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 Chemical Energy from
Natural and Synthetic Gas
 Chemical Energy from
Natural and Synthetic Gas

Yatish T. Shah
CRC Press
Taylor & Francis Group
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© 2017 by Taylor & Francis Group, LLC

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 Dedication

This book is dedicated to my family: Mary, James, Rebecca,

Jonathan, Heather, Keith, Laura, and my eight grandchildren.
Contents
Preface.............................................................................................................................................xxi
Author.............................................................................................................................................xxv

Chapter 1 Introduction...................................................................................................................1
1.1 Introduction........................................................................................................1
1.1.1 Advantages and Disadvantages of Gas as Fuel.....................................5
1.2 Types of Natural Gas and Their Markets and Methods of Production..............6
1.2.1 Conventional versus Unconventional Sources of Natural Gas.............. 7
1.2.2 Unconventional Oil versus Gas........................................................... 10
1.3 Synthesis Gas by Thermal Gasification........................................................... 10
1.3.1 Producer Gas....................................................................................... 11
1.3.2 Syngas or Biosyngas............................................................................ 12
1.4 Biogas, Biomethane, and Biohydrogen Production by Anaerobic
Digestion...................................................................................................12
1.5 Hydrogen Production by Hydrothermal Gasification and Water
Dissociation..............................................................................................14
1.6 Gas Reforming................................................................................................. 15
1.6.1 Steam, Dry, and Tri-Reforming.......................................................... 16
1.6.2 Reforming in Sub- and Supercritical Water........................................ 19
1.6.3 Novel Methods for Reforming............................................................ 19
1.7 Gas Purification and Upgrading.......................................................................20
1.8 Gas Storage and Transportation Infrastructure (Gas Grid).............................. 22
1.9 Gas to Liquid Fuels and Fuel Additives...........................................................25
1.10 Gas for Heat, Electricity, and Mobile Applications.........................................26
1.10.1 Gas Turbines and Microturbines......................................................... 27
1.10.2 Combined Cycles and Cogeneration................................................... 29
1.10.3 Gas Use for Mobile Applications........................................................ 29
References................................................................................................................... 30

Chapter 2 Natural Gas................................................................................................................. 33

2.1 Introduction...................................................................................................... 33
2.1.1 World Gas Reserve.............................................................................. 36
2.1.2 U.S. Natural Gas Resource Estimates................................................. 37
2.2 Methods for Natural Gas Exploration.............................................................. 38
2.2.1 Types of Data Collection..................................................................... 38
2.2.2 Computer-Assisted Exploration and Data Interpretation....................40
2.3 Methods for Drilling and Production of Natural Gas...................................... 41
2.3.1 Vertical Drilling.................................................................................. 42
2.3.2 Horizontal Drilling.............................................................................. 42
2.3.3 Well Completion.................................................................................. 42
2.3.4 Hydraulic Fracturing........................................................................... 43
2.3.4.1 Fracking Hot Spots in the United States.............................46
2.3.4.2 Negative Effects of Hydraulic Fracturing............................46
2.3.5 Production...........................................................................................46
2.3.6 Well Abandonment.............................................................................. 48

vii
viii Contents

2.4 LNG, CNG, and LPG....................................................................................... 48

2.4.1 Liquid Natural Gas.............................................................................. 48
2.4.2 Compressed Natural Gas..................................................................... 50
2.4.3 Liquefied Petroleum Gas..................................................................... 50
2.4.4 Comparison of LPG with Natural Gas................................................ 53
2.5 Coalbed Methane.............................................................................................. 53
2.5.1 CBM Production History.................................................................... 57
2.5.2 Produced Water Characteristics and Management............................. 57
2.5.3 Current Economics of CBM Production............................................. 59
2.5.4 The Future of CBM............................................................................. 59
2.6 Tight Gas..........................................................................................................60
2.6.1 Methods for Tight Gas Recovery........................................................ 62
2.7 Shale Gas.......................................................................................................... 62
2.7.1 Brief History of Shale Gas Development............................................ 63
2.7.2 Shale Gas Resource.............................................................................64
2.7.3 Environmental Impacts of Shale Gas Recovery................................. 65
2.7.4 Water Consumption by Coal Industry versus Shale Gas Industry......66
2.7.5 Economics of Shale Gas......................................................................66
2.8 Deep Gas.......................................................................................................... 67
2.8.1 Historical Perspective and Origin of Deep Gas.................................. 68
2.8.2 General Geologic and Technologic Framework.................................. 70
2.8.3 Economics of Deep Gas Drilling........................................................ 71
2.8.4 The Future of Deep Gas...................................................................... 72
2.9 Gas from Geopressurized Zones...................................................................... 72
2.9.1 Historical Perspectives of Gulf Coast Geopressured Sediments........ 73
2.9.2 Assessment of Recoverable Energy in Gulf Coast and Its Usages...... 74
2.10 Gas Hydrates.................................................................................................... 77
2.10.1 Sources, Sizes, and Importance of Gas Hydrate Deposits.................. 78
2.10.2 Importance of Gas Hydrates on Offshore Oil and Gas
Operations....................................................................................81
2.10.2.1 Drilling................................................................................ 81
2.10.2.2 Production by Enhanced Oil and Gas Recovery
Methods.........................................................................81
2.10.2.3 Natural Gas Hydrates versus Natural Gas in
Transportation...................................................................... 82
2.10.3 Environmental Impacts of Gas Hydrates............................................ 82
2.10.4 Production of Methane from Gas Hydrate Reservoirs........................ 83
2.10.4.1 Thermal Stimulation............................................................84
2.10.4.2 Depressurization..................................................................84
2.10.4.3 Inhibitor Injection................................................................ 85
2.10.4.4 Gas Exchange...................................................................... 85
2.10.4.5 Enhanced Gas Hydrate Recovery Method.......................... 86
2.11 Commercial Application.................................................................................. 87
References................................................................................................................... 88

Chapter 3 Synthesis Gas by Thermal Gasification.................................................................... 113

3.1 Introduction.................................................................................................... 113
3.2 Parameters Affecting Synthesis Gas Production and Its Quality.................. 115
3.2.1 Feedstock........................................................................................... 115
3.2.2 Nature of Gasification Process.......................................................... 118
Contents ix

3.3 Coal and Oil Shale Gasification..................................................................... 119

3.3.1 Synthetic Gas (Producer Gas) Classification Based on Its
Heating Value.................................................................................... 120
3.3.1.1 Low-Btu Gas...................................................................... 120
3.3.1.2 Medium-Btu Gas............................................................... 121
3.3.1.3 High-Btu Gas..................................................................... 121
3.3.2 General Aspects of Coal Gasification............................................... 122
3.3.3 Carbon Dioxide Gasification............................................................. 123
3.3.4 Partial Oxidation............................................................................... 124
3.3.5 Oil Shale Gasification........................................................................ 126
3.4 Gasification of Biomass and Waste................................................................ 127
3.4.1 Types of Biomass.............................................................................. 128
3.4.2 Components of Biomass.................................................................... 128
3.4.3 Composition of Biomass................................................................... 129
3.4.4 Reaction Zones.................................................................................. 131
3.4.4.1 Drying Zone...................................................................... 131
3.4.4.2 Pyrolysis Zone................................................................... 131
3.4.4.3 Reduction Zone.................................................................. 132
3.4.4.4 Combustion Zone............................................................... 132
3.4.5 Properties of Bioproducer Gas.......................................................... 132
3.4.6 Biosyngas.......................................................................................... 133
3.4.7 Gasification of Waste......................................................................... 133
3.5 Cogasification................................................................................................. 134
3.5.1 Advantages........................................................................................ 135
3.5.2 Disadvantages.................................................................................... 136
3.5.3 Typical Examples of Cogasification.................................................. 137
3.5.3.1 Cogasification of Coal and Biomass in Intermittent
Fluidized Bed..................................................................... 137
3.5.3.2 Cogasification of Coal and Biomass in High-Pressure
Fluidized Bed..................................................................... 137
3.5.3.3 Cogasification of Coal and Polyethylene Mixture............. 137
3.5.3.4 High-Pressure Cogasification of Coal with Biomass
and Petroleum Coke........................................................... 138
3.5.3.5 Cogasification of Woody Biomass and Coal with Air
and Steam.......................................................................... 138
3.5.3.6 Cogasification of Coal, Biomass, and Plastic Wastes
with Air/Steam Mixtures in Fluidized Bed....................... 138
3.5.3.7 Coutilization of Biomass and Natural Gas in
Combined Cycles............................................................... 138
3.5.3.8 Steam Gasification of Coal–Biomass Briquettes............... 139
3.5.3.9 Syngas Production by Coconversion of
Methane and Coal in a Fluidized-Bed Reactor................. 139
3.5.3.10 Cogasification of Coal and Biomass in a Dual
Circulating Fluidized-Bed Reactor.................................... 139
3.5.3.11 Cogasification of Coal and Chicken Litter........................ 139
3.5.3.12 Cogasification of Biomass and Waste Filter Carbon......... 139
3.5.3.13 Cogasification of Low-Rank Fuel–Biomass, Coal,
and Sludge Mixture in a Fluidized Bed in the
Presence of Steam.............................................................. 140
3.5.3.14 Cogasification of Residual Biomass/Poor Coal in a
Fluidized Bed..................................................................... 140
x Contents

3.5.3.15 Cogasification of Biomass and Coal for Methanol

Synthesis......................................................................140
3.5.3.16 Underground Cogasification of Coal and Oil Shale.......... 140
3.5.3.17 Cogasification of Petcoke and Coal/Biomass Blend.......... 141
3.5.4 Barriers and Potentials for Future Growth in Cogasification............ 141
3.6 Feed Preparation............................................................................................. 142
3.6.1 Coal Preparation................................................................................ 143
3.6.2 Technological and Environmental Barriers...................................... 144
3.6.3 Pretreatment and Feeding Options for Biomass/Waste.................... 145
3.6.4 Torrefaction....................................................................................... 147
3.6.5 Fast Pyrolysis..................................................................................... 148
3.6.6 Size Reduction................................................................................... 149
3.6.6.1 Wood/Waste Wood............................................................ 150
3.6.6.2 Municipal/Industrial Waste............................................... 150
3.6.6.3 Sewage Sludge................................................................... 151
3.6.6.4 Straw and Miscanthus........................................................ 151
3.6.7 Effects of Feed Treatment for Storage and Transportation
of Biomass......................................................................................... 151
3.6.8 General Issues Regarding Particle Size, Shape, and Density
of Biomass and Feeding Gasifier during Cogasification................... 152
3.6.9 System Design Issues for Cogasification........................................... 153
3.7 Gasification Reactors...................................................................................... 154
3.7.1 Fixed- or Moving-Bed Reactors........................................................ 155
3.7.2 Fluidized-Bed Reactors..................................................................... 158
3.7.3 Entrained-Bed Reactors.................................................................... 159
3.7.4 Comparison of Different Types of Reactors..................................... 161
3.7.4.1 Additional Industrial Perspectives..................................... 161
3.7.5 Best Option of Reactor Technology for Multifuel Coal–Biomass
Gasification........................................................................................ 162
3.7.6 Rotary Kiln Gasifier for Waste......................................................... 163
3.7.6.1 Rotary Kiln Gasification.................................................... 163
3.7.6.2 Callidus Technologies Rotary Kiln Gasifiers.................... 164
3.8 Commercial Gasification Processes............................................................... 164
3.8.1 Historical Town Gas Process............................................................ 164
3.8.2 Typical Commercial Coal Gasification Processes............................ 165
3.8.2.1 Lurgi Gasification.............................................................. 165
3.8.2.2 Koppers–Totzek Gasification............................................. 166
3.8.2.3 Shell Gasification............................................................... 166
3.8.2.4 Texaco Gasification............................................................ 166
3.8.3 Typical Commercial Biomass/Waste Gasification Processes........... 167
3.8.3.1 Twin-Rec............................................................................ 167
3.8.3.2 Schwarze Pumpe............................................................... 167
3.8.3.3 Thermal Converter............................................................ 167
3.8.3.4 Thermoselect Gasifier........................................................ 168
3.8.3.5 TPS Termiska Process....................................................... 168
3.8.4 Typical Commercial Cogasification Processes................................. 169
3.8.4.1 250 MWe IGCC Plant, Nuon Power, Buggenum,
B.V. Willem-Alexander Centrale....................................... 169
3.8.4.2 250 MWe IGCC Plant, Tampa Electric’s Polk Power
Station................................................................................ 169
Contents xi

