JPS63181264A - Electrode/matrix combined body for fuel cell - Google Patents
Electrode/matrix combined body for fuel cellInfo
- Publication number
- JPS63181264A JPS63181264A JP62012812A JP1281287A JPS63181264A JP S63181264 A JPS63181264 A JP S63181264A JP 62012812 A JP62012812 A JP 62012812A JP 1281287 A JP1281287 A JP 1281287A JP S63181264 A JPS63181264 A JP S63181264A
- Authority
- JP
- Japan
- Prior art keywords
- matrix
- layer
- catalyst
- electrode
- fuel cell
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000011159 matrix material Substances 0.000 title claims abstract description 99
- 239000000446 fuel Substances 0.000 title claims description 20
- 239000003054 catalyst Substances 0.000 claims abstract description 101
- 239000000463 material Substances 0.000 claims abstract description 68
- 239000011230 binding agent Substances 0.000 claims abstract description 19
- 239000000843 powder Substances 0.000 claims abstract description 18
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 14
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 14
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 9
- 229910052799 carbon Inorganic materials 0.000 claims description 6
- -1 polytetrafluoroethylene Polymers 0.000 claims description 5
- 229920001577 copolymer Polymers 0.000 claims description 3
- 150000002484 inorganic compounds Chemical class 0.000 claims description 3
- 229910010272 inorganic material Inorganic materials 0.000 claims description 3
- 229910001463 metal phosphate Inorganic materials 0.000 claims description 3
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 2
- 239000004696 Poly ether ether ketone Substances 0.000 claims description 2
- 239000004695 Polyether sulfone Substances 0.000 claims description 2
- 239000004734 Polyphenylene sulfide Substances 0.000 claims description 2
- 239000004917 carbon fiber Substances 0.000 claims description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 2
- 229920006393 polyether sulfone Polymers 0.000 claims description 2
- 229920002530 polyetherether ketone Polymers 0.000 claims description 2
- 229920000069 polyphenylene sulfide Polymers 0.000 claims description 2
- 229920005992 thermoplastic resin Polymers 0.000 claims description 2
- 239000000835 fiber Substances 0.000 claims 1
- 239000000126 substance Substances 0.000 claims 1
- 239000003792 electrolyte Substances 0.000 abstract description 10
- 230000014759 maintenance of location Effects 0.000 abstract description 2
- 239000000758 substrate Substances 0.000 abstract 3
- 239000003795 chemical substances by application Substances 0.000 abstract 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 10
- 238000000034 method Methods 0.000 description 10
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 6
- 239000011148 porous material Substances 0.000 description 6
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 239000005871 repellent Substances 0.000 description 5
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 239000012528 membrane Substances 0.000 description 4
- 230000000717 retained effect Effects 0.000 description 4
- 238000001035 drying Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229910052697 platinum Inorganic materials 0.000 description 3
- 230000002940 repellent Effects 0.000 description 3
- 229910052581 Si3N4 Inorganic materials 0.000 description 2
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 230000007423 decrease Effects 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 239000010419 fine particle Substances 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 229910010271 silicon carbide Inorganic materials 0.000 description 2
- 239000000377 silicon dioxide Substances 0.000 description 2
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 2
- 239000007921 spray Substances 0.000 description 2
- 229910052580 B4C Inorganic materials 0.000 description 1
- LFVLUOAHQIVABZ-UHFFFAOYSA-N Iodofenphos Chemical compound COP(=S)(OC)OC1=CC(Cl)=C(I)C=C1Cl LFVLUOAHQIVABZ-UHFFFAOYSA-N 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- UGACIEPFGXRWCH-UHFFFAOYSA-N [Si].[Ti] Chemical compound [Si].[Ti] UGACIEPFGXRWCH-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- INAHAJYZKVIDIZ-UHFFFAOYSA-N boron carbide Chemical compound B12B3B4C32B41 INAHAJYZKVIDIZ-UHFFFAOYSA-N 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000007766 curtain coating Methods 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 238000007606 doctor blade method Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- 229910000484 niobium oxide Inorganic materials 0.000 description 1
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 1
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 1
- BPUBBGLMJRNUCC-UHFFFAOYSA-N oxygen(2-);tantalum(5+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Ta+5].[Ta+5] BPUBBGLMJRNUCC-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
- 239000002245 particle Substances 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 229910001936 tantalum oxide Inorganic materials 0.000 description 1
- 229910052718 tin Inorganic materials 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 1
- UONOETXJSWQNOL-UHFFFAOYSA-N tungsten carbide Chemical compound [W+]#[C-] UONOETXJSWQNOL-UHFFFAOYSA-N 0.000 description 1
- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
- 229910000859 α-Fe Inorganic materials 0.000 description 1
Classifications
-
- 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
-
- 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
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Inert Electrodes (AREA)
- Fuel Cell (AREA)
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
この発明は燃料電池用室［／マトリックス結合体に関す
るものである。DETAILED DESCRIPTION OF THE INVENTION [Industrial Field of Application] The present invention relates to a chamber/matrix combination for a fuel cell.
