KR20060103631A - Reforming reactor for fuel cell and manufacturing method thereof - Google Patents
Reforming reactor for fuel cell and manufacturing method thereof Download PDFInfo
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- KR20060103631A KR20060103631A KR1020050025432A KR20050025432A KR20060103631A KR 20060103631 A KR20060103631 A KR 20060103631A KR 1020050025432 A KR1020050025432 A KR 1020050025432A KR 20050025432 A KR20050025432 A KR 20050025432A KR 20060103631 A KR20060103631 A KR 20060103631A
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- 239000000446 fuel Substances 0.000 title claims abstract description 53
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 10
- 239000000758 substrate Substances 0.000 claims abstract description 62
- 229910052751 metal Inorganic materials 0.000 claims abstract description 61
- 239000002184 metal Substances 0.000 claims abstract description 61
- 239000003054 catalyst Substances 0.000 claims abstract description 41
- 239000011148 porous material Substances 0.000 claims abstract description 39
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 17
- 238000000034 method Methods 0.000 claims description 15
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 14
- 239000010949 copper Substances 0.000 claims description 14
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 12
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims description 12
- 239000002253 acid Substances 0.000 claims description 12
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 12
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- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 8
- 239000011787 zinc oxide Substances 0.000 claims description 8
- 238000002048 anodisation reaction Methods 0.000 claims description 6
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- 235000006408 oxalic acid Nutrition 0.000 claims description 4
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- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 2
- KRVSOGSZCMJSLX-UHFFFAOYSA-L chromic acid Substances O[Cr](O)(=O)=O KRVSOGSZCMJSLX-UHFFFAOYSA-L 0.000 claims description 2
- 238000007598 dipping method Methods 0.000 claims description 2
- AWJWCTOOIBYHON-UHFFFAOYSA-N furo[3,4-b]pyrazine-5,7-dione Chemical compound C1=CN=C2C(=O)OC(=O)C2=N1 AWJWCTOOIBYHON-UHFFFAOYSA-N 0.000 claims description 2
- 229910017604 nitric acid Inorganic materials 0.000 claims description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims 1
- 239000002245 particle Substances 0.000 claims 1
- 229910052698 phosphorus Inorganic materials 0.000 claims 1
- 239000011574 phosphorus Substances 0.000 claims 1
- 239000012530 fluid Substances 0.000 abstract description 15
- 239000000243 solution Substances 0.000 description 9
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 8
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
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- 238000007743 anodising Methods 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 5
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- 230000000694 effects Effects 0.000 description 4
- 230000005611 electricity Effects 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 3
- 239000003792 electrolyte Substances 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 239000005518 polymer electrolyte Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000005229 chemical vapour deposition Methods 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- NFFYXVOHHLQALV-UHFFFAOYSA-N copper(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Cu].[Cu] NFFYXVOHHLQALV-UHFFFAOYSA-N 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000000151 deposition Methods 0.000 description 1
- 238000007606 doctor blade method Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000003487 electrochemical reaction Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000003628 erosive effect Effects 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000006057 reforming reaction Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 238000004804 winding Methods 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
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- 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
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
- C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
- C01B3/26—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
- H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
- H01M8/0625—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material in a modular combined reactor/fuel cell structure
- H01M8/0631—Reactor construction specially adapted for combination reactor/fuel cell
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- C01B2203/02—Processes for making hydrogen or synthesis gas
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Abstract
본 발명은 연료전지용 개질 반응기 및 그 제조방법에 관한 것으로서, 보다 상세하게는 평균 직경 0.001 내지 1000㎛의 기공이 형성된 금속 기재, 및 상기 금속 기재에 부착된 개질 촉매를 포함하는 연료전지용 개질 반응기 및 그 제조방법에 관한 것이다. The present invention relates to a reforming reactor for a fuel cell and a manufacturing method thereof, and more particularly to a reforming reactor for a fuel cell including a metal substrate having pores having an average diameter of 0.001 to 1000 µm, and a reforming catalyst attached to the metal substrate. It relates to a manufacturing method.