3.8.4.3 High-Temperature Winkler Gasifier.................................. 170

3.8.4.4 Potential Issues and Options for the Commercial
Process Configurations of Cogasification.......................... 170
3.8.5 Commercial Gasification of Oil Shale.............................................. 172
3.9 Underground Coal Gasification...................................................................... 172
3.9.1 Underground Gasification Reactors.................................................. 175
3.9.2 Methods for Underground Gasification............................................. 175
3.9.2.1 Shaft Methods.................................................................... 177
3.9.2.2 Shaftless Methods.............................................................. 177
3.9.3 Potential Problem Areas with In Situ Gasification........................... 178
3.9.4 Controlled Retracting Injection Point Technique.............................. 179
3.9.5 Criteria for Underground Coal Gasification Site Selection............... 179
3.9.5.1 Thickness, Depth, and Dip of Coal Seam......................... 179
3.9.5.2 Amount of Coal, Coal Rank, and Other Coal
Properties.....................................................................180
3.9.5.3 Groundwater and Land Use Requirements
and Restrictions................................................................. 181
3.10 Molten Media Gasification Processes............................................................ 181
3.10.1 Kellogg–Pullman Molten Salt Process............................................. 181
3.10.2 Atgas Molten Iron Coal Gasification................................................ 182
3.10.3 Rummel–Otto Molten Salt Gasification............................................ 182
3.10.4 Rockwell Molten Salt Gasification Process...................................... 183
3.10.5 Alden Process for Biomass Gasification Using Molten Salts............ 184
3.11 Plasma Gasification........................................................................................ 184
3.11.1 Energy from MSW by Plasma Gasification...................................... 185
3.12 Solar Gasification........................................................................................... 187
3.12.1 Solar Gasification Reactors and Processes........................................ 188
3.13 Catalytic Gasification..................................................................................... 189
3.14 Indirect Gasification....................................................................................... 193
3.14.1 Battelle Indirectly Heated Gasifier.................................................... 196
3.15 Global Gasification Experience...................................................................... 197
References................................................................................................................. 198

Chapter 4 Biogas and Biohydrogen Production by Anaerobic Digestion.................................. 219

4.1 Introduction.................................................................................................... 219
4.2 Mechanism of Anaerobic Digestion for Methane.......................................... 221
4.2.1 Hydrolysis and Liquefaction.............................................................. 221
4.2.2 Acidogenesis...................................................................................... 222
4.2.3 Methanogenesis................................................................................. 223
4.2.4 Microbes and the Effects of Operating Conditions...........................224
4.3 Hydrogen Production by Anaerobic Digestion............................................... 227
4.3.1 Mechanism of Fermentative Hydrogen Production.......................... 228
4.3.2 Environmental Factors Affecting Hydrogen Production.................. 229
4.3.2.1 Inocula and Pretreatment................................................... 229
4.3.2.2 Substrate............................................................................ 230
4.3.2.3 pH...................................................................................... 231
4.3.2.4 Hydraulic Retention Time................................................. 232
4.3.2.5 Temperature....................................................................... 232
xii Contents

4.3.2.6 Effects of Products, Metal Ions, Nitrogen, and

Phosphorous.................................................................232
4.3.2.7 Design of Digester............................................................. 234
4.3.3 Brief Literature Assessment on Biohydrogen Production................. 234
4.4 Codigestion..................................................................................................... 238
4.4.1 Advantages and Disadvantages......................................................... 239
4.4.1.1 Advantages......................................................................... 239
4.4.1.2 Disadvantages....................................................................240
4.4.2 Major Applications, Users, and Related Issues with Codigestion...... 241
4.5 Feedstock Effects on Biogas Production........................................................ 241
4.5.1 Single Substrate................................................................................. 241
4.5.1.1 Coir Pith............................................................................. 241
4.5.1.2 Whey.................................................................................. 243
4.5.1.3 Distillery Spent Wash........................................................244
4.5.1.4 Swine Waste.......................................................................244
4.5.1.5 By-Products of Biodiesel Productions...............................244
4.5.1.6 Palm Oil Mill Effluent....................................................... 245
4.5.1.7 Long-Chain Fatty Acids.................................................... 245
4.5.1.8 Organic Wastes and Energy Crops....................................246
4.5.1.9 Dairy Effluent....................................................................246
4.5.1.10 Tofu Wastewater................................................................ 247
4.5.1.11 Conversion of Lignocellulose to High-Value Products
Employing Microbes......................................................... 247
4.5.2 Multiple Substrates (Codigestion).....................................................248
4.5.2.1 Codigestion with Different Types of Sludge and
Wastewater.........................................................................248
4.5.2.2 Codigestion with Different Types of Manure.................... 256
4.5.2.3 Other Co-Substrates.......................................................... 262
4.6 Effects of Harvesting, Storage, and Pretreatment on Biogas Production.......264
4.7 Digester and Associated Process Configurations for Biogas Production....... 265
4.7.1 Novel Digester Technology...............................................................266
4.8 Process-Related and Economic Considerations for Biogas Production......... 268
4.8.1 Process Monitoring and Control....................................................... 268
4.8.2 Scale-Up............................................................................................ 268
4.8.3 Computer Simulation and Model...................................................... 269
4.8.4 Process Optimization........................................................................ 270
4.8.5 Additional Needs for Codigestion and Process Economics.............. 270
4.9 Purification and Utilization of Biogas and Digestate..................................... 271
4.10 Typical Large-Scale Plants for Biogas Production......................................... 272
References................................................................................................................. 275

Chapter 5 Hydrothermal Gasification........................................................................................ 297

5.1 Introduction.................................................................................................... 297
5.2 Hydrogen Market and Methods for Hydrogen Production............................. 297
5.3 Steam and Hydrogasification of Carbonaceous Materials............................. 299
5.3.1 Mechanism of Steam Gasification.................................................... 299
5.3.2 Feedstock Effect on Steam Gasification...........................................300
5.3.2.1 Coal....................................................................................300
5.3.2.2 Biomass..............................................................................302
Contents xiii

5.3.2.3 Mixed Feedstock...............................................................306

5.3.2.4 Tar......................................................................................308
5.3.2.5 Black Liquor......................................................................308
5.3.2.6 Lignin................................................................................309
5.3.3 Catalysts for Steam Gasification.......................................................309
5.3.3.1 Dolomite, Olivine, and Alkali Metal–Based Catalysts.....309
5.3.3.2 Nickel-Based Catalysts...................................................... 310
5.3.4 Hydrogasification with and without Steam....................................... 310
5.4 Hydrothermal Gasification under Subcritical Conditions.............................. 314
5.4.1 Catalysts for Hydrothermal Gasification........................................... 315
5.5 Hydrothermal Gasification in Supercritical Water......................................... 317
5.6 Water Dissociation Technologies................................................................... 321
5.7 Electrolysis and Its Derivative Technologies.................................................. 323
5.7.1 Alkaline Electrolysis......................................................................... 324
5.7.2 High-Temperature Electrolysis (Process).......................................... 324
5.7.3 High-Pressure Electrolysis (Process)................................................ 325
5.7.4 Photoelectrolysis................................................................................ 325
5.7.5 Photoaided Electrolysis..................................................................... 326
5.7.6 Photovoltaic Electrolysis................................................................... 326
5.7.7 Solar Electrolysis............................................................................... 326
5.8 Photochemical and Its Derivative Technologies............................................. 327
5.8.1 Water Splitting on Semiconductor Catalysts (Photocatalysis).......... 327
5.8.1.1 Titanium Oxide Photocatalysts.......................................... 327
5.8.1.2 Tantalates and Niobates..................................................... 328
5.8.1.3 Transition Metal Oxides.................................................... 328
5.8.1.4 Metal Nitrides and Oxynitrides......................................... 328
5.8.1.5 Metal Sulfides.................................................................... 328
5.8.2 Photobiological Production of Hydrogen from Water....................... 329
5.8.3 Plasma-Induced Photolysis................................................................ 329
5.9 Thermal and Thermochemical Decomposition of Water............................... 330
5.9.1 Thermochemical Decomposition of Water....................................... 331
5.9.1.1 UT-3 Cycle......................................................................... 332
5.9.1.2 Zn–ZnO Cycle................................................................... 332
5.9.1.3 SnO/SnO2 Cycle................................................................. 334
5.9.1.4 Mixed Iron Oxide Cycle.................................................... 334
5.9.1.5 Carbothermal Reduction of Metal Oxides........................ 335
5.9.1.6 Sulfur Family Thermochemical Water-Splitting Cycles......335
5.9.1.7 Sulfur–Iodine Cycle........................................................... 338
5.9.1.8 Westinghouse Process....................................................... 338
5.9.1.9 Copper–Chlorine Cycle..................................................... 339
5.9.1.10 Copper–Sulfate Cycle........................................................ 339
5.10 Other Novel Technologies for Water Dissociation......................................... 341
5.10.1 Chemical Methods............................................................................ 341
5.10.2 Magmalysis....................................................................................... 342
5.10.3 Radiolysis.......................................................................................... 342
5.10.4 Shock Waves and Mechanical Pulses............................................... 343
5.10.5 Catalytic Decomposition of Water.................................................... 343
5.10.6 Plasmolysis........................................................................................ 343
5.10.7 Magnetolysis......................................................................................344
References.................................................................................................................344
xiv Contents

Chapter 6 Gas Reforming.......................................................................................................... 357

6.1 Introduction.................................................................................................... 357
6.2 Types of Gas Reforming................................................................................. 357
6.3 WGS Reaction................................................................................................360
6.3.1 Mechanism........................................................................................360
6.3.1.1 Associative Mechanism..................................................... 361
6.3.1.2 Redox Mechanism............................................................. 361
6.3.2 Role of WGS in Syngas Production.................................................. 362
6.3.3 Reverse Water Gas Shift................................................................... 363
6.3.4 Location of WGS Reactor in Gasification Process........................... 363
6.3.5 High-Temperature Shift Catalysts..................................................... 365
6.3.6 Low-Temperature Shift Catalysts...................................................... 365
6.3.7 Role of WGS in Fuel Cells................................................................ 366
6.4 Steam Reforming............................................................................................ 367
6.4.1 Catalysts for Steam Reforming......................................................... 369
6.4.2 Feedstock Effects.............................................................................. 369
6.4.2.1 Ethanol............................................................................... 369
6.4.2.2 Methanol............................................................................ 371
6.4.2.3 Liquid Hydrocarbons......................................................... 373
6.4.2.4 Glycerol.............................................................................. 374
6.4.2.5 Biomass.............................................................................. 375
6.4.2.6 Mixed Feedstock............................................................... 376
6.4.2.7 Bio-Oil............................................................................... 376
6.5 Dry Reforming............................................................................................... 377
6.5.1 Thermodynamics of Dry Reforming................................................ 379
6.5.2 Mechanisms and Kinetics................................................................. 380
6.5.3 Catalysts for Dry Reforming............................................................. 382
6.5.3.1 Perspectives on Noble Metals, Composites, Oxides,
and Carbide Catalysts........................................................ 382
6.5.3.2 Catalyst Deactivation......................................................... 384
6.5.4 Important Conclusions on Catalysis of Dry Reforming of
Methane................................................................................. 385
6.5.5 Dry Reforming of Higher Hydrocarbons.......................................... 386
6.6 Partial Oxidation/Autothermal/Tri-Reforming.............................................. 386
6.6.1 Partial Oxidation/Autothermal Operation......................................... 386
6.6.2 Tri-Reforming................................................................................... 387
6.6.2.1 Application of Tri-Reforming to Flue Gas from
Combustion Plants............................................................. 388
6.7 Subcritical and Supercritical Reforming........................................................ 389
6.7.1 Aqueous-Phase Reforming................................................................ 390
6.7.1.1 Thermodynamics............................................................... 391
6.7.1.2 Kinetics and Catalysis of APR Process............................. 393
6.7.2 Supercritical Water Reforming......................................................... 398
6.7.2.1 Feedstock Effect on Supercritical Water Reforming......... 399
6.8 Plasma Reforming..........................................................................................404
6.8.1 Dry Reforming of Methane by Cold Plasma.....................................405
6.8.2 Dry Reforming of Methane by Thermal Plasma..............................405
6.9 Novel Reforming Processes............................................................................408
6.9.1 Microwave-Assisted Reforming........................................................408
6.9.2 Solar Reforming................................................................................ 410
Contents xv