第２図は例えば特公昭５８−４５２号公報に示された従
来の燃料電池用電極／マトリックス結合体を示す断面図
であり、図において、（１）はｔ極層材、（２）は触媒
層、（３）は触媒浸み込み層、（４）はマトリックス層
である。FIG. 2 is a sectional view showing a conventional fuel cell electrode/matrix assembly disclosed in, for example, Japanese Patent Publication No. 58-452. In the figure, (1) is the t-electrode layer material, and (2) is the catalyst. The layer (3) is a catalyst impregnated layer, and (4) is a matrix layer.
次に製造方法について説明する。電極基材（１）は導電
性で通電性を有するものであり、例えば、カーボンヘー
ハなどの多孔性の導電性シートをポリテトラフルオロエ
チレン（以下ＰＴＦＥと略称する）の分散液に浸漬する
ことによシ撥水処理を施したものが用いられる。Next, the manufacturing method will be explained. The electrode base material (1) is electrically conductive and has electrical conductivity, and can be prepared by, for example, dipping a porous conductive sheet such as carbon ferrite in a dispersion of polytetrafluoroethylene (hereinafter abbreviated as PTFE). Those that have been treated to be water repellent are used.
触媒層（２）は例えば炭素粉末表面に白金微粒子を担持
させた触媒粉末と結着材としてＰＴＦＥを含む触媒ペー
ストを上記電極基材（１）に塗布することによシ形成し
、例えば３００〜８５０℃前後の温度で熱処理を施した
ものが用いられる。マトリックス層（４）は例えば炭化
珪素粉末と固着材としてＰＴＦＥを含むマトリックスペ
ーストを上記触媒層（２）に塗布することにより形成し
、例えば３００〜１３５０℃前後の温度で熱処理を施し
たものが用いられる。触媒層（２）とマトリックス層（
４）の熱処理は個別に行う場合と、同時に行う場合があ
る。The catalyst layer (2) is formed, for example, by applying a catalyst paste containing catalyst powder in which platinum fine particles are supported on the surface of carbon powder and PTFE as a binder to the electrode base material (1). The material that has been heat-treated at a temperature of around 850° C. is used. The matrix layer (4) is formed by applying a matrix paste containing silicon carbide powder and PTFE as a bonding material to the catalyst layer (2), for example, and heat-treated at a temperature of about 300 to 1350°C. It will be done. Catalyst layer (2) and matrix layer (
The heat treatment in 4) may be performed individually or simultaneously.
上記触媒ペーストとマトリックスペーストノ塗布方法と
しては、スプレー法、カーテン被覆法、ドクターブレー
ド法等の方法がある。上記触媒ペーストを電極基材（１
）に塗布するとき、触媒ペーストが電極基材（１３の内
部に浸み込むことにより、触媒浸み込み層（３）が形成
され、その深さは電極基材（１）の細孔径の大小、撥水
性の強弱、触媒ペーストの粘度の高低等の条件によって
変化する。従って、［極層材ｒｔ）や触媒ペーストの製
造ロットによって触媒浸み込み層（３）の深さは影響を
受けやすい。また、一枚の電極基材（１）の中でも細孔
径の大きさや、撥水性の強さの分布が均一でない場合は
、触媒浸み込み層（３）の深さの分布が均一でなくなる
。さらに、電極基材（１）の撥水処理に用いたＰＴＦＥ
が触媒ペーストの塗布後に３００〜８５０℃前後の温度
で熱処理を行うときに溶融して触媒層（２）の細孔構造
を変化させてしまう。Methods for applying the catalyst paste and matrix paste include a spray method, a curtain coating method, a doctor blade method, and the like. The above catalyst paste was applied to the electrode base material (1
), the catalyst paste soaks into the inside of the electrode base material (13), forming a catalyst-soaked layer (3), the depth of which depends on the size of the pores in the electrode base material (1). , varies depending on conditions such as the strength of water repellency and the viscosity of the catalyst paste.Therefore, the depth of the catalyst soaked layer (3) is likely to be affected by the production lot of the [pole layer material rt) and catalyst paste. . Further, if the size of pores and the distribution of water repellency strength are not uniform even within a single electrode base material (1), the distribution of the depth of the catalyst impregnated layer (3) will not be uniform. Furthermore, the PTFE used for water repellent treatment of the electrode base material (1)
However, when heat treatment is performed at a temperature of about 300 to 850° C. after application of the catalyst paste, the catalyst paste melts and changes the pore structure of the catalyst layer (2).
