WO2022145618A1 - Système de reformage de combustible et méthode de reformage de combustible - Google Patents

Système de reformage de combustible et méthode de reformage de combustible Download PDF

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Publication number
WO2022145618A1
WO2022145618A1 PCT/KR2021/011281 KR2021011281W WO2022145618A1 WO 2022145618 A1 WO2022145618 A1 WO 2022145618A1 KR 2021011281 W KR2021011281 W KR 2021011281W WO 2022145618 A1 WO2022145618 A1 WO 2022145618A1
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WIPO (PCT)
Prior art keywords
fuel
hydrogen
reaction tube
reaction
reforming
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Application number
PCT/KR2021/011281
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English (en)
Korean (ko)
Inventor
송형운
곽현주
윤종혁
정대웅
Original Assignee
고등기술연구원연구조합
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Publication of WO2022145618A1 publication Critical patent/WO2022145618A1/fr

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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
    • B01J38/00—Regeneration or reactivation of catalysts, in general
    • B01J38/02—Heat treatment
    • 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
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • 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
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • 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
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
    • 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

Definitions

  • the present invention relates to a fuel reforming system and a fuel reforming method.
  • a fuel cell is a type of power generation device that generates electric energy by the electrochemical reaction of hydrogen and oxygen extracted from fuel. It is being researched and developed as an alternative.
  • Hydrogen is generally obtained by reforming hydrogen-containing fuels such as alcohol-based fuels (methanol, ethanol, etc.), hydrocarbon-based fuels (methane, butane, propane, etc.), and natural gas-based fuels (liquefied natural gas, etc.) by a fuel reformer.
  • alcohol-based fuels methanol, ethanol, etc.
  • hydrocarbon-based fuels methane, butane, propane, etc.
  • natural gas-based fuels liquefied natural gas, etc.
  • the steam reforming method is mainly used in such a fuel reformer.
  • hydrogen-containing fuel is supplied into the reformer together with water, and reacts with a catalyst in the reformer to produce hydrogen through a hydrogen production reaction. to produce hydrogen
  • heat suitable for the reaction may be supplied by the burner.
  • An object of the present invention is to provide a fuel reforming system and a fuel reforming method capable of improving the life cycle of the reforming catalyst by regenerating the reforming catalyst of the fuel reforming system.
  • Another object of the present invention is to provide a fuel reforming system and a fuel reforming method capable of improving heat conduction efficiency during a reforming reaction and alleviating a temperature deviation problem.
  • Another object of the present invention is to provide a fuel reforming system and a fuel reforming method that can be driven in response to a required load.
  • a fuel reforming system includes a heating furnace; a plurality of reaction tubes installed inside the heating furnace, the reforming catalyst being filled therein, and the reforming reaction in which fuel is converted into reformed gas; a fuel supply unit for supplying a fuel to be reformed to the reaction tube; a hydrogen storage unit storing hydrogen generated in the reaction tube, and selectively supplying hydrogen to the reaction tube; and a burner provided inside the heating furnace to supply heat to the reaction tube, wherein when the hydrogen storage unit supplies hydrogen to the reaction tube, carbon deposited on the reforming catalyst of the reaction tube is separated can be
  • the fuel reforming system and fuel reforming method according to an embodiment of the present invention have the effect of improving the life cycle of the reforming catalyst.
  • heat conduction efficiency during a reforming reaction may be improved, and a temperature deviation problem may be alleviated.
  • the fuel reforming system and fuel reforming method according to an embodiment of the present invention may be driven in response to a required load.
  • FIG. 1 is a schematic configuration diagram of a fuel reforming system according to an embodiment of the present invention.
  • FIG. 2 is a schematic perspective view of a heating furnace and a burner according to an embodiment of the present invention.
  • FIG 3 is a schematic horizontal cross-sectional view of a fuel reforming system according to an embodiment of the present invention.
  • FIG. 4 is a schematic vertical cross-sectional view of a fuel reforming system according to an embodiment of the present invention.
  • FIG. 5 is a schematic cross-sectional view of a reaction tube provided in a fuel reforming system according to an embodiment of the present invention.
  • FIG. 6 is a graph showing the reforming catalyst efficiency of a fuel reforming system and a general fuel reforming system according to an embodiment of the present invention.
  • FIG. 7 is a schematic flowchart of a fuel reforming method according to an embodiment of the present invention.
  • a component when it is said that a component is 'connected', 'supported', or 'contacted' to another component, it may be directly connected, supported, or contacted with the other component, but it is understood that other components may exist in the middle. it should be
  • FIG. 1 is a schematic configuration diagram of a fuel reforming system according to an embodiment of the present invention
