Development of the Shell-Koppers Coal Gasification Process [and Discussion]

Author(s): E. V. Vogt, M. J. Van Der Burgt, J. H. Chesters and J. C. Hoogendoorn

Source: Philosophical Transactions of the Royal Society of London. Series A, Mathematical and
Physical Sciences, Vol. 300, No. 1453, New Coal Chemistry (Mar. 20, 1981), pp. 111-120
Published by: The Royal Society
Stable URL: http://www.jstor.org/stable/36817 .
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Phil. Trans.R. Soc.Lond.A 300, 111-120 (1981)

[ 111 ]

Printed
in GreatBritain

oftheShell-Kopperscoal gasification
Development
process
BY E. V. VOGT AND M. J. VAN DER BURGT
Petroleum
ShellInternationale
Development
MaatschappijB. V., Manufacturing
Division,
Carel van Bylandtlaan30, The Hague, The Netherlands
The Shell-Koppers process for the gasificationof coal under pressure,based on the
principles of entrained-bed technology, is characterized by: practically complete
gasificationof virtuallyall solid fuels; production of a clean gas withoutby-products;
high throughput;high thermal efficiencyand efficientheat recovery; environmental
acceptability.
There are numerouspossible futureapplications forthisprocess. The gas produced
(93-98 vol. % hydrogen and carbon monoxide) is suitable for the manufactureof
hydrogenor reducinggas and, with furtherprocessing,substitutenatural gas (s.n.g.).
Moreover, the gas can be used for the synthesisof ammonia, methanol and liquid
hydrocarbons.
Another possible application of this process is as an integral part of a combinedcycle power stationfeaturingboth gas and steam turbines.The integrationof a ShellKoppers coal gasifierwith a combined-cycle power station will allow of electricity
generation at 42-45 0 efficiencyfora wide range of feed coals.
The development programme includes the operation of a .150 t/day gasifier at
Deutsche Shell's Harburg refinerysince November 1978 and of a 6 t/day pilot plant
a Royal Dutch Shell's Amsterdam laboratories fromDecember 1976 onwards. Both
facilitiesrun very successfully.With hard coal a conversionof 99 % is reached while
producing a gas with only 1 vol. %0 Co2.
The next step will be the constructionand operation of one or two 1000 t/day
prototypeplants which are scheduled forcommissioningin 1983-4. Towards the end
of the 1980s large commercial units with a capacity of 2500 t/day are contemplated.
The economy, especially of these large size units,is very competitive.
DEVELOPMENT

OF THE

SHELL-KOPPERS

PROCESS

Sbell Internationale Petroleum Maatschappij B.V., The Hague, and Krupp-Koppers GmbH
(formerlyHeinrich Koppers GmbH), Essen, have togetherbeen workingon the development
of a high-pressurecoal gasificationprocess since the beginningof 1974. A pilot plant of 6 t/day
intake capacity has been in operation at Shell's AmsterdamLaboratories since December 1976.
As part of this development, Deutsche Shell A.G. decided to set up an experimental plant
employingthis process.
The development of thislarge pilot plant, with a daily throughputof 150 t of coal, drew on
the existingexperience of the two associates in the venture. On the one hand, there was the
experience of Krupp-Koppers, who have built numerous coal gasificationplants employing
the Koppers-Totzek process, workingat atmospheric pressure,and on the other hand there
was Shell's experience obtained fromthe Shell oil gasificationprocess, a high-pressureprocess
also employed in many units operating around the world.
The Shell-Koppers 150 t/day pilot plant has made a series of very successfulruns since its
commissioningin November 1978. The longest run to date has been 240 h.
Although the plant has been built by Krupp-Koppers in cooperation with Shell process and
project engineersin The Hague and Harburg, it is the propertyof Deutsche Shell A.G. and
is operated by that company. The capital and operating costs are expected to approach $50M.