従来の燃料電池用電極／マトリックス結合体は以上のよ
うに構成されているので、触媒ペーストが電極基材（１
）の内部にまで浸み込み、電極凰材（１）の細孔が触媒
粉末と結着材によって埋められるため、電極基材（１）
のガス拡散性が低下するという問題点があった。リブ付
電極のように？を極層材の内部に電解質を保持する方式
の場合には、空孔体積が減少するため、電解質の保持量
が低下し、電池の寿命が短かくなるという問題点があっ
た。また、電極基材（１）に浸み込んだ触媒は電池反応
に有効に利用されないため触媒利用率が低いという問題
点があった。さらに、撥水処理を施した電極基材を用い
る場合は、マトリックス層表面からしかリン酸等の電解
質を塗布含浸できないという問題点があった。Since the conventional fuel cell electrode/matrix combination is constructed as described above, the catalyst paste is attached to the electrode base material (1
), and the pores of the electrode base material (1) are filled with the catalyst powder and binder, so that the electrode base material (1)
There was a problem in that the gas diffusivity of the gas was reduced. Like ribbed electrodes? In the case of a method in which the electrolyte is retained inside the electrode layer material, there is a problem that the pore volume decreases, so the amount of electrolyte retained decreases, and the life of the battery is shortened. In addition, there was a problem in that the catalyst that had penetrated into the electrode base material (1) was not effectively utilized in the battery reaction, resulting in a low catalyst utilization rate. Furthermore, when using an electrode base material that has been subjected to water-repellent treatment, there is a problem in that an electrolyte such as phosphoric acid can be applied and impregnated only from the surface of the matrix layer.
この発明は、上記のような問題点を解消するためになさ
れたもので、電極基材のガス拡散性の向上、電極基材の
電解質の保持量の増加、触媒利用率の向上ができるとと
もに、触媒層表面とマトリックス層表面の両方からリン
酸等の電解質を塗布含浸できる燃料電池用室１’＠／マ
トリックス結合体を得ることを目的とする。This invention was made to solve the above problems, and it is possible to improve the gas diffusivity of the electrode base material, increase the amount of electrolyte retained in the electrode base material, and improve the catalyst utilization rate. The object of the present invention is to obtain a fuel cell chamber 1'@/matrix combination that can be coated and impregnated with an electrolyte such as phosphoric acid from both the surface of the catalyst layer and the surface of the matrix layer.
この発明に係る燃料電池用［極／マトリックス結合体は
、１！極基材と触媒層／マトリ、ツクス結合体とを分離
するとともに、触媒層／マトリックス結合体を多孔質シ
ートの一方の面より触媒粉末と結着材とが充填された触
媒充填層と前記触媒充填層の表面に触媒粉末と結着材と
が付着された触媒付着層とからなる触媒層と、前記多孔
質シートの他方の面よりマトリックス骨格材料と固着材
とが充填されたマトリックス充填層と前記マトリックス
充填層の表面にマトリックス骨格材料と固着材とが付着
されたマトリックス付着層とからなるマトリックス層と
から形成したものである。The electrode/matrix combination for fuel cells according to the present invention is 1! The electrode base material and the catalyst layer/matrix and Tux combined body are separated, and the catalyst layer/matrix combined body is separated from one side of the porous sheet by a catalyst packed layer filled with catalyst powder and a binder and the catalyst. a catalyst layer consisting of a catalyst adhesion layer in which catalyst powder and a binder are adhered to the surface of the packed bed; and a matrix packed layer in which a matrix skeleton material and a binder are filled from the other side of the porous sheet. A matrix layer is formed of a matrix adhesion layer having a matrix skeleton material and a fixing material attached to the surface of the matrix filling layer.
