US3446609A - Gasification with water-containing feed - Google Patents

Gasification with water-containing feed Download PDF

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Publication number
US3446609A
US3446609A US455417A US3446609DA US3446609A US 3446609 A US3446609 A US 3446609A US 455417 A US455417 A US 455417A US 3446609D A US3446609D A US 3446609DA US 3446609 A US3446609 A US 3446609A
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United States
Prior art keywords
water
hydrocarbon
feed
soot
liquid
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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
Application number
US455417A
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English (en)
Inventor
Ernst F Reinmuth
Leonard W Ter Haar
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Shell USA Inc
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Shell Oil Co
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Publication date
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
    • C10L1/322—Coal-oil suspensions
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/32—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air
    • C01B3/34—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents
    • C01B3/36—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents using oxygen; using mixtures containing oxygen as gasifying agents
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09C—TREATMENT OF INORGANIC MATERIALS, OTHER THAN FIBROUS FILLERS, TO ENHANCE THEIR PIGMENTING OR FILLING PROPERTIES ; PREPARATION OF CARBON BLACK  ; PREPARATION OF INORGANIC MATERIALS WHICH ARE NO SINGLE CHEMICAL COMPOUNDS AND WHICH ARE MAINLY USED AS PIGMENTS OR FILLERS
    • C09C1/00—Treatment of specific inorganic materials other than fibrous fillers; Preparation of carbon black
    • C09C1/44—Carbon
    • C09C1/48—Carbon black
    • C09C1/56—Treatment of carbon black ; Purification
    • C09C1/58—Agglomerating, pelleting, or the like by wet methods
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/04—Purifying combustible gases containing carbon monoxide by cooling to condense non-gaseous materials
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G OR C10K; LIQUIFIED PETROLEUM GAS; USE OF ADDITIVES TO FUELS OR FIRES; FIRE-LIGHTERS
    • C10L1/00—Liquid carbonaceous fuels
    • C10L1/32—Liquid carbonaceous fuels consisting of coal-oil suspensions or aqueous emulsions or oil emulsions
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/30—Particle morphology extending in three dimensions
    • C01P2004/32—Spheres
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/60—Particles characterised by their size
    • C01P2004/61—Micrometer sized, i.e. from 1-100 micrometer
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/60—Particles characterised by their size
    • C01P2004/62—Submicrometer sized, i.e. from 0.1-1 micrometer