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112

E. V. VOGT

AND

MI.J. VAN

DER

BURGT

with the pilot plants, designs are being nmadeforone or two 1000
Based oIn the ex-perieince
t/day prototype units whlich.are schieduledfor commissioniilgin I 983-4. The capacities of
subsequent fullycomnmeicialuIlitswill be increased in stages to about 2500 t/day towards the
end of the 1980s.
THE

PROCESS

The Inewvprocess is based on the principle of entrained-bedgasificationat elevated pressure

higlhto ensure that the ash is in the
under slagging coinditions(i.e. at temperaturessufficiently
molten state). Thie main teclhnicalfeaturesof the process are described below.
Coal conversion

Processfeatures

The processis suitable forthe complete gasificationof a wide varietyof solid fuels,such as all
typesof coal and petroleumcoke. Fuels with a high ash content (up to 400 by mass) and high
sulplhurcontent (up to 8 0/' by mass) can be used in the Shell-Koppers gasificationplant without any trouble. Even a high water content in the coal does not pose a technical problem.
However, on economic grounds,particularlywith a view to reducing the oxygen requirement
and improvingthe quality of the gas, the coal is in most cases dried to a moisturecontentof
1-8 ?. by mass.
Since the process requires a solid fuel to be in dust formforgasification,the entireoutput of
a mine, including fines,is acceptable as feed. Unlike fixed-bedor fluidized-bedprocesses,in
the Shell-Koppers processthereis practicallyno limitationon the coal as to ash fusionbehaviour
or caking properties.
A new developmentin hand is the gasificationof vacuum residuesof direct coal liquefaction
plants and other hydrocarbonliquids in a Shell-Koppers type reactor. An advantage of such
a process over the Shell gasificationprocess foroil is that liquids containing unconvertedcoal
and a high percentage of ash can be gasified.
Gas quality
The operation at very high temperaturesensures the formationof a high-qualitysynthesis
gas essentiallyconsistingof hydrogenand carbon monoxide (93-98 vol. 0o foroxygengasification). Tars, phenols and other by-productsare absent; as a rule methaneconcentrationsin the
gas do not exceed 0.2 vol. 00.
Unitcapacity
Both the high temperatures(above 1400 ?C) and the high pressuresare responsibleforthe
high capacities attainable. Short-termtargetsare 50-100 t/h coal per reactor, corresponding
to 2.4-4.8 x 106 m3/day (at s.t.p.) of raw gas.
Depending on the application, the optimum pressurelevel can be selected. Apart fromthe
beneficial effectof the elevated pressure on reactor capacity, there are spin-offsin termsof
increased hleattransferrates in the waste heat boiler, easier gas treatingand a reductionin gas
compressioncosts.
Thermalefficiency
The chemically bound heat in the gas produced with oxygen gasificationis equivalent to
about 79-820?o of the chemically bound heat contained in the coal feed. The recoveryo;fthe

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THE

SHELL-KOPPERS

PROCESS

113

sensible heat fromthe hot gases leaving the reactor accounts for another 12-15 % of the heat
contentof the coal feed. The surplus steam produced by this cooling is generally sufficientto
drive the compressorsof the oxygen plant.
Heat losses to atmosphere are reduced to a minimum. The combined operation of reactor
cooling systemand waste heat boiler resultsin an efficientheat recoveryby the production of
superheated high-pressuresteam (typically540 ?C, 10 MPa).
Environmental
acceptability
A negligible environmentalimpact can be expected from the Shell-Koppers process. The
requirementsforboth process and cooling water have been minimized in both the gasification
and the solids removal sections. The gas produced contains no tars, phenols, condensable
hydrocarbonsor organic sulphur compounds. Physical and chemical means are available for
removinghydrogensulphide and traces of cyanide, carbonyl sulphide and ammonia fromthe
synthesisgas. The only by-productsfromthe process are elementalsulphurand the unavoidable
ash fromthe coal as a non-leachable and inert slag. Depending on the application, the production of waste water is very low or nil.
Flow schemeof the150 t/daypilotplant in Harburg,Germany(figure 1)
Coal is ground and dried to specificationin a coal mill and subsequently pneumatically
transportedto the atmospheric cyclone hoppers (2). In the Harburg plant nitrogenfrom a
liquid nitrogenstorage vessel is used as a carrier gas for the coal. To transportthe coal from

17

9
pulverized
coal

rwa

10wga

b.f.w.