この発明における燃料電池用！［／マトリックス結合体
は、触媒層／マトリックス結合体を独立膜として形成で
き、電極基材の細孔構造に悪影響、を及ぼさずに電極／
マトリックス結合体を製造できるとともに触媒が無駄な
く電池反応に利用できる。For fuel cells in this invention! [/Matrix combination allows the catalyst layer/matrix combination to be formed as an independent membrane, and the electrode/matrix combination can be formed as an independent membrane without adversely affecting the pore structure of the electrode base material.
A matrix composite can be produced, and the catalyst can be used for battery reactions without waste.
この発明による触媒層／マトリックス結合体を安定して
得るためＫは、多孔質シートは気孔率が例えば５０チ以
上（好ましくは７５チ以上）のものが望ましく、例えば
、厚さ８０〜ａＯＯμｍ（好ましくは５０〜２００μｍ
）のカーボン繊維シートが優れている。In order to stably obtain the catalyst layer/matrix combination according to the present invention, the porous sheet preferably has a porosity of, for example, 50 cm or more (preferably 75 cm or more), and has a thickness of, for example, 80 to aOOμm (preferably is 50 to 200 μm
) carbon fiber sheets are superior.
触媒付着層の厚さは例えば１０〜２００μｍ（好ましく
は５０〜１５０μｍ）、マトリックス付着層の厚さは例
えば８０〜３００μｍ（好ましくは５０〜２００μｍ）
にするのが望ましい。また、触媒層全体の厚さは例えば
５０〜４００ ｐｍ （好ましくは１００〜３００ ｐ
ｍ ）、マトリックス層全体の厚さは例えば５０〜５０
０μｍ（好ましくは１００〜３００μｍ）にするのが望
ましい。The thickness of the catalyst adhesion layer is, for example, 10 to 200 μm (preferably 50 to 150 μm), and the thickness of the matrix adhesion layer is, for example, 80 to 300 μm (preferably 50 to 200 μm).
It is desirable to do so. The thickness of the entire catalyst layer is, for example, 50 to 400 pm (preferably 100 to 300 pm).
m), the thickness of the entire matrix layer is e.g.
It is desirable that the thickness be 0 μm (preferably 100 to 300 μm).
上記触媒層は触媒粉末と結着材とからなっている。触媒
粉末は炭素粉末表面に白金微粒子を担持させたものが用
いられ、結着材としては、ポリテトラフルオロエチレン
（ＰＴＦＥ ）やテトヮフルオロエチレンーヘキサフル
オロプロピレン共重合体（以下ＦＥＰと略称する）等の
フッ素樹脂が適している。The catalyst layer is made of catalyst powder and a binder. The catalyst powder used is one in which fine platinum particles are supported on the surface of carbon powder, and the binder is polytetrafluoroethylene (PTFE) or tetrafluoroethylene-hexafluoropropylene copolymer (hereinafter abbreviated as FEP). Fluororesins such as are suitable.
上記マトリックス層はマトリックス骨格材料と固着材と
からなっている。マトリックス骨格材料はカーボン、無
機化合物、金属のリン酸塩等が用いられる。マトリック
ス骨格材料として、無機化合物では、粉末状または繊維
状の酸化ジルコニウム、シリカ、アルミナ、シリカアル
ミナ、酸化ニオブ、酸化タンタル、酸化タングステン、
酸化チタン、窒化珪素、炭化ホウ素、炭化タングステン
、炭化珪素等が用いられ、窒化珪素、炭化珪素が優れて
おり、金属のリン酸塩では、珪素チタン、スズ、アルミ
ニウム、ジルコニウム等とリン酸との塩、例えばＳｉＰ
ｔＯｙ −ＺｒＰｔ０ｙ等が適している。固着材として
はＰＴＦＥやＦＥＰ等のフッ素樹脂が適しているが、マ
トリックス中のリン酸等の電解質の保持性を向上させる
ために、上記固着材に、ポリエーテルスルフォン、ポリ
エーテルエーテルケトン、ポリフェニレンサルファイド
等の親水性の熱可塑性樹脂を含有させておいても好結果
が得られる。The matrix layer is composed of a matrix skeleton material and a bonding material. Carbon, inorganic compounds, metal phosphates, etc. are used as the matrix skeleton material. As matrix skeleton materials, inorganic compounds include powdered or fibrous zirconium oxide, silica, alumina, silica alumina, niobium oxide, tantalum oxide, tungsten oxide,
Titanium oxide, silicon nitride, boron carbide, tungsten carbide, silicon carbide, etc. are used, and silicon nitride and silicon carbide are excellent.As for metal phosphates, silicon titanium, tin, aluminum, zirconium, etc. and phosphoric acid are used. salt, e.g. SiP
tOy -ZrPt0y etc. are suitable. Fluororesins such as PTFE and FEP are suitable as the adhesive material, but in order to improve the retention of electrolytes such as phosphoric acid in the matrix, polyether sulfone, polyether ether ketone, and polyphenylene sulfide are used as the adhesive material. Good results can also be obtained by containing hydrophilic thermoplastic resins such as.
