KR100985052B1 - Anode for direct alcohol fuel cells comprising transition metal oxides, preparation method thereof and direct alcohol fuel cells comprising anode for direct alcohol fuel cells containing transition metal oxides - Google Patents

Anode for direct alcohol fuel cells comprising transition metal oxides, preparation method thereof and direct alcohol fuel cells comprising anode for direct alcohol fuel cells containing transition metal oxides Download PDF

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KR100985052B1
KR100985052B1 KR1020070129152A KR20070129152A KR100985052B1 KR 100985052 B1 KR100985052 B1 KR 100985052B1 KR 1020070129152 A KR1020070129152 A KR 1020070129152A KR 20070129152 A KR20070129152 A KR 20070129152A KR 100985052 B1 KR100985052 B1 KR 100985052B1
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fuel cell
alcohol fuel
direct alcohol
transition metal
negative electrode
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KR20090062060A (en
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우성일
전민구
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한국과학기술원
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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
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • 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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
    • H01M8/1011—Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
    • 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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
    • H01M8/1011—Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
    • H01M8/1013—Other direct alcohol fuel cells [DAFC]
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
    • H01M2004/8684—Negative electrodes
    • 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
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • 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
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

본 발명은 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법 및 전이금속 산화물이 함유된 음극을 포함하는 직접 알코올 연료전지에 관한 것으로서 보다 상세하게는 직접 알코올 연료전지용 음극에 있어서, 음극의 촉매층에 전이금속 산화물을 포함하도록 하여 알코올 산화 활성을 촉진시킴으로써 직접 알코올 연료전지의 성능을 향상시킬 수 있는 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법 및 전이금속 산화물이 함유된 음극을 포함하는 직접 알코올 연료전지에 관한 것이다.The present invention relates to a direct alcohol fuel cell comprising a negative electrode for a direct alcohol fuel cell containing a transition metal oxide, a method for producing the same and a negative electrode containing a transition metal oxide, and more particularly, in a negative electrode for a direct alcohol fuel cell, A cathode for a direct alcohol fuel cell containing a transition metal oxide capable of improving the performance of the direct alcohol fuel cell by promoting the oxidation of the alcohol by including a transition metal oxide in the catalyst layer, a method for preparing the same, and a cathode containing the transition metal oxide It relates to a direct alcohol fuel cell comprising.

전이금속 산화물, 직접 알코올 연료전지, 음극 Transition Metal Oxide, Direct Alcohol Fuel Cell, Cathode

Description

전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법 및 전이금속 산화물이 함유된 음극을 포함하는 직접 알코올 연료전지{Anode for direct alcohol fuel cells comprising transition metal oxides, preparation method thereof and direct alcohol fuel cells comprising anode for direct alcohol fuel cells containing transition metal oxides}Anode for direct alcohol fuel cells comprising transition metal oxides, preparation method about and direct alcohol fuel cells comprising anode for direct alcohol fuel cells containing transition metal oxides}

본 발명은 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법 및 전이금속 산화물이 함유된 음극을 포함하는 직접 알코올 연료전지에 관한 것으로서 보다 상세하게는 직접 알코올 연료전지용 음극에 있어서, 음극의 촉매층에 전이금속 산화물을 포함하도록 하여 알코올 산화 활성을 촉진시킴으로써 직접 알코올 연료전지의 성능을 향상시킬 수 있는 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법 및 전이금속 산화물이 함유된 음극을 포함하는 직접 알코올 연료전지에 관한 것이다.The present invention relates to a direct alcohol fuel cell comprising a negative electrode for a direct alcohol fuel cell containing a transition metal oxide, a method for producing the same and a negative electrode containing a transition metal oxide, and more particularly, in a negative electrode for a direct alcohol fuel cell, A cathode for a direct alcohol fuel cell containing a transition metal oxide capable of improving the performance of the direct alcohol fuel cell by promoting the oxidation of the alcohol by including a transition metal oxide in the catalyst layer, a method for preparing the same, and a cathode containing the transition metal oxide It relates to a direct alcohol fuel cell comprising.