_____

~~~~~~~~~~~steam

6
3

.0

11

16

water
~~~~~~~~~~~~recycle

15
~~~~~~~14

4
12

b7

q13

recycle water

to-filter
ash
slag

1. Shell-Koppers coal gasification process: flow scheme, 150 t/day Harburg pilot plant. 1, Coal filter;
2, cyclone hopper; 3, lock hopper; 4, feed hopper; 5, gasifier; 6,,waste heat boiler; 7, slag breaker; 8, slag
lock hopper; 9, steam drum; 10, b.f.w. preheater; 11, cyclone; 12, ash hopper; 13, ash lock hopper; 14,
venturi; 15, scrubber; 16, h.p. separator; 17, recycle gas compressor.

FIGURE

the cyclone hoppers (2) to the nitrogenpressurized feed hoppers (4) a fullyautomated lock
hopper systemis used. The pneumatic transportof the coal from the feed hoppers to the
burnersis again accomplished with nitrogen.For good control of the process it is essential to
8

Vol. 300.

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114

E. V. VOGT

AND

M.J. VAN

DER

BURGT

be able to measure accurately the coal, oxygen and steam flow to the burners.The success of
the pneumatic feed systemhas been made possible by the development of an accurate and
dependable coal flowmeter.
The reactor is equipped with two diametricallyopposed burnersand consistsessentiallyof
a pressureshell protectedfromthe hot gases by a tube wall in which saturated steam at 5 MPa
is raised. The tube wall is in turn protected by a thin layer of a refractorymaterial. The slag,
which leaves the reactorvia a hole in the bottom,is quenched in water,crushedin a submerged
mill and then lock-hopperedout to atmosphericpressure.
The gases leaving the reactor at about 1500 ?C and 3 MPa are quenched with solid free
recycled synthesisgas of 100 to 800-900 ?C to solidifythe entrained slag particles beforethey
enter the waste heat boiler (6). The gases leave the waste heat boiler at a temperatureof
320 'C. In the waste heat boiler superheated steam at 500 'C and 5 MPa is raised. The waste
heat boiler and the reactor tube wall have a common forcedcirculationsystem.Some 900 of
the solids in the gas are separated in the cyclone (1 1). The remainderof the solids are washed
out with water in a seriesof scrubbersand separators (14, 15, 16) afterthe gas has been further
cooled in two economizers (10). The gas leaving the scrubbershas a solid contentof 1 mg/M3
at s.t.p. and a temperatureof 40 'C.
At present the solids in the circulatingwater used in the scrubbersare removed in a filter.
In futuretheywill be concentratedin a slurry,which will be reinjectedupstreamof the cyclone
(11). The water will then evaporate and all solids leaving the waste heat boiler will eventually
be separated in the cyclone, thus eliminating filtration.This system has already run very
successfullyin our 6 t/day pilot plant at our Amsterdam Laboratories.
Improvements
Apart fromthe recirculationof the solids containingwater, the followingimprovementsare
currentlybeing considered:
(1) recirculationof the solids fromthe cyclone back to the gasifierleading to the situation
that in the end all ash enteringthe reactor leaves the systemin the formof inertnon-leaching
slag;
(2) pressurizingthe lock hoppers and transportingthe coal with syngasinstead of nitrogen,
thus avoiding dilution of the gas with nitrogen;
(3) development of a non-cooled insulated brick-linedreactor;
(4) development of a water quench for applications in which a substantialpart of the CO
in the gas must be used to produce hydrogenby the shiftreaction.
Removalof acid gases
The cooled gas, thus treated,still contains sulphur compounds, which have to be removed.
The process used for their removal will depend on the particular application of the gas produced. Units for the removal of H2S, COS and, if necessary, C02, employing various processes, can be hooked up to the Shell-Koppers gasificationplant. Where the gas is to be used
as fuelor in combined cycle electricitygeneration,the residual sulphurcontentmustbe brought
dowii to whatever levels are demanded by environmentalregulationsforgaseous fuels.
Where the gas is to be used in gas turbinesit is desirable not to remove CO2, as its presence
turbine power outputs.
imnproves

