US3916617A - Process for production of low BTU gas - Google Patents

Process for production of low BTU gas Download PDF

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US3916617A
US3916617A US456425A US45642574A US3916617A US 3916617 A US3916617 A US 3916617A US 456425 A US456425 A US 456425A US 45642574 A US45642574 A US 45642574A US 3916617 A US3916617 A US 3916617A
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molten salt
air
coal
combustion
percent
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Donald E Mckenzie
James R Birk
Samuel J Yosim
Donald A Huber
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Boeing North American Inc
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Rockwell International Corp
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Priority to CA 221742 priority patent/CA1060652A/en
Priority to BE154684A priority patent/BE827096A/xx
Priority to FR7509547A priority patent/FR2274675A1/fr
Priority to JP50036695A priority patent/JPS6015677B2/ja
Priority to DE19752514122 priority patent/DE2514122A1/de
Priority to GB1334875A priority patent/GB1454887A/en
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    • 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
    • C10J3/57—Gasification using molten salts or metals
    • 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
    • C10J3/74—Construction of shells or jackets
    • C10J3/76—Water jackets; Steam boiler-jackets
    • 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
    • C10J2300/0916—Biomass
    • C10J2300/092—Wood, cellulose
    • 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
    • C10J2300/0913—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
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0946—Waste, e.g. MSW, tires, glass, tar sand, peat, paper, lignite, oil shale
    • 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
    • C10J2300/0959—Oxygen
    • 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
    • C10J2300/0986—Catalysts
    • 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
    • C10J2300/0996—Calcium-containing inorganic materials, e.g. lime
    • 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
    • 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
    • C10J2300/1675—Integration of gasification processes with another plant or parts within the plant with the production of electricity making use of a steam turbine
    • 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
    • C10J2300/1846—Partial oxidation, i.e. injection of air or oxygen only
    • 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
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • 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
    • Y02P20/10—Process efficiency
    • Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
    • 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

  • ABSTRACT [22] Filed- Ma 29 1974 A process for partial oxidation and complete gasification of a carbonaceous material to produce a combus- [21] Appl. No.: 456,425 tible gas containing a substantial proportion of carbon monoxide, by introducing the carbonaceous material and air as a preferred source of oxygen into a molten [52] Cl 60/39'02 ffi gk gg i salt containing an alkali metal carbonate and prefera- 51] Int Cl 2 3/00 bly also an alkali metal sulfide, the system being oper- 58 Field of Search 196/118; 48/211, 212', 197 R, Preferably abve f about 20 atmospheres.
  • the gaseous effluent, containing a weight ratio of UNITED STATES PATENTS carbon monoxide to carbon dioxide substantially 1,921,711 8/1933 Wangcmann 48/206 greater than 1, is a low BTU gas.
  • This gas can be re- '1 5/ 1966 m P aim 48/202 acted or combusted outside the molten salt in a sec- 3 223 23 i37 f lg l""t'"'l and reaction zone, such as a conventional boiler, to a a e rancoise a.
  • v 3,704,587 12/1972 Krieb et al. 60 3918 B x recover the heat value of 5 emuem' 3,708,270 1/1973 Birk et al. 48/209 x 4 Claims,.4 Drawin Figures Comsusnou 206 C0A1.
  • This invention relates to a process for the production of low BTU gas by the combustion and gasification of carbonaceous materials, particularly solid sulfur-bearing carbonaceous fuel.
  • the invention particularly relates to a molten salt process for the combustion and gasification of carbonaceous materials, particularly coal, under conditions to obtain partial oxidation and production of a combustible gaseous effluent containing a high ratio of carbon monoxide to carbon dioxide, and, when employing air as the source of oxygen, obtaining a low BTU gaseous effluent of the above type which contains nitrogen, such gas being adapted for complete combustion in a secondary reaction zone.
  • the combustion of the oxygen and carbon occurs indirectly, as described in the above patent, and the alkali metal carbonate, such as sodium carbonate, provides a compatible salt medium at practical operating temperatures, retains heat for conducting the combustion reaction, and also reacts with and neutralizes acidic or undesirable pollutants such as sulfur-containing gases which are formed during combustion of carbonaceous materials, e.g. coal, containing impurities such as sulfur and sulfur-bearing compounds.
  • the alkali metal carbonate such as sodium carbonate
  • a carbonaceous feed is thermally decomposed in a pyrolysis zone by heating it in the absence of oxygen to form char and a gaseous effluent.
  • An optional steam input for gasification of the char material may also be utilized.
  • carbon and oxygen are reacted to form carbon dioxide to provide heat for the pyrolytic decomposition reaction.