본 발명의 연료전지용 개질 반응기는 기공이 형성된 금속기재에 개질촉매가 부착되어 있으므로, 촉매의 부착량이 많고, 상기 개질 반응기의 표면을 따라 유체를 흘려보내는 경우에도 기공 속으로 일부의 유체가 흘러들어가게 되어, 유체 및 열의 흐름 효율이 우수한 장점을 가진다. The reforming reactor for a fuel cell of the present invention has a reforming catalyst attached to a metal substrate having pores, so that the amount of adhesion of the catalyst is large, and some fluid flows into the pores even when the fluid flows along the surface of the reforming reactor. In addition, the fluid and heat flow efficiency is excellent.
연료전지, 개질기, 개질 반응기, 촉매, 기공, 금속 기재 Fuel cells, reformers, reforming reactors, catalysts, pores, metal substrates
Description
도 1은 본 발명의 개질 반응기의 일 예를 모식적으로 나타낸 사시도.1 is a perspective view schematically showing an example of a reforming reactor of the present invention.
[산업상 이용분야][Industrial use]
본 발명은 연료전지용 개질 반응기 및 그 제조방법에 관한 것으로서, 보다 상세하게는 촉매 부착량이 많고, 개질 촉매와 유체 및 열의 접촉 효율이 우수한 연료전지용 개질 반응기 및 그 제조방법에 관한 것이다.The present invention relates to a reforming reactor for a fuel cell and a method of manufacturing the same, and more particularly, to a reforming reactor for a fuel cell and a method for producing the same having a large amount of catalyst adhesion and excellent contact efficiency between the reforming catalyst, fluid and heat.
[종래기술][Private Technology]
일반적으로, 연료 전지는 메탄올, 에탄올 또는 천연가스 등 탄화수소 계열의 유기연료 내에 함유되어 있는 수소를 연료로 하여 일어나는 전기화학 반응에 의하여 화학에너지를 직접 전기에너지로 변화시키는 발전 시스템이다. 유기 연료의 높은 비에너지(specific energy)(예를 들어 메탄올의 비에너지는 6232wh/kg임) 때문에 유기 연료를 사용하는 연료 전지는 설치상 또는 휴대상 모두 극도로 매력적이다. In general, a fuel cell is a power generation system that directly converts chemical energy into electrical energy by an electrochemical reaction generated by using hydrogen contained in a hydrocarbon-based organic fuel such as methanol, ethanol, or natural gas as a fuel. Because of the high specific energy of organic fuels (eg, the specific energy of methanol is 6232 wh / kg), fuel cells using organic fuels are extremely attractive both in installation and in portable applications.
이러한 연료 전지는 사용하는 전해질의 종류에 따라, 인산형 연료전지, 용융탄산염 형 연료전지, 고체 산화물형 연료전지, 고분자 전해질형 연료전지, 및 알칼리형 연료전지 등으로 분류되며, 이들 각각의 연료전지는 근본적으로 같은 원리에 의해 작동하나, 연료의 종류, 운전 온도, 촉매 및 전해질이 서로 다르다.Such fuel cells are classified into phosphoric acid fuel cells, molten carbonate fuel cells, solid oxide fuel cells, polymer electrolyte fuel cells, and alkaline fuel cells according to the type of electrolyte used. Operates essentially on the same principle, but differs in fuel type, operating temperature, catalyst and electrolyte.
이 중에서 근래에 개발되고 있는 고분자 전해질형 연료 전지(Polymer Electrolyte Membrance Fuel Cell: PEMFC)는, 다른 연료 전지에 비하여 출력 특성이 탁월하고 작동 온도가 낮을 뿐 아니라, 빠른 시동 및 응답 특성을 가지며, 자동차와 같은 이동용 전원은 물론, 주택, 공공건물과 같은 분산용 전원 및 전자기기용과 같은 소형 전원 등 그 응용 범위가 넓은 장점을 가지고 있다.Among these, polymer electrolyte fuel cells (PEMFCs), which have been recently developed, have superior output characteristics and lower operating temperatures than other fuel cells, and have fast starting and response characteristics. In addition to the mobile power source, there is a wide range of applications such as distributed power supply such as homes, public buildings and small power supply such as for electronic devices.
