WO2012057380A1 - Système de reformage de biogaz à l'aide de la chaleur perdue, et procédé de reformage de biogaz utilisant ce système - Google Patents

Système de reformage de biogaz à l'aide de la chaleur perdue, et procédé de reformage de biogaz utilisant ce système Download PDF

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WO2012057380A1
WO2012057380A1 PCT/KR2010/007532 KR2010007532W WO2012057380A1 WO 2012057380 A1 WO2012057380 A1 WO 2012057380A1 KR 2010007532 W KR2010007532 W KR 2010007532W WO 2012057380 A1 WO2012057380 A1 WO 2012057380A1
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Prior art keywords
reforming
biogas
type
catalyst
gas
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PCT/KR2010/007532
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English (en)
Korean (ko)
Inventor
송순호
김태수
차효석
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연세대학교 산학협력단
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Publication of WO2012057380A1 publication Critical patent/WO2012057380A1/fr

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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M25/00—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture
    • F02M25/10—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture adding acetylene, non-waterborne hydrogen, non-airborne oxygen, or ozone
    • F02M25/12—Engine-pertinent apparatus for adding non-fuel substances or small quantities of secondary fuel to combustion-air, main fuel or fuel-air mixture adding acetylene, non-waterborne hydrogen, non-airborne oxygen, or ozone the apparatus having means for generating such gases
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M21/00—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form
    • F02M21/02—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form for gaseous fuels
    • F02M21/0203—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form for gaseous fuels characterised by the type of gaseous fuel
    • F02M21/0215—Mixtures of gaseous fuels; Natural gas; Biogas; Mine gas; Landfill gas
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N5/00—Exhaust or silencing apparatus combined or associated with devices profiting by exhaust energy
    • F01N5/02—Exhaust or silencing apparatus combined or associated with devices profiting by exhaust energy the devices using heat
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02B—INTERNAL-COMBUSTION PISTON ENGINES; COMBUSTION ENGINES IN GENERAL
    • F02B43/00—Engines characterised by operating on gaseous fuels; Plants including such engines
    • F02B43/10—Engines or plants characterised by use of other specific gases, e.g. acetylene, oxyhydrogen
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02G—HOT GAS OR COMBUSTION-PRODUCT POSITIVE-DISPLACEMENT ENGINE PLANTS; USE OF WASTE HEAT OF COMBUSTION ENGINES; NOT OTHERWISE PROVIDED FOR
    • F02G5/00—Profiting from waste heat of combustion engines, not otherwise provided for
    • F02G5/02—Profiting from waste heat of exhaust gases
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M21/00—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form
    • F02M21/02—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form for gaseous fuels
    • F02M21/0218—Details on the gaseous fuel supply system, e.g. tanks, valves, pipes, pumps, rails, injectors or mixers
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M21/00—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form
    • F02M21/02—Apparatus for supplying engines with non-liquid fuels, e.g. gaseous fuels stored in liquid form for gaseous fuels
    • F02M21/0218—Details on the gaseous fuel supply system, e.g. tanks, valves, pipes, pumps, rails, injectors or mixers
    • F02M21/0227—Means to treat or clean gaseous fuels or fuel systems, e.g. removal of tar, cracking, reforming or enriching
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M27/00—Apparatus for treating combustion-air, fuel, or fuel-air mixture, by catalysts, electric means, magnetism, rays, sound waves, or the like
    • F02M27/02—Apparatus for treating combustion-air, fuel, or fuel-air mixture, by catalysts, electric means, magnetism, rays, sound waves, or the like by catalysts
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
    • F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
    • F02M31/00—Apparatus for thermally treating combustion-air, fuel, or fuel-air mixture
    • F02M31/02—Apparatus for thermally treating combustion-air, fuel, or fuel-air mixture for heating
    • F02M31/04—Apparatus for thermally treating combustion-air, fuel, or fuel-air mixture for heating combustion-air or fuel-air mixture
    • F02M31/06—Apparatus for thermally treating combustion-air, fuel, or fuel-air mixture for heating combustion-air or fuel-air mixture by hot gases, e.g. by mixing cold and hot air
    • F02M31/08—Apparatus for thermally treating combustion-air, fuel, or fuel-air mixture for heating combustion-air or fuel-air mixture by hot gases, e.g. by mixing cold and hot air the gases being exhaust gases
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/30—Use of alternative fuels, e.g. biofuels

