EP0074394A1 - Nouveaux materiaux carbones et procedes permettant d'obtenir de l'hydrogene et des hydrocarbures legers a partir de ces materiaux - Google Patents

Nouveaux materiaux carbones et procedes permettant d'obtenir de l'hydrogene et des hydrocarbures legers a partir de ces materiaux

Info

Publication number
EP0074394A1
EP0074394A1 EP82901238A EP82901238A EP0074394A1 EP 0074394 A1 EP0074394 A1 EP 0074394A1 EP 82901238 A EP82901238 A EP 82901238A EP 82901238 A EP82901238 A EP 82901238A EP 0074394 A1 EP0074394 A1 EP 0074394A1
Authority
EP
European Patent Office
Prior art keywords
carbon
carbonaceous material
group metal
cobalt
metal component
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP82901238A
Other languages
German (de)
English (en)
Other versions
EP0074394A4 (fr
Inventor
Jack L. Blumenthal
Maksymilian Burk
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Northrop Grumman Space and Mission Systems Corp
Original Assignee
TRW Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by TRW Inc filed Critical TRW Inc
Publication of EP0074394A1 publication Critical patent/EP0074394A1/fr
Publication of EP0074394A4 publication Critical patent/EP0074394A4/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/54—Gasification of granular or pulverulent fuels by the Winkler technique, i.e. by fluidisation
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/54—Gasification of granular or pulverulent fuels by the Winkler technique, i.e. by fluidisation
    • C10J3/56—Apparatus; Plants
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72—Other features
    • C10J3/78—High-pressure apparatus
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2200/00—Details of gasification apparatus
    • C10J2200/06—Catalysts as integral part of gasifiers
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/093—Coal
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0956—Air or oxygen enriched air
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0973—Water
    • C10J2300/0976—Water as steam
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1662—Conversion of synthesis gas to chemicals to methane (SNG)
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/1671—Integration of gasification processes with another plant or parts within the plant with the production of electricity
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/50—Improvements relating to the production of bulk chemicals
    • Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts

Definitions

  • This invention relates to new processes for making hydrogen, oxides of carbon, methane, other light hydrocarbons, and mixtures of two or more of these products by reacting carbonaceous materials comprising carbon, ferrous group metal components, and hydrogen with steam. These processes produce commercially attractive product yields in commercially attractive temperature ranges.
  • the invention also relates to new carbonaceous materials comprising carbon, hydrogen, and ferrous group metal components, particularly nickel and cobalt.
  • new carbonaceous materials comprising carbon, hydrogen, and ferrous group metal components, particularly nickel and cobalt.
  • the methods for making our new carbonaceous materials comprise depositing carbon from carbon monoxide-containing gas mixtures over one or more ferrous group metal initiators.
  • ferrous metal is transferred from the inititor to our carbonaceous material and becomes an integral part of these materials as described above.
  • the ferrous group metal starting materials, called initiators in the deposition reaction to distinguish them from ferro.us group metal components in our new carbonaceous materials can be supported or unsupported ferrous group metals, ores, alloys or mixtures of such species.
  • carbonaceous materials formed at temperatures above about 550oC especially those carbonaceous materials formed above this temperature from cobalt alone or from ferrous group metai components containing at least about 70 percent by weight cobalt, tend to produce substantial quantities of hydrogen in the steam gasification reactions of this invention.
  • the gasification reaction tends to produce hydrogen in large quantities, especially where the carbonaceous material is cobalt-based.
  • the molar ratio of steam fed to carbon gasified is less than about 3, and the steam gasification pressure is in the range of about 10 to about 100 atmospheres, (and therefore nearly equals the amount required for thermodynamic equilibrium)
  • the gasification reaction tends to produce methane in large quantities, especially where the carbonaceous material is nickel-based.
  • the gaseous products initially formed in the steaming reactions of this invention can be converted to gas mixtures richer in hydrocarbons, hydrogen, or both, by lowering the temperature of the gaseous products and contacting these products with either fresh or partially reacted carbonaceous material in the range of about 300°C to about 500oC, and by adjusting the pressure and steam feed rate to produce the desired gases, as explained below.
  • the carbon monoxide-containing gas mixtures used in the deposition processes for making our new carbonaceous materials can be low pressure or high pressure producer or synthesis gases. Such gas mixtures may include substantial quantities of nitrogen and carbon dioxide, but must contain little or no sulfur compounds such as hydrogen sulfide, carbon disulfide or sulfur dioxide. If necessary, carbon monoxide-containing gas mixtures are pretreateo by known methods for removing sulfur-containing gases before carbon deposition begins. Carbon deposition removes some of the carbon from the carbon monoxide-containing gas mixtures at nearly 100 percent thermal efficiency since the heat of reaction may remain as sensible heat in the carbon monoxide- depleted fuel gas stream. The reaction heated, carbon monoxide-depleted gas mixture from the carbon deposition reaction is a good fuel source for generating combined cycle electric power.
  • a surprising and unexpected aspect of our methods for steam gasification of the new carbonaceous materials is that where such carbonaceous materials contain iron as the chief ferrous metal component, such carbonaceous materials have quite low rates of reactivity with steam at temperatures in the range of about 500oC to about 600oC. Steam gasification, of such carbonaceous materials at temperatures above about 700oC is adversely affected by the side reaction of the iron component with steam, ano gasification ceases long before all of the carbon is gasified.
  • our new carbonaceous materials which contain substantial amounts of nickel, cobalt, nickel alloys, cobalt alloys and mixtures thereof, have high reaction rates with steam, and do not suffer from deactivating side reactions.
  • Figure 1 illustrates the range of steam reactivities with several different carbonaceous materials, including those of our invention.
  • Tables 1 and 2 show differences in final product gas composition where the products of steam-carbon gasification of carbonaceous reactants containing different ferrous group metals further react at temperatures below the carbon gasification point of about 500oC.
  • a carbonaceous material comprising about 90 percent carbon and about 9 percent nickel, prepared by carbon deposition on nickel powder, at about 450oC, catalyzed the further conversion of a typical steam-carbon gasification mixture of carbon monoxide, hydrogen and steam at 400oC and about 1 atmosphere pressure in a steady flow reactor.
  • Table 1 shows, nearly ail of the carbon monoxide was converted to methane and carbon dioxide, with very little additional gasification of solid carbon (0.04 gram out of 0.83 gram in 203 minutes).
  • FIG. 3 and Table 3 set forth data obtained from steaming a nickel-based carbonaceous material at 650oC at three different pressures, namely one atmosphere, 4.4 atmospheres, and 7.8, atmospheres. We conducted all these runs in small, fluidized bed, steady flow reactors at a constant steam feed rate of 23 standard cubic centimeters per minute per gram of car ⁇ on initially in the reactor. Figure 3 shows that the carbon gasification rate was nearly linear until substantially ail the carbon was gasified. Moreover, this rate did not vary appreciably with pressure. By contrast, the product composition set forth in Table 3 did change substantially depending on the pressure. As the pressure rose from one atmosphere to 7.8 atmospheres, the methane concentration tripled, the carbon monoxide concentration decreased by a factor of two, the hydrogen concentration decreased from about 53 percent to about 43 percent, and the carbon dioxide concentration rose from about 21 percent to about 31 percent.
  • Figure 4 shows that our new carbonaceous materials can cycle many times between the carbon-rich states entering the steam gasification process of our invention, and the carbon-lean states resulting from the steam gasification processes of our invention.
  • a carbonaceous material comprising about 90 percent carbon and about 9 percent cobalt by depositing carbon from a gas mixture comprising about 85 percent carbon monoxide and about 15 percent hydrogen at 450oC and one atmosphere pressure.
  • Figure 4 shows that the rate of steam gasification did not vary significantly from one cycle to the other.
  • FIG. 9 is a block diagram showing some of the advantages of a preferred embodiment of our new processes for producing methane, or other synthetic natural gas, and electric power, from coal.
  • coal from source 1 passes on path 2 to coal gasification and clean-up zone 3. There, the coal is converted to a gaseous mixture of nitrogen, carbon monoxide, carbon dioxide and hydrogen, and the ash, sulfur and water content of the mixture is reduced to acceptable levels by known methods.
  • One advantage of our processes is that we can make synthetic natural gas by reacting coal with air instead of oxygen. Unlike other synthetic gas manufacturing processes, our processes are compatible with feed stocks containing substantial amounts of nitrogen ana carbon dioxide.
  • the cold, clean product gas then passes along path 4 to carbon deposition zone 5 where formation of our carbonaceous materials Dy deposition over one or more ferrous group metal initiators takes place.
  • Some of the fuel gas may pass along path 6 directly to power generation zone 7, if desired, for combustion with air to generate base load and/or peaking power.
  • Depleted fuel gas passes on path 8 to zone 7 for conversion to power in the same way.
  • Catalytically-active carbon rich carbonaceous material passes on path 9 to steam gasification zone 10 for reaction with steam to produce carbon monoxide, carbon dioxide, hydrogen, methane or possibly other light hydrocarbons, as desired.
  • Carbon lean carbonaceous material is returned on path 11 to carbon deposition zone 5. Nearly all of the heating value of the carbonaceous material can be converted to methane or hydrogen in our steam gasification processes.