상기와 같은 PEMFC는 기본적으로 시스템을 구성하기 위해 전기발생부(또는 스택(stack)), 개질기(Reformer), 연료공급부 등을 구비한다. 전기발생부는 연료 전지의 본체를 형성하며, 연료공급부는 연료를 개질기로 공급한다. 개질기는 연료를 개질하여 수소 가스를 발생시키고 그 수소 가스를 전기발생부로 공급한다. 전기발생부에서는 공급된 수소 가스와 산소를 전기 화학적으로 반응시켜 전기에너지를 발생시킨다.Such a PEMFC basically includes an electric generator (or stack), a reformer, a fuel supply unit, etc. to configure a system. The electricity generating portion forms the main body of the fuel cell, and the fuel supply portion supplies the fuel to the reformer. The reformer reforms the fuel to generate hydrogen gas and supplies the hydrogen gas to the electricity generator. The electricity generating unit generates electric energy by electrochemically reacting the supplied hydrogen gas and oxygen.
이 중에서도 상기 개질기는 수소를 함유한 연료와 물을 개질하여 스택의 전기 생성에 필요한 수소 가스로 전환시키는 개질 반응기를 포함하며, 연료 전지의 수명을 단축시키는 일산화탄소와 같은 유해 물질을 제거하는 장치이다. Among these, the reformer includes a reforming reactor for reforming a hydrogen-containing fuel and water and converting the fuel into hydrogen gas for generating electricity of the stack, and removing the harmful substances such as carbon monoxide, which shortens the life of the fuel cell.
일반적인 개질 반응기는 유로가 형성된 기판에 개질 촉매가 도포된 형태 또는 원통형 관의 내부에 개질 촉매가 채워진 형태를 가지고 있다. 그러나, 기판의 유로 또는 관의 내부가 매끄러운 표면을 가지기 때문에, 촉매의 부착량이 적고, 유체가 한쪽 방향으로만 흘러가게 되므로 개질 촉매와 유체 및 열의 접촉 효율이 좋지 못한 문제점이 있다.A general reforming reactor has a form in which a reforming catalyst is applied to a substrate on which a flow path is formed, or a reforming catalyst is filled in a cylindrical tube. However, since the inside of the channel or tube of the substrate has a smooth surface, there is a problem in that the amount of adhesion of the catalyst is small and the fluid flows only in one direction, so that the efficiency of contact between the reforming catalyst and the fluid and heat is poor.
본 발명은 상기와 같은 문제점을 해결하기 위한 것으로서, 본 발명의 목적은 기공이 형성된 금속 기재와 개질 촉매를 포함하는 연료전지용 개질 반응기 및 그 제조방법을 제공하는 것이다. The present invention is to solve the above problems, it is an object of the present invention to provide a reforming reactor for a fuel cell comprising a metal substrate and a reforming catalyst having pores and a method of manufacturing the same.
본 발명은 상기 목적을 달성하기 위하여, 평균 직경 0.001 내지 1000 ㎛의 기공이 형성된 금속 기재; 및 상기 금속 기재에 부착된 개질 촉매를 포함하는 연료전지용 개질 반응기를 제공한다.The present invention, in order to achieve the above object, a metal substrate having pores with an average diameter of 0.001 to 1000 ㎛; And it provides a reforming reactor for a fuel cell comprising a reforming catalyst attached to the metal substrate.
본 발명은 또한, 양극산화법으로 금속기재에 미세기공(micro pore)을 형성시키는 단계, 미세기공이 형성된 금속기재를 산소 존재 하에서 열처리하여 거대기공(macro pore)를 형성시키는 단계, 및 거대기공이 형성된 금속기재에 개질 촉매를 부착시키는 단계를 포함하는 연료전지용 개질 반응기의 제조방법을 제공한다.The present invention also provides a step of forming micro pores on a metal substrate by anodizing, heat treating the metal substrate on which micro pores are formed in the presence of oxygen to form macro pores, and forming macro pores. It provides a method for producing a reforming reactor for a fuel cell comprising the step of attaching a reforming catalyst to a metal substrate.
