US20060185244A1 - Novel production method of gaseous fuels - Google Patents

Novel production method of gaseous fuels Download PDF

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Publication number
US20060185244A1
US20060185244A1 US10/502,633 US50263304A US2006185244A1 US 20060185244 A1 US20060185244 A1 US 20060185244A1 US 50263304 A US50263304 A US 50263304A US 2006185244 A1 US2006185244 A1 US 2006185244A1
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United States
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gas
aromatic
fuel
supercritical water
compound
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US10/502,633
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English (en)
Inventor
Ki Park
Hiroshi Tomiyasu
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Individual
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    • 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
    • B01J3/00—Processes of utilising sub-atmospheric or super-atmospheric pressure to effect chemical or physical change of matter; Apparatus therefor
    • B01J3/008—Processes carried out under supercritical conditions
    • 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
    • C10J1/00—Production of fuel gases by carburetting air or other gases without pyrolysis
    • C10J1/02—Carburetting air
    • C10J1/16—Carburetting air with solid hydrocarbons
    • 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
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/08—Production of synthetic natural 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
    • C10J2300/093—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
    • C10J2300/0946—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
    • C10J2300/0973—Water
    • C10J2300/0979—Water as supercritical 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
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0983—Additives
    • 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
    • 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
    • Y02P20/54—Improvements relating to the production of bulk chemicals using solvents, e.g. supercritical solvents or ionic liquids