  • FIG. 2 is a schematic perspective view of a heating furnace and a burner according to an embodiment of the present invention
  • FIG. 3 is an embodiment of the present invention is a schematic horizontal cross-sectional view of a fuel reforming system according to an embodiment of the present invention
  • FIG. 4 is a schematic vertical cross-sectional view of a fuel reforming system according to an embodiment of the present invention
  • FIG. 5 is a reaction tube provided in the fuel reforming system according to an embodiment of the present invention It is a schematic cross section.
  • a fuel reforming system 1 is installed in a heating furnace 100 and a heating furnace 100, and a reforming catalyst 230 is filled therein.
  • a plurality of reaction tubes 200 in which a reforming reaction in which fuel is converted into reformed gas occurs, a fuel supply unit 300 supplying a fuel to be reformed to the reaction tube 200, and hydrogen generated in the reaction tube 200 are stored,
  • it may include a hydrogen storage unit 400 for supplying hydrogen to the reaction tube 200 and a burner 500 provided inside the heating furnace 100 to supply heat to the reaction tube.
  • the heating furnace 100 may have an outer cylinder wall made of a refractory material, and may have a cylindrical structure in which a space in which fuel (or off-gas) and combustion air are mixed is formed.
  • a burner 500 may be provided on the inner peripheral surface of the heating furnace 100 .
  • the burner 500 may be provided in a cylindrical structure in which a space is formed to correspond to the shape of the inner circumferential surface of the heating furnace 100 . Accordingly, the inner peripheral surface of the heating furnace 100 and the outer peripheral surface of the burner 500 may contact each other.
  • the burner 500 may supply heat necessary for the reforming reaction.
  • the burner 500 may be provided to correspond to the entire inner circumferential surface of the heating furnace 100 and may be provided as an internal cylindrical off-gas burner to which a metal fiber is applied. However, the burner 500 may be replaced with various burners commonly used in the art.
  • a plurality of reaction tubes 200 may be provided inside the heating furnace 100 . More specifically, the reaction tube 200 may be installed inside the burner 500 .
  • reaction tube 200 a reforming reaction in which a fuel such as natural gas is converted into a reformed gas including hydrogen may occur.
  • a plurality of reaction tubes 200 may be provided in a virtual circle having a predetermined radius based on the center of the heating furnace 100 .
  • nine reaction tubes 200 may be provided along the inner circumferential surface of the heating furnace 100 , and the plurality of reaction tubes 200 may include a first group G1 and a second group G2 arbitrarily selected by three. ) and a third group (G3).
  • the reaction tubes 200 belonging to the same group among the plurality of reaction tubes 200 may not be arranged adjacent to each other.
  • the reaction tubes 200 belonging to the second group G2 or the third group G3 may be disposed on both sides of any one reaction tube 200 belonging to the first group G1.
  • the reaction tube 200 is sequentially along the circumferential direction of the heating furnace 100, the reaction tube 200 belonging to the first group (G1), the reaction tube 200 belonging to the second group (G2) and A reaction tube 200 belonging to the third group G3 may be disposed.
  • the reaction tubes 200 belonging to one group may be disposed at the vertices of an imaginary equilateral triangle.
  • the arrangement and number of the reaction tubes 200 may be variously changed according to structural/design needs.
  • the reaction tube 200 may be provided in a double tube shape.
  • the reaction tube 200 includes an outer tube 210 at least partially disposed opposite the burner 500 and forming an outer surface, an inner tube 220 disposed inside the outer tube, and an outer tube 210 and an inner tube 220 .
  • the lower end of the outer tube 210 of the reaction tube 200 may be blocked, and the lower end of the inner tube 220 may have an open structure. Accordingly, the reforming catalyst 230 between the outer tube 210 and the inner tube 220 is provided inside the reaction tube 200, and the first passage 200a and the first passage 200a to which the reforming target fuel or hydrogen is supplied. A second passage 200b in the inner tube 220 that communicates with and through which the gas that has passed through the first passage 200a is discharged may be formed.
  • only the upper end of the reaction tube 200 may be fixed to the heating furnace 100 .
  • the combustion exhaust gas of the burner 500 is in contact with the outside of the reaction tube 200 or heat exchange is conducted through radiant heat of the burner 500, and the raw material supplied to the upper end of the reaction tube 200 is the outer tube 210 and the inner tube.
  • the reforming reaction proceeds while passing through the reforming catalyst 230 filled between 220 .
  • the reformed gas including hydrogen discharged to the lower end of the reaction tube 200 becomes higher than the upper end of the reforming catalyst 230 , and the reformed gas at high temperature is discharged to the upper end of the reaction tube 200 while rising through the inner tube 220 , which is a riser tube.
  • the reforming gas may transfer heat to the reforming catalyst 230 while passing through the inner tube 220 .
  • a valve having a plurality of inlets formed at an upper end of each of the plurality of reaction tubes 200 may be provided, one of the plurality of inlets is connected to the fuel supply unit 300 , and the other of the plurality of inlets is hydrogen storage It may be connected to the unit 400, another one of the plurality of inlets may be connected to the water gas transfer reactor (410).