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THE SHELL-KOPPERS

PROCESS

115

Blast requirements,
product
gas and thermal
efficiency
Oxygen and steam consumptions are dependent on coal feedstock quality. An oxygen
demand of 0.9-1.0 t per tonne of moisture and ash-free(m.a.f.) coal is fairlytypical of hard
coals; forlow-rankcoals a figureof 0.8 t oxygenper tonne of m.a.f. coal is more representative.
The steam requirementis very low and, in fact, is almost zero for some brown coals and in
cases where air is used as a gasifyingagent. For hard coal it is of the order of 8 ?O on m.a.f. coal.
The raw gas production is about 2000 m3/tfor a good-quality bituminous coal. The gas is
relativelyrich in carbon monoxide and the CO:H2 ratio, on a volume basis, is typicallybetween 1.8 and 2.2 forthe preferredoperation at minimum steam dosage and with recycle gas
as a quenching medium. When water is used to quench the hot gases the CO: H2 ratio of the
gas will be somewhat lower.
The heat contentof the gas is of the order of 11.3 MJ/m3 at s.t.p. The thermalefficiencyof
the gasificationproper is about 820 foroxygen-steamgasification.Apart fromthispercentage
of the total heat in the coal that is recovered as chemical heat in the gas, about 15 ?hof the
heat in the coal to the gasifierbecomes available forsteam-raisingin the waste heat boiler via
the sensible heat in the gas.

coal in: 100%

1.75%reactorheat
to slag
waste heat
14.5% boiler
N

unconverted

coolerin
0.75% solids
82.5%

FIGURE

recovery

raw synthesisgas
2. Shell-Kopperscoal gasification
process:typicallheatbalance of gasifierproper.

The total lheatcontent of syntlhesis

gas and steam representsapprox. 94-97 0.!/0 of the lieat
content of the coal feed (see figure2). It is, howvever,more realistic to coinsiderthoeoverall
thermnal
efficiency,takinginto account the energyconsumptioniof oxygen plant, coal mill and
dryer,coal gasifierand auxiliary equipment. This overall thermnal
efficiencv,calctulatedon a
lower lheatiing
value basis, correspondsto approx. 780% for alaard coal conltaiiniiig 1?2o ash
and 7 00 moisture.

8-2

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AND M.J. VAN DER BURGT

E. V. VOGT

116

COAL

QUALITY

To demonstratethe versatilityof the Shell/Koppers gasificationprocess with regard to feed

has been calculated fora range ofcoals, namely: bituminous
coal quality, the thermalefficiency
ash
and moisturecontent (Illinois no. 6); sub-bituminouscoal (Wyodak);
coal with moderate
coal liquefactionvacuum bottoms; brown coal, high moisture,low ash (German brown coal).
These feedstockscover a fairlywide range of ash and moisturecontents.The calorificvalues,
correspondingly,range from 10 to 29 GJ/tas received coal (table 1).
TABLE

COAL

1. SIIELL-KoPPERS

COAL

GASIFICATION:

FEED

ANALYSES

Wyodak
sub-bituminous

coal
liquefaction
vacuum
bottoms

Gerrman
brown coal

78.1
5.5
10.9
4.3
1.2

75.6
6.0
16.8
0.9
0.7

87.1
5.7
3.3
2.4
1.5

67.5
5.0
26.5
0.5
0.5

ash (mass % as received)

moisture (mass 0 as received)
moisture (mass 00 of coal to gasifier)

12.0
6.5
2.0

5.9
35.0
2.0

17.6
0
0

6.4
5.0
5.0

lower heating value of coal as received/(GJ/t)

25.80

17.16

29.41

9.99

carbon (mass
hydrogen
oxygen
sulphur
nitrogen

TABLE

2.

Illinois
no. 6
bituminous

% m.a.f.)

COAL

SHELL-KOPPERS

DIFFERENT

COALS

(TONNES

GASIFICATION:

PER MILLION

constant plant capacity

coal intake as received
coal to gasifier
oxygen demand (vol. 990% pure)
steam demand
thermal efficiency(%) (l.h.v. basis) gasifier
proper
overall plant after subtraction of own
consumption
TABLE

COAL

3. SIIELL-KoPPERS

COAL,

CUBIC

component

1.5

H20

31.6

H2

64.0

CO

CO2
CG4

0.8

H2S + COS

1.4

N92

0.'5

Ar

0.2

METRES

AND

STEAM

REQUIREMENTS

CO + H2 PRODUCED

coal
liquefaction
vacuum
bottoms

Wyodak
sub-bituminous

573
477
400
36

810
489
395
12

494
494
407
86

1364
626
434
20

83

83

83

79

78

77

77

72

GASIFICATION:

WET

SYNTHESIS

Wyodak
sub-bituminous

coal
liquefactions
vacuum
bottoms

2.6

2.1

32.5

33.6

62.8
1.3

0.3
0.3
0.2

German
brown coal

GAS COMPOSITION

BY VOLUME)

German
brown coal

61.8