이하, 본 발명을 보다 상세하게 설명한다. Hereinafter, the present invention will be described in more detail.
본 발명에서 연료전지용 개질 반응기는 개질기에 포함되는 실질적인 개질 반응부를 의미한다. In the present invention, the reforming reactor for a fuel cell means a substantial reforming reaction unit included in the reformer.
본 발명의 개질 반응기가 특별한 형상으로 한정되는 것은 아니며, 판상, 양 끝단이 개방된 원통형, 판상의 금속기재를 와인딩한 형태, 또는 다른 어떠한 형태 도 가질 수 있고, 양 끝단이 개방된 원통형, 또는 판상의 금속기재를 와인딩한 형태인 것이 바람직하다. The reforming reactor of the present invention is not limited to a particular shape, and may have a plate shape, a cylindrical shape with both ends open, a shape of winding a plate metal substrate, or any other shape, and a cylindrical shape or plate shape with both ends open. It is preferable that the metal base is wound.
도 1은 와인딩한 형태의 금속기재를 포함하는 본 발명의 개질 반응기의 일 예를 모식적으로 나타낸 사시도이다. 도 1에서 보는 바와 같이, 본 발명의 개질 반응기(10)는 평균 직경 0.001 내지 1000㎛의 기공(12)이 형성된 금속 기재(11), 및 상기 금속 기재(11)에 부착된 개질 촉매(13)를 포함한다. 1 is a perspective view schematically showing an example of the reforming reactor of the present invention including a metal substrate in a wound form. As shown in FIG. 1, the reforming
상기 금속기재의 기공은 상기 금속기재의 표면에만 형성될 수도 있으나, 금속기재를 관통하여 유체가 흘러지나갈 수 있도록 형성되는 것이 더 바람직하다. Pores of the metal substrate may be formed only on the surface of the metal substrate, it is more preferably formed so that the fluid can flow through the metal substrate.
상기 금속기재는 알루미늄, 구리, 아연, 철, 티타늄, 지르코늄 및 이들 중 둘 이상을 포함하는 합금으로 이루어진 군에서 선택되는 1종 이상의 금속을 산화시킨 것이며, 보다 바람직하게는 금속기재를 양극산화 및 열처리하여 금속을 산화시킴으로써, 기공을 형성시킨 것이다. The metal substrate is oxidized at least one metal selected from the group consisting of aluminum, copper, zinc, iron, titanium, zirconium, and alloys containing two or more thereof, more preferably anodizing and heat treating the metal substrate. By oxidizing the metal, pores are formed.
따라서, 상기 금속기재는 알루미늄 산화물(Al2O3), 구리산화물(Cu2O3), 아연산화물(ZnO), 철산화물(FeO, Fe2O3, Fe3O4), 티타늄 산화물(TiO2) 및 지르코늄 산화물(ZrO2)로 이루어진 군에서 선택되는 1종 이상의 금속산화물을 포함한다. Therefore, the metal substrate may be aluminum oxide (Al 2 O 3 ), copper oxide (Cu 2 O 3 ), zinc oxide (ZnO), iron oxide (FeO, Fe 2 O 3 , Fe 3 O 4 ), titanium oxide (TiO 2 ) and zirconium oxide (ZrO 2 ) and at least one metal oxide selected from the group consisting of.
상기 금속기재에 형성된 기공의 평균직경은 0.001 내지 1000 ㎛인 것이 바람직하며, 100 내지 1000 ㎛인 것이 더 바람직하다. 기공의 평균직경이 0.001 ㎛미만인 경우에는 촉매 부착시에 기공이 막혀 개질 효율이 오히려 떨어질 수 있으며, 1000 ㎛를 초과하는 경우에는 촉매의 부착량이 감소한다. The average diameter of the pores formed in the metal substrate is preferably 0.001 to 1000 ㎛, more preferably 100 to 1000 ㎛. If the average diameter of the pores is less than 0.001 μm, the pores may be blocked at the time of catalyst adhesion, and the reforming efficiency may be lowered. If the average diameter is more than 1000 μm, the amount of adhesion of the catalyst decreases.