연료전지(fuel cell)는 연료의 산화에 의해서 생기는 화학에너지를 직접 전 기에너지로 변환시키는 전지의 일종이다.A fuel cell is a type of battery that converts chemical energy generated by oxidation of fuel directly into electric energy.

연료전지는 전기에너지를 얻기 위한 반응물이 외부에서 연속적으로 공급되어 반응생성물이 연속적으로 계의 바깥으로 제거된다는 특징이 있으며, 화석연료, 액체연료, 기체연료등 다양한 연료를 사용할 수 있다.The fuel cell is characterized in that the reactants for obtaining electrical energy are continuously supplied from the outside, so that the reaction products are continuously removed from the outside of the system, and various fuels such as fossil fuel, liquid fuel, and gas fuel can be used.

연료전지 중에서 직접 알코올 연료전지(direct alcohol fuel cell, DAFC)는 액상 연료를 사용한다는 장점이 있어서 부피가 작고 휴대가 용이하기 때문에 부피가 작은 전자기기인 휴대폰, PDA(personal digital assistants), 노트북 컴퓨터 등의 적용에 적합하다. 하지만 직접 알코올 연료전지의 음극 및/또는 양극에 사용되는 촉매의 활성이 낮기 때문에 전류 밀도가 낮아 상용화하기에는 어려움이 있다. 또한, 촉매의 사용량 또한 수소를 사용하는 연료전지 보다 많기 때문에 가격적인 측면에서 어려움을 격고 있다. Among the fuel cells, direct alcohol fuel cell (DAFC) has the advantage of using liquid fuel, so it is small and easy to carry, so it is a small electronic device such as mobile phones, personal digital assistants (PDAs), notebook computers, etc. Suitable for the application of However, since the activity of the catalyst used in the anode and / or anode of the direct alcohol fuel cell is low, it is difficult to commercialize because of the low current density. In addition, since the amount of the catalyst used is also higher than that of a fuel cell using hydrogen, there are difficulties in terms of price.

상기의 직접 알코올 연료전지는 알코올의 종류에 따라 여러 가지가 있으며, 이러한 직접 알코올 연료전지의 일예로 직접 메탄올 연료전지(direct methanol fuel cell, DMFC), 직접 에탄올 연료전지(direct ethanol fuel cell, DEFC) 등이 있다.There are various types of direct alcohol fuel cells according to the type of alcohol, and examples of such direct alcohol fuel cells include direct methanol fuel cell (DMFC) and direct ethanol fuel cell (DEFC). Etc.

상기와 같은 직접 알코올 연료전지의 촉매 문제를 해결하기 위해서는 높은 활성을 가지는 촉매의 개발이 필수적이며 이러한 방안의 일환으로 다양한 합금 촉매들의 개발이 시도되어 왔다. 그러나 여러 성분이 함유된 다성분계 합금 촉매는 단일 조성의 촉매에 비해 높은 활성을 나타내는 반면, 다성분계 촉매를 사용함으로써 촉매 생산에 대한 비용이 증가하고, 또한 여러 가지 성분이 촉매에 함유되기 때 문에 단일 조성의 촉매에 비해 대량생산에의 어려움이 있어 이를 해결할 새로운 방안이 절실한 실정이다.In order to solve the catalyst problem of the direct alcohol fuel cell as described above, the development of a catalyst having high activity is essential, and as part of this scheme, various alloy catalysts have been attempted. However, multi-component alloy catalysts containing multiple components show higher activity than catalysts of single composition, whereas the cost of catalyst production increases by using multi-component catalysts, and also because various components are contained in the catalyst. Compared to the catalyst of a single composition, there is a difficulty in mass production, and a new solution to this problem is urgently needed.

본 발명은 직접 알코올 연료전지용 음극에 있어서, 전이금속 산화물을 포함하는 직접 알코올 연료전지용 음극을 제공하고자 한다.In the negative electrode for direct alcohol fuel cell, the present invention is to provide a negative electrode for a direct alcohol fuel cell containing a transition metal oxide.