1.0

0.1

11.3
26.9

55.0

6(.1

0.7

0.2

0.2

0.2

0.5

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0.3

FOR

(AT S.T.P.))

Illinois
no. 6
bituminous

(PERCENTAGES

Illinois
no. 6
bituminous

OXYGEN

THE

PROCESS

SHELL-KOPPERS

117

Tlle data presentedin table 2 are indicative oftheoxygenand steam consumptions,and ofthe
overall thermal efficienciesforthe coal feedstocksspecified.Assuminga constantproduction of
synthesisgas (CO + H2), it is evident that the amount of coal to be processed increases as the
rank, and correspondinglythe heating value, of the coal goes down and as moistureand ash
contentsgo up. Variations in oxygen demand are generally well below 10?/ for the various
feedstocks.
Some details of the gas composition are given in table 3. Hydrogen to carbon monoxide
ratios are not materiallyaffectedby a change in coal feed composition.At CO2 concentrations
not exceeding 5 vol. 00, as shown in table 3, the selective removal of H2S does not normally
presenta problem. Typical CO2 concentrationsare below 2 vol. 0/.
RESULTS

OF

EXPERIMENTS

IN

TIIE

150 t/day

PILOT

PLANT

The plant is at presentin the trial phase in which it is aimed to demonstratethe feasibility
of the various systems.So far the uniithas run fora total of 300 h at pressuresof 1.8-2.0 MPa.
Difficultieshave been experienced with the lock hopper system,but these have now been overcome. Further,there have been problems with foulingof the waste heat boiler. Operation of
the coal transportand flow measuring system,the burners,the reactor and the quench have
been very satisfactory.
OPTIONS

FOR

PROCESS

UTILIZATION

It is a matterofprocessoptimizationto assessforeach project the mosteconomic combination

of heat recovery,power generationand treatingtemperaturesin accordance with the econornic
factors prevailing. An important alternative to the base case is air-blown gasification. This
version is primarilyof interestfor use in situationswhere coal gasificationis integratedwith
combined-cyclepower generation. It could also be considered as a means of producing lowenergyfuel gas forindustrialapplications. Some examples of Shell-Koppers process utilization
are brieflyreviewed below.
Production
of CO-richgasforfuel gas, chemicalsynthesis
and directorereduction
Oxygen-blown gasification with the use of a gas quench (see figure 3 for flow scheme),
coupled to a processforthe removal of sulphurcompounds and carbon dioxide, produces a dry
gas typicallyconsistingof some 30-34 vol. 00 H2, 62-64 vol. 00 CO and a small volume percentage of inerts.The gas as such is very suitable forindustrialheating. The use of coke as a
feedstockand the use of CO2 as a moderator instead of steam will result in gases with a CO
content of 80 vol. 00 and higher.
Production
of hydrogen
or hydrogen-rich
gasfor ammonia,methanol
and Fischer-Tropschtype
synthesis
As shown in figure4, the most common option is to use a water quench and to apply a
CO-shift conversion with a sulphur-tolerantcatalyst followed by selective H2S and CO2
removal.
Production
of methane
(s.n.g.)
The raw gas can be converted into methane by the same process route as described above
forhydrogen-richgas followed by methanation and drying.The diseconomy of the absence of

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118

E. V. VOGT

AND M.J. VAN DER BURGT

gas quench

ew Shl
_ Koppers
steam _ gasifier _,

waste|
heat
boiler

old
removal

|HS|
removal

fuelgas

ash
char
FIGURE 3.

Shell-Kopperscoal gasification
process:typicalblockschemeforfuelgas production.
water
forquenching

steam _gasifier

bole

H2S+CO2

COemoval

hydrogen
or synthesisgas

rectisol or
Sulfinol+MDEA

FIGURE

1t
nt~~~ash
char
s]lag
4. Shell-Kopperscoal gasification
process:typicalblockschemeforhydrogenor synthesis
gas production.

methane in the raw gas, an ostensibledrawback of the Shell-Koppers process in the manufacture of s.n.g., is largely outweighed by the relative simplicityof the processingof the gas.
Integration
of theShell-Koppers
processwithcombined-cycle
powergeneration
The integrationof the Shell-Koppers coal gasificationprocess and electricitygenerationin a
