JP5015706B2 - ナノ複合体イオン錯体を利用した電解質膜及びそれを採用した燃料電池 - Google Patents
ナノ複合体イオン錯体を利用した電解質膜及びそれを採用した燃料電池 Download PDFInfo
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- JP5015706B2 JP5015706B2 JP2007241445A JP2007241445A JP5015706B2 JP 5015706 B2 JP5015706 B2 JP 5015706B2 JP 2007241445 A JP2007241445 A JP 2007241445A JP 2007241445 A JP2007241445 A JP 2007241445A JP 5015706 B2 JP5015706 B2 JP 5015706B2
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- electrolyte membrane
- polymer
- clay
- group
- nanocomposite
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- XCOBTUNSZUJCDH-UHFFFAOYSA-B lithium magnesium sodium silicate Chemical compound [Li+].[Li+].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Na+].[Na+].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3.O1[Si](O2)([O-])O[Si]3([O-])O[Si]1([O-])O[Si]2([O-])O3 XCOBTUNSZUJCDH-UHFFFAOYSA-B 0.000 description 7
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- 239000012153 distilled water Substances 0.000 description 6
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- QHPQWRBYOIRBIT-UHFFFAOYSA-N 4-tert-butylphenol Chemical compound CC(C)(C)C1=CC=C(O)C=C1 QHPQWRBYOIRBIT-UHFFFAOYSA-N 0.000 description 1
- QDOGSLSGLUTSQL-UHFFFAOYSA-N 6-amino-2,4-dichloro-3-methylphenol Chemical compound CC1=C(Cl)C=C(N)C(O)=C1Cl QDOGSLSGLUTSQL-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 1
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- 239000005058 Isophorone diisocyanate Substances 0.000 description 1
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- 125000002252 acyl group Chemical group 0.000 description 1
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- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 description 1
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- CQEYYJKEWSMYFG-UHFFFAOYSA-N butyl acrylate Chemical compound CCCCOC(=O)C=C CQEYYJKEWSMYFG-UHFFFAOYSA-N 0.000 description 1
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- NIMLQBUJDJZYEJ-UHFFFAOYSA-N isophorone diisocyanate Chemical compound CC1(C)CC(N=C=O)CC(C)(CN=C=O)C1 NIMLQBUJDJZYEJ-UHFFFAOYSA-N 0.000 description 1
- 239000003273 ketjen black Substances 0.000 description 1
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- QLNWXBAGRTUKKI-UHFFFAOYSA-N metacetamol Chemical compound CC(=O)NC1=CC=CC(O)=C1 QLNWXBAGRTUKKI-UHFFFAOYSA-N 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- DHAFIDRKDGCXLV-UHFFFAOYSA-N n,n-dimethylformamide;1-methylpyrrolidin-2-one Chemical compound CN(C)C=O.CN1CCCC1=O DHAFIDRKDGCXLV-UHFFFAOYSA-N 0.000 description 1
- 238000007344 nucleophilic reaction Methods 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- PNJWIWWMYCMZRO-UHFFFAOYSA-N pent‐4‐en‐2‐one Natural products CC(=O)CC=C PNJWIWWMYCMZRO-UHFFFAOYSA-N 0.000 description 1
- 238000005191 phase separation Methods 0.000 description 1
- 125000005496 phosphonium group Chemical group 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- CFQCIHVMOFOCGH-UHFFFAOYSA-N platinum ruthenium Chemical compound [Ru].[Pt] CFQCIHVMOFOCGH-UHFFFAOYSA-N 0.000 description 1
- 229910000027 potassium carbonate Inorganic materials 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
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- 230000008961 swelling Effects 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- DVKJHBMWWAPEIU-UHFFFAOYSA-N toluene 2,4-diisocyanate Chemical compound CC1=CC=C(N=C=O)C=C1N=C=O DVKJHBMWWAPEIU-UHFFFAOYSA-N 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
Classifications
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- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
- H01M8/1018—Polymeric electrolyte materials
- H01M8/1069—Polymeric electrolyte materials characterised by the manufacturing processes
- H01M8/1081—Polymeric electrolyte materials characterised by the manufacturing processes starting from solutions, dispersions or slurries exclusively of polymers
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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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04197—Preventing means for fuel crossover
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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
- H01M8/10—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
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
- H01M8/1018—Polymeric electrolyte materials