본 발명은 직접 알코올 연료전지용 음극 제조에 있어서, 전이금속 산화물을 포함하는 직접 알코올 연료전지용 음극의 제조방법을 제공하고자 한다.The present invention is to provide a method for producing a direct alcohol fuel cell negative electrode containing a transition metal oxide in the direct alcohol fuel cell anode production.

본 발명은 직접 알코올 연료전지에 있어서, 전이금속 산화물이 함유된 직접 알코올 연료전지용 음극이 포함된 직접 알코올 연료전지를 제공하고자 한다.The present invention provides a direct alcohol fuel cell including a negative electrode for a direct alcohol fuel cell containing a transition metal oxide.

본 발명은 직접 알코올 연료전지용 음극에 있어서, 음극의 촉매층에 전이금속 산화물을 포함하도록 하여 최대 전력 양을 증가시킬 수 있는 직접 알코올 연료전지용 음극을 제공하고자 한다.The present invention is to provide a direct alcohol fuel cell negative electrode in the negative electrode for direct alcohol fuel cell, which can increase the maximum amount of power by including a transition metal oxide in the catalyst layer of the negative electrode.

본 발명은 직접 알코올 연료전지용 음극 제조에 있어서, 음극의 촉매층으로 사용하는 촉매와 전이금속 산화물을 혼합하는 단계를 포함하도록 하여 최대 전력 양을 증가시킬 수 있는 직접 알코올 연료전지용 음극의 제조방법을 제공하고자 한다.The present invention is to provide a method for producing a direct alcohol fuel cell negative electrode that can increase the maximum amount of power by including a step of mixing a catalyst and a transition metal oxide used as a catalyst layer of the negative electrode in the direct alcohol fuel cell anode production. do.

본 발명은 직접 알코올 연료전지에 있어서, 전이금속 산화물을 직접 알코올 연료전지용 음극에 함유하도록 하여 알코올 산화 활성을 촉진시킴으로써 최대 전력 양을 증가시킬 수 있는 직접 알코올 연료전지를 제공하고자 한다.The present invention is to provide a direct alcohol fuel cell in the direct alcohol fuel cell, by including the transition metal oxide directly in the negative electrode for the alcohol fuel cell to promote the alcohol oxidation activity to increase the maximum amount of power.

본 발명은 직접 알코올 연료전지용 음극에 있어서, 음극의 촉매층에 전이금속 산화물을 포함하도록 하여 알코올 산화 활성을 촉진시킴으로써 직접 알코올 연료전지의 최대 전력 양을 증가시킬 수 있는 전이금속 산화물을 이용한 직접 알코올 연료전지용 음극을 제공할 수 있다.The present invention provides a direct alcohol fuel cell negative electrode, which includes a transition metal oxide in the catalyst layer of the negative electrode to promote alcohol oxidation activity to increase the maximum amount of power of the direct alcohol fuel cell direct alcohol fuel cell using a transition metal oxide A negative electrode can be provided.

본 발명은 직접 알코올 연료전지용 음극 제조에 있어서, 음극의 촉매층에 전이금속 산화물을 포함하도록 하여 알코올 산화 활성을 촉진시킴으로써 직접 알코올 연료전지의 최대 전력 양을 증가시킬 수 있는 전이금속 산화물을 이용한 직접 알코올 연료전지용 음극의 제조방법을 제공할 수 있다.The present invention provides a direct alcohol fuel using a transition metal oxide that can increase the maximum amount of power of the direct alcohol fuel cell by promoting the oxidation of the alcohol by including a transition metal oxide in the catalyst layer of the cathode in the anode for direct alcohol fuel cell production. It is possible to provide a method for producing a battery negative electrode.

본 발명은 직접 알코올 연료전지에 있어서, 음극의 촉매층에 전이금속 산화물을 포함하도록 하여 알코올 산화 활성을 촉진시킴으로써 직접 알코올 연료전지의 최대 전력 양을 증가시킬 수 있는 전이금속 산화물을 이용하여 성능이 향상된 직접 알코올 연료전지를 제공할 수 있다.In the present invention, the direct alcohol fuel cell includes a transition metal oxide in the catalyst layer of the cathode to promote alcohol oxidation activity, thereby directly improving performance by using a transition metal oxide capable of increasing the maximum amount of power of the direct alcohol fuel cell. An alcohol fuel cell can be provided.