상기 금속기재에 형성된 기공의 기공 밀도는 1 내지 100 개/m2인 것이 바람직하며, 10 내지 50 개/m2인 것이 더 바람직하다. 금속기재의 기공도가 1 개/m2 미만인 경우에는 기공 형성의 효과가 미미하며, 100 개/m2를 초과하는 경우에는 충분한 평균직경을 가지는 기공을 형성하기 어렵다. The pore density of the pores formed in the metal substrate is preferably 1 to 100 / m 2 , more preferably 10 to 50 / m 2 . If the porosity of the metal substrate is less than 1 / m 2, the effect of pore formation is insignificant, and if it exceeds 100 / m 2 , it is difficult to form pores having a sufficient average diameter.
상기 금속기재에 부착되는 개질 촉매는 통상적인 개질 촉매를 모두 포함하며, 바람직하게는 백금(Pt), 루테늄(Ru), 구리(Cu), 구리/산화아연(Cu/ZnO), 철(Fe) 및 니켈(Ni)로 이루어진 군으로부터 선택되는 1종 이상이다.The reforming catalyst attached to the metal substrate includes all conventional reforming catalysts, preferably platinum (Pt), ruthenium (Ru), copper (Cu), copper / zinc oxide (Cu / ZnO), iron (Fe) And nickel (Ni).
상기 개질 촉매는 상기 금속기재의 표면 및 기공 내부에 어떤 형태로든 존재할 수 있으며, 바람직하게는 딥핑법으로 개질 촉매를 부착시키거나, 스퍼터링, 열화학증착법(Thermal CVD), 플라즈마강화 화학증착법(Plasma Enhanced CVD; PECVD), 열증발법 또는 전자선(e-beam)증발법 등에서 선택되는 증착법으로 부착시킨 것일 수 있다. The reforming catalyst may be present in any form on the surface of the metal substrate and in the pores. Preferably, the reforming catalyst is attached by a dipping method, sputtering, thermal CVD, plasma enhanced CVD. PECVD), thermal evaporation, or e-beam evaporation.
본 발명의 연료전지용 개질 반응기는 유체 도입부와 유체 배출부가 형성된 밀폐 용기 안에 설치되어 연료 및 물의 혼합연료로부터 수소 가스를 발생시키는 역할을 한다. The reforming reactor for a fuel cell of the present invention is installed in a sealed container in which a fluid inlet and a fluid outlet are formed to generate hydrogen gas from a mixed fuel of fuel and water.
또한, 상기 개질 반응기는 금속 기재의 표면 및 기공 내부에도 개질 촉매를 포함하며, 상기 개질 반응기의 표면을 따라 유체를 흘려보내는 경우에도 상기 금속기재의 표면과 수직한 방향으로 형성된 기공 속으로 일부의 유체가 흘러들어가게 되어, 유체 및 열의 흐름 효율이 우수한 장점을 가진다. In addition, the reforming reactor includes a reforming catalyst on the surface of the metal substrate and inside the pores, and in the case of flowing a fluid along the surface of the reforming reactor, a part of the fluid into the pores formed in a direction perpendicular to the surface of the metal substrate. Is flowed in, the fluid and heat flow efficiency is excellent.
본 발명의 연료전지용 개질 반응기는 양극산화법으로 금속기재에 미세기공(micro pore)을 형성시키는 단계, 미세기공이 형성된 금속기재를 산소 존재 하에서 열처리하여 거대기공(macro pore)를 형성시키는 단계, 및 거대기공이 형성된 금속기재에 개질 촉매를 부착시키는 단계를 포함하는 연료전지용 개질 반응기의 제조방법에 따라 제조될 수 있다. The reforming reactor for a fuel cell of the present invention comprises the steps of forming micro pores on a metal substrate by anodizing, heat treating the metal substrate on which the micro pores are formed in the presence of oxygen, and forming macro pores. It can be prepared according to the method for producing a reforming reactor for a fuel cell comprising the step of attaching a reforming catalyst to the metal substrate having pores.
