Journal of Petroleum Science and Engineering 56 (2007) 1 – 8 www.elsevier.



An introduction to natural gas hydrate/clathrate: The major organic carbon reserve of the Earth
1. Existence of hydrates Gas hydrates belong to a general class of inclusion compounds commonly known as clathrates. A clathrate is a compound of molecular cage structure made of host molecules encapsulating guest molecules. It is also considered a chemical substance consisting of a lattice of one type of molecule trapping and containing a second type of molecule (Sloan, 1998; Taylor et al., 2004). Natural gas clathrates owe their existence to the ability of H2O molecules to assemble via hydrogen bonding and form polyhedral cavities as shown in Figs. 1 and 2. Natural gas hydrate is a naturally occurring ice-like solid (see Fig. 3), which is made of water molecules as the cage forming host and other molecules (mostly methane) as the guest. The guest molecules, like methane or carbon dioxide, are of an appropriate size such that they fit within cavities formed by the host material. Common clathrate compounds of interest are those formed from CO2/H2O and CH4/H2O mixtures: the former for application in carbon sequestration and the latter for methane extraction. The physical appearance of the natural gas hydrate is like other crystalline substances. At standard pressure and temperature, a methane hydrate molecule contains approximately 160 volumes of methane for each volume of water. Until recently, methane hydrates, known to scientists for almost 200 years, have remained a scientific curiosity. It was not until the 1930's that it was realized that methane hydrate was responsible for plugging natural gas pipelines, particularly those located in cold environments. For the next 40 years, a small body of researchers investigated the physics of various clathrates, including the construction of the first predictive models of their formation. A prime focus of this work was (and continues to be) the development of chemical additives and other methods to inhibit hydrate formation.
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The United States Geological Survey (USGS) estimates that there are more organic carbon reserves around the earth as methane hydrate than all other forms of fossil fuels combined (Booth et al., 1996). The Department of Energy (DOE) considers about 1% recovery of methane from the known methane hydrate reserves within the U.S. enough (over 2000 TCF) to satisfy the U.S. consumption for the next eight decades. As it is demonstrated in the pie-chart, Fig. 4, the amount of organic carbon contained in natural gas hydrate reserves around the globe is estimated to be twice the amount contained in all fossil fuels on Earth. By fossil fuels it is meant coal, oil and conventional natural gas reserves all around the world. According to the U.S. Geological Survey, the estimated global natural gas hydrate reserves are in the range from 100,000 to about 300,000,000 trillion cubic feet. This estimate when compared with the 13,000 trillion cubic feet of conventional natural gas reserves demonstrates the vastly more abundant natural gas hydrates around the globe. Interest in methane hydrate as an energy resource was initially ignited in 1960s' by Russian scientists who claimed contribution from hydrates during conventional gas drilling in the Messoyakha field, Siberia. The U.S. was a leader in the 1970s' in this area. In mid-1990's, two countries, with a large energy demand but limited resources (Japan and India), began to explore the possibility of extracting methane from hydrates. The U.S. research effort got a big push in Year 2000 with the passage of the Methane Hydrate Research and Development Act. Under the Act, the U.S. DOE coordinated a five-year effort by the Federal Agencies “to promote the research, identification, assessment, exploration, and development of methane hydrate resources”. Advances in the basic understanding of hydrates have occurred during these 5 years, including several hydrate-specific