본 발명은 전이금속 산화물을 포함하는 직접 알코올 연료전지용 음극을 나타낸다.The present invention represents a negative electrode for a direct alcohol fuel cell containing a transition metal oxide.

본 발명은 직접 알코올 연료전지용 음극에 있어서, 음극의 촉매에 전이금속 산화물을 포함하는 직접 알코올 연료전지용 음극을 나타낸다.The present invention relates to a direct alcohol fuel cell negative electrode in the negative electrode for a direct alcohol fuel cell, comprising a transition metal oxide in the catalyst of the negative electrode.

상기의 직접 알코올 연료전지는 알코올이 메탄올(methanol)인 직접 알코올 연료전지를 나타낸다.The direct alcohol fuel cell represents a direct alcohol fuel cell in which the alcohol is methanol.

상기의 직접 알코올 연료전지는 알코올이 에탄올(ethanol)인 직접 알코올 연료전지를 나타낸다.The direct alcohol fuel cell represents a direct alcohol fuel cell in which the alcohol is ethanol.

상기의 직접 알코올 연료전지에서 연료전지 음극의 촉매는 백금(Pt) 촉매를 사용할 수 있다.In the direct alcohol fuel cell, a catalyst of the fuel cell anode may use a platinum (Pt) catalyst.

상기의 직접 알코올 연료전지에서 연료전지 음극의 촉매는 백금/루테늄(Pt/Ru) 합금 촉매를 사용할 수 있다.In the direct alcohol fuel cell, the catalyst of the fuel cell anode may use a platinum / ruthenium (Pt / Ru) alloy catalyst.

상기의 직접 알코올 연료전지 음극의 촉매에 포함되는 전이금속 산화물은 Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Te, Ru, Rh, Pd, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, W, Re, Os, Ir의 군으로부터 선택되는 전이금속의 산화물 중에서 선택되는 1종 또는 2종 이상의 혼합물을 사용할 수 있다. The transition metal oxides included in the catalyst of the direct alcohol fuel cell anode are Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Te, Ru, Rh, From the group of Pd, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, W, Re, Os, Ir One or a mixture of two or more selected from the oxides of the transition metals selected may be used.

상기의 직접 알코올 연료전지 음극의 촉매에 포함되는 전이금속 산화물은 음극 촉매에 촉매 중량 대비 1∼30％ 포함되도록 사용할 수 있다.The transition metal oxide included in the catalyst of the direct alcohol fuel cell negative electrode may be used so as to include 1 to 30% by weight of the catalyst in the negative electrode catalyst.

본 발명은 음극의 촉매에 전이금속 산화물을 혼합하는 단계를 포함하는 직접 알코올 연료전지용 음극의 제조방법을 나타낸다.The present invention shows a method for producing a negative electrode for a direct alcohol fuel cell comprising the step of mixing a transition metal oxide to the catalyst of the negative electrode.

본 발명은 직접 알코올 연료전지용 음극 제조에 있어서, 음극의 촉매에 전이금속 산화물을 혼합하는 단계를 포함하는 직접 알코올 연료전지용 음극의 제조방법 을 나타낸다.The present invention relates to a method for producing a cathode for a direct alcohol fuel cell, comprising the step of mixing a transition metal oxide to the catalyst of the anode in the anode for direct alcohol fuel cell production.

상기의 직접 알코올 연료전지는 알코올이 메탄올(methanol)인 직접 알코올 연료전지를 나타낸다.The direct alcohol fuel cell represents a direct alcohol fuel cell in which the alcohol is methanol.

상기의 직접 알코올 연료전지는 알코올이 에탄올(ethanol)인 직접 알코올 연료전지를 나타낸다.The direct alcohol fuel cell represents a direct alcohol fuel cell in which the alcohol is ethanol.