상기 양극산화법은 금속기재를 산 용액에 침지시킨 후, 전압을 걸어 산화시키는 방법을 말하며, 산 용액의 침식작용으로 금속기재에 미세기공을 형성시킨다. The anodizing method refers to a method of oxidizing a metal substrate by immersing the metal substrate in an acid solution, and applying a voltage to form a micropore in the metal substrate by erosion of the acid solution.
상기 양극산화법에 사용되는 금속기재는 알루미늄, 구리, 아연, 철 및 이들 중 둘 이상을 포함하는 합금으로 이루어진 군에서 선택되는 1종 이상의 금속을 포함하는 것이 바람직하다. The metal substrate used in the anodization method preferably includes at least one metal selected from the group consisting of aluminum, copper, zinc, iron, and alloys containing two or more thereof.
상기 양극산화법에 사용되는 산 용액은 전해액의 역할을 하며, 산 용액에 포함되는 산의 농도는 1 부피% 내지 50 부피%인 것이 바람직하고, 5 부피% 내지 10 부피% 인 것이 더 바람직하다. 상기 산의 농도가 1 부피% 미만인 경우에는 양극산화의 효과가 미미하며, 50 부피%를 초과하는 경우에는 과도한 산화로 금속기재의 구조가 붕괴될 수 있다.The acid solution used in the anodic oxidation method serves as an electrolyte, and the concentration of the acid contained in the acid solution is preferably 1% by volume to 50% by volume, more preferably 5% by volume to 10% by volume. If the acid concentration is less than 1% by volume, the effect of anodization is insignificant, and if it exceeds 50% by volume, the structure of the metal substrate may collapse due to excessive oxidation.
상기 산 용액은 옥살산, 황산, 크롬산, 및 질산으로 이루어진 군에서 선택되는 1종 이상의 산을 포함하는 것이 바람직하며, 그 중에서도 옥살산, 황산, 또는 이들의 혼합물을 포함하는 것이 더 바람직하다. The acid solution preferably includes at least one acid selected from the group consisting of oxalic acid, sulfuric acid, chromic acid, and nitric acid, more preferably oxalic acid, sulfuric acid, or mixtures thereof.
상기 양극산화법에서 금속기재에 인가되는 전압은 10 내지 50 V인 것이 바람직하며, 20 내지 40 V인 것이 더 바람직하다. 또한, 상기 전압은 직류전압인 것이 바람직하다. 인가 전압이 직류 10 V 미만인 경우에는 양극 산화 반응의 발생이 미미하며, 50 V를 초과하는 경우에는 높은 반응 속도로 인한 반응기 온도 제어의 어려움이 있다.In the anodic oxidation method, the voltage applied to the metal substrate is preferably 10 to 50 V, more preferably 20 to 40 V. In addition, the voltage is preferably a DC voltage. When the applied voltage is less than 10 V DC, the occurrence of the anodic oxidation reaction is insignificant, and when it exceeds 50 V, there is a difficulty in controlling the reactor temperature due to the high reaction rate.
상기 양극산화법으로 미세기공이 형성된 금속 기재를 산소 존재 하에서 열처리하여 거대기공(macro pore)를 형성시킨다. 이 때, 상기 열처리 온도는 500 내지 700 ℃인 것이 바람직하며, 550 내지 600 ℃인 것이 더 바람직하다. 열처리 온도가 500℃ 미만인 경우에는 산화 반응의 발생이 미미하며, 700 ℃를 초과하는 경우에는 금속 기재의 용융 및 휘발로 인한 구조 붕괴의 우려가 있다. The metal substrate on which the micropores are formed by the anodization is heat-treated in the presence of oxygen to form macropores. At this time, the heat treatment temperature is preferably 500 to 700 ° C, more preferably 550 to 600 ° C. If the heat treatment temperature is less than 500 ° C, the occurrence of oxidation reactions is insignificant, and if it exceeds 700 ° C, there is a fear of structural collapse due to melting and volatilization of the metal substrate.