  • CO is obtained as the major product from the partial combustion and gasification process occurring in the molten salt. Subsequent heat generation is attained by combustion of the CO to CO carried out in a boiler separate from the molten salt.
  • US. Pat. No. 3,567,412 to Lefrancois et al describes a process for the production of synthesis gas in which a two-zone furnace is utilized for the gasification of carbonaceous materials, in one zone of which steam and a carbonaceous material are added to an alkali metal carbonate melt. The resulting char is transferred to the second melt-containing zone where it is catalytically combusted to provide heat for the gasification reaction by maintaining at least a critical minimum concentration of 0.4 weight percent sodium sulfate.
  • U8. Pat. No. 3,252,773 to Solomon et al discloses a carbon-containing solid material and steam brought into contact with a melt comprising an alkali metal compound under conditions such that a hydrogen-rich gas is formed along with; a resultant char.
  • heat may be supplied forthe gasification reaction by combusting the resultant char with air, a requirement of the system being that any heat generation occur as the direct combustion of carbon by the reaction of carbon and oxygen to form carbon dioxide.
  • the Pelczarski et al US. Pat. Nos. 3,533,739 and 3,526,478 disclose the gasification of solid sulfur-bearing fuel wherein the fuel is injected into a molten iron bath maintained at a temperature above about 1400C, and a limited quantity of oxygen or air is also injected into the bath. Carbon contained in the fuel is absorbed by the iron and preferentially reacts with the air or oxygen to form carbon monoxide which then passes upwardly through the iron bath. A molten layer of limebearing slag is maintained on the surface of the molten iron bath to function as a fluxing agent for the ash and to cause the sulfur absorbed by the molten iron to be 3 desorbed and to react with the lime to form calcium sulfide.
  • a portion of the slag is continuously withdrawn thereby continuously removing sulfur from the iron bath.
  • the mixture of gases from thecombustion reac.-: tion including carbon monoxide can then be reacted with oxygen to form Carbon dioxide thereby generatin additional heat.
  • a particular object of the invention is'the provision of a process for partial oxidation of a carbonaceous material in a molten alkali metal salt medium for production of a gaseous effluent containing a high proportion. of combustible gases, particularly carbon monoxide and hydrogen, such gaseous effluent then being adapted for further and complete combustion in a secondary, reaction zone or cornbustor, to utilize the heat value of the kali metal carbonates, or preferably consisting essentially of a major portion of an alkali metal carbonate and a minor portion of an alkali metal sulfate orsulfide.
  • the source of oxygen preferably air,'is employed in a proportion such as to provide an amount of oxygen substantially below the amount stoichiometrically required for complete combustion of the carbonaceous material.
  • air employed is used in a proportion to provide less than about 60 percent of the amount of oxygen stoichiometrically required for complete oxidation or combustion.
  • Other reaction parameters are controlled so as to favor incomplete combustion of the carbonaceous material, and'maximize production of CO, consistent with maintenance of the molten salt temperature at a desired value, aswell as adequate throughput of coal or carbonaceousmaterial in the most economical manner.
  • coal or other carbonaceous material containing sulfur can also serve as a source of the Sn]- fide.
  • the temperature of the molten salt is maintained between about l400 and about 2000F (about 760 to 1 100C), particularly between about l,600 and about 1,800F (about 870 980C) where coal is the carbonaceous material.
  • the result is a gaseous eflluent from the gasification and combustion reactionsw'hich contains a substantially greater volume of COthan CO generally at least 5:1 and up to 20:1, and which also the present. 3
  • .-4 contains other combustible gases such as hydrogen and hydrocarbons 1, I; l r
  • the retention of the sulfur'and ash from the fuel'in the melt eliminates the requirement for a stack gas sulfur oxide removal system and an electrostatic, precipitator.
  • These materials can be removed fromthe reaction zone with a continuous stream of molten salt, the contaminants removed from I such stream, and the regenerated stream of molten salt tible gases such as carbon monoxide and hydrogen can then be brought into :a second combustion zone or unit, which may be ,in the form of a. conventional utility 'boiler, and reacted therein with oxygen of the air to oxidize the combustible gases to CO and water with the release of heat.
  • FIG. 1 is a flow chart illustrating generally the process of the present invention
  • FIG. 2 is a schematic illustration of apreferred form of reactor containing the molt en salt
  • FIG. 3 is aflo w chart of an alternative molten salt combustion process according to the invention, employing a pressurized gas feed;
  • FIG. 4 is a graph illustrating the effect of carboncontent of the melt on CO/CO ratio obtained during partial combustion in the molten salt reactor. 1
  • the air is introduced into the molten salt in a proportion to provide an amount of oxygen less than about 60 percent of that theoretically required for complete combustion of the carbonaceous material to CO and H 0.