6.9.3 Nuclear Heat–Aided Reforming........................................................ 410

6.9.4 Other Novel Reforming Processes.................................................... 410
6.10 Novel Reforming Reactors............................................................................. 411
6.10.1 Steam Reforming Reactors............................................................... 411
6.10.2 Annular Bed Reformer...................................................................... 412
6.10.3 Plate-Type Reformers........................................................................ 412
6.10.4 Membrane Reformers........................................................................ 412
6.10.5 Autothermal Reformers..................................................................... 413
6.10.6 Ion Transport Membrane Reformers................................................. 413
6.10.7 Sorbent-Enhanced Reformers........................................................... 413
6.10.8 Plasma Reformers.............................................................................. 413
6.10.9 Micro-Channel Reformers................................................................ 414
6.10.10 Microwave-Assisted Reformer.......................................................... 414
6.10.11 Solar Steam Reforming Reactors...................................................... 415
References................................................................................................................. 418

Chapter 7 Gas Processing, Purification, and Upgrading........................................................... 435

7.1 Introduction.................................................................................................... 435
7.2 Natural Gas Processing.................................................................................. 435
7.2.1 Processing Details............................................................................. 437
7.2.2 Process Steps for the Production of Pipeline-Quality Natural
Gas and NGLs................................................................................... 438
7.2.2.1 Oil and Condensate Removal............................................ 438
7.2.2.2 Water Removal.................................................................. 439
7.2.2.3 Sulfur and Carbon Dioxide Removal................................440
7.2.2.4 Nitrogen Extraction........................................................... 443
7.2.2.5 Helium (He) Extraction..................................................... 443
7.2.2.6 Separation of NGLs...........................................................444
7.2.2.7 NGL Fractionation............................................................. 445
7.3 Factors Affecting the Level of Impurities in Syngas..................................... 445
7.3.1 Effects of Cogasification of Coal and Biomass/Waste
on Tar Release........................................................................... 446
7.3.2 Roles of Mineral Matters and Slagging in Cogasification................ 447
7.3.3 Product Cleaning and Separation Mechanisms................................448
7.3.3.1 Behavior of Nitrogen, Chlorine, and Sulfur......................448
7.3.3.2 Bottom and Fly Ash Characteristics and Role
of Alkalis................................................................... 449
7.3.3.3 Ash and Slag Utilizations.................................................. 451
7.3.3.4 Assessment of Synergy during Pyrolysis.......................... 451
7.4 Technologies for Particulate Removal............................................................ 453
7.4.1 Cyclones............................................................................................ 454
7.4.2 Filtration............................................................................................ 454
7.4.2.1 Ceramic Filters.................................................................. 454
7.4.2.2 Metal Candle Filters.......................................................... 455
7.4.2.3 Low-Temperature Baghouse Filters................................... 455
7.4.3 Electrostatic Precipitators................................................................. 456
7.4.4 Wet Scrubbers................................................................................... 457
7.4.5 Technologies Used in Typical Industrial Processes.......................... 459
7.5 Technologies for Tar Removal........................................................................ 459
7.5.1 Physical..............................................................................................460
xvi Contents

7.5.1.1 Oil Loop Tar Removal.......................................................460

7.5.1.2 Water Loop Tar Removal...................................................460
7.5.1.3 Venturi Wet Scrubbers.......................................................460
7.5.2 Chemical/Catalytic Treatments......................................................... 461
7.5.2.1 Thermal Cracking.............................................................. 461
7.5.2.2 Hydrogenation.................................................................... 461
7.5.2.3 Plasma Conversion............................................................. 461
7.5.2.4 Catalytic Steam Reforming............................................... 462
7.6 Technologies for Sulfur Removal................................................................... 463
7.6.1 Low-Temperature Processes.............................................................. 463
7.6.1.1 SULFURTRAP Process by Chemical Products
(Oklahoma City, Oklahoma)..............................................464
7.6.1.2 Low-Temperature Amine Process (Bionomic
Industries, Mahwah, New Jersey)......................................464
7.6.1.3 MV Technologies H2SPlus System...................................465
7.6.1.4 Merichem LO-CAT™ Process for Sulfur Removal..........466
7.6.2 Brief Industrial Assessment of Sulfur Removal Technologies.........469
7.6.3 COS Hydrolysis.................................................................................469
7.6.4 Sulfur Recovery Unit........................................................................469
7.7 Technologies for Nitrogen and CO2 Removal................................................ 470
7.7.1 CO2 Removal in Integrated Gasification Combined-Cycle Plants.... 470
7.8 Technologies for Removal of Chlorides, Alkalis, and Heavy Metals............ 471
7.9 Some Perspectives on Low-Temperature and Low-Pressure
Syngas-Cleaning Process............................................................................... 472
7.10 RTI High-Temperature Impurity Removal Processes.................................... 473
7.10.1 RTI’s Scale-Up Experience for High-Temperature Removal............ 475
References................................................................................................................. 476

Chapter 8 Gas Storage and Transport Infrastructure................................................................. 487

8.1 Introduction.................................................................................................... 487
8.2 Natural Gas Storage....................................................................................... 489
8.2.1 Types of Underground Storage.......................................................... 490
8.2.1.1 Depleted Gas Reservoirs................................................... 491
8.2.1.2 Aquifers............................................................................. 492
8.2.1.3 Salt Caverns....................................................................... 493
8.3 Natural Gas Transport.................................................................................... 494
8.3.1 Pipeline Control and Safety.............................................................. 496
8.3.2 Natural Gas Distribution................................................................... 497
8.4 Storage and Transport of CNG and Gas Hydrates......................................... 498
8.4.1 Gas Hydrates..................................................................................... 498
8.4.2 Compressed Natural Gas................................................................... 499
8.5 Methods for Storage and Transport of LNG and LPG...................................500
8.5.1 LNG Storage and Transport..............................................................500
8.5.2 LPG Storage and Transport...............................................................504
8.6 Storage and Transport of Syngas.................................................................... 505
8.6.1 Methanation.......................................................................................506
8.6.2 Syngas and SNG Storage...................................................................506
8.6.2.1 Options for Large-Scale Storage.......................................506
8.6.2.2 Aboveground Syngas Storage Methods.............................507
Contents xvii

8.6.2.3 Underground Syngas Storage Methods.............................508

8.6.2.4 Major Storage and Transportation Issues with Syngas......509
8.7 Storage and Transportation of Biogas and Biomethane................................. 510
8.7.1 Biogas Storage................................................................................... 511
8.7.2 Biomethane Storage.......................................................................... 512
8.7.3 Biomethane Transport....................................................................... 513
8.8 Methods of Hydrogen Storage........................................................................ 513
8.8.1 Physical Storage................................................................................ 515
8.8.1.1 Storage Vessels and Their Transport................................. 515
8.8.1.2 Liquid Hydrogen................................................................ 516
8.8.1.3 Physical Hydrogen Storage in Mobile Applications.......... 516
8.8.2 Other Physical Methods.................................................................... 518
8.8.2.1 Carbon Nanotubes and Adsorption................................... 518
8.8.2.2 Clathrate Hydrates............................................................. 518
8.8.2.3 Glass Capillary Arrays and Microspheres......................... 518
8.8.3 Chemical Storage for Static and Mobile Applications...................... 519
8.8.3.1 Metal Hydrides.................................................................. 519
8.8.3.2 Nonmetal Hydrides............................................................ 519
8.8.3.3 Metal-Organic Frameworks............................................... 520
8.8.4 Future Challenges.............................................................................. 521
8.9 Hydrogen Transport........................................................................................ 521
8.9.1 Pipeline Transport of Gaseous Hydrogen (CGH2)............................ 521
8.9.2 Tube Trailer Transport of Gaseous Hydrogen (CGH2)...................... 522
8.9.3 Road Tanker and Ship Transports of Liquid Hydrogen.................... 523
8.10 Natural Gas and Hydrogen Grids................................................................... 523
8.10.1 Grid Integrations............................................................................... 525
8.10.2 Levels of Grid Applications.............................................................. 527
8.10.3 Role of Gas Storage........................................................................... 527
References................................................................................................................. 528

Chapter 9 Natural and Synthetic Gas for Productions of Liquid Fuels and Their Additives.... 543
9.1 Introduction.................................................................................................... 543
9.1.1 Paths for GTL Conversions...............................................................544
9.2 Conversion of Syngas to Methanol................................................................. 545
9.2.1 Chemistry.......................................................................................... 545
9.2.2 Catalysts............................................................................................ 547
9.2.3 Syngas Requirements........................................................................ 548
9.2.4 Commercial Reactors and Processes................................................ 548
9.3 Conversion of Methanol to Dimethyl Ether, Gasoline, and Olefins............... 549
9.3.1 Mobil MTG Process.......................................................................... 551
9.3.1.1 Chemistry of Reactions..................................................... 552
9.3.1.2 Process Description........................................................... 553
9.3.1.3 Advantages and Disadvantages of MTG Process.............. 554
9.3.2 Methanol to Olefins Process.............................................................. 555
9.3.2.1 Catalyst, Reactor, and Process........................................... 556
9.3.2.2 UOP/Hydro MTO Process................................................. 557
9.3.2.3 DMTO Process.................................................................. 558
9.4 FT Synthesis................................................................................................... 558
9.4.1 Product Distribution.......................................................................... 560
9.4.2 Catalysts............................................................................................ 561
xviii Contents

9.4.3 FT Reactor Options...........................................................................564

9.4.3.1 Multitubular Fixed-Bed Reactor........................................564
9.4.3.2 Entrained-Flow Reactor.....................................................564
9.4.3.3 Fluidized-Bed and Circulating Catalyst Reactors.............564
9.4.3.4 Slurry Reactors.................................................................. 565
9.4.4 Product Separations and Upgrading.................................................. 565
9.4.5 FT Commercialization...................................................................... 565
9.4.5.1 Sasol................................................................................... 566
9.4.5.2 PetroSA.............................................................................. 566
9.4.5.3 Shell Middle Distillate Synthesis...................................... 566
9.4.5.4 Ras Laffan, Qatar.............................................................. 566
9.4.5.5 UPM (Finland).................................................................. 566
9.4.5.6 Others................................................................................ 567
9.4.5.7 An Integrated Process for Biomass to Biodiesel Oil
Production via FT Synthesis (BTL)................................... 567
9.4.5.8 Conventional GTL versus Smaller Scale GTL.................. 569
9.5 Mixed Alcohol Synthesis............................................................................... 570
9.5.1 Chemical Reactions and Product Distributions................................ 570
9.5.2 Catalyst Performance Comparisons.................................................. 573
9.5.3 Process............................................................................................... 574
9.5.4 Alcohol Separation............................................................................ 575
9.5.5 Process Commercialization............................................................... 576
9.6 Isosynthesis..................................................................................................... 576
9.6.1 Catalysts............................................................................................ 577
9.7 Oxosynthesis................................................................................................... 578
9.7.1 Chemistry.......................................................................................... 579
9.7.2 Catalysts and Associated Commercial Processes............................. 580
9.7.2.1 Cobalt Carbonyl Catalyst................................................... 581
9.7.2.2 Phosphine-Modified Cobalt............................................... 581
9.7.2.3 Phosphine-Modified Rhodium.......................................... 582
9.8 Syngas Fermentation...................................................................................... 583
9.8.1 Biochemistry of Gas Fermentation................................................... 584
9.8.2 Acetogens.......................................................................................... 585
9.8.3 Parameters for Fermentation Process Optimization......................... 586
9.8.4 Commercialization............................................................................ 587
9.9 Role of Hydrogen in Refinery Operations...................................................... 589
9.9.1 Hydrogenation................................................................................... 589
9.9.2 Hydrocracking................................................................................... 590
9.9.3 Hydrodesulfurization........................................................................ 590
9.9.4 Hydrodemetallization........................................................................ 592
9.9.5 Hydrodenitrogenation (HDN) and Hydrodeoxygenation (HDO)...... 592
9.10 Comparison of Liquid Fuel Production with Other Methods........................ 593
References................................................................................................................. 594

Chapter 10 Gas for Heat, Electricity, and Mobile Applications.................................................. 613

10.1 Introduction.................................................................................................... 613
10.1.1 Versatility of Natural and Synthetic Gas.......................................... 613
10.1.1.1 Power Generation............................................................... 613
10.1.1.2 Domestic, Industrial, and Agricultural Uses..................... 614
Contents xix