상기 열처리에 의해 형성된 거대기공은 0.001 내지 1000 ㎛의 평균직경을 가지며, 바람직하게는 100 내지 1000 ㎛의 평균직경을 가진다. The macropores formed by the heat treatment have an average diameter of 0.001 to 1000 μm, and preferably have an average diameter of 100 to 1000 μm.
상기 방법으로 기공이 형성된 금속기재에 촉매를 부착시켜 본 발명의 연료전지용 개질 반응기를 제조할 수 있다. By attaching the catalyst to the metal substrate having the pores formed in the above method, the reforming reactor for a fuel cell of the present invention may be manufactured.
상기 촉매의 부착방법은 기공이 형성된 금속기재를 촉매 용액에 딥핑한 후 건조시키는 방법, 스프레이 코팅법, 또는 닥터블레이드법 등의 습식 코팅 방법과 스퍼터링, 열화학증착법(Thermal CVD), 플라즈마강화 화학증착법(Plasma Enhanced CVD; PECVD), 열증발법 또는 전자선(e-beam)증발법 등에서 선택되는 증착법으로 부착시키는 방법이 있다. The method of attaching the catalyst is a method of dripping a metal substrate having pores into a catalyst solution and then drying it, a wet coating method such as a spray coating method, or a doctor blade method, and sputtering, thermal CVD, and thermally enhanced chemical vapor deposition ( Plasma Enhanced CVD (PECVD), thermal evaporation, or e-beam evaporation may be applied by a deposition method selected from evaporation.
상기 금속기재에 부착되는 개질 촉매는 통상적인 개질 촉매가 모두 사용될 수 있으며, 바람직하게는 백금(Pt), 루테늄(Ru), 구리(Cu), 구리/산화아연(Cu/ZnO), 철(Fe) 및 니켈(Ni)로 이루어진 군으로부터 선택되는 1종 이상이 사용될 수 있다. The reforming catalyst attached to the metal substrate may be any conventional reforming catalyst, preferably platinum (Pt), ruthenium (Ru), copper (Cu), copper / zinc oxide (Cu / ZnO), iron (Fe) ) And one or more selected from the group consisting of nickel (Ni) can be used.
이하, 본 발명의 바람직한 실시예를 기재한다. 다만, 하기의 실시예는 본 발명의 바람직한 일 실시예일 뿐, 본 발명이 하기 실시예에 의해 한정되는 것은 아니다.Hereinafter, preferred embodiments of the present invention are described. However, the following examples are only preferred embodiments of the present invention, and the present invention is not limited to the following examples.
[실시예]EXAMPLE
실시예 1Example 1
두께 50 ㎛, 폭 1 cm, 길이 10 cm인 판상(plate)의 알루미늄을 0.5 mm의 간격을 가지도록 길이방향으로 와인딩하여, 도 1의 금속기재와 같은 형태로 와인딩된 원통형 구조를 형성하였다. 상기 원통형 알루미늄 기재를 옥살산(H2C2O4) 수용액(5 중량% 농도)에 침지하고, 상온에서 DC 50 V의 전압을 걸어 양극산화 처리하여 알루미늄 기재에 미세기공을 형성시켰다.50 μm thick, 1 cm wide and 10 cm long The plate-shaped aluminum was wound in the longitudinal direction to have a distance of 0.5 mm, thereby forming a cylindrical structure wound in the same shape as the metal substrate of FIG. 1. The cylindrical aluminum substrate was immersed in an aqueous solution of oxalic acid (H 2 C 2 O 4 ) (5 wt% concentration), and subjected to anodizing at a voltage of DC 50 V to form micropores in the aluminum substrate.
상기 미세기공이 형성된 알루미늄 기재를 산소 환경에서 500 ℃로 열처리하여 거대기공을 형성시켰다. The aluminum substrate having the micropores was heat-treated at 500 ° C. in an oxygen environment to form macropores.