Definitions

  • This invention relates to a process for preparing gas mixtures containing hydrogen and carbon monoxide.
  • it relates to gasification of liquid hydrocarbon feeds containing small amounts of Water.
  • the gasification of hydrocarbons by partial oxidation to produce H -CO mixtures is a Well-known commercial process. This process generally involves intimately mixing hydrocarbon and an oxidant, such as air, in a combustion chamber in carefully controlled proportions. The mixed gases enter a reaction zone, wherein the conversion of hydrocarbon feed to hydrogen, CO, and minor amounts of carbon, is completed. After subsequent processing which may include heat recovery, carbon removal, and water scrubbing of the gas, the carbon-free product may be used as synthesis gas or fuel gas for any of a variety of purposes. Examples of these processes are found in Oil and Gas Journal, vol. 63, No. 14, pp. 108-9 (Apr. 5, 1965).
  • soot gas mixtures obtained by hydrocarbon gasification always contain some free carbon, hereafter referred to as soot.
  • soot-in-oil suspension It is known to recover this soot by water-quenching and washing the gases, and by aggregating soot particles to pellets by treatment of the resulting aqueous soot slurry with small amounts of oil, or by recovering the soot as a soot-in-oil suspension.
  • soot-in-oil slurry is useful as a fuel, it usually cannot be completely consumed at or near the gasification unit and transport to other areas is costly.
  • soot formation is reduced by feeding a fuel comprising a liquid hydrocarbon and a minor amount of water to the gasification process.
  • Water is supplied to the liquid hydrocarbon feed in small amounts sufficient to reduce soot formation; appropriate amounts of water are less than 4%, preferably 0.1 to 4%, and more especially 0.3 to 0.7% by weight of the total fuel intake.
  • Any liquid hydrocarbon or hydrocarbon mixture may be used as gasification fuel, ranging from lower parafiins and naphthas to residual oils. Even normally gaseous hydrocarbons, such as propane, could be used if they were supplied to the reactor in the liquid phase, which is the essential requirement of reactor feed for practice of the invention.
  • Water may be injected into the fuel prior to atomization to pressurize the fuel up to feed pressure, which may be from about 60 to about 160 atmospheres.
  • feed pressure which may be from about 60 to about 160 atmospheres.
  • feed pressure which may be from about 60 to about 160 atmospheres.
  • water may be injected into the hydrocarbon prior to preheat of the feed. Feed preheat may be anywhere from about to about 350 0, however, it is essential that the feed remain in the liquid phase until vaporization in the atomizer.
  • feed pressures may be from 60 to atmospheres, and the reactor pressure is less than 40 atmospheres.
  • reactor pressures are from about 1 to about 6 atmospheres; when oxygen is used as an oxidant, higher pressures of 3 to about 40 atmospheres are more suitable.
  • Gasification reaction conditions are generally temperatures of 1000-1600 0., preferably 1100-1500 C., and pressures of 1-40 atmospheres. Both hydrocarbon and oxygen feed are advantageously preheated to temperatures not exceeding 350 C. in the practice of the invention.
  • Oxygen is supplied in amounts suflicient to completely react to form the desired products; oxygen/hydrocarbon ratios will vary depending on desired products, hydrocarbon mol weight, etc.
  • a moderator such as steam or CO may also be supplied to the reactor.
  • oxygen content of the oxidant, oxygen/fuel ratio, and equipment design free carbon liberated may be from about 0.1 to about 5% w. basis hydrocarbon feed.
  • soot Gasification of liquid feeds always contain soot, which, as discussed above, must be removed from the gases by some treatment.
  • the most effective treatment has been found to be a water wash or quench wherein the soot is recovered as an aqueous slurry.
  • This slurry cannot be disposed of as waste because of pollution problems.
  • the slurry may be concentrated and the carbon either pelletized or recovered as a soot-in-oil slurry by preferential wetting of the soot with e.g. a light hydrocarbon oil which is easily separated from the aqueous phase.
  • the resulting soot agglomerates contain about 10 to 15% w.
  • soot-containing oil may be mixed with liquid hydrocarbon feed such that the resulting mixture contains a certain 3 critical amount of water (i.e. less than 4%, preferably 0.3 to 0.7% by weight).
  • vessel 1 represents a storage tank for liquid hydrocarbon from which the liquid fuel is pumped by pump 3 through a line 2.
  • Pump 3 is a lowpressure pump which pressurizes the liquid fuel after passing the pump to not more than about 6 atmospheres.
  • Water is supplied to line 4 and pump 5 which is driven by a driving means 6 which may include also a dosing mechanism to line 7.
  • a driving means 6 which may include also a dosing mechanism to line 7.
  • a driving means 6 which may include also a dosing mechanism to line 7.
  • Pump 9 pressurizes the mixture up to 60-160 atmospheres.
  • the mixture is preheated before entering the reactor, preferably at a point not far from the reactor, in heat exchanger 12.
  • the mixture is introduced through a pressure atomizer 13 into reactor 14, wherein the degree of atomization is very fine due to the circumstance that a small amount of water is present in the fuel stream.
  • the reactor is an open vertical chamber, unobstructed by packing and the like. The water protects the brick lining of the reactor at the hottest place. As a result of its cooling effect on evaporation. Soot-containing gases produced in the reactor are drawn off through line 15 for further processing.
  • Suitable control means 16 operating the dosing device '6 and receiving its signal from a fiowmeter present in line 2 is schematically indicated in the drawing by dotted lines 17 and 18 respectively.
  • Auxiliary equipment, such as inlet and outlet lines, valves, other control means, etc. have been omitted.
  • liquid water is added in an amount of from about 0.3 to 0.7% by weight of the total hydrocarbon feed.
  • a process for partial oxidation of a liquid hydrocarbon feed wherein hydrocarbon and water is fed in the liquid phase to a reaction zone andis contacted therein with an oxygen-containing gas at elevated temperatures to produce a gaseous mixture comprising carbon monoxide and hydrogen and small amounts of free carbon, recovering free carbon from the gaseous mixture by contacting the gaseous mixture with water to form an aqueous slurry of carbon particles, contacting the aqueous slurry with liquid hydrocarbon to form a slurry of carbon in hydrocarbon, and blending at least a portion of the carbon-hydrocarbon slurry with hydrocarbon feed, the liquid water content being from 0.01 to 4% by weight of the resulting reactor feed.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • General Chemical & Material Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)
US455417A 1964-05-14 1965-05-13 Gasification with water-containing feed Expired - Lifetime US3446609A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB20187/64A GB1056184A (en) 1964-05-14 1964-05-14 Processes for preparing gas mixtures containing hydrogen and carbon monoxide
GB3771764 1964-09-15