以下、この発明の一実施例を図について説明する。第１
図において、（１）は電極基材、（５）は触媒層、（６
）はマトリックス層、（７）は多孔質シートであシ、触
媒層（５）とマトリックス層（６）とで一体の触媒層／
マトリックス結合体を形成している。An embodiment of the present invention will be described below with reference to the drawings. 1st
In the figure, (1) is the electrode base material, (5) is the catalyst layer, and (6) is the electrode base material.
) is a matrix layer, (7) is a porous sheet, and the catalyst layer (5) and matrix layer (6) are integrated.
Forms a matrix conjugate.
触媒層／マトリックス結合体は多孔質シート（７）の一
方の面より触媒粉末と結着材とが充填された触媒充填層
（８）と前記触媒充填層（８）の表面に触媒粉末と、結
着材とが付着された触媒付着層（９）とからなる触媒層
（５）と、前記多孔質シート（７）の他方の面よりマト
リックス骨格材料と固着材とが充填されたマトリックス
充填層αＯと前記マトリ・リクス充填層αｄの表面に７
１１ツクス骨格材料と固着材とが付着されたマトリック
ス付着層αυとから形成されたものである。The catalyst layer/matrix combination includes a catalyst packed layer (8) filled with catalyst powder and a binder from one side of a porous sheet (7), a catalyst powder on the surface of the catalyst packed layer (8), a catalyst layer (5) consisting of a catalyst adhesion layer (9) to which a binding material is attached; and a matrix packed layer filled with a matrix skeleton material and a binding material from the other side of the porous sheet (7). 7 on the surface of αO and the matrix packed layer αd.
It is formed from a matrix adhesion layer αυ to which a 11Tx skeleton material and a fixing material are attached.
次に製造方法について説明する。電極基材（１）は、厚
さ例えば３００μｍ、気孔率例えば７５チのカーボンペ
ーパをＰＴＦＥの分散液に浸漬後乾燥して、例えば８６
０℃の温度で熱処理して撥水処理を施した。Next, the manufacturing method will be explained. The electrode base material (1) is prepared by immersing a carbon paper having a thickness of, for example, 300 μm and a porosity of, for example, 75 cm in a PTFE dispersion and then drying it.
Water repellent treatment was performed by heat treatment at a temperature of 0°C.
触媒層（５）は次のようにして製造した。多孔質シ−）
（７）として厚さ例えば１００μｍ％完孔率例えば８
０係のカーボンペーパを用いた。この多孔質シート（７
）に炭素粉末表面に白金微粒子を担持させた触媒粉末と
結着材としてＰＴＦＥを充填して触媒充填層（８）を得
た。次にこの触媒充填層（８）の表面に上記触媒充填層
（８）と全く同じ組成の触媒粉末と結着材としてＰＴＦ
Ｅを付着して触媒付着層（９）を得た。なお、触媒粉末
と結着材は水性のペーストを調整して多孔質シート（７
）への充填及び付着をリバースロールコータ法などによ
勺行なった。続いて乾燥して、例えば８６０℃の温度で
熱処理して触媒層（５）を完成させた。触媒層（５）全
体の厚さは例えば２００μｍであり、触媒付着層（８）
の厚さは例えば１５０μｍであった。The catalyst layer (5) was manufactured as follows. porous sea)
(7) Thickness, for example, 100μm% porosity, for example, 8
0 carbon paper was used. This porous sheet (7
) was filled with catalyst powder in which platinum fine particles were supported on the carbon powder surface and PTFE as a binder to obtain a catalyst packed bed (8). Next, the surface of this catalyst packed bed (8) is coated with catalyst powder having exactly the same composition as the catalyst packed bed (8) and PTF as a binder.