and academia discussing Fig. A thematic symposium on “Gas hydrates and clathrates” was organized during the 2005 Spring National Meeting of the American Chemical Society in San Diego. Ames. Sarah A.A. below are the titles and authors. government. “Natural Gas-Hydrates — A potential energy source for the 21st century” by Y. Shelli R. Makogon⁎. John Pohlman. Costas Tsouris⁎ 8. 1. Akihiro Yamasaki. As it is shown in Fig. “Resource potential of methane hydrate coming into focus” by Ray Boswell⁎ 2. and Juan Diaz 4. “Effect of pressure vessel size on the formation of gas hydrates” by Scott D. Methane clathrate dual structure. Warren Wood. Charles Woods Fig. Phelps⁎ 7. Makogon 3. The schematic drawing of one type of natural gas clathrate structure in which a methane molecule is encaged by a lattice of water molecules. 2000) was extended by an amendment through 2010 as part of the Energy Policy Act of 2005. “Raman spectroscopy of a hydrated CO2/water composite” by Monsuru O. Michael D. Osegovic⁎. About this special issue This special issue is primarily dedicated to natural gas hydrate. 1753. S. The two-day symposium consisted of 28 invited speakers from industry. 5). followed by brief summaries of the 20 papers that are included herein: 1. (Courtesy of NETL). .R. Yousef Atallah. Joseph Gettrust. 2. Olga Y. David A. Fumio Kiyono. Many issues are under investigation by hydrate researchers around the world. Jennifer Dearman. an unconventional energy source that has the potential to supplant the world's energy supply. “Investigations into surfactant/gas–hydrate relationship” by Rudy Rogers⁎. future energy source. Of those presented. Shelby Walker. Audra L. Lance. Holman. Tommy J. Max 5. and global distribution of hydrate. Methane hydrates have been discovered in the subsurface in permafrost regions. Holditch. “Methane hydrate exploration on the mid-Chilean coast: A geochemical and geophysical survey” by Richard Coffin⁎. Lai⁎ 6. and T. Tadashi Masuyama 9. hydrate formation and dissociation properties. but most occur in oceanic sediments hundreds of meters below the sea floor where water depths are greater than about 500 m. “Formation of HFC-134a hydrate by static mixing” by Hideo Tajima⁎. The Methane Hydrate Research and Development Act (H. Riestenberg. Toru Nagata. These include implications on the global carbon cycle. McCallum. Zatsepina. “Growth kinetics of ethane hydrate from a seawater solution at an ethane gas interface” by John P. David E. Rebecca Plummer. Joan Gardner. Michael J. physical and chemical properties. 5 natural gas hydrates have been discovered at numerous locations along continental margins as well as in the Arctic. Scott D. Guochang Zhang. Tatro. We have attempted to represent papers reporting on the latest research in these areas.Y. seafloor stability. long-term climatechange effects. McCallum. Riestenberg.F. 2. As research is progressing. expeditions in the polar region and in the deep water on the continental shelves around the world (see Fig.2 Editorial the latest research issues and advances in the field of gas hydrates and clathrates. it may lead to an environmentally-benign methane extraction method in a not too distant future. Ross Downer. “Effects of gas hydrates on the chemical and physical properties of seawater” by Chung-Chieng A. CA. Gborigi. Leila Hamdan.

P.usgs. and Arvind Gupta 14. “A novel high-pressure apparatus to study hydrate– sediment interactions” Michael Eaton. Taylor⁎. 19. Kneafsey⁎. Mason. “Methane gas hydrate effect on sediment acoustic and strength properties” by W. Winters. In the 1st invited paper. To address this and other questions. Boswell (2007) (NETL/U. Ladner 12. environmental. Castaldi⁎. Link. Lichtner “Down-hole combustion method for gas production from methane hydrates” by Marco J. Gbaruko. The paper discusses significant developments over the past 5 years that have sharpened the focus of R and D into methane hydrate's resource . 2004). Charles E. 20. Igwe. Waite. 10. Taylor⁎. “Effect of bubble size and density on methane conversion to hydrate” by Jonathan Lekse. “Methane hydrate formation and dissociation in a partially saturated core-scale sand Sample" by Timothy J. Dirk D. and Edward P. and R. A: pure methane hydrate. More than half of the carbon is locked up in gas hydrates (Source: www.A. D. Chief among these is the potential for methane hydrate to serve as a significant new resource to help meet long-term energy demands. and I.Editorial 3 Fig. William J. Moridis. L. Gbaruko⁎. Gilbert. C. research to make methane production from hydrates a reality" by Charles E. Yue Zhou. Stanmire Tomov. Distribution of organic carbon in Earth reservoirs (excluding dispersed carbon in rocks and sediments. which equals nearly 1000 times this amount).J.F. Tsimpanogiannis⁎. “Characterization of methane hydrate host sediments using synchrotron-computed microtomogra- 16.Y. and Niall Eglish “Gas hydrates and clathrates: flow assurance. Huan Feng. “Effect of surfactant carbon chain length on hydrate formation kinetics” Takamichi Daimaru. Yegulalp “Methane hydrate research at NETL. Charles E. 3. 