  • the air is employed in an amount to provide from about 30 percent to about 60 percent, preferably from about 35 to about 45 percent, of the amount of oxygen theoretically required for complete combustion of the carbonaceous material. If more than 60 percent of the oxygen needed for complete stoichiometric combustion is provided, then the resulting gas has a carbon monoxidezcarbon dioxide ratio generally less than one, which is undesirably low. If less than about 30 percent of the oxygen stoichiometrically required for complete combustion is provided, then unburned coal or char begins to accumulate in the molten salt until its viscosity becomes too high.
  • the invention process and the conditions of operation are chosen so as to obtain from the partial combustion reaction in the molten salt, a combustible gas product containing as much CO as possible and as high a BTU content as possible, with the minimum amount of heat evolution in the molten salt as possible, sufficient to maintain the salt in the molten state.
  • the combustible product gas will provide a maximum amount of heat in the secondary combustion zone.
  • Air is the preferred source of reactant gaseous oxygen for use in the present process. While oxygenenriched air or pure oxygen can be used, thereby resulting in a combustible product gas of higher BTU content, the use of oxygen would ordinarily be economically undesirable for the production of such combustible product gas, since this would ordinarily require an oxygen plant. Accordingly, the present invention will be particularly described and illustrated using air as the source of oxygen.
  • the present process finds its. principal and significant utility when integrated'into a conventional coal-fired steam plant.
  • the molten salt furnace can thus be considered as an additional step in the treatment of the coal prior to its combustion in the boiler.
  • This step takes the pulverized coal and converts it into a high temperature (about 980C.) low heat content (about BTU/scf) fuel gas.
  • This low BTU fuel gas is then burned in the boiler as a non-polluting fuel.
  • the ash and sulfur are retained in the melt and removed in the auxiliary equipment associated with the molten salt furnace.
  • the low BTU gas which is generated is burned on site.
  • the air and the carbonaceous material, preferably coal, are fed into the molten salt, which is maintained at a temperature generally ranging from about l400F to about 2000F (about 760C to ll0OC), and in preferred practice the temperature of the molten salt is maintained between about 1600 and about 1800F. (about 870C to 980C).
  • a temperature preferably from about l600 to about 2000F is utilized. It is desirable to maintain the temperature low enough so that essentially no oxides of nitrogen are formed during the partial combustion reaction and so that particulate emission is minimized.
  • the initial molten salt mixture can contain either alkali metal sulfate or sulfide. It preferably consists essentially of sodium carbonate containing from about 1 to 15 wt. percent sodium sulfate, an amount between about 3 and 10 wt. percent sodium sulfate being particularly preferred. Alternatively, a binary or ternarymixture of the carbonates of sodium, potassium and lithium can be employed, a preferred binary mixture being the Na CO -K CO eutectic.
  • the sulfur compound may be added initially as sulfate, it being converted to sulfide under steady-state conditions. Any of the sulfates vof the foregoing alkali metals may be utilized.
  • Sodium sulfate is generally preferred because of its ready availability and low cost.
  • the sulfur (as sulfide) content of the molten salt can also be furnished either wholly or partially from the sulfur content of the carbonaceous material, e.g., coal, employed, so that alkali metal sulfate or sulfide need not then be added initially tothe alkali metal carbonate.
  • the sodium sulfide is considered to catalyze the combustion reaction by a complex reaction mechanism. While various exemplary intermediate reactions may be postulated, precise knowledge as to the details of the reaction mechanism is still lacking. Thus it is not intended that the present invention be considered limited by the following explanation.
  • the net overall reaction that occurs is the partial oxidation of the carbonaceous material or coal.
  • the combination of the oxygen and carbon is believed to occur indirectily in that each of such components reacts separately with a component present in the molten salt.
  • the alkali metal sulfide e.g., sodium sulfide
  • the alkali metal carbonate provides a compatible salt medium at practical operating temperatures and acts as a dispersing medium for both the fuel being combusted and the primary air used for the combustion.
  • the carbonate melt neutralizes the acidic pollutants, such as oxides of sulfur and chlorine-containing gases, formed in the partial oxidation reaction, and retains the resulting products.
  • the carbonate melt also acts as a heat sink, with high heat transfer rates for absorbing and distributing the heat of combustion, as a heat source for the distillation of the volatile matter of the fuel, and as an absorbent for the ash from the fuel.
  • carbonaceous materials i.e., those providing an effective source of reactive carbon
  • all of the common forms of carbonaceous fuels can be used including coal, coke, fuel oil, petroleum residue, lignite, peat, wood, photographic film, plastics, pesticides and their containers, and municipal wastes such as household trash and garbage, and sewage sludge; industrial wastes such as polyvinyl chloride and I scrap rubber, and agricultural wastes including plant and animal waste material.