E was deposited to obtain a catalyst deposited layer (9). In addition, the catalyst powder and the binder are prepared by preparing an aqueous paste and forming a porous sheet (7
) was filled and adhered by a reverse roll coater method. Subsequently, the catalyst layer (5) was completed by drying and heat treatment at a temperature of, for example, 860°C. The total thickness of the catalyst layer (5) is, for example, 200 μm, and the catalyst adhesion layer (8)
The thickness was, for example, 150 μm.
この触媒層（５）は可撓性があシ、手で持って取扱い可
能な自己支持性を有する独立膜となった。This catalyst layer (5) was a flexible, self-supporting independent membrane that could be held and handled by hand.
マトリックス層（６）は次のようにして製造した。The matrix layer (6) was manufactured as follows.
上記触媒層（５）を形成した多孔質シート（７）を反転
して、マ） ＋Ｊラックス格材料として炭化珪素粉末を
、固着材としてＰＴＦＥを充填してマトリックス充填層
００を得た。次に、この々トリックス充填Ｍ ｔｍの表
面に上記マトリックス充填層ａＯと全く同じ組成で、マ
トリックス骨格材料として炭化珪素粉末を、固着材とし
てＰＴＦＥを付着させて、マトリックス付着層αｐを得
た。なお、マトリックス骨格材料と固着材は水性のペー
ストを調製して多孔質シート（７）への充填及び付着を
リバースロールコータ法などによカ行なった。続いて、
乾燥して、例えば２５０℃の温度で熱処理して、マトリ
ックス層（６）全完成させた。マトリックス層（６）全
体の厚さは例えば２００μｍでアシ、マトリックス付着
層（１）の厚さは例えば１５０μｍであった。これで、
触媒層（５）とマトリックス層（６）が一体となった触
媒層／マトリックス結合体が得られた。この触媒層／マ
トリックス結合体は、可撓性があシ手で持って取扱い可
能な自己支持性を有する独立膜となった。上記の方法で
得た電極基材（１）及び触媒層／マトリックス結合体は
□電池組立時にＮ層して一体化して！！／マトリックス
結合体とした。The porous sheet (7) on which the catalyst layer (5) was formed was inverted and filled with silicon carbide powder as the +J lux rated material and PTFE as the fixing material to obtain a matrix-filled layer 00. Next, on the surface of each of the trix-filled M tm, silicon carbide powder was adhered as a matrix skeleton material and PTFE as a fixing material with exactly the same composition as the matrix-filled layer aO, to obtain a matrix adhesion layer αp. Note that the matrix skeleton material and the fixing material were prepared as an aqueous paste, and filled and adhered to the porous sheet (7) by a reverse roll coater method or the like. continue,
The matrix layer (6) was completely completed by drying and heat treatment at a temperature of, for example, 250°C. The overall thickness of the matrix layer (6) was, for example, 200 μm, and the thickness of the matrix adhesion layer (1) was, for example, 150 μm. with this,
A catalyst layer/matrix combination in which the catalyst layer (5) and matrix layer (6) were integrated was obtained. This catalyst layer/matrix combination was a self-supporting independent membrane that was flexible and could be handled by hand. The electrode base material (1) and catalyst layer/matrix combination obtained by the above method are □ integrated into N layers during battery assembly! ! /matrix conjugate.
前記の実施例では、触媒ペースト及びマ） ＩＪラック
スーストの多孔質シート（７）への充填・付着のための
塗工はリバースロールコータ法を用いたが、スプレー法
等も用いることが可能である。しかし、リバースロール
コータ法が最も適している。また前記の実施例では、電
極基材（１）と触媒層／マ）ＩＪワックス合体は電池組
立時に積層して一体化したが、予め、スプレまたは圧延
ロール等によシ両者を一体化しておいてもよい。さらに
、前記実施例では、電極基材（１）に撥水処理を怖じた
カーボンペーパを用いたが、を極基材（１）内に電解質
を保持する方式の、例えばリブ付置ｌｉｔ材であっても
よく、この場合、従来の電極基材（１）に触媒ペースト
を直接塗布する方法に比較して、浸み込み触媒層のない
分だけリン酸等の電解質を多く保持できる効果がある。In the above example, a reverse roll coater method was used to fill and adhere the catalyst paste and IJ Luxoaste to the porous sheet (7), but a spray method etc. can also be used. It is. However, the reverse roll coater method is most suitable. Furthermore, in the above embodiment, the electrode base material (1) and the catalyst layer/ma) IJ wax combination were laminated and integrated at the time of battery assembly. You can stay there. Furthermore, in the above embodiment, carbon paper that is not subject to water-repellent treatment was used as the electrode base material (1), but it is also possible to use a ribbed lit material that retains the electrolyte within the electrode base material (1). In this case, compared to the conventional method of directly applying a catalyst paste to the electrode base material (1), there is an effect that a large amount of electrolyte such as phosphoric acid can be retained due to the lack of a permeated catalyst layer.
