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Japanese-to-English technical translation by U.S. patent agent/chemist.
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Japanese to English: Ruel Cell and Manufacturing Method Thereof General field: Law/Patents Detailed field: Chemistry; Chem Sci/Eng
Source text - Japanese 特開平４－３６６５５８
(http://www6.ipdl.inpit.go.jp/Tokujitu/tjsogodbk.ipdl)
Translation - English (19) Japanese Patent Office (JP) (12) Official Gazette for Unexamined Patent Applications (A) (11) Disclosure Number: H4-366558A(43) Disclosure Date: Sept. 9, 1992
(51) Int. Cl.5H01M 4/90B01J 23/89 Ident. Code Agency Internal Control No.M 9062-4KM 8017-4G FI Indicator of Technology
Examination Request Status: Not Requested. No. of Claims: 4 (4 pages total)
(21) Filing Number: Patent Filing No. Hei 3-139309(22) Date of Application: June 12, 1991
(71) Applicant: 000005234 Fuji Electric Co., Ltd.. 1-1 Tanabe Shinden, Kawasaki-ku Kawasaki-shi, Kanagawa-ken(72) Inventor: Hirobumi ENOMOTO c/o Fuji Electric Co., Ltd.. 1-1 Tanabe Shinden, Kawasaki-ku Kawasaki-shi, Kanagawa-ken(72) Inventor: Shuzo WARATANI c/o Fuji Electric Co., Ltd.. 1-1 Tanabe Shinden, Kawasaki-ku Kawasaki-shi, Kanagawa-ken(72) Agent: Iwao YAMAGUCHI, Attorney
(54) [Title of Invention] Fuel Cell and Manufacturing Method Thereof
(57) [Abstract]
[Object] The object of the present invention is to obtain a catalyst used for a fuel cell which has excellent initial characteristics and stability.
[Composition of the Invention] A ternary alloy is formed from platinum, iron, and nickel. Hydroxides of iron and nickel are deposited on platinum-supporting carbon, and the mixture is heat treated at a temperature of 800°C to 1000°C, followed by bonding using a binder to laminate the treated mixture on an electrode catalyst layer.
[Scope of the Patent Claims]
[Claim 1] A fuel cell having an electrode catalyst layer on an electrode base material;
wherein the electrode catalyst layer is formed by using a binder to bind together a catalyst supporting a ternary alloy of platinum, iron, and nickel on a carbon support.
[Claim 2] A method for manufacture of a fuel cell;
wherein the method comprises:
a first step of causing deposition and attachment of nickel hydroxide and iron hydroxide on platinum-supporting carbon;
a second step of preparing catalyst by heat treating the hydroxide deposition-treated carbon at a temperature of 800°C to 1000°C; and
a third step of laminating onto an electrode base material an electrode catalyst layer formed by binding together the catalyst using a binder.
[Claim 3] The method for manufacture of a fuel cell according to claim 2;
wherein deposition and attachment of the hydroxides is performed by:
adding ammonia water to a mixed solution of nitric acid salts to adjust pH to 8 to form a suspension solution;
performing ultrasonic dispersion of the suspension solution to prepare a uniform mixed solution; and
causing the uniform mixed solution to contact the platinum-supporting carbon.
[Claim 4] The method for manufacture of a fuel cell according to claim 2;
wherein the heat treatment is performed under flowing nitrogen gas.
[Detailed Description of the Invention]
[0001]
[Field of Industrial Use]
This invention relates to an electrode catalyst layer of a fuel cell, and this invention particularly relates to the catalyst substance and manufacturing method thereof.
[0002]
[Conventional Technology]
Generally a gas diffusion electrode used for a fuel cell is formed by lamination of an electrode catalyst layer (formed by using polytetrafluoroethylene to bind a catalyst powder which supports a precious metal catalyst) on a porous carbon electrode base material which has excellent electrical conductivity.
[0003] Due to the uniform presence of three phases (i.e., the catalyst, phosphoric acid electrolyte, and supplied reactive gas (i.e., hydrogen or oxygen)), an electrochemical reaction occurs, and direct electrical energy is obtained.