  • coal is the preferred carbonaceous material.
  • the present process is further advantageous in its ability to handle a wide variety of coals, including lignite, subbituminous bituminous, and anthracite coals, without any need for pre-treatment of caking coals. Tar formation is also absent in the present process.
  • an additional catalyst in the molten salt other than the alkali metal sulfide for the above reduction reaction.
  • Iron compounds have been found to be good catalysts for this reaction, employing an amount of iron ranging from about 0.5 to about 3 weight percent of the melt.
  • the iron can be added in the elemental form or preferably in the form of compounds containing iron,
  • iron sulfide such as iron sulfide or iron sulfate.
  • impurities present in the carbonaceous material are retained in the melt.
  • the amount and type of impurities present in the melt will vary depending upon the source of carbonaceous material or feed.
  • the most common impurities are ash and sulfur, the sulfur generally being present as a sulfur compound such as sodium sulfide in the melt.
  • a portion of the alkali carbonate melt is withdrawn continuously and processed in a regeneration system which removes the ash and sulfur compounds retained in the melt and returns the regenerated sodium carbonate back to the molten salt furnace.
  • a typical impurity removal process for this purpose is described in above U.S. Pat. Nos. 3,710,737 and 3,708,270.
  • the effluent gas mixture from the partial combustion reaction in the molten salt contains carbon monoxide and carbon dioxide having a volumetric ratio of CO to CO substantially greater than I, and generally ranging from about :1 to about 20:1.
  • a combustible gaseous effluent according to the invention can contain from about 90 to about 95 percent CO and about 5 to about percent CO by volume, based on these two components.
  • the effluent gas will also contain hydrogen and hydrocarbons, together with nitrogen and water. It has been found that CO concentrations in the gaseous effluent will increase with (1) reduction in the percentage of oxygen stoichiometrically required for complete combustion, (2) increasing carbon content in the melt, (3) higher temperatures of reaction and (4) increasing sulfide content of the melt.
  • the carbon content of the melt can range, for example, from about I to about 10 percent.
  • the combustible effluent gas containing the above noted high ratios of carbon monoxide to carbon dioxide has a relatively low BTU heating value, which can range from about to about 200 BTU per cubic foot.
  • a secondary burner or combustion zone such as a boiler
  • the major portion of the heat of reaction from the overall heat of combustion by complete combustion of the carbonaceous material to CO is released in the secondary combustion zone.
  • the molten salt'combustion system is operated at a pressure between I and 20 atmospheres, preferably between 5 and 10 atmospheres. By operating at pressures above atmospheric, a higher throughput of coal and air is obtained than at atmospheric pressure. Thereby the combustion reaction can be accomplished in a smaller vessel for a given rate of coal feed to the vessel.
  • a carbonaceous feed material 10 such as coal or a waste material
  • air 12 as a source of reactive oxygen
  • molten salt furnace or reactor 14 containing a Na CO -Na s melt.
  • Furnace 14 is maintained at a pressure between 5 and I0 atmospheres.
  • the air may be introduced in the bottom portion of the reactor zone so as to pass upwardly through the melt and thereby provide for an intimate mixing of the air, coal, and molten salt.
  • the heat generated by such oxidation reaction is sufficient to maintain the melt in the molten condition within the desired temperature ranges noted above for effective partial oxidation and substantially complete gasification of the carbonaceous fuel according to the invention.
  • a combustible gaseous effluent 16 from the molten salt furnace 14 contains CO and CO in the above noted volumetric ratio of CO to CO substantially greater than 1, and preferably at least 5 to l, and also contains H H 0, and N and small amounts of hydrocarbons.
  • Such low BTU gaseous effluent preferably having a heating value in excess of 100, and most desirably of the order of about to about 200 BTU per standard cubic foot, is introduced or injected into a secondary burner or boiler 18, together with air 20.
  • the resulting gaseous combustion products pass out of the boiler 18 by way of a conduit 22.
  • Such gaseous combustion products consist essentially of CO H 0, and N
  • Such completely oxidized combustion products can be vented or passed into a heat exchanger (not shown) for extraction of additional sensible heat, e.g., for preheating boiler feed water.
  • Operation of the molten salt furnace takes place preferably at a pressure between 5 and I0 atmospheres, although a pressure just high enough above ambient to allow the fuel gas generated to be injected into the fuel nozzles of the boiler is also suitable.
  • a reactor vessel 100 contains a body of molten salt 102, e.g. comprising sodium carbonate and l to 15 wt. percent sodium sulfide.
  • the reactor is provided with an insulated air or water cooling jacket 104, and there is provided a primary air inlet 106 and an air manifold distributor system 108, and coal inlets 110, the air manifold and coal inlets being interconnected.