Definitions

  • the present invention relates to a biogas reforming system using waste heat and a biogas reforming method using the same. Specifically, 1) a gas engine using biogas as a main fuel, and 2) recovering heat from exhaust gas of the biogas engine. A heat exchanger for raising the temperature of the biogas for use, and 3) catalytic reforming the reformed biogas heated through the heat exchanger into a synthesis gas containing hydrogen, and then introducing the reformed gas into the biogas engine.
  • the present invention relates to a biogas reforming system and a reforming method using waste heat including a reformer.
  • a distributed power source using a gas engine is highly durable and easy to miniaturize, and since it has advantages in terms of cost, it can be commercialized relatively easily.
  • distributed power generation using a gas engine can recover waste heat and improve work loss to improve thermal efficiency, and there is no great difficulty in producing electric power using renewable energy such as biogas along with fossil fuel such as natural gas. It has advantages.
  • Ilbas et al., 2006 measured the laminar flame rates of hydrogen-air and hydrogen-methane-air mixed gases and reported that combustion rates and flammability increased with increasing hydrogen concentration (Ilbas M, Crayford AP, Yilmaz I, Bowen PJ, Syred N. Laminarburning velocities of hydrogen-ir and hydrogen-methane-air mixture: an experimental study.Int J Hydrogen Energy 2006; 31: 1768--79). In the case of gaseous fuels such as methane, hydrogenation has been found to have a significant effect on engine power.
  • the present invention has developed a biogas fuel reforming technology for an on-board type small gas engine generator which does not need to separately supply hydrogen for addition while improving the thermal efficiency of the small gas engine generator.
  • the present invention is to provide a system and method for reforming the waste heat of the exhaust gas to maintain the active temperature of the reforming catalyst, using the same to produce a reformed gas containing hydrogen to enable smooth hydrogen addition to the biogas.
  • the purpose is to provide a system and method for reforming the waste heat of the exhaust gas to maintain the active temperature of the reforming catalyst, using the same to produce a reformed gas containing hydrogen to enable smooth hydrogen addition to the biogas.
  • the present invention provides a heat exchanger for improving the temperature of the reforming biogas and reforming catalyst by recovering heat from the exhaust gas of the biogas engine.
  • a heat exchanger, and 3) waste heat including a reformer for reforming the reformed biogas heated through the heat exchanger into a synthesis gas containing hydrogen and introducing the reformed gas into a biogas engine. It provides a biogas reforming system using.
  • the present invention 1) recovering the exhaust heat of the biogas engine to heat the reforming biogas and reforming catalyst, ii) the hydrogen by using the catalyst as a heated biogas It provides a biogas reforming method using waste heat comprising the step of reforming the synthesis gas included, and iii) introducing the generated reformed gas into the biogas engine.
  • the reforming system and reforming method may use a burner for supplying additional energy required for the reforming reaction if the recovered exhaust heat is not sufficient to cause the reforming reaction, which burner is a gas burner that burns biogas. , An electric heater or a plasma burner.
  • non-fixed (fixed type), fixed (fixed type), U-type (U-type), cylindrical coil (shell and coil type), so that the exhaust gas and the reforming biogas can be exchanged without mixing Plate type or double pipe type heat exchangers may be used.
  • the flow rate of the biogas reformed by the reformer is determined according to the amount of hydrogen gas required by the biogas engine and the reforming efficiency of the catalyst, and the type and size of the heat exchanger is adjusted according to the determined flow rate of the reforming biogas. desirable.
  • the reforming catalyst may be monolith, pellet, or powder type, and the volume of the reforming catalyst may be determined according to the flow rate of biogas introduced into the catalyst for the reforming reaction.
  • Reforming catalyst reaction of the reformer may be a mixture of carbon dioxide reforming reaction (CO 2 reforming), and the reaction is preferred, the carbon dioxide reforming (CO 2 reforming), and partial oxidation reforming (partial oxidation reforming) to increase the efficiency.
  • CO 2 reforming carbon dioxide reforming reaction
  • partial oxidation reforming partial oxidation reforming
  • the reforming catalyst is preferably a precious metal such as platinum (Pt), rhodium (Rh), palladium (Pd), ruthenium (Ru).
  • the thermal efficiency of the small gas engine generator can be improved, and the biogas fuel reforming for the small gas engine generator of the on-board type, which does not need to separately supply hydrogen for addition. You can implement the system.
  • FIG. 1 is an overall configuration diagram of a biogas reforming system of the present invention.
  • FIG. 2 is a cross-sectional view showing an embodiment of a heat exchanger and a reformer constituting the biogas reforming system of the present invention.
  • FIG 3 is a cross-sectional view of a floating type heat exchanger used in the biogas reforming system of the present invention.
  • FIG. 4 is a cross-sectional view of a fixed type heat exchanger used in the biogas reforming system of the present invention.
  • FIG. 5 is a cross-sectional view of a U-type heat exchanger used in the biogas reforming system of the present invention.
  • FIG. 6 is a cross-sectional view of a shell and coil type heat exchanger used in the biogas reforming system of the present invention.
  • FIG. 7 is a cross-sectional view of a plate type heat exchanger used in the biogas reforming system of the present invention.
  • FIG. 8 is a cross-sectional view of a double pipe type heat exchanger used in the biogas reforming system of the present invention.