[0004] FIG. 1 is a schematic cross-sectional diagram showing the structure of an electrode of the fuel cell. The fuel cell has an electrode base material 1, which utilizes porous carbon having a flow path for air or hydrogen, and an electrode layer 5 formed by blending PTFE 4 to impart a suitable degree of water repellence to a catalyst 3 which supports a platinum catalyst 2. Due to the occurrence at the catalyst particle surface in this electrode catalyst layer of a three-phase coexisting state (i.e. with the phosphoric acid electrolyte and the fed reaction gas (i.e. hydrogen or air)), an electrochemical reaction occurs, and direct electrical energy can be obtained.
[0005] A catalyst using platinum, which is highly resistant to corrosion by high temperature phosphoric acid, has conventionally be used as the catalyst in a conventional phosphoric acid type fuel cell. The catalyst performs an extremely important role in the electrode reaction and is required for increasing stability and activity of the catalyst in order to improve working life and output of the cell.
[0006] The conventional method of manufacture of the platinum catalyst generally uses liquid phase reduction. Specifically, acid treatment using nitric acid, glacial acetic acid, and the like is performed in order to make the platinum-supporting carbon black readily disperse in the liquid phase, and thereafter, the platinum needed for supporting is added as a chloroplatinic acid aqueous solution, and platinum reduction is performed at a liquid temperature of 40°C to 90°C by dropwise addition of hydrazine as a reducing agent.
[0007] To further increase activity of the catalyst, alloying is performed by addition to the platinum-supporting catalyst of a second metal component such as vanadium, chromium, cobalt, nickel, iron, and the like. Firstly, the above mentioned reduced platinum catalyst is dispersed again in aqueous solution, and the second metal is deposited and attached to the carbon surface as a hydroxide by use of an alkaline agent such as potassium hydroxide, sodium hydroxide, ammonia water, and the like. This treated catalyst is filtered and water-washed, dried, and then subjected to heat treatment at 800°C to 1000°C in an inert atmosphere to manufacture the alloy catalyst. Technology is widely known which attempts to improve catalyst activity of an alloy catalyst by adding other group IV - VIII transition metals to this type of platinum catalyst. Furthermore, for stability and activity improvement, ternary catalysts have been introduced such as a platinum-chromium-cobalt catalyst (Unexamined Laid-open Patent Application No. S59-141160), a platinum-iron-cobalt catalyst (Unexamined Laid-open Patent Application No. S62-163746), a platinum-nickel-cobalt catalyst (Unexamined Laid-open Patent Application No. S63-190254), and the like.
[0008]
[Problem to Be Solved by the Invention]
However, due to the display of a lowering of characteristics over a comparatively short time interval even when initial activity is excellent, stability remains to be improved for such catalysts. In consideration of the above mentioned points, the object of the present invention is to provide a fuel cell which has excellent characteristics and stability by the development of a novel catalyst substance, and a manufacturing method thereof.
[0009]
[Means to Solve the Problem]
The above mentioned object is achieved by the present invention which forms an electrode catalyst layer on an electrode base material, wherein the electrode catalyst layer is formed by using a binder to bind together a catalyst supporting a ternary alloy of platinum, iron, and nickel on a carbon support. Moreover, the above mentioned object is achieved by the present invention which includes: a first step of causing deposition and attachment of nickel hydroxide and iron hydroxide on platinum-supporting carbon, a second step of preparing catalyst by heat treating the hydroxide deposition-treated carbon at a temperature of 800°C to 1000°C, and a third step of laminating onto an electrode base material an electrode catalyst layer formed by binding together the catalyst using a binder.
[0010]
[Operation of the Invention]
A platinum-iron-nickel ternary alloy catalyst is formed which incorporates iron and nickel and which has excellent stability and high initial activity in comparison to a binary catalyst. Therefore, it is possible to cause an improvement of both catalyst activity and stability.