10.1.1.3  Transportation................................................................... 614
10.1.1.4   Other Factors Affecting or Enhancing Gas Utility........... 615
10.1.2 Important Concepts and Tools to Expand Usefulness of Gas
in Energy and Fuel Industry.............................................................. 617
10.2 The Centralized Power System...................................................................... 618
10.3 The Distributed Power System....................................................................... 619
10.3.1 Future of Distributed Generation...................................................... 621
10.3.1.1   Technical Constraints....................................................... 621
10.3.1.2  Cost Competitiveness....................................................... 622
10.3.1.3  Regulatory Barriers.......................................................... 622
10.3.1.4   Impact on Climate Change and Global Warming............. 622
10.4 Smart Electrical Grid for Centralized and Distributed Power
Management............................................................................................... 622
10.4.1 Smart Electrical Grid........................................................................ 623
10.4.2 Benefits and Requirements of Smart Electrical Grid........................ 624
10.4.3 Smart Grid Technology Assessment, Development,
Standardization, and Optimization................................................... 624
10.5 Gas Turbine.................................................................................................... 626
10.5.1 Theory of Operation.......................................................................... 626
10.5.2 Advantages and Disadvantages of Gas Turbine Engines.................. 627
10.5.3 Gas Turbines in Surface Vehicles..................................................... 627
10.5.4 Marine Applications.......................................................................... 628
10.5.5 Recent Advances in Technology....................................................... 628
10.6 Micro-Turbines............................................................................................... 628
10.6.1 Micro-Turbines versus Reciprocating Engines................................. 629
10.6.2 Micro-Turbines in Transportation Industry....................................... 630
10.6.3 State-of-the-Art Micro-Turbines....................................................... 630
10.6.4 Methods to Improve Gas Micro-Turbine Performance..................... 630
10.7 Combined Cycle and IGCC Technology for Power Generation..................... 632
10.7.1 Combined Cycle Power Plants.......................................................... 632
10.7.1.1   Single-Shaft versus Multi-Shaft Options......................... 635
10.7.2 Integrated Combined Cycles............................................................. 635
10.8 Combined Heat and Power Generation–Cogeneration
and Trigeneration.................................................................................. 638
10.8.1 Micro-CHP........................................................................................ 642
10.9 NGV (CNG and LNG) and LPG Vehicles...................................................... 643
10.9.1 NGV (CNG and LNG) Vehicles........................................................ 643
10.9.1.1   Advantages of CNG.......................................................... 645
10.9.1.2   Disadvantages of CNG.....................................................646
10.9.1.3  LNG-Fueled Vehicles.......................................................646
10.9.2 LPG Vehicles..................................................................................... 647
10.9.3 LPG versus NGV Vehicles................................................................ 650
10.10 Fuel Cell......................................................................................................... 650
10.10.1 Types of Fuel Cells............................................................................ 651
10.10.1.1 Proton Exchange Membrane Fuel Cells........................... 652
10.10.1.2 Phosphoric Acid Fuel Cell................................................ 652
10.10.1.3 High-Temperature Fuel Cells (SOFC)............................. 652
10.10.1.4 Hydrogen-Oxygen Fuel Cell (Bacon Cell)....................... 653
10.10.1.5 MCFC............................................................................... 653
10.10.2 Theoretical versus Practical Energy Efficiency................................ 655
xx Contents

10.10.3 Applications....................................................................................... 655

10.10.3.1 Power................................................................................ 655
10.10.3.2 Fuel Cell Vehicles............................................................. 656
10.10.4 Markets and Economics.................................................................... 657
References................................................................................................................. 658

Index............................................................................................................................................... 675
Preface
As the world is engaged in realigning the energy and fuel portfolio, which is currently fossil fuel
dominated, to one that is more balanced between fossil, nuclear, and renewable energies, one source
of fuel that is considered as playing the role of not only a “bridge or transition fuel” but also an
“ultimate or end fuel” is gas. While for several decades coal and oil have been the dominant forces
for heating, electrical power generation, and fuel for transportation industry, recent concerns about
global warming and carbon emissions from these sources have led to more push toward the use of
renewable energy sources such as biomass, waste, solar, wind, geothermal, and water, as well as
more recognition of carbon-free nuclear energy. Unfortunately, the commercial development of
energy and fuel from renewables will take time to economically compete with existing fossil energy
resources and their infrastructure.
The development of renewable and nuclear energy at the large scale faces many challenges.
Biomass has low mass and energy density compared to coal and oil. They are difficult to transport
long distances and they are not as easy to store as coal and oil. The same is true for waste. In gen-
eral, municipal solid waste is also highly heterogeneous and it can only be used from local sources.
For these reasons, the development of stand-alone, large-scale, and sustainable power or fuel plants
from these sources is highly problematic. Small-scale plants cannot compete with the economy of
scale of fossil fuel plants. Furthermore, the infrastructure for their storage and transport is not well
developed. Their penetration in the energy and fuel industry may require a different strategy than
one used for fossil fuels. This different strategy is addressed in my previous book Energy and Fuel
Systems Integration, CRC Press, New York (2015). Similarly, both solar and wind energy are time
and location dependent and cannot provide large-scale sustainable power without backup power
supply by fossil or nuclear energy or backup energy storage. Their large-scale implementation will
also require hybrid energy system strategy. The possible hybrid structures for this purpose are also
discussed in my previous book. Solar and wind energy are not highly energy efficient and their
infrastructures also need to be further developed. The large-scale commercial experience for power
generation from these sources of energy is in its early stages of development.
While enhanced geothermal system has an enormous potential for its role in energy and fuel
industry, the needed infrastructure and commercial experience for it to become a reality is also still
at the development stage. Finally, as shown in my book Water for Energy and Fuel Production,
CRC Press, New York (2014), water also has an enormous potential for providing unlimited supply
of energy and fuel; however, both infrastructure and commercial experience to tap this still needs
to be developed. Nuclear energy, in some parts of the world, still suffers from social and political
acceptance and, as shown in my previous book Energy and Fuel Systems Integration, CRC Press,
New York (2015), it will require a different strategy (more toward helping renewable energy pen-
etration and its use for nonelectrical applications) to gain more public acceptance.
While the world must pursue, more aggressively, obtaining energy and fuels from renewable
sources, the resolutions of the issues outlined in the previous paragraph will take time. While renew-
able sources of energy and fuel have distinct advantages over fossil fuels, their commercial produc-
tion must economically compete with fossil fuels. In the meantime, one fuel that has the potential
to be a true “transition or bridge fuel” or even the “ultimate or end fuel” is gas. This book illustrates
this point by examining all the roles of natural and synthetic gas in the energy and fuel industry.
Gaseous compounds containing carbon and/or hydrogen are what make gas a source of energy
and fuel. These compounds, such as methane, ethane, propane, butane (and other volatile hydrocar-
bons), syngas (mixture of hydrogen and carbon monoxide), and hydrogen have high heating values
and can be used to generate energy and other types of fuels. These fuels can be basically obtained
from two sources: natural and man-made. Gas from a natural source (obtained from underground)
recovered by conventional or unconventional method is called natural gas. This gas predominantly

xxi
xxii Preface

contains methane as a source of energy and fuel. Man-made gas is called “synthetic gas” and it can
be obtained by three different methods, as detailed later. The composition of synthetic gas varies
depending on the process used to produce it. While natural gas only comes from nonrenewable
sources, synthetic gas can come from both nonrenewable and renewable sources.
Just like coal and oil, natural gas is a fossil fuel obtained from underground, from the bottom
of the ocean or from an arctic environment. In the past, natural gas was recovered from relatively
shallow and easy-to-access natural gas reservoirs by conventional drilling techniques. Just like con-
ventional oil well, this source of natural gas is rapidly depleting. Natural gas often contains oil, and
this type of gas is called associated gas. Natural gas can also be obtained from stand-alone pure gas
reservoirs, called nonassociated gas.
Recent developments in and success of the process of hydraulic fracturing and horizontal (or direc-
tional) drilling have allowed successful access to gas trapped in deeper (even more than 15,000 ft) and
tighter and more compressed matrices underground. These techniques have allowed us to access
unconventional gas such as deep gas, tight gas, gas from geo-pressurized zones, shale gas, and gas
from coal bed methane. In the United States, the biggest revolution occurred in the production of
shale gas. Along with these unconventional gas sources, gas hydrates (mixture of water and meth-
ane) are obtained from the ocean floor and in arctic conditions. All these combined unconventional
gas resources have vast potential, and our improved ability to tap them has led us into the “gas age.”
With recent successes, the United States is now the world’s leading producer of natural gas. This
expanding supply has allowed us to replace coal by natural gas in power plants and diesel oil in
large vehicles by Liquid Natural Gas (LNG), Liquid Petroleum Gas or Liquid Propane Gas (LPG),
and Compressed Natural Gas (CNG). This “shale gas” revolution has allowed us to replace more
harmful coal and oil by gas, which has made it a “transition or bridge fuel.” Thus, we are slowly
transitioning from a coal and oil–based economy to a natural gas–based economy.
Natural gas or methane is cleaner than coal and oil. It contains significantly larger hydrogen
to carbon ratio (4) compared to the ones for coal (less than 1) and refined oil (around 1.2–1.6).
It does not contain other harmful chemicals that cannot be handled upfront and are prevented
from emission into the environment. Unlike coal, natural gas can be used for both large- and
small-scale (like micro turbines and engines) power applications in a convenient manner. While
natural gas has low mass and energy density compared to oil, LNG, LPG, and CNG have been
found to be good substitutes for diesel oil in large vehicles and their use is both economically and
environmentally competitive and gaining ground. A gallon of CNG has about 25% of the energy
content of a gallon of diesel fuel and LNG has 60% of the volumetric energy density of diesel fuel.
LPG has a typical specific calorific value of 46.1 MJ/kg compared with 42.5 MJ/kg for fuel oil
and 43.5 MJ/kg for premium-grade gasoline. However, its energy density per volume (26 MJ/L)
is lower than either that of gasoline or fuel oil. Its density (about 0.5–0.58 kg/L) is lower than
that of gasoline (about 0.71–0.77 kg/L). All old coal-based power plants in the United States are
gradually being replaced by those operated by natural gas. Natural gas usage in power plants is
expected to double by 2040 and surpass that of coal. Similarly, the use of natural gas is expected
to surpass that of oil by 2025.
Synthetic gas can be produced by three distinct methods: (a) thermal gasification of all carbona-
ceous materials or refining of oil to produce hydrocarbons such as propane, butane, etc.; (2s) anaero-
bic digestion of cellulosic waste; and (3) hydrothermal processes involving either gasification in the
presence of steam, sub- and supercritical water, and/or hydrogen for all carbonaceous materials
or water dissociation to produce hydrogen. These three methods produce synthetic gas of different
compositions.
Unlike coal- and petroleum-based oil, gas can be produced synthetically by gasification and
reforming of both nonrenewable and renewable carbonaceous materials. The feedstock for the
production of synthetic gas can be coal, oil, biomass, waste, or a mixture of these. The thermal
gasification of coal is a commercially proven technology. The refining of oil to produce hydro-
carbons such as propane, butane, etc., is also a commercial technology. The gasification of other
Preface xxiii