以上のように、この発明によれば、燃料電池用ｔ［／マ
） ＩＪラックス合体を電極基材と触媒層／マトリック
ス結合体とを分離し、触媒層／マトリックス結合体を多
孔質シートの一方の面より触媒粉末と結着材とが充填さ
れた触媒充填層と前記触媒充填層の表面に触媒粉末と結
着材とが付着された触媒付着層とからなる触媒層と、前
記多孔質シートの他方の面よりマトリックス骨格材料と
固着材とが充填されたマトリックス充填層と前記マトリ
ックス充填層°の表面にマトリックス骨格材料と固着材
とが付着されたマトリックス付着層とからなるマトリッ
クス層とから構成したので、電極基材のガス拡散性が良
好で、電池として構成した場合、出力電圧が高く、長寿
命で品質の安定したものが得られ、また、触媒層表面と
マトリックス層表面の両方からリン酸等の電解質を塗布
含浸でき、塗布含浸時間が短縮できるものが得られる効
果がある。As described above, according to the present invention, the electrode base material and the catalyst layer/matrix combination are separated from the electrode base material and the catalyst layer/matrix combination in the IJ lux combination for fuel cells, and the catalyst layer/matrix combination is placed on one side of the porous sheet. a catalyst layer comprising a catalyst packed layer filled with catalyst powder and a binder from a surface thereof, and a catalyst adhesion layer with catalyst powder and a binder adhered to the surface of the catalyst packed layer; and the porous sheet. A matrix layer consisting of a matrix filled layer filled with a matrix skeleton material and a fixing material from the other side of the matrix, and a matrix adhesion layer having a matrix skeleton material and a fixing material attached to the surface of the matrix filled layer. Therefore, the gas diffusivity of the electrode base material is good, and when configured as a battery, a battery with high output voltage, long life, and stable quality can be obtained. There is an effect that an electrolyte such as an acid can be coated and impregnated, and the coating and impregnating time can be shortened.
第１図はこの発明の一実施例による燃料電池用電極／マ
トリックス結合体を示す断面図、第２図は従来の燃料電
池用電極／マトリックヌ結合体を示す断面図である。
図において、（１）は電極基材、（５）は触媒層、（６
）はマトリックス層、（７）は多孔質シー）、（８１は
触媒充填層、（９）は触媒付着層、ＧＯはマトリックス
充填層、αηはマトリックス付着層である。
なお、図中、同一符号は同一、又は相補部分を示す。FIG. 1 is a sectional view showing a fuel cell electrode/matrix combination according to an embodiment of the present invention, and FIG. 2 is a sectional view showing a conventional fuel cell electrode/matrix combination. In the figure, (1) is the electrode base material, (5) is the catalyst layer, and (6) is the electrode base material.
) is a matrix layer, (7) is a porous sheet), (81 is a catalyst packed layer, (9) is a catalyst adhesion layer, GO is a matrix packed layer, and αη is a matrix adhesion layer. In addition, the same reference numerals are used in the figure. indicate the same or complementary parts.
Claims (9)
る燃料電池用電極／マトリックス結合体において、触媒
層／マトリックス結合体が多孔質シートの一方の面より
触媒粉末と結着材とが充填された触媒充填層と前記触媒
充填層の表面に触媒粉末と結着材とが付着された触媒付
着層とからなる触媒層と、前記多孔質シートの他方の面
よりマトリックス骨格材料と固着材とが充填されたマト
リックス充填層と前記マトリックス充填層の表面にマト
リックス骨格材料と固着材とが付着されたマトリックス
付着層とからなるマトリックス層とから構成されたこと
を特徴とする燃料電池用電極／マトリツクス結合体。(1) In a fuel cell electrode/matrix combination consisting of an electrode base material and a catalyst layer/matrix combination, the catalyst layer/matrix combination is filled with catalyst powder and a binder from one side of the porous sheet. A catalyst layer consisting of a catalyst packed layer and a catalyst adhesion layer in which a catalyst powder and a binder are attached to the surface of the catalyst packed layer, and a matrix skeleton material and a binder from the other side of the porous sheet. An electrode/matrix for a fuel cell, characterized in that it is constituted by a matrix layer consisting of a matrix filling layer filled with and a matrix adhesion layer having a matrix skeleton material and a fixing material attached to the surface of the matrix filling layer. conjugate.