[0011]
[Working Example]
The present invention will be explained using a working example. First, 9 g of a carbon black, such as acetylene black and the like, was weighed out and was added to 200 mL of purified water. Thereafter, a chloroplatinic acid aqueous solution (1 g as Pt) was added, and the mixture was heated to 60°C. After temperature had become constant, 2N NaOH solution was added to adjust the mixture to pH 10, and a 3% hydrazine solution was added dropwise to perform reduction of the chloroplatinic acid. After reduction, the mixture was filtered on a glass filter, was water-washed, and was dried to obtain the platinum-supporting catalyst. Size of platinum crystallites of this platinum-supporting catalyst was 28Å.
[0012] Alloying of the platinum-supporting catalyst obtained in this manner will be described below. Firstly, the platinum-supporting catalyst was dispersed in 200 mL of purified water. Separately, cobalt nitrate (0.15 g as cobalt (Co)) and iron nitrate (0.15 g as iron (Fe)) were weighed out and dissolved in 50 mL of purified water. Furthermore, ammonia water was added to this solution to adjust pH to 8, and ultrasonic dispersion equipment was used to produce a uniform mixed solution of iron hydroxide and nickel hydroxide. This solution was added to the solution of dispersed platinum-supporting catalyst, ammonia water was added dropwise to adjust pH to 9, and the catalyst and solution were sufficiently contacted for 1 to 5 hours. Then the mixture was filtered using a glass filter, was water-washed, and was dried. Thereafter, heat treatment was performed at 800°C to 1000°C in flowing nitrogen gas. A catalyst carrying the ternary alloy 2A was obtained in this manner.
[0013] Platinum crystallite size of the alloy catalyst produced in this manner was 33Å. Compared to the conventional alloy catalyst, the obtained platinum-iron-nickel ternary alloy catalyst was characterized in that both initial activity and stability were excellent. The initial characteristics and change of crystallite size after 1000 hours are shown in Table 1.
[0015]
[Effect of the Invention]
According to this invention, an electrode catalyst layer is formed on an electrode base material, wherein the electrode catalyst layer is formed by using a binder to bind together a catalyst supporting a ternary alloy of platinum, iron, and nickel on a carbon support. Moreover, catalyst is prepared by: a first step of causing deposition and attachment of nickel hydroxide and iron hydroxide on platinum-supporting carbon, a second step of preparing catalyst by heat treating the hydroxide deposition-treated carbon at a temperature of 800°C to 1000°C, and a third step of laminating onto an electrode base material an electrode catalyst layer formed by binding together the catalyst using a binder. Therefore a ternary alloy catalyst is obtained which has a small crystallite size and has little change of crystallite size over time. A fuel cell can thus be obtained which has excellent characteristics and stability.
[Simple Explanation of Figures]
[FIG. 1] This is a schematic cross-sectional diagram which shows the electrode structure of the fuel cell.
[Explanation of Item Numbering]
1 … electrode base material
2 … platinum
2A … ternary alloy
3 … catalyst
4 … PTFE
[FIG. 1]
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Experience
Years of experience: 27. Registered at ProZ.com: Oct 2009.
STEVEN WAYNE JOHNSTON
801 Country Place Drive, #109, Houston, TX 77079
Phone: 281-556-1709
E-mail: [email protected]
WWW site: www.japaneseology.com
SKYPE: StevenWJohnston
Service: Japanese to English translation, specializing in patents and technology
NATIVE LANGUAGE: English
TRANSLATION, PATENT SEARCH & DRAFTING, DOCUMENT REVIEW & TECHNICAL WRITING
Language pair: Japanese into English (12 years experience)
Membership: American Translators Association, Japan Association of Translators (both about 12 years), American Intellectual Property Law Association, Japan Translation Federation. Registered with the U.S. Patent Office as US Patent Agent No. 63,097.
Certification: Japanese-to-English patent translation, April of 2011, Japan Translation Federation (registration no. 6259).
Japanese-to-English science-technology translation, Sept. of 2011, Japan Translation Federation.
SUBJECT MATTER SPECIALIZATION
Patents, engineering, chemistry-plastics, physics-electronics, software, and business. Japanese document review for litigation.