또한, 개질 촉매인 구리 분말을 이소프로필알코올에 분산시켜 촉매 용액을 제조한 후, 상기 거대기공이 형성된 알루미늄 기재를 상기 촉매 용액에 침지하고, 90 ℃에서 건조하여 연료전지용 개질 반응기를 제조하였다.In addition, after dispersing a copper powder as a reforming catalyst in isopropyl alcohol to prepare a catalyst solution, the aluminum substrate having the macropores was immersed in the catalyst solution, and dried at 90 ° C. to produce a reforming reactor for a fuel cell.
실시예 2Example 2
산 용액으로 황산(H2SO4) 수용액(5 중량% 농도)를 사용한 것을 제외하고는 실시예 1과 동일한 방법으로 연료전지용 개질 반응기를 제조하였다. A reforming reactor for a fuel cell was manufactured in the same manner as in Example 1, except that sulfuric acid (H 2 SO 4 ) aqueous solution (5 wt% concentration) was used as the acid solution.
실시예 3Example 3
인가전압을 DC 30V로 한 것을 제외하고는 실시예 1과 동일한 방법으로 연료전지용 개질 반응기를 제조하였다. A reforming reactor for a fuel cell was manufactured in the same manner as in Example 1 except that the applied voltage was changed to DC 30V.
실시예 4Example 4
열처리온도를 700 ℃로 한 것을 제외하고는 실시예 1과 동일한 방법으로 연료전지용 개질 반응기를 제조하였다. A reforming reactor for a fuel cell was manufactured in the same manner as in Example 1 except that the heat treatment temperature was 700 ° C.
실시예 5Example 5
구리(Cu)를 스퍼터링하여 촉매를 부착시킨 것을 제외하고는 실시예 1과 동일한 방법으로 연료전지용 개질 반응기를 제조하였다. A reforming reactor for a fuel cell was manufactured in the same manner as in Example 1 except that the catalyst was attached by sputtering copper (Cu).
본 발명의 실시예 1 내지 6에 따라 제조된 개질 반응기를 통과한 개질 반응기체는 연료와의 접촉 면적이 넓어 수소기체의 생성 효과가 우수하고, 일산화탄소의 발생량이 낮은 효과가 있다.The reforming reactor body which has passed through the reforming reactor prepared according to Examples 1 to 6 of the present invention has a wide contact area with the fuel, which is excellent in the effect of generating hydrogen gas and has a low effect of generating carbon monoxide.
본 발명의 연료전지용 개질 반응기는 기공이 형성된 금속기재에 개질촉매가 부착되어 있으므로, 촉매의 부착량이 많고, 상기 개질 반응기의 표면을 따라 유체를 흘려보내는 경우에도 기공 속으로 일부의 유체가 흘러들어가게 되어, 유체 및 열의 흐름 효율이 우수한 장점을 가진다. The reforming reactor for a fuel cell of the present invention has a reforming catalyst attached to a metal substrate having pores, so that the amount of adhesion of the catalyst is large and some fluid flows into the pores even when the fluid flows along the surface of the reforming reactor. In addition, the fluid and heat flow efficiency is excellent.
Claims (14)
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR101019234B1 (en) * | 2009-04-14 | 2011-03-04 | 한국에너지기술연구원 | Method for producing metal structure catalyst for compact reforming reactor, metal structure catalyst, metal structure catalyst module |
| US8173309B2 (en) | 2007-02-12 | 2012-05-08 | Samsung Sdi Co., Ltd. | Reformer for fuel cell, and fuel cell system comprising the same |
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2005
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US8173309B2 (en) | 2007-02-12 | 2012-05-08 | Samsung Sdi Co., Ltd. | Reformer for fuel cell, and fuel cell system comprising the same |
| KR101019234B1 (en) * | 2009-04-14 | 2011-03-04 | 한국에너지기술연구원 | Method for producing metal structure catalyst for compact reforming reactor, metal structure catalyst, metal structure catalyst module |
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