  • a gas engine containing biogas as a main fuel and 2) recovering heat from exhaust gas of the biogas engine to increase the temperature of the reforming biogas.
  • biogas reforming method using the system 1) recovering the exhaust heat of the biogas engine to heat the reforming biogas, ii) reforming the heated biogas into a synthesis gas containing hydrogen using a catalyst And iii) introducing the generated reformed gas into a biogas engine.
  • biogas In the case of a gas engine generator using biogas as a fuel, carbon dioxide contained in biogas interferes with combustion, resulting in lower overall thermal efficiency and combustion rate than conventional fossil fuels, but adding hydrogen gas having a fast reaction rate to the biogas. This can improve the overall combustion efficiency of the biogas engine.
  • catalyst activation temperature is so high as about 400 °C to 800 °C because a lot of energy input is required, but in the system of the present invention heat exchange to obtain energy for maintaining the catalyst activation temperature from the waste heat of the exhaust gas from the engine Install the machine.
  • the biogas flowing into the gas engine is discharged to the outside through the exhaust pipe in the form of high temperature exhaust gas after combustion reaction inside the cylinder of the engine. This can then be fed back into the gas engine, which in turn improves the overall thermal efficiency of the biogas engine.
  • the heat exchanger may be used in a variety of forms, preferably as shown in Figures 3 to 8, so that the exhaust gas and the reforming biogas is not mixed with each other, floating type (floating type)
  • floating type floating type
  • a fixed type, U-type, shell and coil type, plate type or double pipe type heat exchanger may be used.
  • the biogas supplied with heat from the exhaust gas through the heat exchanger is reformed into a synthesis gas including hydrogen gas through a catalytic reforming reaction in the reformer, and the apparatus including the heat exchanger is installed at a point close to the engine for effective heat recovery. It is preferable.
  • the temperature of the biogas after the heat exchanger is changed according to the flow rate.
  • the flow rate of the biogas required for the reforming reaction is determined according to the required amount of hydrogen reforming gas and the reforming efficiency of the catalyst, and the type and dimensions of the heat exchanger are also affected by the determined flow rate of the biogas.
  • the reformer is a device that supports the reforming catalyst and serves to transfer waste heat of the exhaust gas to the catalyst as well as the heat exchanger.
  • the type of catalyst filled in the reformer may vary depending on the type of fuel and reforming, but can be largely divided into a metal catalyst and a noble metal catalyst, and the temperature and reforming efficiency at which the reforming reaction is activated vary for each catalyst.
  • a metal catalyst to be commonly used may include nickel (Ni), platinum (Pt) as a noble metal catalyst, Rhodium (Rh), palladium (Pd), ruthenium (Ru) and the like can be used.
  • the catalyst activation temperature is relatively low and the active area of the catalyst due to carbon deposition is reduced.
  • the first is a steam reforming method currently used commercially to obtain high purity hydrogen.
  • the steam reforming method is mainly used in steam reforming reaction using natural gas, methane (CH 4 ), carbon dioxide (CO 2 ), carbon monoxide (CO), hydrogen (H 2 ), water (H 2 O), carbon (C Components such as) may be present in the reaction. Reactions that may occur from the steam reforming reaction are as follows.
  • the steam reforming process is a unit reaction process that primarily produces high concentrations of hydrogen by reforming natural gas from which sulfur is removed, and has a higher yield of hydrogen production per mole of methane than the partial oxidation and autothermal reforming processes. It can be called a method.
  • the process size should be large and the response characteristics to the steady state to the load fluctuations are slow.
  • the forward reaction is advantageous only at high temperature and low pressure conditions.
  • the second reforming process is a partial oxidation reforming method, in which a synthesis gas is obtained by supplying oxygen of less than the stoichiometry required for complete combustion with fuel at the same time, accompanied by a weak exothermic reaction by the partial oxidation reaction. .
  • the partial oxidation reforming process does not necessarily require an external heat source, so the reactor is relatively small in size and has excellent initial start-up and load response characteristics.
  • the hydrogen production efficiency is relatively low compared to other processes. Has its drawbacks.
  • the general partial oxidation scheme is as follows.
  • CO 2 reforming process is being actively conducted as part of an effort to chemically convert global warming gas carbon dioxide into a more useful compound, which is a synthesis gas containing a higher concentration of carbon monoxide than a conventional steam reforming reaction. Can be obtained.
  • a general carbon dioxide reaction is as follows.
  • the catalyst can be used in various forms such as monolith, pellet, powder type.
  • the size and volume of the catalyst may be determined in consideration of the flow rate of the biogas flowing into the catalyst for the reforming reaction, in which case the concept of Gas Hourly Space Velocity (GHSV) may be used.
  • GHSV Gas Hourly Space Velocity
  • the equation of gas space velocity is:
  • a separate burner may be installed to supply energy.
  • the position of the gas burner is determined in consideration of effective heat transfer, and may be formed to heat the heat exchanger and the reformer as shown in FIG. 1, or may be formed directly on an exhaust gas line entering the heat exchanger as shown in FIG. 2. have.
  • the burner may be a gas burner that heats exhaust gas, heat exchanger, reformer, etc. with heat released by mixing and burning biogas, oxygen, and air,
  • burners such as an electric heater and a plasma burner may be used.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