gas-turbine-steam-turbinecycle offersan efficientand environmentallyacceptable means of
meetingfutureenergyrequirements.
The process lends itselfto the full utilization of the high efficiencyof gas turbineswith high
inlet temperatures,owing to the high proportionof electricitygenerated in the gas turbine,
namely up to 600% in an advanced scheme (see, for example, figure5). At the same time an
efficientsteam cycle can be maintained by the production of high-qualitysteam in the waste
heat boiler of the gasifier.
The particulate-freepressurizedfuel gas produced in the gasifieris a low-medium-energy
fuel gas which gives a low production of NO, in the gas turbinecombustor.
Both the air-blown and the oxygen-blownversionsof the Shell-Koppers process can be used
of 42-45 00 forgas turbineswithinlet temperatures
at approximatelythe same stationefficiency
of about 1200 0C, which are expected to be available in the mid-1980s.
ECONOMICS
The investmentfor a gas plant to synthesize36 x 106 m3/day (at s.t.p.), based on U.S.
location in mid-1979, is estimated at $793M. This figureapplies to the processingof a hard

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THE

119

PROCESS

SHELL-KOPPERS

steam turbine

|f
coal
coa

Shell waste
heat
Kop.pers _-

_andsolids
H2S

stack

_combus-

gas turbine

compressor
FIGURE

lue gas
to

5. Shell-Koppers coal gasification process plant; combined cycle power.

indirect gasoline

synthesis

_directgasoline
synthesis

medium-energy

gas

coal costs/($/(J)
FIGURE

6. Shell-Koppers coal gasification: coal conversion costs; economics for various applications.

Basis: Illinois, U.S.A.;

dollar values at mid-1979.

coal containing 100 0 ash and 10 0 moisture,and includes the investmentof coal handling and
storage,coal mill and dryer,oxygen plant, water treatment,ash disposal facilitiesand off-sites.
Excluded is the investmentin plants for the furtherprocessing of the dry, particulate and
sulphur-freesynlthesisgas. The correspondingcost of the synthesis gas before and after

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120

E. V. VOGT

AND

M.J. VAN

DER

BURGT

conversioninto methylfuel, and subsequentlyto gasoline on a heating value basis, is shown as

a functionof the coal feed unit cost in figure6. For a low-costcoal feed,as would be available
from open-cast mining of large coal reserves,the synthesisgas cost would amount to some
$2.8/GJ. For deep-mined coal, as available in Europe, the cost could be as high as $4.7/GJ.
The correspondingfiguresformethylfuel are $6.2 and $9.0/GJ and forgasoline $5.7-7.6 and
$8.5-10.4/GJ respectively.The economics of Shell-Koppers coal gasificationare only marginally affectedby variations in coal rank, ash contentor moisturecontent. Only the costs of the
coal mill and dryerand of the ash disposal facilitiesare significantly
influenced,but thesehave
a minor impact on the overall economics.
Discussion
on Energy).The enthusiasm and clarity with
J. H. CHESTERS(Chairmanof the WattCommission
which the last three papers have been presented makes the production of oil fromcoal seem
rather easy, and freeof serious developmentproblems apart fromscaling-up.
I know, however, that certain plants have experienced trouble owing to the abrasion of
refractoriesby high-velocitydust-laden gases - sufficientindeed, to put certain sectionsout of
were of the typesuccessfullyemployed
commissionin days ratherthan years. As the refractories
in catalytic crackersand were installed with great care, I should like to ask whetherany of the
speakers have experienced such troubles,and if so how theyovercame them.

J. C. HOOGENDOORN.In the Fischer-Tropsch process for production of liquid fuels from

synthesisgas made by Lurgi pressure gasification,only minor use is made of refractoriesin
some of the process steps (furnaces,etc.) but these are normal standard applications that pose
no specificproblems.
M. J. VAN DER BURGT. At Shell, in the 150 t/daypilot plant in Harburg, Germany,no abrasion
problems were experienced during 750 h of operation.

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