feedstock (like biomass, waste, etc.) is also being aggressively developed at both small and large
scales. Cogasification of coal/biomass/waste mixtures is gaining momentum due to its impact on
carbon emission into the environment.
Unlike natural gas, synthetic gas contains many fuel components, such as all volatile hydro-
carbons, hydrogen, carbon monoxide, and other gaseous impurities depending on the nature of
feedstock and gasification conditions. Synthetic gas produced in this manner has been given many
names, such as “producer gas,” “town gas,” “wood gas,” “syngas,” “water gas,” etc., depending on
its composition. Producer gas can also be described as high-, medium-, or low-Btu gas depending
on its methane and nitrogen concentrations. Thus, synthetic gas can replace natural gas for heating
and power production. The most useful form of synthetic gas for liquid fuel production is “syngas,”
which is a mixture of hydrogen and carbon monoxide that can be converted to a variety of liquid
fuels and chemicals by the well-recognized Fischer–Tropsch synthesis, iso-synthesis, oxo-synthesis,
and methanol and mixed alcohol production processes. Often, gas produced by the gasification
technology is called by the generic name “synthesis gas,” which is synonymous to “syngas.” Unlike
natural gas, the sources for synthesis gas are unlimited.
Both methane and hydrogen can also be produced by the biological process of “anaerobic diges-
tion,” which can be carried out in the absence of oxygen and with the help of suitable microor-
ganisms. The gas produced by this method is called “biogas” or “bio-hydrogen.” With the use
of methanogenic bacteria, the “biogas” produced mainly contains methane and carbon dioxide.
Landfill gas is a type of “biogas” largely containing methane and carbon dioxide. Anaerobic diges-
tion processes can also produce bio-hydrogen with the help of appropriate microorganisms. In the
presence of methanogenic bacteria, the produced “biogas” has a methane concentration of about
55% (the remainder being mostly carbon dioxide) as opposed to conventional natural gas that has
a methane concentration of about 95%. The methane concentration in “biogas” is, however, very
similar to that in “shale gas.” Biogas can be refined to produce “bio-syngas,” which is very similar
to syngas produced from thermal gasification technologies.
The third type of synthetic gas is hydrogen or gas concentrated with hydrogen produced by two
separate methods. Gas containing a high concentration of hydrogen can be produced by gasifica-
tion in the presence of steam and sub- and supercritical water with or without hydrogenation of all
carbonaceous materials. These processes are generally considered as “hydrothermal gasification.”
The second method involves the dissociation of water by electrolysis and photocatalytic, photobio-
logical, thermal, thermochemical, and other novel methods. These methods generally produce pure
hydrogen. Many consider hydrogen to be the “ultimate fuel” because it contains no carbon. The
world will be much safer and cleaner if all the energy is provided from carbon-free sources. Thus,
technological developments and commercialization of all types of “synthetic gas production,” and
in particular hydrogen production, will make large-scale synthetic gas production the end game (not
just a transition game like natural gas) for energy and fuel industry.
Natural and synthetic gas can be converted to syngas with the desired composition of hydrogen
and carbon monoxide by the process of “gas reforming” so that the mixture can be used to produce
liquid fuels, fuel additives, and chemicals via Fischer–Tropsch synthesis, iso-synthesis, oxo-synthesis,
and others. Gas reforming is one of the most important technologies for natural and synthetic gas and
its further development can transform the role of gas from a “bridge fuel” to more of an “end fuel”
through the production of syngas and hydrogen from methane and other carbonaceous materials. One
type of gas reforming, namely, dry reforming, which involves the use of carbon dioxide to convert
synthetic gas or carbonaceous materials to syngas, can also be an answer to reduce carbon dioxide
emission. The book critically evaluates the effectiveness of various available technologies for gas
reforming. Further developments in various types of reforming processes will further accentuate the
role of “synthetic gas” as the “ultimate fuel.”
Unlike coal and oil, natural gas, and various types of synthetic gas, can be easily cleaned up and
upgraded to the desired level so that using them for power, heat, and liquid fuel applications does not
result in harmful emissions into the environment. Both natural and synthetic gases also need to be
xxiv Preface

cleaned to prepare them for storage and the transport. The book evaluates all the available technolo-
gies to clean and upgrade gas coming from different sources.
One of the reasons natural gas is becoming so important in the energy and fuel industry is that
its storage and transportation infrastructure is well established and it is constantly expanding. The
concept of gas grid, analogous to smart electrical grid, is being developed and this will make gas,
heat, and electricity the dominant future forces of the energy and fuel industry. Natural gas storage
technologies in all its forms (natural gas, LNG, LPG, CNG) are well established on a regional basis
and progress is constant. While the natural gas infrastructure can be used for hydrogen in small
quantities (5 to 15 vol%), the storage and transportation infrastructure for hydrogen is still at the
research stage. Once that is developed, gas will truly become the “ultimate fuel.” The book evalu-
ates storage and transportation options for natural gas, syngas, and hydrogen.
The book also evaluates various end usages of natural gas, syngas, and hydrogen. Various gas-
to-liquid fuel technologies and the role of hydrogen in refinery industries are assessed. Hydrogen is
the most valuable commodity in the fuel industry. The book evaluates the role of methane, syngas,
and hydrogen in large- and small-scale power production. Over next twenty years, gas will be the
most dominant fuel in the power industry, surpassing coal and oil by a large margin. ExxonMobil
predicts that by 2040, gas will generate 30% of the total electricity as opposed to its current value
of 20%. The use of gas in small-scale power generation is rapidly rising. The use of gas for various
heating purposes will also rapidly expand. Another area where the use of gas is rapidly expanding
is the vehicle industry where LNG, LPG, and CNG are replacing gasoline and diesel fuels, and the
use of fuel cell is on rise. The use of hydrogen for both stationary and mobile fuel cells is gaining
momentum. The book evaluates all of these applications of gas in a critical manner.
In summary, this book differs from numerous other books on natural gas, synthesis gas, and
hydrogen published previously in that it presents the unified and collective role of gas in the energy
and fuel industry. It addresses both the “transition” as well as the “end game” role of gas. Most
people believe hydrogen and electricity will be the pivotal sources of energy in the future. Syngas
chemistry for the production of liquid fuels and chemicals has a vast future because syngas can be
obtained from both natural gas and man-made synthetic gas. The development of smart gas grid
will make the use of gas for heat, power, and liquid fuel unavoidable in the years to come.
This comprehensive book on natural and synthetic gas will be useful to all researchers involved
in the development of new technologies for energy and fuel. It will be a good reference for graduate
courses on energy and fuel and can serve as a graduate-level text on the subject of gas as a source
of fuel and energy.
Author
Dr. Yatish T. Shah received his BSc in chemical ­engineering from
the University of Michigan, Ann Arbor, Michigan and MS and ScD in
chemical engineering from Massachusetts Institute of Technology,
Cambridge, Massachusetts. He has more than 40 years of academic
and industrial experience in energy-related areas. He was chairman
of the Department of Chemical and Petroleum Engineering at the
University of Pittsburgh, dean of the College of Engineering at the
University of Tulsa and Drexel University, chief research officer at
Clemson University, and provost at Missouri University of Science
and Technology, University of Central Missouri, and Norfolk State
University. He was also a visiting scholar at Cambridge University
in the United Kingdom and a visiting professor at the University of California, Berkley, and Institut
für Technische Chemie I der Universität Erlangen, Nürnberg, Germany. Dr. Shah has written
six books related to energy: Gas-Liquid-Solid Reactor Design (published by McGraw-Hill, 1979),
Reaction Engineering in Direct Coal Liquefaction (published by Addison-Wesley, 1981), Cavitation
Reaction Engineering (published by Plenum Press, 1999), Biofuels and Bioenergy—Processes and
Technologies (published by CRC Press, 2012), Water for Energy and Fuel Production (published
by CRC Press, 2014) and Energy and Fuel Systems Integration (CRC Press, 2015). He has also
­published more than 250 refereed reviews, book chapters, and research technical publications in the
areas of energy, environment, and reaction engineering. He is an active consultant to numerous indus-
tries and government organizations in the energy areas.

xxv
 1 Introduction

1.1 INTRODUCTION
There are 10 sources of energy and fuel on earth. These are coal, oil, gas, biomass, waste, nuclear
energy, solar energy, wind energy, geothermal energy, and water. They can also be divided into three
categories: fossil fuels (coal, oil, and natural gas), nuclear energy, and renewables (biomass, waste,
solar energy, wind energy, geothermal energy, and water). Currently, about 85% of our energy needs
are supplied by fossil fuels. Among fossil fuels, coal and oil have been the dominant sources for our
fuel supply for power and transportation, respectively. In recent years, due to environmental con-
cerns, while the use of coal for power production is declining, the use of gas for power production is
on the rise. Use of natural gas in transportation industry is also slowly increasing.
Three fossil fuels, namely, coal, oil, and natural gas, were formed many hundreds of millions of
years ago before the Age of Dinosaurs—hence the name “fossil fuels.” The age they were formed
is called the Carboniferous (named after carbon) Period. It was part of the Paleozoic Era. The
Carboniferous Period occurred from about 360 to 286 million years ago. At the time, the land was
covered with swamps filled with huge trees, ferns, and other large leafy plants. The water and seas
were filled with algae. Besides trees and vegetables, the remains of animals were also buried in
the ground.
Natural gas is a fossil fuel formed when layers of buried plants, gases, and animals are exposed
to intense heat and pressure over thousands of years. The energy that the plants originally obtained
from the sun is stored in the form of chemical bonds in natural gas. Natural gas is a nonrenew-
able resource because it cannot be replenished on a human time frame. Natural gas is the gas
­component of coal, shale, oil, and water (in the form of clathrate hydrates under certain temperature
and ­pressure conditions) formation. It is found with coal as coalbed methane (CBM), with oil as
associated gas, with shale matrix as shale gas and as solid crystalline inclusion compounds, and
with water as gas hydrates in arctic conditions and at the bottom of the sea. It can be used to generate
heat, power, and liquid fuels and chemicals. It can be used for both static and mobile applications.
Energy in 6000 cubic feet (ft3) of natural gas is equivalent to 1 barrel of oil.
While the high-velocity gas generates wind energy, this book is focused on the conversion of
chemical energy from gas to heat, electricity, and liquid fuels. This chemical energy is generally
obtained from natural gas recovered from underground or synthetic gas produced from a variety of
nonrenewable and renewable sources.
The useful chemical constituents of natural and synthetic gas are largely methane, syngas (mix-
ture of hydrogen and carbon monoxide), and hydrogen. Other lower hydrocarbons, ethane, and
particularly propane and butane, are also used as fuels. Olefins such as ethylene and propylene are
often used as raw materials to produce chemicals, polymers, etc. In this book we will mainly focus
on various aspects of chemical constituents such as methane, syngas, hydrogen, propane (liquefied
petroleum gas [LPG]), and butane and their roles in the energy and fuel industry. Collectively, these
are called gaseous fuels. The scope of this book is to describe in detail the production, cleaning,
upgrade, storage, and transport of gaseous fuels that occurred naturally and the ones that are man-
made. The book also illustrates versatile applications of natural and synthetic gas for a variety of
end products.
While both coal and oil contain a large number of aliphatic, olefin, and aromatic hydrocarbons,
which can provide energy, the processing of coal and oil for heat and power productions also results
in the production of harmful by-products and emissions. On the other hand, gas containing volatile
hydrocarbons (mostly methane), syngas, and hydrogen provide fuel for energy in a cleaner form.

1
2 Chemical Energy from Natural and Synthetic Gas

Unlike coal and oil, natural or synthetic gas can be pretreated to produce high-quality pure meth-
ane, syngas, or hydrogen fuels, which can be used for numerous downstream applications. Both
methane and hydrogen have high hydrogen to carbon ratios than coal or oil, making them cleaner
and more efficient fuels. While the processing of coal and oil generates a significant amount of car-
bon dioxide, which is harmful to the environment, natural gas produces much lower carbon dioxide
than coal during power production and much less harmful emissions than oil in heat and transpor-
tation applications. Harmful environmental effect by burning syngas is even lower and there is no
carbon emission during the use of hydrogen.
The average emissions rates in the United States from natural gas–fired power plants are
1135 lb/MWh of carbon dioxide, 0.1 lb/MWh of sulfur dioxide, and 1.7 lb/MWh of nitrogen oxides
[1]. Thus, compared to the average air emissions from coal-fired generation, natural gas produces half
as much carbon dioxide, less than a third as much nitrogen oxides, and 1% as much sulfur oxides at
the power plant [1]. All new power plants in the United States are planning to use natural gas instead
of coal. An Massachusetts Institute of Technology (MIT) study [2] indicates that the use of natural
gas will be nearly doubled by 2040. Other projections shown in Figure 1.1 [3] indicate that natural
gas will compete well with oil in the future.
The increased share of natural gas in the global energy mix is not sufficient on its own to put the
world on a carbon emission path consistent with an average global temperature rise of no more than
2°C. As shown in Table 1.1, natural gas is still not as good as renewable fuels and nuclear energy for
its carbon emission. In the long term, more use of renewable energy and carbon-free nuclear energy
is needed. The large-scale hydrogen production from natural or synthetic gas can, of course, make
gas the ultimate source of fuel and energy along with renewable energy. At present time, nuclear
power, renewable energy, and carbon capture and sequestration are relatively expensive next to gas.
Until we make renewable energies and hydrogen commercially cheaper compared to fossil fuels,
natural gas will remain the “transition fuel.”