  • the valve may be provided as, for example, a 3-way valve.
  • the inlet connected to the fuel supply unit 300 is opened so that the fuel to be reformed can be introduced into the reaction tube 200 , and the inlet connected to the hydrogen storage unit 400 is opened during the catalyst regeneration operation to open the reaction tube 200 . ), high-purity hydrogen can be supplied.
  • the inlet of the valve may be selectively opened and closed in response to the hydrogen generating operation or the catalyst regeneration operation.
  • the reformed gas discharged from the reaction tube 200 may sequentially pass through the water gas transfer reactor 410 and the gas purifier 420, PSA. Through this series of processes, the hydrogen contained in the reformed gas is purified to high purity.
  • High purity hydrogen purified by the gas purifier 420 may be stored in the hydrogen storage unit 430 .
  • the hydrogen storage unit 430 may store high-purity hydrogen purified through a reforming process and a refining process. In this case, the hydrogen storage unit 430 may supply stored hydrogen to the reaction tube 200 during the catalyst regeneration operation.
  • the fuel reforming system 1 may improve reforming catalyst efficiency by supplying hydrogen stored in the hydrogen storage unit 400 to the reaction tube 200 .
  • carbon (C) is deposited on the surface of the reforming catalyst during the reforming reaction, and as carbon (C) deposition proceeds, the efficiency of the reforming catalyst may decrease.
  • by supplying hydrogen stored in the hydrogen storage unit 400 to the reaction tube 200 deposition on the surface of the reforming catalyst through a metallization reaction (C)
  • the converted carbon may be discharged as methane (CH 4 ).
  • the catalyst regeneration operation may be performed in the other reaction tubes 200 in which the hydrogen generating operation does not proceed.
  • FIG. 6 is a graph showing the reforming catalyst efficiency (c1) of the fuel reforming system and the reforming catalyst efficiency (c2) of a general fuel reforming system according to an embodiment of the present invention.
  • the efficiency of the reforming catalyst continuously decreases and thus has a relatively short replacement cycle L1.
  • the replacement cycle may mean a time for which the reforming catalyst efficiency reaches the reforming catalyst efficiency limit value T1.
  • the fuel reforming system 1 according to an embodiment of the present invention includes sections r1, r2, r3, r4, r5, r6, r7, r8 for improving the efficiency of the reforming catalyst through repeated catalyst regeneration operations. may be included, and thus may have an improved replacement cycle L2.
  • the fuel reforming system 1 may be driven by following a required load.
  • the reaction tube 200 may be provided in nine, and the plurality of reaction tubes 200 are arbitrarily selected by three in a first group (G1), a second group (G2), and a third group (G3). can be classified.
  • the reaction tube 200 belonging to the first group G1 may perform a hydrogen generation operation, and the reaction tube 200 belonging to the second group G2 and the third group G3 ( 200) may perform a catalyst regeneration operation.
  • reaction tube 200 belonging to the first group G1 and the second group G2 may perform a hydrogen generation operation, and the half tube belonging to the third group G3 ( 200) may perform a catalyst regeneration operation.
  • the reaction tube 200 belonging to the first group G1 , the second group G2 , and the third group G3 may perform a hydrogen generation operation.
  • the efficiency of the reforming catalyst 230 due to carbon deposition among the reaction tubes 200 belonging to the group that does not perform the hydrogen generation operation is recognized as below a predetermined efficiency.
  • the step of supplying the reforming target fuel to the reaction tube 200 through the fuel supply unit 300 ( S10 ) may be performed first.
  • hydrogen-containing fuels such as alcohol-based fuels (methanol, ethanol, etc.), hydrocarbon-based fuels (methane, butane, propane, etc.), and natural gas-based fuels (liquefied natural gas, etc.) may be used.
  • a step ( S20 ) of generating a mixed gas including hydrogen through a reforming reaction in the reaction tube 200 may be performed.
  • the reforming target fuel may be reformed by the reforming catalyst 230 while flowing through the first passage 200a of the reaction tube 200 . Thereafter, the gas mixture on which the reforming reaction is completed may be discharged through the second passage 200b.
  • a step of purifying the mixed gas generated in the reaction tube 200 to extract high-purity hydrogen and storing it in the hydrogen storage unit 400 may be performed.
  • a hydrogen generation operation may be performed through such a series of processes.
  • the catalyst regeneration operation may be performed through the step S40 of supplying hydrogen stored in the hydrogen storage unit 400 to the reaction tube 200 .
  • hydrogen may separate carbon on the surface of the reforming catalyst through a methanation reaction with the reforming catalyst 230 .
  • the fuel reforming system 1 and the fuel reforming method according to the embodiment of the present invention described above may improve the life cycle of the reforming catalyst through the catalyst regeneration operation.
  • the burner including the metal fiber heat transfer efficiency during the reforming reaction may be improved and the temperature deviation problem may be alleviated.
  • there is an effect that the load following operation is possible by adjusting the number of reaction tubes that perform the hydrogen generating operation in response to the required load.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)