Definitions

  • the present invention is related to a method of producing gas fuel, in which low quality fuel such as coal and flame retardant waste such as various plastics and resins are decomposed in supercritical water with a catalyst, so that resultant gas can be utilized as gas fuel.
  • plastics for example, foamed polystyrene
  • foamed polystyrene some types of plastics
  • resins polymeric compounds
  • coal While coal is very stable in supercritical water, it is known to be possible to extract oily components depending on a type of coal. However, the extracted oily components have a composition containing a large amount of oxygen, thereby making it difficult to use as fuel.
  • a novel process of producing gas fuel in which low quality fuel such as coal and various kinds of plastics and resins (polymeric compounds) collected as waste are decomposed to gas in supercritical water, so that the resultant gas is effectively utilized as fuel.
  • polymeric compounds and aromatic/condensed hydrocarbons are decomposed in supercritical water with ruthenium oxide (IV) as a catalyst.
  • the resultant gas components through the decomposition are collected as gas fuel.
  • polymeric compounds and aromatic/condensed hydrocarbons i.e. materials to be decomposed to obtain gas fuel
  • materials to be decomposed to obtain gas fuel are immerged in supercritical water.
  • a reaction occurs in the materials to be decomposed in supercritical water with ruthenium oxide (IV) as a catalyst.
  • the materials are composed into gas components and organic residue, and the gas component is collected as gas fuel.
  • the novel method of producing gas fuel includes the following steps.
  • polymeric compounds and aromatic/condensed hydrocarbons are decomposed in supercritical water with ruthenium oxide (IV) as a catalyst to produce gas components as a result of the decomposition.
  • the gas components, which are produced through the decomposition of the polymeric compounds and aromatic/condensed hydrocarbons, are collected to use as gas fuel.
  • the material to be decomposed it is possible to decompose industrial waste such as polymeric compounds as well as aromatic/condensed hydrocarbons. For example, it is possible to decompose up to 92% of naphthalene to obtain flammable gas as described above.
  • the present invention is similarly applicable to coal, which is very stable in supercritical water, and it is possible to convert coal into flammable gas with ruthenium oxide (IV) as a catalyst. In other words, it is possible to modify coal into high quality fuel (low molecular weight hydrocarbons such as methane and hydrogen) without containing harmful metal, and nitrogen and sulfur components.
  • the material for obtaining fuel it is possible to use industrial waste such as plastics and resins, thereby producing gas fuel with low cost and contributing to industrial waste treatment.
  • polymeric compounds and aromatic/condensed hydrocarbons i.e. materials to be decomposed for obtaining gas fuel
  • materials to be decomposed for obtaining gas fuel are immerged in supercritical water.
  • a reaction occurs in the materials to be decomposed in supercritical water with ruthenium oxide as a catalyst.
  • the materials are composed into gas components and organic residue, and the gas components are collected as gas fuel.
  • it is possible to utilize the resultant gas generated through the decomposition of polymeric compounds and aromatic/condensed hydrocarbons as gas fuel.
  • the materials to be processed for obtaining gas fuel include a compound having a polymeric structure such as polyvinylchloride (PVC), fiber reinforced plastics (FRP), Teflon resins (PTFE), polypropylene (PP), polyethylene (PE), polystyrene (PS), and Daiflon (PFA); and a compound having an aromatic ring structure such as naphthalene and coal. That is, such flame retardant materials and low quality fuel are used as the materials to be processed, thereby effectively utilizing materials.
  • PVC polyvinylchloride
  • FRP fiber reinforced plastics
  • PTFE Teflon resins
  • PP polypropylene
  • PE polyethylene
  • PS polystyrene
  • PFA Daiflon
  • FIG. 1 is a gas chromatogram showing low molecular weight hydrocarbons obtained through decomposition of polystyrene
  • FIG. 2 is a gas chromatogram showing hydrogen obtained through decomposition of polystyrene
  • FIG. 3 is a gas chromatogram showing carbon dioxide obtained through decomposition of polystyrene
  • FIG. 4 is a gas chromatogram showing low molecular weight hydrocarbons obtained through decomposition of naphthalene
  • FIG. 5 is a gas chromatogram showing hydrogen obtained through decomposition of naphthalene
  • FIG. 6 is a gas chromatogram showing carbon dioxide obtained through decomposition of naphthalene
  • FIG. 7 is a gas chromatogram showing low molecular weight hydrocarbons obtained through decomposition of Taiheiyo coal
  • FIG. 8 is a gas chromatogram showing hydrogen obtained through decomposition of Taiheiyo coal.
  • FIG. 9 is a gas chromatogram showing carbon dioxide obtained through decomposition of Taiheiyo coal.
  • a novel process of producing gas fuel in which polymeric compounds and aromatics/condensed hydrocarbons are decomposed in supercritical water with ruthenium oxide (IV) RuO 2 as a catalyst, and the resultant gas is collected as gas fuel.
  • a critical state water is heated to 374° C., i.e. a critical temperature, at 22.1 MPa, i.e. a critical pressure.
  • a pressure is controlled by an amount of water and reaches 22.1 MPa or higher.
  • Water in such a state is called supercritical water. It has been known that decomposition is facilitated in supercritical water.
  • ruthenium oxide (IV) is used as a catalyst. It has been experimentally confirmed that ruthenium oxide (IV) efficiently decomposes organic compounds in any states of liquid, solid, linear structures and cyclic structures to produce gas in supercritical water. Accordingly, in the present invention, ruthenium oxide (IV) is used as a catalyst for decomposing organic compounds in supercritical water.
  • Materials to be processed for obtaining gas fuel include a compound having an aromatic ring structure such as naphthalene and coal; and a compound having a polymeric structure such as polyvinylchloride (PVC), fiber reinforced plastics (FRP), Teflon resins (PTFE), polypropylene (PP), polyethylene (PE), polystyrene (PS), and Daiflon (PFA) as flame retardant materials.
  • PVC polyvinylchloride
  • FRP fiber reinforced plastics
  • PTFE Teflon resins
  • PP polypropylene
  • PE polyethylene
  • PS polystyrene
  • PFA Daiflon
  • polystyrene as the polymeric compound was decomposed in an experiment, as follows: 100 mg of polystyrene (apparent quantity; 0.960 mmol with —C 8 H 8 — as a unit), 20 mg of ruthenium oxide (IV), and 3 ml of water were placed in a batch-type supercritical water reactor. After the reactor was sealed, the reactor was heated to conduct a reaction at 450° C. for 2 hours. After cooling, the reactor was connected with a vacuum glass line, and produced gas components were analyzed with on-line gas chromatography. An oily organic residue was extracted using chloroform and collected from a water phase. As a result, 99% of polypropylene was decomposed into gas components, and a trace amount (1.1 mg) of the organic residue remained.
  • the obtained gases are flammable gases (methane, ethane, propane, hydrogen) and carbon dioxide.
  • Carbon dioxide can be selectively collected through calcium hydroxide solution, thereby imposing no influence on the environment.
  • the organic residue has a trace amount, and it was confirmed that there is no influence on the environment upon processing.
  • naphthalene as the aromatic/condensed-aromatic compound was decomposed in an experiment, as follows:
  • naphthalene 0.780 mmol
  • 3 ml of water 100 mg were placed in a batch-type supercritical water reactor. After the reactor was sealed, the reactor was heated to conduct a reaction at 450° C. for 3 hours. After cooling, the reactor was connected with a vacuum glass line, and produced gas components were analyzed with on-line gas chromatography. An organic residue was extracted using chloroform and collected from a water phase. As a result, 92% of naphthalene was decomposed into gas components, and a trace amount (8.5 mg) of the organic residue remained.
  • the obtained gases are flammable gases (methane, a trace amount of ethane, a trace amount of propane, hydrogen) and carbon dioxide.
  • Carbon dioxide can be selectively collected through calcium hydroxide solution, thereby imposing no influence on the environment.
  • a trace amount of the organic residue was mainly unreacted naphthalene, and it was confirmed that the organic residue can be used again as the material to be processed.
  • the obtained gases are flammable gases (methane, a trace amount of ethane, a trace amount of propane, hydrogen) with no harmful components (nitrogen component, sulfur component or heavy metal).
  • Carbon dioxide can be selectively collected through calcium hydroxide solution, thereby imposing no influence on the environment.
  • a trace amount of the organic residue can be stored in a glass bottle, thereby imposing no negative influence on the environment.
  • polystyrene polymeric compound
  • naphthalene aromatic/condensed-aromatic compound
  • low molecular weight hydrocarbons methane, ethane, propane
  • hydrogen is produced.
  • ruthenium oxide (IV) functions as a catalyst of reductive decomposition.
  • carbon dioxide indicates that ruthenium oxide (IV) functions as a catalyst of oxidative decomposition.
  • ruthenium oxide (IV) decomposes a polymeric compound, i.e. large linear macromolecules, into low molecular hydrocarbons through reduction and oxidation.
  • naphthalene indicates that an aromatic compound having a stable conjugated ring structure is oxidized, and at the same time, is opened reductively to produce low molecular hydrocarbons.
  • ruthenium oxide (IV) functions as a catalyst for decomposing many organic compounds in supercritical water through reduction and oxidation.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • General Chemical & Material Sciences (AREA)
  • Separation, Recovery Or Treatment Of Waste Materials Containing Plastics (AREA)
  • Catalysts (AREA)
US10/502,633 2002-02-06 2004-02-04 Novel production method of gaseous fuels Abandoned US20060185244A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2002028957A JP4121283B2 (ja) 2002-02-06 2002-02-06 超臨界水中における酸化ルテニウム（ｉｖ）を触媒とした気体燃料の生成方法
JP2002028957 2002-02-06