Quadrillion Btu
1990 History 2013 Projections
120

100

27% Natural gas 29%

80

23% 8% Renewables 10%

7% 1% Liquid biofuels 1%
60 8% Nuclear 8%
7%
23% 18% Coal 18%
40

Petroleum and
20 40% 36% 33%
other liquids

0
1980 1990 2000 2013 2020 2030 2040

FIGURE 1.1 Energy consumption projection by fuel type. (From U.S. Energy Information Administration,
Annual energy outlook 2015, EIA, Washington, DC, 2015, www.eia.gov/forecasts/aeo/, accessed on April, 2015.)
Another random document with
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 “Besides,” he was saying, “she hasn’t proper respect for me ... her father.
Sometimes I think it’s the ideas she got from you and from going abroad to
school.”
“What a nasty thing to say! But if you want the truth, I think it’s because
you’ve never been a very good father. Sometimes I’ve thought you never
wanted children. You’ve never paid much attention to them ... not even to
Jack ... while he was alive. It wasn’t ever as if they were our children.
You’ve always left them to me ... alone.”
The thin neck stiffened a little and he said, “There are reasons for that.
I’m a busy man.... I’ve given most of my time, not to making money, but to
doing things to better the world in some way. If I’ve neglected my children
it’s been for a good reason ... few men have as much on their minds. And
there’s been the book to take all my energies. You’re being unjust, Olivia.
You never could see me as I am.”
“Perhaps,” said Olivia. (She wanted to say, “What difference does the
book make to any one in the world? Who cares whether it is written or
not?”) She knew that she must keep up her deceit, so she said, “You needn’t
worry, because Sabine is going away to-morrow and Jean will go with her.”
She sighed. “After that your life won’t be disturbed any longer. Nothing in
the least unusual is likely to happen.”
“And there’s this other thing,” he said, “this disloyalty of yours to me
and to all the family.”
Stiffening slightly, she asked, “What can you mean by that?”
“You know what I mean.”
She saw that he was putting himself in the position of a wronged
husband, assuming a martyrdom of the sort which Aunt Cassie practised so
effectively. He meant to be a patient, well-meaning husband and to place
her in the position of a shameful woman; and slowly, with a slow, heavy
anger, she resolved to circumvent his trick.
“I think, Anson, that you’re talking nonsense. I haven’t been disloyal to
any one. Your father will tell you that.”
“My father was always weak where women are concerned, and now he’s
beginning to grow childish. He’s so old that he’s beginning to forgive and
condone anything.” And then after a silence he said, “This O’Hara. I’m not
such a fool as you think, Olivia.”
 For a long time neither of them said anything, and in the end it was
Olivia who spoke, striking straight into the heart of the question. She said,
“Anson, would you consider letting me divorce you?”
The effect upon him was alarming. His face turned gray, and the long,
thin, oversensitive hands began to tremble. She saw that she had touched
him on the rawest of places, upon his immense sense of pride and dignity. It
would be unbearable for him to believe that she would want to be rid of him
in order to go to another man, especially to a man whom he professed to
hold in contempt, a man who had the qualities which he himself did not
possess. He could only see the request as a humiliation of his own precious
dignity.
He managed to grin, trying to turn the request to mockery, and said,
“Have you lost your mind?”
“No, Anson, not for a moment. What I ask is a simple thing. It has been
done before.”
He did not answer her at once, and began to move about the room in the
deepest agitation, a strange figure curiously out of place in the midst of
Horace Pentland’s exotic, beautiful pictures and chairs and bibelots—as
wrong in such a setting as he had been right a month or two earlier among
the museum of Pentland family relics.
“No,” he said again and again. “What you ask is preposterous! To-
morrow when you are less tired you will see how ridiculous it is. No ... I
couldn’t think of such a thing!”
She made an effort to speak quietly. “Is it because you don’t want to put
yourself in such a position?”
“It has nothing to do with that. Why should you want a divorce? We are
well off, content, comfortable, happy....”
She interrupted him, asking, “Are we?”
“What is it you expect, Olivia ... to live always in a sort of romantic
glow? We’re happier than most.”
“No,” she said slowly. “I don’t think happiness has ever meant much to
you, Anson. Perhaps you’re above such things as happiness and
unhappiness. Perhaps you’re more fortunate than most of us. I doubt if you
have ever known happiness or unhappiness, for that matter. You’ve been
uncomfortable when people annoyed you and got in your way, but ... that’s
all. Nothing more than that. Happiness ... I mean it in the sensible way ...
has sometimes to do with delight in living, and I don’t think you’ve ever
known that, even for a moment.”
He turned toward her saying, “I’ve been an honest, God-fearing,
conscientious man, and I think you’re talking nonsense!”
“No, not for a moment.... Heaven knows I ought to know the truth of
what I’ve been saying.”
Again they reached an impasse in the conversation and again they both
remained silent, disturbed perhaps and uneasy in the consciousness that
between them they had destroyed something which could never be restored;
and yet with Olivia there was a cold, sustained sense of balance which came
to her miraculously at such times. She felt, too, that she stood with her back
against a wall, fighting. At last she said, “I would even let you divorce me
—if that would be easier for you. I don’t mind putting myself in the
wrong.”
Again he began to tremble. “Are you trying to tell me that....”
“I’m not telling you anything. There hasn’t been anything at all ... but ...
but I would give you grounds if you would agree.”
He turned away from her in disgust. “That is even more impossible.... A
gentleman never divorces his wife.”
“Let’s leave the gentlemen out of it, Anson,” she said. “I’m weary of
hearing what gentlemen do and do not do. I want you to act as yourself, as
Anson Pentland, and not as you think you ought to act. Let’s be honest. You
know you married me only because you had to marry some one ... and I ... I
wasn’t actually disreputable, even, as you remind me, if my father was
shanty Irish. And ... let’s be just too. I married you because I was alone and
frightened and wanted to escape a horrible life with Aunt Alice.... I wanted
a home. That was it, wasn’t it? We are both guilty, but that doesn’t change
the reality in the least. No, I fancy you practised loving me through a sense
of duty. You tried it as long as you could and you hated it always. Oh, I’ve
known what was going on. I’ve been learning ever since I came to
Pentlands for the first time.”
He was regarding her now with a fixed expression of horrid fascination;
he was perhaps even dazed at the sound of her voice, slowly, resolutely,
tearing aside all the veils of pretense which had made their life possible for
so long. He kept mumbling, “How can you talk this way? How can you say
such things?”
Slowly, terribly, she went on and on: “We’re both guilty ... and it’s been
a failure, from the very start. I’ve tried to do my best and perhaps
sometimes I’ve failed. I’ve tried to be a good mother ... and now that Sybil
is grown and Jack ... is dead, I want a chance at freedom. I’m still young
enough to want to live a little before it is too late.”
Between his teeth he said, “Don’t be a fool, Olivia.... You’re forty years
old....”
“You needn’t remind me of that. To-morrow I shall be forty. I know it ...
bitterly. But my being forty makes no difference to you. To you it would be
all the same if I were seventy. But to me it makes a difference ... a great
difference.” She waited a moment, and then said, “That’s the truth, Anson;
and it’s the truth that interests me to-night. Let me be free, Anson.... Let me
go while being free still means something.”
Perhaps if she had thrown herself at his feet in the attitude of a wretched,
shameful woman, if she had made him feel strong and noble and heroic, she
would have won; but it was a thing she could not do. She could only go on
being coldly reasonable.
“And you would give up all this?” he was saying. “You’d leave
Pentlands and all it stands for to marry this cheap Irishman ... a nobody, the
son perhaps of an immigrant dock-laborer.”
“He is the son of a dock-laborer,” she answered quietly. “And his mother
was a housemaid. He’s told me so himself. And as to all this.... Why,
Anson, it doesn’t mean anything to me ... nothing at all that I can’t give up,
nothing which means very much. I’m fond of your father, Anson, and I’m
fond of you when you are yourself and not talking about what a gentleman
would do. But I’d give it all up ... everything ... for the sake of this other
thing.”
For a moment his lips moved silently and in agitation, as if it were
impossible for him to answer things so preposterous as those his wife had
just spoken. At last he was able to say, “I think you must have lost your
mind, Olivia ... to even think of asking such a thing of me. You’ve lived
here long enough to know how impossible it is. Some of us must make a
stand in a community. There has never been a scandal, or even a divorce, in
the Pentland family ... never. We’ve come to stand for something. Three
hundred years of clean, moral living can’t be dashed aside so easily....
We’re in a position where others look up to us. Can’t you see that? Can’t
you understand such a responsibility?”
For a moment she had a terrible, dizzy, intoxicating sense of power, of
knowing that she held the means of destroying him and all this whited
structure of pride and respectability. She had only to begin by saying,
“There was Savina Pentland and her lover....” The moment passed quickly
and at once she knew that it was a thing she could not do. Instead, she
murmured, “Ah, Anson, do you think the world really looks at us at all? Do
you think it really cares what we do or don’t do? You can’t be as blind as
that.”
“I’m not blind ... only there’s such a thing as honor and tradition. We
stand for something....”
She interrupted him. “For what?”
“For decency, for a glorious past, for stability ... for endless things ... all
the things which count in a civilized community.”
He really believed what he was saying; she knew that he must have
believed it to have written all those thousands of dull, laborious words in
glorification of the past.
He went on. “No, what you ask is impossible. You knew it before you
asked.... And it would be a kindness to me if you never mentioned it again.”
He was still pale, but he had gained control of himself and his hands no
longer trembled; as he talked, as his sense of virtue mounted, he even grew
eloquent, and his voice took on a shade of that unction which had always
colored the voice of the Apostle to the Genteel and made of him a
celebrated and fashionable cleric. Perhaps for the first time since his
childhood, since the days when the red-haired little Sabine had mocked his
curls and velvet suits, he felt himself a strong and powerful person. There
was a kind of fierce intoxication in the knowledge of his power over Olivia.
In his virtuous ardor he seemed for a moment to become a positive, almost
admirable person.
At length she said quietly, “And what if I should simply go away ...
without bothering about a divorce?”
The remark shattered all his confidence once more; and she knew that
she had struck at the weakest point in all his defense—the fear of a scandal.
“You wouldn’t do that!” he cried. “You couldn’t—you couldn’t behave like
a common prostitute!”
“Loving one man is not behaving like a common prostitute.... I never
loved any other.”
“You couldn’t bring such a disgrace on Sybil, even if you don’t care for
the rest of us.”
(“He knew, then, that I couldn’t do such a thing, that I haven’t the
courage. He knows that I’ve lived too long in this world.”) Aloud she said,
“You don’t know me, Anson.... In all these years you’ve never known me at
all.”
“Besides,” he added quickly, “he wouldn’t do such a thing. Such a
climber isn’t likely to throw over his whole career by running away with a
woman. You’d find out if you asked him.”
“But he is willing. He’s already told me so. Perhaps you can’t understand
such a thing.” When he did not answer, she said ironically, “Besides, I don’t
think a gentleman would talk as you are talking. No, Anson.... I don’t think
you know what the world is. You’ve lived here always, shut up in your own
little corner.” Rising, she sighed and murmured, “But there’s no use in talk.
I am going to bed.... I suppose we must struggle on as best we can ... but
there are times ... times like to-night when you make it hard for me to bear
it. Some day ... who knows ... there’s nothing any longer to keep me....”
She went away without troubling to finish what she had meant to say,
lost again in an overwhelming sense of the futility of everything. She felt,
she thought, like an idiot standing in the middle of an empty field, making
gestures.
 CHAPTER X