상기의 직접 알코올 연료전지용 음극 제조시 연료전지 음극의 촉매는 백금(Pt) 촉매를 사용할 수 있다.In the production of the anode for the direct alcohol fuel cell, a catalyst of the fuel cell anode may use a platinum (Pt) catalyst.

상기의 직접 알코올 연료전지용 음극 제조시 연료전지 음극의 촉매는 백금/루테늄(Pt/Ru) 합금 촉매를 사용할 수 있다.In the production of the anode for the direct alcohol fuel cell, the catalyst of the fuel cell anode may use a platinum / ruthenium (Pt / Ru) alloy catalyst.

상기의 직접 알코올 연료전지용 음극 제조시, 직접 알코올 연료전지용 음극의 촉매에 혼합되는 전이금속 산화물은 Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Te, Ru, Rh, Pd, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, W, Re, Os, Ir의 군으로부터 선택되는 전이금속의 산화물 중에서 선택되는 1종 또는 2종 이상의 혼합물을 사용할 수 있다. In the preparation of the negative electrode for the direct alcohol fuel cell, the transition metal oxide mixed in the catalyst of the negative electrode for the direct alcohol fuel cell is Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Te, Ru, Rh, Pd, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, W, One or a mixture of two or more selected from oxides of transition metals selected from the group of Re, Os and Ir can be used.

상기의 직접 알코올 연료전지용 음극 제조시 직접 알코올 연료전지용 음극의 촉매와 혼합되는 전이금속 산화물은 음극 촉매에 촉매 중량 대비 1∼30％으로 혼합할 수 있다.In the preparation of the negative electrode for a direct alcohol fuel cell, the transition metal oxide mixed with the catalyst of the negative electrode for a direct alcohol fuel cell may be mixed with the negative electrode catalyst at 1 to 30% by weight of the catalyst.

본 발명은 상기에서 언급한 음극의 촉매에 전이금속 산화물이 포함된 직접 알코올 연료전지용 음극을 함유하는 직접 알코올 연료전지를 포함한다.The present invention includes a direct alcohol fuel cell containing a negative electrode for a direct alcohol fuel cell containing a transition metal oxide in the catalyst of the above-mentioned negative electrode.

본 발명은 상기에서 언급한 직접 알코올 연료전지용 음극 제조에 있어서, 음극의 촉매에 전이금속 산화물을 혼합하는 단계를 포함하는 직접 알코올 연료전지용 음극의 제조방법에 의해 제조한 음극이 함유된 직접 알코올 연료전지를 포함한다.The present invention provides a direct alcohol fuel cell containing a negative electrode prepared by the method for producing a negative electrode for a direct alcohol fuel cell, which includes mixing a transition metal oxide to a catalyst of the negative electrode in the above-mentioned negative electrode for a direct alcohol fuel cell. It includes.

상기 직접 알코올 연료전지에서 알코올은 메탄올 또는 에탄올인 직접 알코올 연료전지를 나타낸다.In the direct alcohol fuel cell, alcohol represents a direct alcohol fuel cell which is methanol or ethanol.

본 발명의 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법에 있어서, 다양한 성분, 함량 등의 조건에 의해 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법에 대해 조사한바, 본 발명의 목적을 달성하기 위해서는 상기에서 언급한 조건에 의해 전이금속 산화물을 함유하는 직접 알코올 연료전지용 음극, 이의 제조방법을 제공하는 것이 바람직하다.In the negative electrode for a direct alcohol fuel cell containing a transition metal oxide of the present invention, a method for producing the same, the negative electrode for a direct alcohol fuel cell containing a transition metal oxide under the conditions of various components, content, etc. In order to achieve the object of the present invention, it is preferable to provide a negative electrode for a direct alcohol fuel cell containing a transition metal oxide under the above-mentioned conditions, and a method for manufacturing the same.

이하 본 발명의 내용을 실시예 및 시험예를 통하여 구체적으로 설명한다. 그러나, 이들은 본 발명을 보다 상세하게 설명하기 위한 것으로 본 발명의 권리범위가 이들에 의해 한정되는 것은 아니다.Hereinafter, the present invention will be described in detail with reference to Examples and Test Examples. However, these are intended to explain the present invention in more detail, and the scope of the present invention is not limited thereto.