Abstract

Un système de reformage de combustible selon un mode de réalisation de la présente invention comprend : un four de chauffage ; une pluralité de tubes de réaction qui sont installés à l'intérieur du four de chauffage et ont un catalyseur de reformage qui est rempli à l'intérieur de ceux-ci et dans lesquels a lieu une réaction de reformage pour convertir le combustible en gaz reformé ; une unité d'alimentation en combustible pour fournir un combustible devant être reformé aux tubes de réaction ; une unité de stockage d'hydrogène pour stocker l'hydrogène généré dans les tubes de réaction et fournir sélectivement de l'hydrogène aux tubes de réaction ; et un brûleur disposé à l'intérieur du four de chauffage pour fournir de la chaleur au tube de réaction, lorsque l'unité de stockage d'hydrogène fournit de l'hydrogène aux tubes de réaction, du carbone déposé sur le catalyseur de reformage des tubes de réaction pouvant être séparé.
PCT/KR2021/011281 2020-12-30 2021-08-24 Système de reformage de combustible et méthode de reformage de combustible WO2022145618A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR10-2020-0187393 2020-12-30
KR1020200187393A KR102316259B1 (ko) 2020-12-30 2020-12-30 연료 개질 시스템 및 연료 개질 방법

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11814288B2 (en) 2021-11-18 2023-11-14 8 Rivers Capital, Llc Oxy-fuel heated hydrogen production process
US11859517B2 (en) 2019-06-13 2024-01-02 8 Rivers Capital, Llc Power production with cogeneration of further products
US11891950B2 (en) 2016-11-09 2024-02-06 8 Rivers Capital, Llc Systems and methods for power production with integrated production of hydrogen

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20030045965A (ko) * 2001-12-03 2003-06-12 (주)세티 연료전지용 연료개질기
JP2009119307A (ja) * 2007-11-09 2009-06-04 Japan Science & Technology Agency 触媒の再生方法
KR20090081997A (ko) * 2008-01-25 2009-07-29 에스케이에너지 주식회사 고성능 메탈 화이버 버너를 이용한 수증기 개질장치 및상기 수증기 개질장치가 포함된 수소 스테이션
KR100971743B1 (ko) * 2007-12-27 2010-07-21 삼성에스디아이 주식회사 연료 전지 시스템 및 연료 전지 시스템용 개질기
KR102149149B1 (ko) * 2020-01-29 2020-08-28 연세대학교 산학협력단 수소 생산 장치 및 이를 이용한 수소 생산 방법

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20030045965A (ko) * 2001-12-03 2003-06-12 (주)세티 연료전지용 연료개질기
JP2009119307A (ja) * 2007-11-09 2009-06-04 Japan Science & Technology Agency 触媒の再生方法
KR100971743B1 (ko) * 2007-12-27 2010-07-21 삼성에스디아이 주식회사 연료 전지 시스템 및 연료 전지 시스템용 개질기
KR20090081997A (ko) * 2008-01-25 2009-07-29 에스케이에너지 주식회사 고성능 메탈 화이버 버너를 이용한 수증기 개질장치 및상기 수증기 개질장치가 포함된 수소 스테이션
KR102149149B1 (ko) * 2020-01-29 2020-08-28 연세대학교 산학협력단 수소 생산 장치 및 이를 이용한 수소 생산 방법

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11891950B2 (en) 2016-11-09 2024-02-06 8 Rivers Capital, Llc Systems and methods for power production with integrated production of hydrogen
US11859517B2 (en) 2019-06-13 2024-01-02 8 Rivers Capital, Llc Power production with cogeneration of further products
US11814288B2 (en) 2021-11-18 2023-11-14 8 Rivers Capital, Llc Oxy-fuel heated hydrogen production process

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