Toward morning the still, breathless heat broke without warning into a
fantastic storm which filled all the sky with blinding light and enveloped
the whole countryside in a wild uproar of wind and thunder, leaving the
dawn to reveal fields torn and ravaged and strewn with broken branches,
and the bright garden bruised and battered by hail.
At breakfast Anson appeared neat and shaven and smooth, as though
there had been no struggle a few hours before in the drawing-room, as if the
thing had made no impression upon the smooth surface which he turned
toward the world. Olivia poured his coffee quietly and permitted him to kiss
her as he had done every day for twenty years—a strange, cold, absent-
minded kiss—and stood in the doorway to watch him drive off to the train.
Nothing had changed; it seemed to her that life at Pentlands had become
incapable of any change.
And as she turned from the door Peters summoned her to the telephone
to receive the telegram from Jean and Sybil; they had been married at seven
in Hartford.
She set out at once to find John Pentland and after a search she came
upon him in the stable-yard talking with Higgins. The strange pair stood by
the side of the red mare, who watched them with her small, vicious red
eyes; they were talking in that curious intimate way which descended upon
them at the mention of horses, and as she approached she was struck, as she
always was, by the fiery beauty of the animal, the pride of her lean head,
the trembling of the fine nostrils as she breathed, the savagery of her eye.
She was a strange, half-evil, beautiful beast. Olivia heard Higgins saying
that it was no use trying to breed her ... an animal like that, who kicked and
screamed and bit at the very sight of another horse....
Higgins saw her first and, touching his cap, bade her good-morning, and
as the old man turned, she said, “I’ve news for you, Mr. Pentland.”
A shrewd, queer look came into his eyes and he asked, “Is it about
Sybil?”
 “Yes.... It’s done.”
She saw that Higgins was mystified, and she was moved by a desire to
tell him. Higgins ought to know certainly among the first. And she added,
“It’s about Miss Sybil. She married young Mr. de Cyon this morning in
Hartford.”
The news had a magical effect on the little groom; his ugly, shriveled
face expanded into a broad grin and he slapped his thigh in his enthusiasm.
“That’s grand, Ma’am.... I don’t mind telling you I was for it all along. She
couldn’t have done better ... nor him either.”
Again moved by impulse, she said, “So you think it’s a good thing?”
“It’s grand, Ma’am. He’s one in a million. He’s the only one I know who
was good enough. I was afraid she was going to throw herself away on Mr.
O’Hara.... But she ought to have a younger man.”
She turned away from him, pleased and relieved from the anxiety which
had never really left her since the moment they drove off into the darkness.
She kept thinking, “Higgins is always right about people. He has a second
sight.” Somehow, of them all, she trusted him most as a judge.
John Pentland led her away, out of range of Higgins’ curiosity, along the
hedge that bordered the gardens. The news seemed to affect him strangely,
for he had turned pale, and for a long time he simply stood looking over the
hedge in silence. At last he asked, “When did they do it?”
“Last night.... She went for a drive with him and they didn’t come back.”
“I hope we’ve been right ...” he said. “I hope we haven’t connived at a
foolish thing.”
“No.... I’m sure we haven’t.”
Something in the brilliance of the sunlight, in the certainty of Sybil’s
escape and happiness, in the freshness of the air touched after the storm by
the first faint feel of autumn, filled her with a sense of giddiness, so that she
forgot her own troubles; she forgot, even, that this was her fortieth birthday.
“Did they go in Sabine’s motor?” he asked.
“Yes.”
Grinning suddenly, he said, “She thought perhaps that she was doing us
a bad turn.”
“No, she knew that I approved. She did think of it first. She did propose
it....”
 When he spoke again there was a faint hint of bitterness in his voice.
“I’m sure she did. I only hope she’ll stop her mischief with this. In any
case, she’s had a victory over Cassie ... and that’s what she wanted, more
than anything....” He turned toward her sharply, with an air of anxiety. “I
suppose he’ll take her away with him?”
“Yes. They’re going to Paris first and then to the Argentine.”
Suddenly he touched her shoulder with the odd, shy gesture of affection.
“It’ll be hard for you, Olivia dear ... without her.”
The sudden action brought a lump into her throat, and yet she did not
want to be pitied. She hated pity, because it implied weakness on her part.
“Oh,” she said quickly, “they’ll come back from time to time.... I think
that some day they may come back here to live.”
“Yes.... Pentlands will belong to them one day.”
And then for the first time she remembered that there was something
which she had to tell him, something which had come to seem almost a
confession. She must tell him now, especially since Jean would one day
own all of Pentlands and all the fortune.
“There’s something I didn’t tell you before,” she began. “It’s something
which I kept to myself because I wanted Sybil to have her happiness ... in
spite of everything.”
He interrupted her, saying, “I know what it is.”
“You couldn’t know what I mean.”
“Yes; the boy told me himself. I went to him to talk about Sybil because
I wanted to make sure of him ... and after a time he told me. It was an
honorable thing for him to have done. He needn’t have told. Sabine would
never have told us ... never until it was too late.”
The speech left her feeling weak and disconcerted, for she had expected
anger from him and disapproval. She had been fearful that he might treat
her silence as a disloyalty to him, that it might in the end shatter the long,
trusting relationship between them.
“The boy couldn’t help it,” he was saying. “It’s a thing one can’t
properly explain. But he’s a nice boy ... and Sybil was so set on him. I think
she has a good, sensible head on her young shoulders.” Sighing and turning
toward her again, he added, “I wouldn’t speak of it to the others ... not even
to Anson. They may never know, and if they don’t what they don’t know
won’t hurt them.”
The mystery of him, it seemed, grew deeper and deeper each time they
talked thus, intimately, perhaps because there were in the old man depths
which she had never believed possible. Perhaps, deep down beneath all the
fierce reticence of his nature, there lay a humanity far greater than any she
had ever encountered. She thought, “And I have always believed him hard
and cold and disapproving.” She was beginning to fathom the great strength
that lay in his fierce isolation, the strength of a man who had always been
alone.
“And you, Olivia?” he asked presently. “Are you happy?”
“Yes.... At least, I’m happy this morning ... on account of Sybil and
Jean.”
“That’s right,” he said with a gentle sadness. “That’s right. They’ve done
what you and I were never able to do, Olivia. They’ll have what we’ve
never had and never can have because it’s too late. And we’ve helped them
to gain it.... That’s something. I merely wanted you to know that I
understood.” And then, “We’d better go and tell the others. The devil will
be to pay when they hear.”
She would have gone away then, but an odd thought occurred to her, a
hope, feeble enough, but one which might give him a little pleasure. She
was struck again by his way of speaking, as if he were very near to death or
already dead. He had the air of a very old and weary man.
She said, “There’s one thing I’ve wanted to ask you for a long time.” She
hesitated and then plunged. “It was about Savina Pentland. Did she ever
have more than one child?”
He looked at her sharply out of the bright black eyes and asked, “Why
do you want to know that?”
She tried to deceive him by shrugging her shoulders and saying casually,
“I don’t know ... I’ve become interested lately, perhaps on account of
Anson’s book.”
“You ... interested in the past, Olivia?”
“Yes.”
“Yes, she only had one child ... and then she was drowned when he was
only a year old. He was my grandfather.” Again he looked at her sharply.
“Olivia, you must tell me the truth. Why did you ask me that question?”
Again she hesitated, saying, “I don’t know ... it seemed to me....”
“Did you find something? Did she,” he asked, making the gesture toward
the north wing, “did she tell you anything?”
She understood then that he, marvelous old man, must even know about
the letters. “Yes,” she said in a low voice, “I found something ... in the
attic.”
He sighed and looked away again, across the wet meadows. “So you
know, too.... She found them first, and hid them away again. She wouldn’t
give them to me because she hated me ... from our wedding-night. I’ve told
you about that. And then she couldn’t remember where she’d hid them ...
poor thing. But she told me about them. At times she used to taunt me by
saying that I wasn’t a Pentland at all. I think the thing made her mind darker
than it was before. She had some terrible idea about the sin in my family for
which she must atone....”
“It’s true,” said Olivia softly. “There’s no doubt of it. It was written by
Toby Cane himself ... in his own handwriting. I’ve compared it with the
letters Anson has of his.” After a moment she asked, “And you ... you’ve
known it always?”
“Always,” he said sadly. “It explains many things.... Sometimes I think
that those of us who have lived since have had to atone for their sin. It’s all
worked out in a harsh way, when you come to think of it....”
She guessed what it was he meant. She saw again that he believed in
such a thing as sin, that the belief in it was rooted deeply in his whole
being.
“Have you got the letters, Olivia?” he asked.
“No ... I burned them ... last night ... because I was afraid of them. I was
afraid that I might do something shameful with them. And if they were
burned, no one would believe such a preposterous story and there wouldn’t
be any proof. I was afraid, too,” she added softly, “of what was in them ...
not what was written there, so much as the way it was written.”
He took her hand and with the oddest, most awkward gesture, kissed it
gently. “You were right, Olivia dear,” he said. “It’s all they have ... the
others ... that belief in the past. We daren’t take that from them. The strong
daren’t oppress the weak. It would have been too cruel. It would have
destroyed the one thing into which Anson poured his whole life. You see,
Olivia, there are people ... people like you ... who have to be strong enough
to look out for the others. It’s a hard task ... and sometimes a cruel one. If it
weren’t for such people the world would fall apart and we’d see it for the
cruel, unbearable place it is. That’s why I’ve trusted everything to you.
That’s what I was trying to tell you the other night. You see, Olivia, I know
you ... I know there are things which people like us can’t do.... Perhaps it’s
because we’re weak or foolish—who knows? But it’s true. I knew that you
were the sort who would do just such a thing.”
Listening to him, she again felt all her determination slipping from her. It
was a strange sensation, as if he took possession of her, leaving her
powerless to act, prisoning her again in that terrible wall of rightness in
which he believed. The familiar sense of his strength frightened her,
because it seemed a force so irresistible. It was the strength of one who was
more than right; it was the strength of one who believed.
She had a fierce impulse to turn from him and to run swiftly, recklessly,
across the wet meadows toward Michael, leaving forever behind her the
placid, beautiful old house beneath the elms.
“There are some things,” he was saying, “which it is impossible to do ...
for people like us, Olivia. They are impossible because the mere act of
doing them would ruin us forever. They aren’t things which we can do
gracefully.”
And she knew again what it was that he meant, as she had known
vaguely while she stood alone in the darkness before the figures of Higgins
and Miss Egan emerged from the mist of the marshes.
“You had better go now and telephone to Anson. I fancy he’ll be badly
upset, but I shall put an end to that ... and Cassie, too. She had it all planned
for the Mannering boy.”
2

Anson was not to be reached all the morning at the office; he had gone,
so his secretary said, to a meeting of the Society of Guardians of Young
Working Girls without Homes and left express word that he was not to be
disturbed. But Aunt Cassie heard the news when she arrived on her morning
call at Pentlands. Olivia broke it to her as gently as possible, but as soon as
the old lady understood what had happened, she went to pieces badly. Her
eyes grew wild; she wept, and her hair became all disheveled. She took the
attitude that Sybil had been seduced and was now a woman lost beyond all
hope. She kept repeating between punctuations of profound sympathy for
Olivia in the hour of her trial, that such a thing had never happened in the
Pentland family; until Olivia, enveloped in the old, perilous calm, reminded
her of the elopement of Jared Pentland and Savina Dalgedo and bade her
abruptly to stop talking nonsense.
And then Aunt Cassie was deeply hurt by her tone, and Peters had to be
sent away for smelling-salts at the very moment that Sabine arrived,
grinning and triumphant. It was Sabine who helped administer the smelling-
salts with the grim air of administering burning coals. When the old lady
grew a little more calm she fell again to saying over and over again, “Poor
Sybil.... My poor, innocent little Sybil ... that this should have happened to
her!”
To which Olivia replied at last, “Jean is a fine young man. I’m sure she
couldn’t have done better.” And then, to soften a little Aunt Cassie’s
anguish, she said, “And he’s very rich, Aunt Cassie ... a great deal richer
than many a husband she might have found here.”
The information had an even better effect than the smelling-salts, so that
the old lady became calm enough to take an interest in the details and asked
where they had found a motor to go away in.
“It was mine,” said Sabine dryly. “I loaned it to them.”
The result of this statement was all that Sabine could have desired. The
old lady sat bolt upright, all bristling, and cried, with an air of suffocation,
“Oh, you viper! Why God should have sent me such a trial, I don’t know.
You’ve always wished us evil and now I suppose you’re content! May God
have mercy on your malicious soul!” And breaking into fresh sobs, she
began all over again, “My poor, innocent little Sybil.... What will people
say? What will they think has been going on!”
“Don’t be evil-minded, Aunt Cassie,” said Sabine sharply; and then in a
calmer voice, “It will be hard on me.... I won’t be able to go to Newport
until they come back with the motor.”
“You!... You!...” began Aunt Cassie, and then fell back, a broken
woman.
“I suppose,” continued Sabine ruthlessly, “that we ought to tell the
Mannering boy.”
 “Yes,” cried Aunt Cassie, reviving again, “Yes! There’s the boy she
ought to have married....”
“And Mrs. Soames,” said Sabine. “She’ll be pleased at the news.”
Olivia spoke for the first time in nearly half an hour. “It’s no use. Mr.
Pentland has been over to see her, but she didn’t understand what it was he
wanted to tell her. She was in a daze ... only half-conscious ... and they
think she may not recover this time.”
In a whisper, lost in the greater agitation of Aunt Cassie’s sobs, she said
to Sabine, “It’s like the end of everything for him. I don’t know what he’ll
do.”