  • the coal inlets can also serve for introduction of alkali metal carbonate into the reactor.
  • the reactor is also provided with a melt outlet 112 and a gaseous outlet 114.
  • the outlet 114 is provided with a conventional demister 116 for removing liquid and solid particulates from the effluent gas.
  • the reactor is also provided in the interior thereof with an overflow weir 118, to maintain a constant level of molten salt, and a drain 120. Air is supplied to the reaction or partial oxidation zone 122 comprised of the salt melt 102 through the air distributor system 108.
  • the carbonaceous material is partially combusted to C0, C and H 0, with release of hydrogen and hydrocarbons into the resulting gases.
  • the partial combustion and the gasification take place rapidly at relatively low temperatures, e.g. of the order of l,7001,800F, because of the high contact areas and high heat transfer rates, and more importantly, because of the catalytic effect of the sodium sulfide dissolved in the melt.
  • the gaseous effluent exiting the reactor at 114 contains at least 5 to l volumetric ratio of carbon monoxide to carbon dioxide, together with hydrogen, hydrocarbons and water, and also nitrogen from the air supply.
  • This side stream is quenched in water, which dissolves the sodium carbonate and sulfur compounds.
  • the insoluble ash and any uncombusted carbon are removed from the solution by clarification and/or filtration, preferably in the presence of CO to decrease silicate formation.
  • Carbonation of the filtrate with flue gas and steam stripping are employed to regenerate the sodium carbonate and release hydrogen sulfide.
  • the hydrogen sulfide is processed in a conventional manner for recovery of elemental sulfur or sulfuric acid.
  • the sodium carbonate is crystallized out of its water solution, and after addition of makeup, is returned to the molten salt furnace.
  • integration of the molten salt combustion and gasification process of the present invention into a conventional coal-fired steam plant can be achieved by incorporating the molten salt furnace and its associated auxiliary equipment into the coal feed system of the boiler.
  • the molten salt furnace can thus be considered as an additional initial step in the treatment of the coal prior to combustion of the product gas in the boiler.
  • the integration of the molten salt furnace system into a conventional power plant can be done in various ways, the simplest involving the installation of the molten salt furnace as a supplementary unit upstream of the boiler.
  • Operation of the molten salt furnace at a pressure just high enough above ambient to allow injection of the gas generated into the boiler, as in conventional operation, has the disadvantage that it requires a large cross section molten salt furnace, since the controlling parameter involved is the superficial velocity of the fuel gas generated.
  • operation of this furnace can be carried out under pressure. Typically a pressure of 5 atmospheres will decrease the diameter of the furnace by a factor of 2.2.
  • the amount of energy required to compress the primary air feed is however appreciable and, for economic reasons, it is important that this energy be recovered by expanding either the fuel gas produced or the off-gas from the system through a gas turbine.
  • a process and system employing such concept is illustrated in FIG. 3 of the drawing.
  • air is compressed in a compressor 200, and fed together with coal at 202 into a molten salt furnace 204.
  • the combustion gases at 208 are introduced into a gas turbine 210, generating power for operation of compressor 200, and the expanded gases from the gas turbine are introduced at 212 into a waste heat boiler 214 which generates the steam for a steam turbine 216 for the steam cycle portion of the plant.
  • the process also includes a melt regeneration system 218, described above.
  • a combination molten salt furnace and secondary combustion chamber can be used as a substitute for the combustion chamber of a conventional gas turbine.
  • the fuel gas from the molten salt furnace can be fed directly to a gas turbine to generate power, and the turbine discharge gas which is still uncombusted and containing a major portion of CO with respect to CO according to the invention, is fed to a power plant boiler functioning as the secondary combustion zone to effect complete combustion of the fuel gas from the molten salt furnace.
  • a major advantage of this embodiment is that the gas turbine expansion lowers the temperature of the fuel gas by several hundred degrees, with a consequent decrease in the combustion temperature in the secondary combustor and therefore a reduction in the oxides of nitrogen present in the stack gases.
  • the advantages of the above-noted alternative embodiments employing a compressed air feed and a gas turbine include a significant reduction in molten EXAMPLE 1 Gasification of Kentucky No. 9 Seam Coal, at 1,800F.
  • the moisture content of the. gas exiting the reaction zone was calculated assuming saturation at the temperature measured. Furnace heat was used to maintain the desired temperature of the melt.
  • the salt bed utilized in these tests had a composition at the start of these tests of 803 percent sodium carbonate, 134 percent sodium sulfate and 63 percent ash.
  • the coal was ground and dried before being fed by means of a screw feeder to a bench-"scale reactor containing the molten salt mixture.