La présente invention se rapporte à un système destiné à reformer du biogaz à l'aide de la chaleur perdue et à un procédé de reformage de biogaz utilisant le système. Le système de reformage de biogaz comprend de façon détaillée : 1) un moteur à gaz utilisant du biogaz comme combustible principal ; 2) un échangeur de chaleur récupérant la chaleur provenant du gaz d'échappement du moteur à biogaz afin d'augmenter la température du biogaz de reformage ; et 3) un reformeur acheminant le biogaz de reformage dans le moteur à biogaz une fois que le biogaz de reformage chauffé au moyen de l'échangeur de chaleur a été catalytiquement reformé à l'aide d'un gaz de synthèse contenant de l'hydrogène.
PCT/KR2010/007532 2010-10-29 2010-10-29 Système de reformage de biogaz à l'aide de la chaleur perdue, et procédé de reformage de biogaz utilisant ce système WO2012057380A1 (fr)

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KR1020100106697A KR101136234B1 (ko) 2010-10-29 2010-10-29 폐열을 이용한 바이오가스 개질 시스템 및 바이오가스 개질 방법
KR10-2010-0106697 2010-10-29

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KR101480801B1 (ko) 2013-05-08 2015-01-12 한국화학연구원 이산화탄소 개질반응용 모노리스 촉매, 이의 제조방법 및 이를 이용한 합성가스의 제조방법
KR102435378B1 (ko) 2020-08-21 2022-08-22 조선대학교산학협력단 플라즈마-매트릭스 버너 부분산화 개질기 기반의 태양연료 생산 시스템
KR102483101B1 (ko) * 2020-12-28 2023-01-02 한국에너지기술연구원 암모니아 분해 반응을 이용한 연소 시스템

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JP2005214013A (ja) * 2004-01-27 2005-08-11 Mitsubishi Heavy Ind Ltd メタン含有ガスを供給ガスとした発電システム
JP2009185625A (ja) * 2008-02-04 2009-08-20 Nissan Motor Co Ltd 内燃機関の燃料改質および廃熱回収装置と、燃料改質および廃熱回収方法
KR20100000543A (ko) * 2008-06-25 2010-01-06 한국기계연구원 엔진의 개질가스 공급시스템
JP2010025031A (ja) * 2008-07-22 2010-02-04 Toyota Motor Corp 燃料改質装置
KR20100079282A (ko) * 2008-12-31 2010-07-08 연세대학교 산학협력단 개질기를 이용한 엔진의 유해배출물 저감 장치, 이에사용되는 개질기 및 이를 이용한 엔진의 유해배출물 저감방법

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2005214013A (ja) * 2004-01-27 2005-08-11 Mitsubishi Heavy Ind Ltd メタン含有ガスを供給ガスとした発電システム
JP2009185625A (ja) * 2008-02-04 2009-08-20 Nissan Motor Co Ltd 内燃機関の燃料改質および廃熱回収装置と、燃料改質および廃熱回収方法
KR20100000543A (ko) * 2008-06-25 2010-01-06 한국기계연구원 엔진의 개질가스 공급시스템
JP2010025031A (ja) * 2008-07-22 2010-02-04 Toyota Motor Corp 燃料改質装置
KR20100079282A (ko) * 2008-12-31 2010-07-08 연세대학교 산학협력단 개질기를 이용한 엔진의 유해배출물 저감 장치, 이에사용되는 개질기 및 이를 이용한 엔진의 유해배출물 저감방법

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