US3904387A - Fuel gas manufacture - Google Patents

Fuel gas manufacture Download PDF

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Publication number
US3904387A
US3904387A US500817A US50081774A US3904387A US 3904387 A US3904387 A US 3904387A US 500817 A US500817 A US 500817A US 50081774 A US50081774 A US 50081774A US 3904387 A US3904387 A US 3904387A
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United States
Prior art keywords
sulfur
process according
gasifying
gaseous mixture
carbonaceous matter
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.)
Expired - Lifetime
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US500817A
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English (en)
Inventor
Norbert J Kertamus
Warnie L Sage
Mark A Paisley
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.)
Babcock and Wilcox Co
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Babcock and Wilcox Co
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Publication date
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Priority to US500817A priority Critical patent/US3904387A/en
Priority to CA222,596A priority patent/CA1038165A/fr
Application granted granted Critical
Publication of US3904387A publication Critical patent/US3904387A/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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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
    • 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
    • C10J3/02—Fixed-bed gasification of lump fuel
    • C10J3/06—Continuous processes
    • C10J3/14—Continuous processes using gaseous heat-carriers
    • 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
    • C10J3/02—Fixed-bed gasification of lump fuel
    • C10J3/20—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
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/48—Apparatus; Plants
    • C10J3/482—Gasifiers with stationary fluidised bed
    • 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
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72—Other features
    • C10J3/82—Gas withdrawal means
    • C10J3/84—Gas withdrawal means with means for removing dust or tar from the gas
    • 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
    • C10J2300/0943—Coke
    • 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
    • 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
    • C10J2300/0983—Additives
    • C10J2300/0993—Inert particles, e.g. as heat exchange medium in a fluidized or moving bed, heat carriers, sand
    • 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
    • C10J2300/1603—Integration of gasification processes with another plant or parts within the plant with gas treatment
    • C10J2300/1606—Combustion processes
    • 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
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1807—Recycle loops, e.g. gas, solids, heating medium, water