<실시예> <Examples>

백금(Pt) 촉매 1g을 나피온 이오노머(ionomer) 용액 및 이소프로필알코올이 1:10의 부비피로 혼합된 용액 100ml에 혼합한 다음 테프론 판에 스프레이 건을 이용하여 분사하고 건조한 것을 양극으로 사용하였다.1 g of a platinum (Pt) catalyst was mixed with 100 ml of a solution of Nafion ionomer solution and isopropyl alcohol mixed in a 1:10 volume volume, and then sprayed onto a Teflon plate using a spray gun, and dried was used as an anode.

백금/루세늄(Pt/Ru) 합금촉매(백금:루세늄 = 1:1 at.％)와 산화철(Fe2O3) 나노 입자를 90:10의 질량비로 혼합한 혼합물 1g을 나피온 이오노머(ionomer) 용액 및 이소프로필알코올이 1:10의 부비피로 혼합된 용액 100ml에 혼합한 다음 테프론 판에 스프레이 건을 이용하여 분사하고 건조한 것을 음극으로 사용하였다.1 g of a mixture of a platinum / ruthenium (Pt / Ru) alloy catalyst (platinum: rusenium = 1: 1 at.%) And iron oxide (Fe 2 O 3 ) nanoparticles in a mass ratio of 90:10 was added to the Nafion ionomer ( The ionomer solution and isopropyl alcohol were mixed into 100 ml of a 1:10 volume mixture, and then sprayed onto a Teflon plate using a spray gun, and a dry one was used as a cathode.

각각의 촉매가 코팅된 테프론 판을 서로 마주보게 한 뒤 테프론 판 가운데 사이에 나피온 전해질 막을 넣고 120℃, 1000psi에서 3분간 압착하였다. 이후 양쪽의 테프론 판을 제거하여 막/전극 복합체(Membrane Electrode Assemblies, MEA)를 얻었다. Each catalyst-coated Teflon plate was faced to each other, and then the Nafion electrolyte membrane was placed between the middle of the Teflon plate and pressed at 120 ° C. and 1000 psi for 3 minutes. Thereafter, both Teflon plates were removed to obtain a membrane / electrode assembly (Membrane Electrode Assemblies, MEA).

<비교예>Comparative Example

백금(Pt) 촉매 1g을 나피온 이오노머(ionomer) 용액 및 이소프로필알코올이 1:10의 부비피로 혼합된 용액 100ml에 혼합한 다음 테프론 판에 스프레이 건을 이용하여 분사하고 건조한 것을 양극으로 사용하였다.1 g of a platinum (Pt) catalyst was mixed with 100 ml of a solution of Nafion ionomer solution and isopropyl alcohol mixed in a 1:10 volume volume, and then sprayed onto a Teflon plate using a spray gun, and dried was used as an anode.

백금/루세늄(Pt/Ru) 합금촉매(백금:루세늄 = 1:1 at.％) 1g을 나피온 이오노머(ionomer) 용액 및 이소프로필알코올이 1:10의 부비피로 혼합된 용액 100ml에 혼합한 다음 테프론 판에 스프레이 건을 이용하여 분사하고 건조한 것을 음극으로 사용하였다.1 g of platinum / ruthenium (Pt / Ru) alloy catalyst (platinum: rucenium = 1: 1 at.%) Is mixed into 100 ml of a solution containing a Nafion ionomer solution and isopropyl alcohol in a 1:10 volume The Teflon plate was then sprayed with a spray gun and the dry one was used as the cathode.

각각의 촉매가 코팅된 테프론 판을 서로 마주보게 한 뒤 테프론 판 가운데 사이에 나피온 전해질 막을 넣고 120℃, 1000psi에서 3분간 압착하였다. 이후 양쪽 의 테프론 판을 제거하여 막/전극 복합체(MEA)를 얻었다. Each catalyst-coated Teflon plate was faced to each other, and then the Nafion electrolyte membrane was placed between the middle of the Teflon plate and pressed at 120 ° C. and 1000 psi for 3 minutes. Thereafter, both Teflon plates were removed to obtain a membrane / electrode composite (MEA).