  • Air was fed at a rate of about 1.6 to about 2.1 scfm (ftflmin. at standard conditions of 70F and 14.7 psia) to the reactor, and the coal feed at a rate of about 11 to about 19 g/min. Air rates and coal rates were chosen to give 1 ft/sec superficial velocity for the product gas exiting the'salt bed.
  • Each run was made employing the same time pattern, the runs being 1 hour in length, with 6 hour being allowed to reach steady state. This series of tests was carried out at a melt temperature of approximately 1800F (about 980C) using four different air stoichiometries, as noted in Table 1 below.
  • the ratio of COICO is substantially greater than 11 and ranges from about'3 to 1 for 46 percent theoretical 1 air to about 9 to 1 for 33 percent theoretical air.
  • the ratio of CO/CO; is substantially less 'gas, the particulate loading is about 2 grams/scf, with close to-50 percent of the particulates being carbon.
  • the bench scale equipment employed in these tests was not designed for demisting of the melt nor the deentrainment of air-home solids so that the particulate emission is not an absolute value to be expected in acl4 and in the CO/CO ratio with time apparently as a result of decrease in the carbon content of the melt with time.
  • Example 1 As seen from curves A and B, the CO/CO vol- (927C.) ume ratios at superficial air velocity of 1 ft/sec were The procedure of Example 1 was Substantially fob substantially higher than at 3 ft/sec, for corresponding lowed in running another series of tests at four different percentages of carbon the melt air stoichiometn'es, similar to Example 1 in which .From the q q It IS Seen that the mventlon prosteady-state conditions were attained, but in this case an effluent Improved procedure for the the molten salt bed temperature was maintained at of low BTU gas by a m9lten combusnon f about 1700F.
  • Air was introduced into the molten comprises: salt maintained at a temperature of about l700F.
  • salt maintained at a temperature of about l700F.
  • FIG. 4 shows the plot of such CO/CO ratio against percent carbon in the melt, for superficial air velocities of l and 3 ft. per second, as represented by curves A and B, respectively. It was noted that during these runs there was a gradual decrease in the CO concentration 25 wt. percent sodium sulfide;

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CA 221742 CA1060652A (en) 1974-03-29 1975-03-10 Process for production of low btu gas
BE154684A BE827096A (fr) 1974-03-29 1975-03-24 Procede de production de gaz combustible
FR7509547A FR2274675A1 (fr) 1974-03-29 1975-03-26 Procede de production de gaz combustible
JP50036695A JPS6015677B2 (ja) 1974-03-29 1975-03-26 燃焼性ガスの製造方法
DE19752514122 DE2514122A1 (de) 1974-03-29 1975-03-29 Verfahren zur erzeugung eines brennbaren gases
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US4007786A (en) * 1975-07-28 1977-02-15 Texaco Inc. Secondary recovery of oil by steam stimulation plus the production of electrical energy and mechanical power
US4013427A (en) * 1975-01-31 1977-03-22 Dr. C. Otto & Comp. G.M.B.H. Slag bath generator
US4017271A (en) * 1975-06-19 1977-04-12 Rockwell International Corporation Process for production of synthesis gas
US4033113A (en) * 1974-10-07 1977-07-05 Clean Energy Corporation Steam generation with coal
FR2370785A1 (fr) * 1976-11-10 1978-06-09 Saarbergwerke Ag Procede pour eliminer les composes du soufre, en particulier h2s, d'un gaz de synthese
US4169583A (en) * 1974-10-07 1979-10-02 Clean Energy Corporation Apparatus for reducing ore
WO1980002116A1 (en) * 1979-04-02 1980-10-16 Rockwell International Corp Disposal of pcb
US4295331A (en) * 1978-03-07 1981-10-20 Uriel Rekant Process for the production of energy from solid hydrocarbon fuels
US4420464A (en) * 1981-10-26 1983-12-13 Rockwell International Corporation Recovery of vanadium from carbonaceous materials
US4444007A (en) * 1982-03-12 1984-04-24 Chevron Research Company Method for combined cycle electrical power generation
US4447262A (en) * 1983-05-16 1984-05-08 Rockwell International Corporation Destruction of halogen-containing materials
US4455153A (en) * 1978-05-05 1984-06-19 Jakahi Douglas Y Apparatus for storing solar energy in synthetic fuels
US4608058A (en) * 1984-09-12 1986-08-26 Houston Industries, Incorporated Steam supply system for superposed turine and process chamber, such as coal gasification
US4668429A (en) * 1985-06-27 1987-05-26 Texaco Inc. Partial oxidation process
US4668428A (en) * 1985-06-27 1987-05-26 Texaco Inc. Partial oxidation process
US4682985A (en) * 1983-04-21 1987-07-28 Rockwell International Corporation Gasification of black liquor
WO1988000610A1 (en) * 1986-07-11 1988-01-28 Dynecology Inc. Process for the thermal decomposition of toxic refractory organic substances
US4773918A (en) * 1984-11-02 1988-09-27 Rockwell International Corporation Black liquor gasification process
US4803061A (en) * 1986-12-29 1989-02-07 Texaco Inc. Partial oxidation process with magnetic separation of the ground slag
EP0591703A3 (de) * 1992-09-23 1995-01-04 Bayer Ag Verfahren zur Verstromung von Kunststoffabfällen.