Definitions

  • the present invention relates to gasification and more particularly to a continuous process for yielding a combustible gas from the gasification of char or coke.
  • coal as a fuel in electric generating power plants has been on a decline in recent years due to enviwith heated gaseous sulfur dioxide to produce a gaseous mixture of carbon monoxide and elemental sulfur. Entrained solids are removed from the gaseous mixture and the latter is cooled through indirect heat exchange so as to condense the sulfurthereby leaving a gas comprised primarily of carbon monoxide and having the prerequisite heat value to qualify as a fuel.
  • the condensed sulfur is burned in the presence of heated air to produce a gaseous mixture of sulfur dioxide and nitrogen which is then passed through a conventional sulfur dioxide recovery system to effect separation of the nitrogen and sulfur dioxide, the latter is then heated preparatory to use as the gasifying agent.
  • Oxygen from a separate source, may be added during the sulfur dioxide heating stage in the event that the gasification temperature drops below the level required ronmental constraints which rendered the conversion of coal to electricity uneconomieal. Since coal is by far the most abundant of all fossil fuel reserves, the development of a process for producing clean fuel gas from coal or its by-products would reduce our dependence on natural gas and oil while providing an economical fuel capable of meeting the new environmental standards.
  • the upper temperature level during gasification is of prime concern due to reaction rates or kinetics.
  • the present invention relates to processes for obtaining carbon monoxide fuel gas from the reaction of gaseous sulfur dioxide with char or coke.
  • An alternate embodiment of the invention dispenses with the need for a separate source of oxygen by pro-' trioxide, the latter is then heated to a temperature level causing the dissociation of sulfur trioxide into oxygen enriched sulfur dioxide to be used as the gasifying agent.
  • FIG. I is a schematic representation of a system embodying the invention as related to a process for yielding a combustible gas from the gasification of char or coke..
  • FIG. 2 is a schematic representation of an alternate system embodying the invention.
  • FIGS. 1 and 2 are schematic illustrations of systems which are related to processes whereby sulfur dioxide is used to gasify carbonaceous matter to yield a combustible'fuel gas.
  • hot carbonaceous matter 12 is supplied to a gasifier 14 to be contacted therein by a heated continuous stream 16 of concentrated sulfur dioxide.
  • the carbonaceous matter 12 must contain less than 1%, by weight, of hydrogen C and is either char derived from a conventional gasification process or coke such as that used for various met allurgical processes.
  • the sulfur dioxide reacts with the char or coke to produce a gaseous mixture 18 of carbon monoxide and elemental sulfur.
  • the ehar'or coke contained within the gasifi er '14 may be either in a fixed or fluidized state the latter condition being maintained by theflowing stream of heated sulfur dioxide. 7 1 I I
  • the gaseous mixture 18 is conveyed from the gasifier 14 to a gas-solids separator for the removal of ungasifled particulates 22.
  • Th e gas-solids separator, 20 is one of many presently known in the art, for example. a mechani cal or bed-filjteritype separator. g,
  • the Substantially solids-free gaseous mixture 24 of carbon monoxide and elemental sulfurexiting from the separator 2i) is conveyed to a sulfur condenser which is a known indirect type heat exchanger. for example, a shell and tube heat exchanger. preferably one having the gaseous mixture 24 flowing through th'ef tubes and the enteringcoolant 28 passing ov er th'e tubes. and exiting as shownby 28A.
  • the heat ex changer paramcf c'rs are such that the'gaseous mixture" 24; Within the condenser 26, maintained afacontrolled temperature in the ran ge' of 280F to 3 l'5F to dissociate the carbon monoxide and elemental sulfur as follows: i l
  • Thejco n ibustible fuel gas 30 produced in a 'c'cordanc'e with the present invention has a carbon monoxide content in the range of 95to l()%and a heatvalu ein ex cess' 'c'wf-3 00'Btu/scf.
  • The'fuel gas 30 leaving thc coh: denser 26 is a'high quality clean gas which m; beuscd as fuelin a second-stage combustioii' device oras a feed gas for petrochemical applications.
  • the elemental sulfur contained within the gaseous mixture 24 is liquified in the condenscrZQand is thereafter conveyed as liquid sulfur 32 to a sulfur burner 34 and associated combustion chamber 36 of a type known inthe'artffor example.
  • the burner and combustion chamber disclosed -in'U.S. Pat. No. -3,723.068 is-" sued on Mar. 27. 1973, in the name of R. A. Mcllroy' et al.
  • the liquidsulfur 32* is entrained by a regulated quantity of heated air 38 and burned to producea'gaseous mixture of sulfur dioxide a nd nitrogen as follolvs: V 1..
  • thecooled gaseous mixture 40A exiting from the fluid heater 42, is conveyed to a sulfur dioxide concentrator 50 wherein the nitrogen 52 is removed thereby leaving a concentrated gaseous stream 16A containing in excess of 99% of sulfur dioxide.
  • the concentrator 50 is of a typeknown in the art. for example. the recovery. system disclosed in US. Pat. No. 3.758.668 issued on Sept. 1 l, l973'.- in the name of Lapple et al, and which employs a slurry, containing magnesium oxide, to absorb the sulfur dioxidefrom the gaseous mixture 40A.
  • magnesium sulfide crystals which are thereafter separated from the slurry and heatcdto reduce the water of crystallization, and arepelletized with carbon and a binder to form pellets which are thermally treated for dissociation into reactive -magnesium oxide particles and gaseous sulfur dioxide, the former being returned to the absorption zone of the recovery system.
  • the gaseous stream 16A, of sulfur dioxide, exiting from the concentrator 50 is routed to-.:the lower chamber 46of fluid heater'42. to be heatedby the refractory particles circulating therethrpugh
  • the heated gaseous stream 16 of sulfur dioxide leaving the lower chamber 46 isconveyed to the gasifierlfifor the manufacture of combustible fuel gas.
  • Aaseparate source 54 of nitro-; gen-freeoxygen is available to supply a regulated quan-. tity of oxygen 56.to the lower chamber 4 6 for oxygen enrichment of the gaseous strcamvlfi of sulfur dioxide; whenever-required, to maintainthe temperature necessary for sustained reaction withinv the gasifier 14.
  • Themcatalytie oxidation stage takes place at .areaction temperature of less than 1800F. usuallyjin the range of 70091 10 850F and is expressed as follows:-' t
  • the gaseous mixture 6 4, .exitingfrom..the catalytic oxidizer 62, may contain up to 85% diluent nitrogen with sulfur trioxide.
  • Thc gaseousmixture 654 is fed-to a sulfur trioxide concentrator 66 for theseparation of ni trog en 8 and concentrated sulfur trioxide 70.
  • The, separation stage is" effected by, using highly concentrated sulfurieacid to scrub outthe sulfur trioxide thereby obtaining sulfur trij'oxidc, enriched sulfuric acid, the latter is then conveyed fto an evaporator.which gasifics the sulfur trioxide.
  • the gaseous stream 70 of sulfur trioxide. exiting from the concentrator (viris routed to thelowc'r chamber 46 of fluid heater 42 to be heated by the refractory particles circulating there'through.
  • the heat, supplied in chamber 46 is at a jt'emperaturelin..excessof 18003 thereby decomposing the gaseous sulfur trioxide to 0xygen enriched sulfur dioxide.as expressed belowp so-i so. v. 0.
  • the heated gaseous stream 16 of sulfur dioxide cnrichcd with up to 33% oxygen is conveyed to the gasifier 14 for the manufacture of combustible fuel gas.
  • a process for converting hot carbonaceous matter to gaseous fuel comprised primarily of carbon monoxide. and including the steps of:
  • step of gasifying the carbonaceous matter comprises gasifying char.
  • step of gasifying the carbonaceous matter comprises gasifying coke.
  • step of fluidizing said carbonaceous matter comprises fluidizing with heated gaseous sulfur oxides.
  • step of thermally reacting the condensed sulfur in the presence of air includes burning the sulfur to produce a gaseous mixture of sulfur dioxide and nitrogen.
  • step of heating the gaseous sulfur oxides includes decomposing sulfur trioxide to sulfur dioxide and oxygen.
  • step of gasifying the carbonaceous matter comprises gasifying carbonaceous matter having less than one percent by weight of hydrogen.
  • step of heating the sulfur oxides comprises heating said sulfur oxides to a temperature in excess of 1800F.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Industrial Gases (AREA)
US500817A 1974-08-26 1974-08-26 Fuel gas manufacture Expired - Lifetime US3904387A (en)