17. and the Nigerian Liquified Natural Gas Project” by B.H. W.S. Devinder Mahajan⁎. by Yukio Yanagisawa 11. and Roger Flood 13. C. Pecher 15. Barry M. Nwokeoma Fig. 18. economic perspectives. and Peter C. C: methane hydrate in F-110 sand (Taylor et al. Photographs of methane hydrate made in a 1 L cell. Freifeld. 4. Winters⁎. B: methane hydrate in sea sand. Jones. Liviu Tomutsa. Akihiro Yamasaki⁎. C.. phy (CMT)” by Keith W. and Devinder Mahajan⁎ “Predicting gas generation by depressurization of gas hydrates where the sharp-interface assumption is not valid” by Shahab Gerami and Mehran Pooladi–Darvish⁎ “Parametric study of methane hydrate dissociation in oceanic sediments driven by thermal stimulation” by Ioannis N. Maša Prodanoviæ. George J. Taylor. N. the Methane Hydrate R & D Act of 2000 was enacted — promoting unprecedented collaboration between six federal agencies and enabling 5 years of government-industry–academia R & D partnerships. Yongkoo Seol. The first three papers discuss the resource potential of methane hydrate as an energy source. DOE) discusses increasing recognition of the potentially vast global occurrence of methane hydrate that has raised a number of critical public interest questions. and Tuncel M.

5. He contends that the rate of modern civilization growth in the future will depend on numerous factors. Ethane hydrate crystals that have the macroscopic appearance of concentric rings were nucleated and grown from a seawater solution under a range of supersaturations. Osegovic et al. 1997). The goal of the expedition was to survey regions of possible hydrate accumulations by integrating data from seismic surveys. This work is representative of worldwide interest in developing hydrate to supplant conventional natural gas reserves. CO2. Distribution of natural gas hydrates around the globe (Max et al. based on WOCE ocean observations. measurement of the shallow SMI and vertical sulfate diffusion. and other gases. Coffin et al. This sample pattern was based on a previous deep towed acoustics geophysics system (DTAGS) seismic survey.4 Editorial Fig.. coupled with the seismic survey and heat flow provides a more thorough indication of the presence of deep sediment methane gas pockets. The nucleation rate was determined by plotting the increase in the number of observed particles with time and approached a maximum rate implying a diffusion limited process. (2007) (Naval Research Laboratory) summarize data from a methane hydrate exploration that was conducted off the Mid-Chilean margin (west of Concepción) during October 2004. In paper 6. the reserves are sufficient for 41 years for oil and 66 years for natural gas. and heat flow probing. Lai (2007) (Los Alamos National Laboratory) presents analysis of individual profiles on the seafloor and continental margins that imply dissociation of gas hydrates occurs according to temperature and pressure (depth) conditions at the hydrate phase boundary. McCallum . Analysis of the relationship among seawater temperature. The 2nd paper by Makogon et al. The disk crystals eventually agglomerated to completely cover the interface. as of 1 January 2005. (2007) (Texas A & M) presents various energy scenarios. According to British Petroleum (BP). the proven hydrocarbon reserves are 161. Papers 4 through 8 describe laboratory studies that are underway to enhance our understanding of hydrates of CH4.9 billion tons of oil and 179. potential. Piston cores were collected at 13 sites along a NE–SW transect. the oceanic hydrates provide a huge biochemical fuel source that is continually generating internal heat in the world oceans. A new source of fossil fuel is needed and gas hydrates may be this source. In the 5th paper. According to Lai. In the study region. An understanding of the formation of hydrate at gas/liquid interfaces is of interest for its potential role in clogging gas pipelines. “apparent oxygen utilization” (AOU) and the concentration of CO2. The role of microbes in altering the chemical and physical properties of seawater is also discussed. In paper 4. In the 3rd paper. At the current level of consumption. The data presented in this paper reflects the distribution and changes of energy sources over time with oil and natural gas as the primary present fuels. (2007) (MDS. but the quality and quantity of energy used will be among the most important factors. This may explain the observed ocean warming at the intermediate depth during last several decades. geochemical analysis of porewater samples from piston cores.5 trillion m3 of natural gas. reveal some characteristics that are not part of a stoichiometric relation. LLC) reports the growth rate and morphology of gas hydrate at an interface of seawater and ethane gas.