Publications (1)

Publication Number Publication Date
US3446609A true US3446609A (en) 1969-05-27

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ID=26254516

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US455417A Expired - Lifetime US3446609A (en) 1964-05-14 1965-05-13 Gasification with water-containing feed

Country Status (7)

Country Link
US (1) US3446609A (fr)
BE (2) BE663816A (fr)
ES (1) ES312828A1 (fr)
FR (2) FR1436287A (fr)
GB (1) GB1056184A (fr)
NL (2) NL6506075A (fr)
OA (1) OA01724A (fr)

Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3778240A (en) * 1969-08-11 1973-12-11 Int Materials Corp Coking prevention system
US4259414A (en) * 1979-11-29 1981-03-31 Rca Corporation Non-air polluting, non-pyrolytic upgrading of coal for cleaner and more effective electrical power generation
US5112527A (en) * 1991-04-02 1992-05-12 Amoco Corporation Process for converting natural gas to synthesis gas
US20070009425A1 (en) * 2003-05-27 2007-01-11 Wolf Johnssen Method for producing alkali metal hydrides and hydrogen
US8303676B1 (en) * 2008-02-19 2012-11-06 Proton Power, Inc. Conversion of C-O-H compounds into hydrogen for power or heat generation
US9023243B2 (en) 2012-08-27 2015-05-05 Proton Power, Inc. Methods, systems, and devices for synthesis gas recapture
US9254461B2 (en) 2014-01-10 2016-02-09 Proton Power, Inc. Methods, systems, and devices for liquid hydrocarbon fuel production, hydrocarbon chemical production, and aerosol capture
US9382482B2 (en) 2014-03-05 2016-07-05 Proton Power, Inc. Continuous liquid fuel production methods, systems, and devices
US9698439B2 (en) 2008-02-19 2017-07-04 Proton Power, Inc. Cellulosic biomass processing for hydrogen extraction
US9890332B2 (en) 2015-03-08 2018-02-13 Proton Power, Inc. Biochar products and production
US10005961B2 (en) 2012-08-28 2018-06-26 Proton Power, Inc. Methods, systems, and devices for continuous liquid fuel production from biomass

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4762528A (en) * 1986-09-05 1988-08-09 Reichl Eric H Fluid fuel from coal and method of making same