<시험예> 직접 메탄올 연료전지의 성능 향상 관찰Test Example Observation of Performance Improvement of Direct Methanol Fuel Cell

상기 실시예 및 비교예에서 제조한 각각의 막/전극 복합체(MEA)를 직접 메탄올 연료전지에 적용하여 직접 메탄올 연료전지의 성능을 측정하고 그 결과를 도 1에 나타내었다. Each membrane / electrode composite (MEA) prepared in Examples and Comparative Examples was applied directly to a methanol fuel cell to measure the performance of the direct methanol fuel cell, and the results are shown in FIG. 1.

상기에서 직접 메탄올 연료전지의 성능 측정은 70℃에서 이루어졌으며, 음극에는 1M 농도의 메탄올 용액을 0.5ml/min으로 공급하였고, 양극에는 산소 기체를 100cc/min으로 공급하였다. The performance of the direct methanol fuel cell was measured at 70 ° C., a 1 M methanol solution was supplied at 0.5 ml / min to the cathode, and oxygen gas was supplied at 100 cc / min to the anode.

도 1의 결과에서처럼 산화철이 함유되지 않은 음극을 나타내는 비교예의 막/전극 접합체를 사용한 직접 메탄올 연료전지(■)에서는 69mW/cm2의 최대 전력을 얻었으나, 산화철이 함유된 음극을 나타내는 실시예의 막/전극 접합체를 사용한 직접 메탄올 연료전지(○)에서는 73mW/cm2의 최대 전력을 얻었다. In the direct methanol fuel cell (■) using the membrane / electrode assembly of Comparative Example showing the negative electrode free of iron oxide as shown in the results of FIG. 1, the maximum power of 69 mW / cm 2 was obtained, but the membrane of the embodiment showing the negative electrode containing iron oxide was obtained. In the direct methanol fuel cell (○) using the / electrode assembly, a maximum power of 73 mW / cm 2 was obtained.

특히 실시예의 음극에서는 비교예의 음극과 비교시 촉매의 사용량을 적게 하였으나, 촉매의 활성 향상으로 인해 연료전지의 성능이 향상되었음을 나타내고 있다.In particular, the amount of catalyst used is reduced in the negative electrode of the negative electrode in comparison with the negative electrode of the comparative example, but the performance of the fuel cell is improved due to the improved activity of the catalyst.

상술한 바와 같이, 본 발명의 바람직한 실시예를 참조하여 설명하였지만 해당 기술 분야의 숙련된 당업자라면 하기의 특허청구범위에 기재된 본 발명의 사상 및 영역으로부터 벗어나지 않는 범위 내에서 본 발명을 다양하게 수정 및 변경시킬 수 있음을 이해할 수 있을 것이다. As described above, although described with reference to a preferred embodiment of the present invention, those skilled in the art will be variously modified and modified within the scope of the present invention without departing from the spirit and scope of the invention described in the claims below. It will be appreciated that it can be changed.

본 발명의 음극의 촉매에 전이금속 산화물을 포함하는 직접 알코올 연료전지용 음극은 종래 촉매만 사용한 직접 알코올 연료전지용 음극에 비교시 촉매를 적게 사용해도 촉매의 활성이 향상되어 전체적으로 직접 알코올 연료전지의 성능이 향상됨을 알 수 있다.The negative electrode for a direct alcohol fuel cell including a transition metal oxide in the catalyst of the negative electrode of the present invention has improved catalytic activity even when less catalyst is used as compared to a negative electrode for a direct alcohol fuel cell using only a conventional catalyst, thereby improving overall performance of the direct alcohol fuel cell. It can be seen that the improvement.

따라서 본 발명에 의해 직접 알코올 연료전지의 성능을 보다 향상시킬 수 있어, 직접 알코올 연료전지를 사용하는 분야에서 생산성 향상을 기대할 수 있다.Therefore, according to the present invention, the performance of the direct alcohol fuel cell can be further improved, and productivity can be expected in the field of using the direct alcohol fuel cell.