The hydrate formation patterns depended on the rate of hydrate formation per pressure and temperature conditions. An attempt was made to calculate the hydration number for the CO2 hydrate composite and also the percentage of liquid CO2 and water loss during formation. The authors conclude that mesoscale experiments such as those in the SPS. and C18) were tested. (2007) (Oak Ridge National Laboratory) investigated formation of a sinking carbon dioxide (CO2) hydrate composite as an alternative to direct liquid CO2 injection and pure CO2 hydrate formation for ocean carbon sequestration. Plug-like hydrate was agglomerated HFC-134a bubbles covered with hydrate. The Raman shifts corresponding to CO2 and water molecules as well as shifts in peak positions due to different CO2 phases were obtained. The variability of pressure and/or induction time for hydrate formation was not eliminated by using the SPS. it was estimated that power consumption could be reduced by about 40% with the use of the C4 surfactant in the hydrate formation process. The observed differences were attributed to increased bubble surface area. (2007) (Oak Ridge National Laboratory) describe the effect of pressure vessel size on gas hydrate formation. the pressure and temperature conditions feasible for continuously forming HFC-134a hydrate were determined. In the 7th paper. Japan) the authors propose a more efficient continuous gas hydrate formation method using a static mixer. From the experimental results.Editorial 5 et al. (2007) (NETL/U.45 L pressurized vessels at pressure and temperature conditions equivalent to approximately 1. the applications of gas hydrate research are expanding into fields of energy and environmental management. The catalytic effects. Papers 9 and 10 describe the effect of surfactants on hydrate formation.S.) presents results showing how anionic synthetic surfactants helped develop an industrial gas-hydrate storage process for natural gas and how naturally-occurring in situ anionic biosurfactants influence the formation and placement of gas hydrates in ocean sediments. lifetime of bubbles. The Raman spectra of the composite showed that both liquid and hydrate phases of CO2 were present. The authors observed during investigation that the ability to convert methane to hydrate was enhanced by foaming of the methane-water solution using a surfactant. but it appeared to be less dramatic (small coefficients of variation) when compared with a 450 mL Parr vessel. A Seafloor Process Simulator (SPS) consisting of a 72 L vessel was used for mesoscale experiments investigating the nature of hydrate nucleation and dissociation at pressures and temperatures required for stability of hydrates of CH4 and CO2. Lekse et al. The same experiments were duplicated in a smaller (0. and the hydrate formation rate determined by the rate of pressure decrease caused by hydrate formation. C12. In recent years. mechanisms. It was found that experiments in the SPS resulted in hydrates consistently forming at lower overpressures and in shorter induction times than equivalent experiments in the smaller vessel. In the 8th paper by Tajima et al. Gborigi et al. The 9th paper by Rogers and his group (2007) (Mississippi State U. was important in this conversion reaction. Raman spectroscopy was used as a tool to understand the formation and spectroscopy of a semi-solid sinking CO2 hydrate composite formed using a coflow injector in the 72 L and 0. The density of the foam. gas concentration. and the resulting hydrate was observed as plug-like hydrate and hydrate slurry. Paper 10 by Daimaru et al. Energy saving potential was estimated when the C4 surfactant was applied to a natural gas transportation scenario in the form of hydrates.45 L) Parr vessel. The experiments indicate that seafloor biosurfactants can be produced rapidly in situ to achieve threshold concentrations whereby hydrates are promoted. and the effects of carbon chain length and concentration were systematically investigated. while the hydrate slurry consisted of small hydrate particles dispersed in water. may perhaps be more representative of hydrate accumulation in the natural environment. The Bacillus subtilis bacterium that is indigenous to gas hydrate mounds in the Gulf of Mexico was cultured in the laboratory. or a combination of the above. along with bubble