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP4673098B2 (ja) * 2005-03-15 2011-04-20 中部電力株式会社 還元雰囲気の超臨界水を用いた磁性体の合成方法

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3983028A (en) * 1974-07-01 1976-09-28 Standard Oil Company (Indiana) Process for recovering upgraded products from coal
US4597363A (en) * 1981-02-27 1986-07-01 Melvin Emelock Hydrogen generator for motor vehicle
US5616154A (en) * 1992-06-05 1997-04-01 Battelle Memorial Institute Method for the catalytic conversion of organic materials into a product gas
US6551719B2 (en) * 1999-12-20 2003-04-22 Furuyametal Co., Ltd. Reaction vessel of oxidization and decomposition processing equipment by supercritical water and method for manufacturing the same

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3983028A (en) * 1974-07-01 1976-09-28 Standard Oil Company (Indiana) Process for recovering upgraded products from coal
US4597363A (en) * 1981-02-27 1986-07-01 Melvin Emelock Hydrogen generator for motor vehicle
US5616154A (en) * 1992-06-05 1997-04-01 Battelle Memorial Institute Method for the catalytic conversion of organic materials into a product gas
US6551719B2 (en) * 1999-12-20 2003-04-22 Furuyametal Co., Ltd. Reaction vessel of oxidization and decomposition processing equipment by supercritical water and method for manufacturing the same

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JP2003226885A (ja) 2003-08-15
KR100562069B1 (ko) 2006-03-16
KR20030016354A (ko) 2003-02-26
JP4121283B2 (ja) 2008-07-23

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