Abstract

Des materiaux carbones comprenant des quantites importantes de carbone, et des quantites inferieures d'hydrogene et de composants metalliques du groupe du fer, notamment du nickel et du cobalt, reagissent avec la vapeur a des faibles temperatures, et produisent des quantites interessantes du point de vue commercial de gaz tel que de l'hydrogene, du methane, des oxydes carboniques et d'autres hydrocarbures plus legers.
EP19820901238 1981-03-27 1982-03-11 Nouveaux materiaux carbones et procedes permettant d'obtenir de l'hydrogene et des hydrocarbures legers a partir de ces materiaux. Withdrawn EP0074394A4 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US24859781A 1981-03-27 1981-03-27
US248597 1981-03-27

Publications (2)

Publication Number Publication Date
EP0074394A1 true EP0074394A1 (fr) 1983-03-23
EP0074394A4 EP0074394A4 (fr) 1984-04-04

Family

ID=22939799

Family Applications (1)

Application Number Title Priority Date Filing Date
EP19820901238 Withdrawn EP0074394A4 (fr) 1981-03-27 1982-03-11 Nouveaux materiaux carbones et procedes permettant d'obtenir de l'hydrogene et des hydrocarbures legers a partir de ces materiaux.

Country Status (10)

Country Link
EP (1) EP0074394A4 (fr)
JP (1) JPS58500445A (fr)
BR (1) BR8207244A (fr)
CA (1) CA1197098A (fr)
IL (1) IL65225A (fr)
IT (1) IT1191176B (fr)
NL (1) NL8220132A (fr)
PL (1) PL235658A1 (fr)
WO (1) WO1982003380A1 (fr)
ZA (1) ZA821679B (fr)

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4873214A (en) * 1984-12-24 1989-10-10 Trw Inc. Carbonaceous material for production of hydrogen from low heating value fuel gases
DE3600432A1 (de) * 1985-05-21 1987-02-05 Gutehoffnungshuette Man Verfahren zum vergasen eines kohlenstoffhaltigen brennstoffs, insbesondere kohle
GB8524894D0 (en) * 1985-10-09 1985-11-13 Shell Int Research Producing hydrogen-containing gas
US4756696A (en) * 1985-12-06 1988-07-12 Amp Incorporated Solder joint inspection feature for surface mount connectors
CN102537917A (zh) * 2012-02-02 2012-07-04 王海波 带调温器的锅炉烟气余热回收装置
CN105419897A (zh) * 2015-11-26 2016-03-23 广东拓丰实业有限公司 一种助燃型生物质成型燃料

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2422440A1 (fr) * 1977-07-21 1979-11-09 Trw Inc Matiere carbonee de haute activite et procede pour sa production, ainsi que son application

Family Cites Families (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2686819A (en) * 1949-09-01 1954-08-17 Kellogg M W Co Synthesis of methane
ZA763382B (en) * 1975-06-18 1977-05-25 Battelle Memorial Institute Converting fuels
US4134907A (en) * 1977-07-21 1979-01-16 Hazen Research, Inc. Process for enhancing the fuel value of low BTU gas
US4265868A (en) * 1978-02-08 1981-05-05 Koppers Company, Inc. Production of carbon monoxide by the gasification of carbonaceous materials
US4211669A (en) * 1978-11-09 1980-07-08 Exxon Research & Engineering Co. Process for the production of a chemical synthesis gas from coal
US4242103A (en) * 1979-06-04 1980-12-30 Union Carbide Corporation Cyclic two step process for production of methane from carbon monoxide
US4242104A (en) * 1979-10-09 1980-12-30 Union Carbide Corporation Cyclic process for producing methane with catalyst regeneration
US4284416A (en) * 1979-12-14 1981-08-18 Exxon Research & Engineering Co. Integrated coal drying and steam gasification process

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2422440A1 (fr) * 1977-07-21 1979-11-09 Trw Inc Matiere carbonee de haute activite et procede pour sa production, ainsi que son application

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See also references of WO8203380A1 *

Also Published As

Publication number Publication date
JPH0463913B2 (fr) 1992-10-13
EP0074394A4 (fr) 1984-04-04
IT1191176B (it) 1988-02-24
IL65225A (en) 1985-09-29
WO1982003380A1 (fr) 1982-10-14
ZA821679B (en) 1983-01-26
NL8220132A (nl) 1983-02-01
BR8207244A (pt) 1983-03-01
IT8267385A0 (it) 1982-03-26
CA1197098A (fr) 1985-11-26
PL235658A1 (fr) 1982-11-08
JPS58500445A (ja) 1983-03-24
IL65225A0 (en) 1982-05-31

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Inventor name: BLUMENTHAL, JACK L.

Inventor name: BURK, MAKSYMILIAN