EP0693305A1 (en) 1994-07-21 1996-01-24 Rockwell International Corporation Molten salt destruction of composite materials
US5640706A (en) * 1993-04-02 1997-06-17 Molten Metal Technology, Inc. Method and apparatus for producing a product in a regenerator furnace from impure waste containing a non-gasifiable impurity
NL1008832C2 (nl) * 1998-04-07 1999-10-08 Univ Delft Tech Werkwijze voor het omzetten van een koolstofomvattend materiaal, een werkwijze voor het bedrijven van een brandstofcel en een werkwijze voor het bedrijven van een brandstofcelstapel.
US5984987A (en) * 1983-04-18 1999-11-16 Boeing North American, Inc. Black liquor gasification process
US20080141591A1 (en) * 2006-12-19 2008-06-19 Simulent Inc. Gasification of sulfur-containing carbonaceous fuels
WO2012102843A1 (en) * 2011-01-28 2012-08-02 Energy Independence Of America Corp. Method and apparatus for making liquid iron and steel
US8277766B2 (en) 2010-12-27 2012-10-02 Hnat James G Methods for the concentration of vanadium from carbonaceous feedstock materials
US8685281B2 (en) 2011-07-21 2014-04-01 Battelle Energy Alliance Llc System and process for the production of syngas and fuel gasses
US20160046880A1 (en) * 2014-08-14 2016-02-18 Johnny D. Combs Waste to Fuel System

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FR2509634B1 (fr) * 1981-07-20 1986-10-10 Cirta Ct Int Rech Tech Appliqu Procede de destruction de produits a base de matieres organiques contenant du soufre et/ou des halogenes et applications de celui-ci
US4423702A (en) * 1982-01-22 1984-01-03 Ashworth Robert A Method for desulfurization, denitrifaction, and oxidation of carbonaceous fuels
DE3434004C2 (de) * 1984-09-15 1987-03-26 Dornier System Gmbh, 7990 Friedrichshafen Verfahren und Vorrichtung zur Müllvergasung
RU2160300C2 (ru) * 1998-09-15 2000-12-10 Новосибирский государственный проектно-изыскательский институт "ВНИПИЭТ" Способ переработки твердых органических отходов, установка и деструктор для его осуществления
RU2408528C2 (ru) * 2008-08-06 2011-01-10 Институт химии нефти Сибирского отделения Российской академии наук Способ получения водорода
CN107858167B (zh) * 2017-12-21 2023-07-28 辽宁中电投电站燃烧工程技术研究中心有限公司 一种高碱煤与污泥联合热解装置及方法

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US3533739A (en) * 1968-04-01 1970-10-13 Black Sivalls & Bryson Inc Combustion of sulfur-bearing carbonaceous fuel
US3567412A (en) * 1968-08-12 1971-03-02 Pullman Inc Gasification of carbonaceous fuels
US3704587A (en) * 1970-02-07 1972-12-05 Steinkohlen Elektrizitaet Ag Control system for a gas-turbine installation
US3708270A (en) * 1970-10-01 1973-01-02 North American Rockwell Pyrolysis method
US3710737A (en) * 1970-10-01 1973-01-16 North American Rockwell Method for producing heat
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Cited By (37)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4033113A (en) * 1974-10-07 1977-07-05 Clean Energy Corporation Steam generation with coal
US4169583A (en) * 1974-10-07 1979-10-02 Clean Energy Corporation Apparatus for reducing ore
US4013427A (en) * 1975-01-31 1977-03-22 Dr. C. Otto & Comp. G.M.B.H. Slag bath generator
US4017271A (en) * 1975-06-19 1977-04-12 Rockwell International Corporation Process for production of synthesis gas
US4007786A (en) * 1975-07-28 1977-02-15 Texaco Inc. Secondary recovery of oil by steam stimulation plus the production of electrical energy and mechanical power
FR2370785A1 (fr) * 1976-11-10 1978-06-09 Saarbergwerke Ag Procede pour eliminer les composes du soufre, en particulier h2s, d'un gaz de synthese
US4295331A (en) * 1978-03-07 1981-10-20 Uriel Rekant Process for the production of energy from solid hydrocarbon fuels
US4455153A (en) * 1978-05-05 1984-06-19 Jakahi Douglas Y Apparatus for storing solar energy in synthetic fuels
WO1980002116A1 (en) * 1979-04-02 1980-10-16 Rockwell International Corp Disposal of pcb
US4420464A (en) * 1981-10-26 1983-12-13 Rockwell International Corporation Recovery of vanadium from carbonaceous materials