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US1644146A (en) * 1923-05-02 1927-10-04 Robert D Pike Method of manufacturing oil gas
US2665980A (en) * 1950-05-05 1954-01-12 Texas Co Process for generation of carbon monoxide
US2999741A (en) * 1958-05-29 1961-09-12 Texaco Inc Production of carbon monoxide and hydrogen
US3097082A (en) * 1963-07-09 Gasification of hydrocarbon fuel oils
US3147093A (en) * 1962-03-14 1964-09-01 Texaco Inc Recovery of carbon from water
US3232727A (en) * 1961-12-13 1966-02-01 Texaco Inc Synthesis gas generation

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3097082A (en) * 1963-07-09 Gasification of hydrocarbon fuel oils
US1644146A (en) * 1923-05-02 1927-10-04 Robert D Pike Method of manufacturing oil gas
US2665980A (en) * 1950-05-05 1954-01-12 Texas Co Process for generation of carbon monoxide
US2999741A (en) * 1958-05-29 1961-09-12 Texaco Inc Production of carbon monoxide and hydrogen
US3232727A (en) * 1961-12-13 1966-02-01 Texaco Inc Synthesis gas generation
US3147093A (en) * 1962-03-14 1964-09-01 Texaco Inc Recovery of carbon from water

Cited By (16)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3778240A (en) * 1969-08-11 1973-12-11 Int Materials Corp Coking prevention system
US4259414A (en) * 1979-11-29 1981-03-31 Rca Corporation Non-air polluting, non-pyrolytic upgrading of coal for cleaner and more effective electrical power generation
US5112527A (en) * 1991-04-02 1992-05-12 Amoco Corporation Process for converting natural gas to synthesis gas
US20070009425A1 (en) * 2003-05-27 2007-01-11 Wolf Johnssen Method for producing alkali metal hydrides and hydrogen
US9698439B2 (en) 2008-02-19 2017-07-04 Proton Power, Inc. Cellulosic biomass processing for hydrogen extraction
US8303676B1 (en) * 2008-02-19 2012-11-06 Proton Power, Inc. Conversion of C-O-H compounds into hydrogen for power or heat generation
US8696775B2 (en) 2008-02-19 2014-04-15 Proton Power, Inc Conversion of C—O—H compounds into hydrogen for power or heat generation
US9023124B2 (en) 2008-02-19 2015-05-05 Proton Power, Inc Conversion of C—O—H compounds into hydrogen for power or heat generation
US9561956B2 (en) 2008-02-19 2017-02-07 Proton Power, Inc. Conversion of C-O-H compounds into hydrogen for power or heat generation
US9023243B2 (en) 2012-08-27 2015-05-05 Proton Power, Inc. Methods, systems, and devices for synthesis gas recapture
US10005961B2 (en) 2012-08-28 2018-06-26 Proton Power, Inc. Methods, systems, and devices for continuous liquid fuel production from biomass
US9254461B2 (en) 2014-01-10 2016-02-09 Proton Power, Inc. Methods, systems, and devices for liquid hydrocarbon fuel production, hydrocarbon chemical production, and aerosol capture
US10144875B2 (en) 2014-01-10 2018-12-04 Proton Power, Inc. Systems, and devices for liquid hydrocarbon fuel production, hydrocarbon chemical production, and aerosol capture
US10563128B2 (en) 2014-01-10 2020-02-18 Proton Power, Inc. Methods for aerosol capture
US9382482B2 (en) 2014-03-05 2016-07-05 Proton Power, Inc. Continuous liquid fuel production methods, systems, and devices
US9890332B2 (en) 2015-03-08 2018-02-13 Proton Power, Inc. Biochar products and production

Also Published As

Publication number Publication date
FR1436287A (fr) 1966-04-22
BE663815A (fr) 1965-11-12
BE663816A (fr) 1965-11-12
NL6506074A (fr) 1965-11-15
GB1056184A (en) 1967-01-25
NL6506075A (fr) 1965-11-15
OA01724A (fr) 1969-12-15
FR1436288A (fr) 1966-04-22
ES312828A1 (es) 1965-12-16

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