EDUCATION
M.S., California Institute of Technology, Pasadena, California, 1980
Major: Env. Engineering. Concentration: Chemical Engineering
Jessie Smith Noyes Foundation Fellowship
M.S., Louisiana State University, Baton Rouge, LA, 1976
Major: Chemical Engineering
Enzyme process development thesis. Taught computer programming.
B.S., Louisiana State University, Baton Rouge, LA, 1973
Major: Chemical Physics
Alumni Fund Academic Scholarship. I.H. Gotlieb Memorial Scholarship. Sigma Pi Sigma (Physics Honor Society)
PROFESSIONAL EXPERIENCE
Japanese-English Technical Translator & Technical Writer: 1994 - Present
JTech Translations (owner, translator, writer), Houston, Texas
Translation of Japanese patents and technical journal articles into English for the semiconductor, chemical, plastics, and other industries. Translation for both filing and information. Japanese document review. Patent searching and screening, including the Japanese PATOLIS system. Translation of numerous JPO office action documents. Also general technical writing and patent searching, particularly in-house for the local petrochemical industry for 8 years, including 3 years in the intellectual property dept. One publication. Certified as a Japanese-to-English patent translator by the Japan Translation Federation.
Product Development Engineer: 1994 - 1997
Tredegar Films Corporation, Terre Haute, Indiana
Develop plastic film products with US, European, and Japanese clients. Development of films for disposable consumer products and medical devices.
Process Development Engineer: 1980 - 1994
Ethyl Corporation, Houston, Texas (1989 - 1994)
Developed silicon semiconductor crystal growth processes for the semiconductor and silicon photovoltaic industries. Japanese customer technical service. Japanese-English technical translation. Japanese patent searching. Several patents. One publication.
Ethyl Corporation, Baton Rouge, Louisiana (1980 - 1989)
Designed, built, and operated pilot plants. Bench-scale process development. Three patents. One publication.
Research Associate: 1976 - 1978
Center for Wetland Resources, Baton Rouge, Louisiana
Developed trace chemical analytical methods and equipment. Study of chemistry of trace contaminants in sediments.
PUBLICATIONS:
(1) Johnston, S. W., “Construction of a 12.5” Tri-Shiefspiegler,” Telescope Making Magazine, Fall of 1986, pp. 44 - 51. (applied optics, accompanied by presentation at 1987 TSP conference)
(2) Marlett, E. M., Fey, F. W., Johnston, S. W., & Kaesz, H. D., “Stabilization of Amine Alanes,” US Patent No. 4,730,070 (1988).
(3) Marlett, E. M., Fey, F. W., Johnston, S. W., & Kaesz, H. D., “Stabilization of Amine Alanes," US Patent No. 4,782,171 (1988).
(4) Marlett, E. M., Fey, F. W., Johnston, S. W., & Kaesz, H. D., “Stabilization of Amine Alanes,” US Patent No. 4,866,191 (1988).
(5) Johnston, S. W. & Kurz, J. D., “Multiple Czochralski Crystal Growth Using Polysilicon Granules,” (16p-ZK-4) Oyobutsurigakukai Koenkai Yokoshu, pub. of The Japan Society of Applied Physics, vol. 53, no.1 (19920916) p. 213. (semiconductor crystal growth, accompanied by presentation at The Japan Society of Applied Physics Fall 1992 Meeting)
(6) Johnston, S. W. & Wikman, A. O., “Particulate Matter Feeding Apparatus,” Japanese Unexamined Laid-open Patent Application No. H06-205960A (1994).
(7) Johnston, S. W., “Using Japanese Online Patent Information,” Fourth Annual NTIS/JICST Conference: Japanese Scientific & Technical Information, Boston, Massachusetts, 14 & 15 July 1994, pub. by U.S. National Technical Information Service (searching and using Japanese language technical literature, accompanied by presentation at JSTI conference in Boston).
(8) Johnston, S. W. & Wikman, A. O., “Apparatus for Recharging a Heated Receptacle with Particulate Matter at a Controlled Velocity,” US Patent No. 5,419,462 (1995).
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