size. and surface specificities imparted by synthetic surfactants in the gas storage process and imparted by biosurfactants in porous media are discussed. with 100 mL inner volume. (2007) (University of Tokyo) describes an experimental study to establish the effect of surfactants on hydrate formation kinetics. Its biosurfactant was separated and found to catalyze gas hydrates in porous media. etc. DOE) describe research to economically store methane as hydrates that may open many commercial opportunities such as transport of stranded gas. off-peak storage of line gas.3 km depth in the ocean. Flowing HFC-134a gas was mixed with water in a static mixer. A series of surfactants with sodium sulfonic acid groups in common but of different carbon chain lengths (C4. The biosurfactants accumulate and promote hydrate formation on specific mineral surfaces such as sodium montmorillonite. In paper 11. Hydrate formation rates were measured by a batchtype method with a high-pressure vessel made of stainless steel. . The dissolution rate of CO2 hydrate composite in water was also studied. total volume of the SPS. (2007) (National Institute of Advanced Industrial Science and Technology.

In a series of experiments. Various parameters obtained from analysis of the CMT data are presented for all three sediment samples. To date. a large data set from laboratory studies are available for pure methane hydrates for which kinetic models have been proposed but reproducible data collection in the presence of sediments has proved challenging. (2007) (Columbia U. The study describes the applicability of the computed microtomography (CMT) technique that utilizes an intense X-ray synchrotron source to characterize sediment samples. (3) dependence of shear strength on pore space contents. (2007) (USGS) report in paper 14 the interaction of methane gas hydrate with host sediment. thermal perturbations on the sand/water/gas system were performed to form methane hydrate and studied their reverse behavior. of oceanic versus permafrost origins could be significantly different and impact hydrate behavior. The analytical models assume that decomposition happens at a sharp-interface that divides the medium into two regions. pressure reduction propagates from the interface into the hydrate zone. that once contained methane trapped as hydrates. (2) effect of different hydrate formation mechanisms on measured acoustic properties. They consider a semianalytical model of the problem based on local equilibrium and build upon previous studies to understand the effect of various parameters on methane production. etc. These data could help delineate possible range of parameters where methane production could be economically viable. In addition. and transport. Calgary) and 17 by Tsimpanogiannis and Lichtner (2007) (Los Alamos National Laboratory) examine methane hydrate dissociation in porous media caused by thermal stimulation of the system. Methane hydrate was formed and dissociated under various conditions in a large X-ray transparent pressure vessel. While previous studies focused on porous media with relevance to permafrost regions. A number of analytical models have been reported for predicting gas production from gas hydrates. the sharp-interface assumption is not valid and much needs to be learned in the production area. a visualization of the connecting pathways through the pore space of the sediment. porosities. leading to decomposition of the hydrate throughout the hydrate zone. In paper 15. which formed in high gas flux environments. The unit was designed to confine artificial and natural sediments in a pressure vessel and mimic oceanic conditions to study various aspects of hydrate research. several detailed studies have shown that in the presence of a mobile (gas or water) phase in the hydrate cap. and. In order to develop or improve understanding of hydrates under natural environments that may lead to a methane recovery method. can cement coarse-grained sediment. X-ray computed tomography (CT) was used to determine local density changes during the experiment. The authors studied kinetics of methane hydrate formation/decomposition in depleted sediments from a well-studied hydrate site. Under these conditions. the increasing significance of hydrates in oceanic sediments warrants further studies on this aspect. permeabilities. the