US4444007A (en) * 1982-03-12 1984-04-24 Chevron Research Company Method for combined cycle electrical power generation
US5984987A (en) * 1983-04-18 1999-11-16 Boeing North American, Inc. Black liquor gasification process
US4682985A (en) * 1983-04-21 1987-07-28 Rockwell International Corporation Gasification of black liquor
US4447262A (en) * 1983-05-16 1984-05-08 Rockwell International Corporation Destruction of halogen-containing materials
EP0125383A3 (en) * 1983-05-16 1986-07-16 Rockwell International Corporation Destruction of halogen-containing materials
US4608058A (en) * 1984-09-12 1986-08-26 Houston Industries, Incorporated Steam supply system for superposed turine and process chamber, such as coal gasification
US4773918A (en) * 1984-11-02 1988-09-27 Rockwell International Corporation Black liquor gasification process
US4668428A (en) * 1985-06-27 1987-05-26 Texaco Inc. Partial oxidation process
US4668429A (en) * 1985-06-27 1987-05-26 Texaco Inc. Partial oxidation process
WO1988000610A1 (en) * 1986-07-11 1988-01-28 Dynecology Inc. Process for the thermal decomposition of toxic refractory organic substances
US4803061A (en) * 1986-12-29 1989-02-07 Texaco Inc. Partial oxidation process with magnetic separation of the ground slag
EP0591703A3 (de) * 1992-09-23 1995-01-04 Bayer Ag Verfahren zur Verstromung von Kunststoffabfällen.
US5640706A (en) * 1993-04-02 1997-06-17 Molten Metal Technology, Inc. Method and apparatus for producing a product in a regenerator furnace from impure waste containing a non-gasifiable impurity
EP0693305A1 (en) 1994-07-21 1996-01-24 Rockwell International Corporation Molten salt destruction of composite materials
NL1008832C2 (nl) * 1998-04-07 1999-10-08 Univ Delft Tech Werkwijze voor het omzetten van een koolstofomvattend materiaal, een werkwijze voor het bedrijven van een brandstofcel en een werkwijze voor het bedrijven van een brandstofcelstapel.
WO1999052166A3 (en) * 1998-04-07 2000-01-20 Univ Delft Tech Method of converting a carbon-comprising material, method of operating a fuel cell stack, and a fuel cell
US6607853B1 (en) 1998-04-07 2003-08-19 Technische Universitiet Delft Method of converting a carbon-comprising material, method of operating a fuel cell stack, and a fuel cell
US20080141591A1 (en) * 2006-12-19 2008-06-19 Simulent Inc. Gasification of sulfur-containing carbonaceous fuels
US20100088958A1 (en) * 2006-12-19 2010-04-15 Simulent Energy Inc. Mixing and feeding aqueous solution of alkali metal salt and particles of sulfur-containing carbonaceous fuel for gasification
US8529648B2 (en) 2006-12-19 2013-09-10 Arthur L. Kohl Mixing and feeding aqueous solution of alkali metal salt and particles of sulfur-containing carbonaceous fuel for gasification
US8277766B2 (en) 2010-12-27 2012-10-02 Hnat James G Methods for the concentration of vanadium from carbonaceous feedstock materials
WO2012102843A1 (en) * 2011-01-28 2012-08-02 Energy Independence Of America Corp. Method and apparatus for making liquid iron and steel
US8685281B2 (en) 2011-07-21 2014-04-01 Battelle Energy Alliance Llc System and process for the production of syngas and fuel gasses
WO2013012473A3 (en) * 2011-07-21 2014-05-08 Battelle Energy Alliance, Llc System and process for the production of syngas and fuel gasses
US9011725B2 (en) 2011-07-21 2015-04-21 Battelle Energy Alliance Llc System and process for the production of syngas and fuel gasses
US20160046880A1 (en) * 2014-08-14 2016-02-18 Johnny D. Combs Waste to Fuel System
US9714391B2 (en) * 2014-08-14 2017-07-25 Johnny D. Combs Waste to fuel system

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CA1060652A (en) 1979-08-21
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FR2274675B1 (OSRAM) 1981-03-20
GB1454887A (en) 1976-11-03
DE2514122A1 (de) 1975-10-09
JPS50134003A (OSRAM) 1975-10-23
BE827096A (fr) 1975-09-24

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