特徴とする特許請求の範囲第１項記載の燃料電池用電極
／マトリックス結合体。(2) The electrode/matrix assembly for a fuel cell according to claim 1, wherein the porous sheet has a porosity of 50% or more.
繊維シートであることを特徴とする特許請求の範囲第１
項または、第２項に記載の燃料電池用電極／マトリック
ス結合体。(3) Claim 1, wherein the porous sheet is a carbon fiber sheet with a thickness of 80 to 300 μm.
or the fuel cell electrode/matrix assembly according to item 2.
を特徴とする特許請求の範囲第１項ないし第８項のいず
れかに記載の燃料電池用電極／マトリックス結合体。(4) The electrode/matrix assembly for a fuel cell according to any one of claims 1 to 8, wherein the catalyst adhesion layer has a thickness of 10 to 300 μm.
あることを特徴とする特許請求の範囲第１項ないし第４
項のいずれかに記載の燃料電池用電極／マトリックス結
合体。(5) Claims 1 to 4 characterized in that the thickness of the matrix adhesion layer is 80 to 300 μm.
The fuel cell electrode/matrix combination according to any one of Items 1-2.
、テトラフルオロエチレン−ヘキサフルオロプロピレン
共重合体等のフッ素樹脂であることを特徴とする特許請
求の範囲第１項ないし第５項のいずれかに記載の燃料電
池用電極／マトリックス結合体。(6) Any one of claims 1 to 5, wherein the binder of the catalyst layer is a fluororesin such as polytetrafluoroethylene or tetrafluoroethylene-hexafluoropropylene copolymer. The fuel cell electrode/matrix combination according to claim 1.
チレン、テトラフルオロエチレン−ヘキサフルオロプロ
ピレン共重合体等のフッ素樹脂を含有していることを特
徴とする特許請求の範囲第１項ないし第６項のいずれか
に記載の燃料電池用電極／マトリックス結合体。(7) Claims 1 to 6 characterized in that the fixing material of the matrix layer contains a fluororesin such as polytetrafluoroethylene or tetrafluoroethylene-hexafluoropropylene copolymer. An electrode/matrix combination for a fuel cell according to any one of the above.
ォン、ポリエーテルエーテルケトン、ポリフエニレンサ
ルファイド等の親水性の熱可塑性樹脂を含有しているこ
とを特徴とする特許請求の範囲第１項ないし第６項のい
ずれかに記載の燃料電池用電極／マトリックス結合体。(8) Claims 1 to 1, characterized in that the fixing material of the matrix layer contains a hydrophilic thermoplastic resin such as polyether sulfone, polyether ether ketone, or polyphenylene sulfide. The electrode/matrix combination for a fuel cell according to any one of Item 6.
合物、金属のリン酸塩から選ばれた少なくとも１種の物
質粉末または繊維であることを特徴とする特許請求の範
囲第１項ないし第８項のいずれかに記載の燃料電池用／
マトリックス結合体。(9) Claims 1 to 8, characterized in that the skeleton material of the matrix layer is at least one substance powder or fiber selected from carbon, inorganic compounds, and metal phosphates. For fuel cells described in any of the above/
matrix conjugate.
Priority Applications (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62012812A JPH0628163B2 (en) | 1987-01-21 | 1987-01-21 | Fuel cell electrode / matrix combination |
| US07/139,571 US4847173A (en) | 1987-01-21 | 1987-12-30 | Electrode for fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62012812A JPH0628163B2 (en) | 1987-01-21 | 1987-01-21 | Fuel cell electrode / matrix combination |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS63181264A true JPS63181264A (en) | 1988-07-26 |
| JPH0628163B2 JPH0628163B2 (en) | 1994-04-13 |
Family
ID=11815794
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62012812A Expired - Fee Related JPH0628163B2 (en) | 1987-01-21 | 1987-01-21 | Fuel cell electrode / matrix combination |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0628163B2 (en) |
-
1987
- 1987-01-21 JP JP62012812A patent/JPH0628163B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0628163B2 (en) | 1994-04-13 |
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