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US500817A US3904387A (en) 1974-08-26 1974-08-26 Fuel gas manufacture
CA222,596A CA1038165A (fr) 1974-08-26 1975-03-18 Procede de fabrication de gaz combustible

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Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4396594A (en) * 1981-12-28 1983-08-02 Rockwell International Corporation Sulfur dioxide reduction process
US4483693A (en) * 1974-11-20 1984-11-20 The Ralph M. Parsons Co. Reforming of hydrocarbons in the presence of sulfur
EP0400836A1 (fr) * 1989-05-24 1990-12-05 Florida Institute Of Phosphate Research Centrale thermique à charbon avec contrôle de la pollution et sous produits utilisables
US5686056A (en) * 1996-02-05 1997-11-11 Bechtel Group, Inc. Methods and apparatus for purifying hydrogen sulfide
US6024932A (en) * 1993-05-11 2000-02-15 Gas Research Institute Method for the conversion of gypsum to elemental sulfur
US20100284899A1 (en) * 2009-05-11 2010-11-11 Dieter Kita Generation of sulfur trioxide and sulfuric acid
US20110033370A1 (en) * 2009-08-05 2011-02-10 General Electric Company System and method for sulfur recovery
US9802153B2 (en) 2016-03-04 2017-10-31 Bogdan Wojak Sulphur-assisted carbon capture and utilization (CCU) methods and systems

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3745109A (en) * 1970-10-01 1973-07-10 North American Rockwell Hydrocarbon conversion process
US3840354A (en) * 1972-03-23 1974-10-08 Us Interior Three-stage gasification of coal
US3870480A (en) * 1971-03-19 1975-03-11 Exxon Research Engineering Co Process and apparatus for the production of combustible gases

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3745109A (en) * 1970-10-01 1973-07-10 North American Rockwell Hydrocarbon conversion process
US3870480A (en) * 1971-03-19 1975-03-11 Exxon Research Engineering Co Process and apparatus for the production of combustible gases
US3840354A (en) * 1972-03-23 1974-10-08 Us Interior Three-stage gasification of coal

Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4483693A (en) * 1974-11-20 1984-11-20 The Ralph M. Parsons Co. Reforming of hydrocarbons in the presence of sulfur
US4396594A (en) * 1981-12-28 1983-08-02 Rockwell International Corporation Sulfur dioxide reduction process
EP0400836A1 (fr) * 1989-05-24 1990-12-05 Florida Institute Of Phosphate Research Centrale thermique à charbon avec contrôle de la pollution et sous produits utilisables
US6024932A (en) * 1993-05-11 2000-02-15 Gas Research Institute Method for the conversion of gypsum to elemental sulfur
US5686056A (en) * 1996-02-05 1997-11-11 Bechtel Group, Inc. Methods and apparatus for purifying hydrogen sulfide
US20100284899A1 (en) * 2009-05-11 2010-11-11 Dieter Kita Generation of sulfur trioxide and sulfuric acid
US8052949B2 (en) * 2009-05-11 2011-11-08 Thermo Fisher Scientific Inc. Generation of sulfur trioxide and sulfuric acid
US8679435B2 (en) 2009-05-11 2014-03-25 Thermo Fisher Scientific Inc. Generation of sulfur trioxide and sulfuric acid
US20110033370A1 (en) * 2009-08-05 2011-02-10 General Electric Company System and method for sulfur recovery
US7901646B2 (en) * 2009-08-05 2011-03-08 General Electric Company System and method for sulfur recovery
US9802153B2 (en) 2016-03-04 2017-10-31 Bogdan Wojak Sulphur-assisted carbon capture and utilization (CCU) methods and systems

Also Published As

Publication number Publication date
CA1038165A (fr) 1978-09-12

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