- H01M8/102—Polymeric electrolyte materials characterised by the chemical structure of the main chain of the ion-conducting polymer
- H01M8/1027—Polymeric electrolyte materials characterised by the chemical structure of the main chain of the ion-conducting polymer having carbon, oxygen and other atoms, e.g. sulfonated polyethersulfones [S-PES]
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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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
- H01M8/1018—Polymeric electrolyte materials
- H01M8/1041—Polymer electrolyte composites, mixtures or blends
- H01M8/1044—Mixtures of polymers, of which at least one is ionically conductive
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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
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
- H01M8/1018—Polymeric electrolyte materials
- H01M8/1041—Polymer electrolyte composites, mixtures or blends
- H01M8/1046—Mixtures of at least one polymer and at least one additive
- H01M8/1051—Non-ion-conducting additives, e.g. stabilisers, SiO2 or ZrO2
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
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- 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
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- 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
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- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T428/00—Stock material or miscellaneous articles
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- Y10T428/2913—Rod, strand, filament or fiber
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Description
S−DCDPS(0.1モル)、DCDPS(0.35モル)、HFIPDP(0.459モル)及び炭酸カリウム(0.55モル)を利用して、NMP(120mL)及びトルエン(100mL)を溶媒として使用して150℃で12時間還流して形成された水を除去した後、それ以上水がディーンストック装置を通じて出ないことを確認し、トルエンを前記ディーンストック装置の弁を通じて除去した。次いで、2時間にわたって反応混合物の温度を180℃に上昇させた後、この温度で4時間縮合重合反応を実施した。
HFIPDPの代わりにビスフェノールAを使用したことを除いては、実施例1と同じ方法によって実施して電解質膜及び燃料電池を完成した。
二種のジオールであるHFIPDP(30重量%)ビスフェノールA(70重量%)を使用したことを除いては、実施例1と同じ方法によって実施してスルホン化ポリスルホンナノ複合体を合成した。このとき、使用したクレーは、ラポナイトであり、膜を製造する時にポリベンズイミダゾール5質量部が付加された混合物に8:400:0.8混合重量比の多価アルコールのアクリル酸エステルであるポリ(メタクリル酸メチル−co−アクリル酸ブチル−co−メタクリル酸ヒドロキシエチル)、溶媒である1−プロパノール及び硬化剤である1,6−ヘキサメチレンジイソシアネートを付加及び混合したことを除いては、実施例1と同じ方法によって実施して電解質膜及び燃料電池を完成した。
MMTの代わりにラポナイトを使用したことを除いては、実施例1と同じ方法によって実施して電解質膜及び燃料電池を完成した。
MMTの代わりにラポナイトを使用したことを除いては、実施例2と同じ方法によって実施して電解質膜及び燃料電池を完成した。
非変性クレーを添加していないことを除いては、実施例1と同じ方法によって実施して電解質膜及び燃料電池を完成した。
電解質膜としてナフィオン112膜を使用したことを除いては、実施例1と同じ方法によって実施して燃料電池を完成した。
電解質膜としてナフィオン115膜を使用したことを除いては、実施例1と同じ方法によって実施して燃料電池を完成した。
ポリベンズイミダゾールの含量が10質量部であり、非変性クレーであるMMTを使用していないことを除いては、実施例1と同じ方法によって実施して電解質膜及び燃料電池を完成した。
Claims (9)
- スルホン酸基を有する高分子、及び、前記高分子中に分散され、層状構造を有する非変性クレーの複合体であるナノ複合体と、窒素原子の塩基性基を有している高分子との反応結果物であるナノ複合体イオン錯体を含み、
前記層の間に前記スルホン酸基を有する高分子がインタカレーションされているか、または、前記層が剥離されており、
前記スルホン酸基を有する高分子は、下記化学式1で表示されるスルホン化ポリスルホンであることを特徴とする、電解質膜。
pは、0ないし4の整数であり、
Xは、−C(CF 3 ) 2 −、−C(CH 3 ) 2 −または−PY’(=O)−(Y’は、HまたはC 6 H 5 である)であり、
Mは、Na、K、またはHであり、
mは、0.1ないし10の実数であり、nは、0.1ないし10の実数であり、kは、5ないし500の実数である。 - 前記スルホン化ポリスルホンは、下記化学式2で表示されることを特徴とする請求項1に記載の電解質膜。
- 前記塩基性高分子は、ポリベンズイミダゾール、ポリ(4−ビニルピリジン)、ポリエチレンイミン、(アクリルアミド−塩化ジアリルジメチルアンモニウム)共重合体、ポリ(塩化ジアリルジメチルアンモニウム)、ポリアクリルアミド系、ポリウレタン系、ポリアミド系、ポリイミン系、ポリウレア系、ポリベンゾオキサゾール系、ポリベンズイミダソール系及びポリピロリドン系からなる群から選択された一つ以上であることを特徴とする、請求項1に記載の電解質膜。
- 前記塩基性高分子の含量は、スルホン酸基を有する高分子100質量部を基準として0.1ないし40質量部であることを特徴とする請求項1に記載の電解質膜。
- 多価アルコールのアクリル酸エステルと硬化剤との硬化反応結果物であるアクリル系高分子がさらに含まれることを特徴とする、請求項1に記載の電解質膜。
- 前記非変性クレーは、スメクタイト系クレーであることを特徴とする、請求項1に記載の電解質膜。
- 前記スメクタイト系クレーは、モンモリロナイト、ベントナイト、サポナイト、ベイデライト、ノントロナイト、ヘクトライト及びスチーブンサイトからなる群から選択された一つ以上であることを特徴とする、請求項6に記載の電解質膜。
- 前記スルホン化ポリスルホンの数平均分子量は、1万ないし30万であり、質量平均分子量は、2万ないし50万であり、スルホン化度は、40ないし80%であることを特徴とする、請求項1に記載の電解質膜。
- カソード、アノード及びこれらの間に位置して請求項1ないし8のうち何れか1項に記載の電解質膜を備える、燃料電池。
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---|---|---|---|---|
KR100986493B1 (ko) * | 2008-05-08 | 2010-10-08 | 주식회사 동진쎄미켐 | 연료전지용 고분자 전해질 막 |
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KR100708713B1 (ko) * | 2005-09-24 | 2007-04-17 | 삼성에스디아이 주식회사 | 나노복합체, 나노복합 전해질막 및 이를 이용한 연료전지 |
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JP2011052222A (ja) | 2011-03-17 |
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US8039520B2 (en) | 2011-10-18 |
US20080176126A1 (en) | 2008-07-24 |
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CN101150196A (zh) | 2008-03-26 |
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