hydrate zone and the dissociated zone. (2007) (Brookhaven National Laboratory) studied the hydrate–sediment interaction. The last four papers (16–20) present studies to understand hydrate behavior during gas production. The authors studied: (1) the effects of gas hydrate and ice on acoustic velocity in different sediment types. Papers 16 by Gerami and Pooladi–Darvish (2007) (U. The 18th paper by Castaldi et al.) considers natural gas as an excellent fuel for transition to a hydrogen economy. The best fuel for a transition to . However. Winters et al. two at various depths from the Blake Ridge area (a well-known hydrate-prone region) and one from Georges Bank.6 Editorial Papers 12–15 focus on the study of sediment (host)/ hydrate (guest) interactions. whereas hydrate formed from methane dissolved in the pore fluid may not. it is important to be able to mimic natural conditions in a laboratory and study dynamics of methane hydrates in host sediments. (2007) (Brookhaven National Laboratory/Stony Brook University). Sediment properties such as pore-size distributions. while pressure and temperature were monitored. The following paper 13 by Kneafsey et al. Acoustic models based on measured Vp indicate that hydrate. a new experimental apparatus namely FISH (Flexible Integrated Study of Hydrates) is described. A wide range in acoustic p-wave velocities (Vp) were measured in coarse-grained sediment for different pore space occupants. and (4) pore-pressure effects during undrained shear. Detailed results of the tomographic analysis performed on the deepest sample (667 m) from Blake Ridge are presented as 2D and 3D images which show several mineral constituents. The availability of accurate data on the formation/decomposition cycle and acoustic properties of hydrates will aid in developing a much sought after economical method to extract methane from this vast resource. following segmentation into pore and grain space. an important aspect of gas hydrate studies that needs further examination. Jones et al. (2007) (Lawrence Berkeley National Laboratory) focused on a series of experiments to collect data for validating numerical models of gas hydrate behavior in porous media. In paper 12 by Eaton et al. thermodynamics. the internal grain/pore microstructure.

petrol. Gas hydrates and clathrates: Flow assurance. 192–198 (this issue). Open-File Report 96–272.01. Gborigi.C.A.R. Journal of Petroleum Science and Engineering 56.. A novel high-pressure apparatus to study hydrate–sediment interactions. Yegulalp.2005.2005. Riestenberg.. Mahajan.2005.. Gardner. their environmental and economic perspectives with respect to their prospects as storage and transport alternative to the liquefied natural gas (LNG) technology.petrol.005. doi:10.M. C. S. Igwe. Prodanović. H. Resource potential of methane hydrate coming into focus.1753.09. D. K.. J...C. Gas hydrates are also being looked upon as a future energy source in Nigeria.1016/j.. an understanding of which is needed to develop a commercially viable extraction method in the near future. References Booth. Journal of Petroleum Science and Engineering 56. Journal of Petroleum Science and Engineering 56. Walker.. 32–41 (this issue). (2007) (NETL/U. 2007. Journal of Petroleum Science and Engineering 56. 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Laboratory research is accomplished in one of the numerous high-pressure hydrate cells: thermal conductivity of hydrates (synthetic and natural) at temperature and pressure. A. Fischer. Nwokeoma. (2007) (Abia State University. S.O. Gbaruko.029. are hit with multifold increase in a short span of few years. Castaldi. Flood.07. The paper discusses chemistry and mechanism of gas hydrate formation.S. The laboratory results are used in the computational models and the results from the computational modeling is used to help direct future laboratory research. the 20 contributions included in this volume cut across several hydrate R & D areas to give the reader appreciation of the system complexity. In closing.D.. 2000.1016/j. doi:10.012. With its high H/ C ratio. R.S. Yanagisawa. Calculations and simulations using FEMLAB™ show that the method offers an energy efficient and environmental friendly way to produce natural gas from hydrate reservoirs.007. H.J.. doi:10. 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