The confusion of the day seemed to increase rather than to die away.
Aunt Cassie was asked to stay to lunch, but she said it was impossible to
consider swallowing even a crust of bread. “It would choke me!” she cried
melodramatically.
“It is an excellent lunch,” urged Olivia.
“No ... no ... don’t ask me!”
But, unwilling to quit the scene of action, she lay on Horace Pentland’s
Regence sofa and regained her strength a little by taking a nap while the
others ate.
At last Anson called, and when the news was told him, the telephone
echoed with his threats. He would, he said, hire a motor (an extravagance
by which to gage the profundity of his agitation) and come down at once.
And then, almost immediately, Michael telephoned. “I have just come
down,” he said, and asked Olivia to come riding with him. “I must talk to
you at once.”
She refused to ride, but consented to meet him half-way, at the pine
thicket where Higgins had discovered the foxcubs. “I can’t leave just now,”
she told him, “and I don’t think it’s best for you to come here at the
moment.”
For some reason, perhaps vaguely because she thought he might use the
knowledge as a weapon to break down her will, she said nothing of the
elopement. For in the confusion of the day, beneath all the uproar of scenes,
emotions and telephone-calls, she had been thinking, thinking, thinking, so
that in the end the uproar had made little impression upon her. She had
come to understand that John Pentland must have lived thus, year after year,
moving always in a secret life of his own, and presently she had come to the
conclusion that she must send Michael away once and for all.
As she moved across the meadow she noticed that the birches had begun
to turn yellow and that in the low ground along the river the meadows were
already painted gold and purple by masses of goldenrod and ironweed. With
each step she seemed to grow weaker and weaker, and as she drew near the
blue-black wall of pines she was seized by a violent trembling, as if the
sense of his presence were able somehow to reach out and engulf her even
before she saw him. She kept trying to think of the old man as he stood
beside her at the hedge, but something stronger than her will made her see
only Michael’s curly black head and blue eyes. She began even to pray ...
she (Olivia) who never prayed because the piety of Aunt Cassie and Anson
and the Apostle to the Genteel stood always in her way.
And then, looking up, she saw him standing half-hidden among the
lower pines, watching her. She began to run toward him, in terror lest her
knees should give way and let her fall before she reached the shelter of the
trees.
In the darkness of the thicket where the sun seldom penetrated, he put
his arms about her and kissed her in a way he had never done before, and
the action only increased her terror. She said nothing; she only wept quietly;
and at last, when she had gained control of herself, she struggled free and
said, “Don’t, Michael ... please don’t ... please.”
They sat on a fallen log and, still holding her hand, he asked, “What is
it? What has happened?”
“Nothing.... I’m just tired.”
“Are you willing to come away with me? Now?” And in a low, warm
voice, he added, “I’ll never let you be tired again ... never.”
She did not answer him, because it seemed to her that what she had to
tell him made all her actions in the past seem inexplicable and cheap. She
was filled with shame, and tried to put off the moment when she must
speak.
“I haven’t been down in three days,” he was saying, “because there’s
been trouble in Boston which made it impossible. I’ve only slept an hour or
two a night. They’ve been trying to do me in ... some of the men I always
trusted. They’ve been double-crossing me all along and I had to stay to
fight them.”
He told her a long and complicated story of treachery, of money having
been passed among men whom he had known and trusted always. He was
sad and yet defiant, too, and filled with a desire to fight the thing to an end.
She failed to understand the story; indeed she did not even hear much of it:
she only knew that he was telling her everything, pouring out all his sadness
and trouble to her as if she were the one person in all the world to whom he
could tell such things.
And when he had finished he waited for a moment and then said, “And
now I’m willing to chuck the whole dirty business and quit ... to tell them
all to go to hell.”
Quickly she answered, “No, you mustn’t do that. You can’t do that. A
man like you, Michael, daren’t do such a thing....” For she knew that
without a battle life would mean nothing to him.
“No ... I mean it. I’m ready to quit. I want you to go with me.”
She thought, “He says this ... and yet he stayed three days and nights in
Boston to fight!” She saw that he was not looking at her, but sitting with his
head in his hands; there was something broken, almost pitiful, in his
manner, and it occurred to her that perhaps for the first time he found all his
life in a hopeless tangle. She thought, “If I had never known him, this might
not have happened. He would have been able to fight without even thinking
of me.”
Aloud she said, “I can’t do it, Michael.... It’s no use. I can’t.”
He looked up quickly, but before he could speak she placed her hand
over his lips, saying, “Wait, Michael, let me talk first. Let me say what I’ve
wanted to say for so long.... I’ve thought.... I’ve done nothing else but think
day and night for the past three days. And it’s no good, Michael.... It’s no
good. I’m forty years old to-day, and what can I give you that will make up
for all you will lose? Why should you give up everything for me? No, I’ve
nothing to offer. You can go back and fight and win. It’s what you like more
than anything in the world ... more than any woman ... even me.”
Again he tried to speak, but she silenced him. “Oh, I know it’s true ...
what I say. And if I had you at such a price, you’d only hate me in the end. I
couldn’t do it, Michael, because ... because in the end, with men like you
it’s work, it’s a career, which is first.... You couldn’t bear giving up. You
couldn’t bear failure.... And in the end that’s right, as it should be. It’s what
keeps the world going.”
He was watching her with a look of fascination in his eyes, and she knew
—she was certain of it—that he had never been so much in love with her
before; but she knew, too, from the shadow which crossed his face (it
seemed to her that he almost winced) and because she knew him so well,
that he recognized the truth of what she had said.
“It’s not true, Olivia.... You can’t go back on me now ... just when I need
you most.”
“I’d be betraying you, Michael, if I did the other thing. It’s not me you
need half so much as the other thing. Oh, I know that I’m right. What you
should have in the end is a young woman ... a woman who will help you. It
doesn’t matter very much whether you’re terribly in love with her or not ...
but a woman who can be your wife and bear your children and give dinner
parties and help make of you the famous man you’ve always meant to be.
You need some one who will help you to found a family, to fill your new
house with children ... some one who’ll help you and your children to take
the place of families like ours who are at the end of things. No, Michael ...
I’m right.... Look at me,” she commanded suddenly. “Look at me and you’ll
know that it’s not because I don’t love you.”
He was on his knees now, on the carpet of scented pine-needles, his arms
about her while she stroked the thick black hair with a kind of hysterical
intensity.
“You don’t know what you’re saying, Olivia. It’s not true! It’s not true!
I’d give up everything.... I don’t want the other thing. I’ll sell my farm and
go away from here forever with you.”
“Yes, Michael, you think that to-day, just now ... and to-morrow
everything will be changed. That’s one of the mean tricks Nature plays us.
It’s not so simple as that. We’re not like Higgins and ... the kitchen-maid ...
at least not in some ways.”
“Olivia ... Olivia, do you love me enough to....”
She knew what he meant to ask. She thought, “What does it matter?
Why should I not, when I love him so? I should be harming no one ... no
one but myself.”
And then, abruptly, through the mist of tears she saw through an opening
in the thicket a little procession crossing the meadows toward the big house
at Pentlands. She saw it with a terrible, intense clarity ... a little procession
of the gardener and his helper carrying between them on a shutter a figure
that lay limp and still, and following them came Higgins on foot, leading
his horse and moving with the awkward rolling gait which afflicted him
when his feet were on the ground. She knew who the still figure was. It was
John Pentland. The red mare had killed him at last. And she heard him
saying, “There are some things which people like us, Olivia, can’t do.”

What happened immediately afterward she was never able to remember

very clearly. She found herself joining the little procession; she knew that
Michael was with her, and that there could be no doubt of the tragedy....
John Pentland was dead, with his neck broken. He lay on the shutter, still
and peaceful, the bitter lines all melted from the grim, stern face, as he had
been when she came upon him in the library smelling of dogs and
woodsmoke and whisky. Only this time he had escaped for good....
And afterward she remembered telling Michael, as they stood alone in
the big white hall, that Sybil and Jean were married, and dismissing him by
saying, “Now, Michael, it is impossible. While he was living I might have
done it.... I might have gone away. But now it’s impossible. Don’t ask me.
Please leave me in peace.”
Standing there under the wanton gaze of Savina Pentland, she watched
him go away, quietly, perhaps because he understood that all she had said
was true.
3

In the tragedy the elopement became lost and forgotten. Doctors came
and went; even reporters put in an awkward appearance, eager for details of
the death and the marriage in the Pentland family, and somehow the
confusion brought peace to Olivia. They forgot her, save as one who
managed everything quietly; for they had need just then of some one who
did not break into wild spasms of grief or wander about helplessly. In the
presence of death, Anson forgot even his anger over the elopement, and late
in the afternoon Olivia saw him for the first time when he came to her
helplessly to ask, “The men have come to photograph the portraits. What
shall we do?”
 And she answered, “Send them away. We can photograph ancestors any
time. They’ll always be with us.”
Sabine volunteered to send word to Sybil and Jean. At such times all her
cold-blooded detachment made of her a person of great value, and Olivia
knew that she could be trusted to find them because she wanted her motor
again desperately. Remembering her promise to the old man, she went
across to see Mrs. Soames, but nothing came of it, for the old lady had
fallen into a state of complete unconsciousness. She would, they told
Olivia, probably die without ever knowing that John Pentland had gone
before her.
Aunt Cassie took up her throne in the darkened drawing-room and there,
amid the acrid smell of the first chrysanthemums of the autumn, she held a
red-eyed, snuffling court to receive the calls of all the countryside. Again
she seemed to rise for a time triumphant and strong, even overcoming her
weakness enough to go and come from the gazeboed house on foot, arriving
early and returning late. She insisted upon summoning Bishop Smallwood
to conduct the services, and discovered after much trouble that he was
attending a church conference in the West. In reply to her telegram she
received only an answer that it was impossible for him to return, even if
they delayed the funeral ... that in the rôle of prominent defender of the
Virgin Birth he could not leave the field at a moment when the power of his
party was threatened.
It seemed for a time that, as Sabine had hoped, the whole structure of the
family was falling about them in ruins.
As for Olivia, she would have been at peace save that three times within
two days notes came to her from Michael—notes which she sent back
unopened because she was afraid to read them; until at last she wrote on the
back of one, “There is nothing more to say. Leave me in peace.” And after
that there was only silence, which in a strange way seemed to her more
unbearable than the sight of his writing. She discovered that two persons
had witnessed the tragedy—Higgins, who had been riding with the old man,
and Sabine, who had been walking the river path—walking only because
Jean and Sybil had her motor. Higgins knew only that the mare had run off
and killed his master; but Sabine had a strangely different version, which
she recounted to Olivia as they sat in her room, the day after.
 “I saw them,” she said, “coming across the meadow.... Cousin John, with
Higgins following. And then, all at once, the mare seemed to be frightened
by something and began to run ... straight in a line for the gravel-pit. It was
a fascinating sight ... a horrible sight ... because I knew—I was certain—
what was going to happen. For a moment Cousin John seemed to fight with
her, and then all at once he leaned forward on her neck and let her go.
Higgins went after him; but it was no use trying to catch her.... One might
as well have tried to overtake a whirlwind. They seemed to fly across the
fields straight for the line of elders that hid the pit, and I knew all the while
that there was no saving them unless the mare turned. At the bushes the
mare jumped ... the prettiest jump I’ve ever seen a horse make, straight
above the bushes into the open air....”
For a moment Sabine’s face was lighted by a macabre enthusiasm. Her
voice wavered a little. “It was a horrible, beautiful sight. For a moment they
seemed almost to rise in the air as if the mare were flying, and then all at
once they fell ... into the bottom of the pit.”
Olivia was silent, and presently, as if she had been waiting for the
courage, Sabine continued in a low voice, “But there’s one thing I saw
beyond any doubt. At the edge of the pit the mare tried to turn. She would
have turned away, but Cousin John raised his crop and struck her savagely.
There was no doubt of it. He forced her over the elders....” Again after a
pause, “Higgins must have seen it, too. He followed them to the very edge
of the pit. I shall always see him there, sitting on his horse outlined against
the sky. He was looking down into the pit and for a moment the horse and
man together looked exactly like a centaur.... It was an extraordinary
impression.”
She remembered him thus, but she remembered him, too, as she had seen
him on the night of the ball, slipping away through the lilacs like a shadow.
Rising, she said, “Jean and Sybil will be back to-morrow, and then I’ll be
off for Newport. I thought you might want to know what Higgins and I
knew, Olivia.” For a moment she hesitated, looking out of the window
toward the sea. And at last she said, “He was a queer man. He was the last
of the great Puritans. There aren’t any more. None of the rest of us believe
anything. We only pretend....”
But Olivia scarcely heard her. She understood now why it was that the
old man had talked to her as if he were very near to death, and she thought,