도 1은 실시예 및 비교예에서 제조한 막/전극 접합체를 각각 직접 알코올 연료전지에 사용시 직접 알코올 연료전지의 성능 결과를 나타낸 그래프이다.1 is a graph showing the performance results of a direct alcohol fuel cell when the membrane / electrode assembly prepared in Examples and Comparative Examples is used in a direct alcohol fuel cell, respectively.

Claims (12)

직접 알코올 연료전지용 음극에 있어서, In the negative electrode for direct alcohol fuel cell, 음극의 백금/루테늄 합금 촉매에 Sc, Cr, Fe, Cu, Zn, Y, Zr, Nb, Mo, Te, Rh, Pd, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, Re, Os, Ir의 군으로부터 선택되는 전이금속의 산화물 중에서 1종 또는 2 종 이상의 혼합물인 전이금속 산화물을 음극 촉매 중량 대비 10％ 포함하는 직접 알코올 연료전지용 음극.Pt, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Sc, Cr, Fe, Cu, Zn, Y, Zr, Nb, Mo, Te, Rh, Pd Catalytic catalyst weight of a transition metal oxide which is one or a mixture of two or more of oxides of transition metals selected from the group of Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, Re, Os and Ir A direct alcohol fuel cell negative electrode containing 10% compared. 제1항에 있어서, 알코올은 메탄올 또는 에탄올인 것을 특징으로 하는 직접 알코올 연료전지용 음극.The negative electrode of claim 1, wherein the alcohol is methanol or ethanol. 삭제delete 삭제delete 삭제delete 직접 알코올 연료전지용 음극 제조에 있어서, In the manufacture of a cathode for a direct alcohol fuel cell, 음극의 백금/루테늄 합금 촉매에 Sc, Cr, Fe, Cu, Zn, Y, Zr, Nb, Mo, Te, Rh, Pd, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, Re, Os, Ir의 군으로부터 선택되는 전이금속의 산화물 중에서 1종 또는 2 종 이상의 혼합물인 전이금속 산화물을 음극 촉매 중량 대비 10％ 혼합하는 단계를 포함하는 것을 특징으로 하는 직접 알코올 연료전지용 음극의 제조방법.Pt, Ag, Cd, La, Ce, Pr, Nd, Pm, Sm, Eu, Sc, Cr, Fe, Cu, Zn, Y, Zr, Nb, Mo, Te, Rh, Pd Catalytic catalyst weight of a transition metal oxide which is one or a mixture of two or more of oxides of transition metals selected from the group of Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Hf, Ta, Re, Os and Ir Method for producing a direct alcohol fuel cell negative electrode comprising the step of mixing 10% compared. 제6항에 있어서, 알코올은 메탄올 또는 에탄올인 것을 특징으로 하는 직접 알코올 연료전지용 음극의 제조방법.7. The method of claim 6, wherein the alcohol is methanol or ethanol. 삭제delete 삭제delete 삭제delete 특허청구범위 제1항의 직접 알코올 연료전지용 음극 또는 특허청구범위 제6항의 방법에 의해 제조한 직접 알코올 연료전지용 음극을 포함하는 직접 알코올 연료전지.A direct alcohol fuel cell comprising the direct alcohol fuel cell negative electrode of claim 1 or a direct alcohol fuel cell negative electrode produced by the method of claim 6. 제11항에 있어서, 알코올은 메탄올 또는 에탄올인 것을 특징으로 하는 직접 알코올 연료전지.12. The direct alcohol fuel cell of claim 11, wherein the alcohol is methanol or ethanol.
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JP2005063677A (en) * 2003-08-11 2005-03-10 Nitto Denko Corp Fuel cell
KR20070046021A (en) * 2004-11-25 2007-05-02 가부시키가이샤 리코 Electrode catalyst, method for preparation thereof, direct alcohol fuel cell

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JP2005063677A (en) * 2003-08-11 2005-03-10 Nitto Denko Corp Fuel cell
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