JP6204382B2 - 水素生成用レドックスフロー電池 - Google Patents
水素生成用レドックスフロー電池 Download PDFInfo
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- JP6204382B2 JP6204382B2 JP2014560318A JP2014560318A JP6204382B2 JP 6204382 B2 JP6204382 B2 JP 6204382B2 JP 2014560318 A JP2014560318 A JP 2014560318A JP 2014560318 A JP2014560318 A JP 2014560318A JP 6204382 B2 JP6204382 B2 JP 6204382B2
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- hydrogen
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- 229910052739 hydrogen Inorganic materials 0.000 title claims description 42
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims description 40
- 239000001257 hydrogen Substances 0.000 title claims description 40
- 239000003792 electrolyte Substances 0.000 claims description 73
- 239000003054 catalyst Substances 0.000 claims description 57
- 238000003860 storage Methods 0.000 claims description 26
- 230000003647 oxidation Effects 0.000 claims description 21
- 238000007254 oxidation reaction Methods 0.000 claims description 21
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 21
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 19
- 239000001301 oxygen Substances 0.000 claims description 19
- 229910052760 oxygen Inorganic materials 0.000 claims description 19
- 239000012528 membrane Substances 0.000 claims description 17
- 238000000034 method Methods 0.000 claims description 15
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 11
- AFVFQIVMOAPDHO-UHFFFAOYSA-N Methanesulfonic acid Chemical group CS(O)(=O)=O AFVFQIVMOAPDHO-UHFFFAOYSA-N 0.000 claims description 10
- 239000007789 gas Substances 0.000 claims description 10
- 229910052799 carbon Inorganic materials 0.000 claims description 8
- 239000002105 nanoparticle Substances 0.000 claims description 8
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- 150000001875 compounds Chemical class 0.000 claims description 6
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- 229940098779 methanesulfonic acid Drugs 0.000 claims description 5
- 239000000654 additive Substances 0.000 claims description 4
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- 239000011261 inert gas Substances 0.000 claims description 4
- 150000002894 organic compounds Chemical class 0.000 claims description 4
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 claims description 3
- 239000000460 chlorine Substances 0.000 claims description 3
- 229910052801 chlorine Inorganic materials 0.000 claims description 3
- 230000001590 oxidative effect Effects 0.000 claims description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 2
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- 238000006243 chemical reaction Methods 0.000 description 50
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- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 6
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- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 5
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- 229910052684 Cerium Inorganic materials 0.000 description 4
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- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 4
- 150000002431 hydrogen Chemical class 0.000 description 4
- CWQXQMHSOZUFJS-UHFFFAOYSA-N molybdenum disulfide Chemical group S=[Mo]=S CWQXQMHSOZUFJS-UHFFFAOYSA-N 0.000 description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
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- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 2
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- XMPZTFVPEKAKFH-UHFFFAOYSA-P ceric ammonium nitrate Chemical compound [NH4+].[NH4+].[Ce+4].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O XMPZTFVPEKAKFH-UHFFFAOYSA-P 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 239000008367 deionised water Substances 0.000 description 2
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- 238000007599 discharging Methods 0.000 description 2
- 230000009977 dual effect Effects 0.000 description 2
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- 150000002484 inorganic compounds Chemical class 0.000 description 2
- 229910010272 inorganic material Inorganic materials 0.000 description 2
- 238000009434 installation Methods 0.000 description 2
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- 239000000463 material Substances 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 238000013508 migration Methods 0.000 description 2
- 230000005012 migration Effects 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 229910052961 molybdenite Inorganic materials 0.000 description 2
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- 229910052697 platinum Inorganic materials 0.000 description 2
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- 238000004611 spectroscopical analysis Methods 0.000 description 2
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- QIJNJJZPYXGIQM-UHFFFAOYSA-N 1lambda4,2lambda4-dimolybdacyclopropa-1,2,3-triene Chemical compound [Mo]=C=[Mo] QIJNJJZPYXGIQM-UHFFFAOYSA-N 0.000 description 1
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 description 1
- GGZZISOUXJHYOY-UHFFFAOYSA-N 8-amino-4-hydroxynaphthalene-2-sulfonic acid Chemical compound C1=C(S(O)(=O)=O)C=C2C(N)=CC=CC2=C1O GGZZISOUXJHYOY-UHFFFAOYSA-N 0.000 description 1
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- ZAKOWWREFLAJOT-CEFNRUSXSA-N D-alpha-tocopherylacetate Chemical compound CC(=O)OC1=C(C)C(C)=C2O[C@@](CCC[C@H](C)CCC[C@H](C)CCCC(C)C)(C)CCC2=C1C ZAKOWWREFLAJOT-CEFNRUSXSA-N 0.000 description 1
- 108091006149 Electron carriers Proteins 0.000 description 1
- 229910003178 Mo2C Inorganic materials 0.000 description 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 description 1
- 229920000557 Nafion® Polymers 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 239000004809 Teflon Substances 0.000 description 1
- 229920006362 Teflon® Polymers 0.000 description 1
- 239000007983 Tris buffer Substances 0.000 description 1
- NJSSICCENMLTKO-HRCBOCMUSA-N [(1r,2s,4r,5r)-3-hydroxy-4-(4-methylphenyl)sulfonyloxy-6,8-dioxabicyclo[3.2.1]octan-2-yl] 4-methylbenzenesulfonate Chemical compound C1=CC(C)=CC=C1S(=O)(=O)O[C@H]1C(O)[C@@H](OS(=O)(=O)C=2C=CC(C)=CC=2)[C@@H]2OC[C@H]1O2 NJSSICCENMLTKO-HRCBOCMUSA-N 0.000 description 1
- SKAXWKNRKROCKK-UHFFFAOYSA-N [V].[Ce] Chemical compound [V].[Ce] SKAXWKNRKROCKK-UHFFFAOYSA-N 0.000 description 1
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- 229910052786 argon Inorganic materials 0.000 description 1
- HKVFISRIUUGTIB-UHFFFAOYSA-O azanium;cerium;nitrate Chemical compound [NH4+].[Ce].[O-][N+]([O-])=O HKVFISRIUUGTIB-UHFFFAOYSA-O 0.000 description 1
- 239000002551 biofuel Substances 0.000 description 1
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- 239000012018 catalyst precursor Substances 0.000 description 1
- 125000002091 cationic group Chemical group 0.000 description 1
- XQTIWNLDFPPCIU-UHFFFAOYSA-N cerium(3+) Chemical compound [Ce+3] XQTIWNLDFPPCIU-UHFFFAOYSA-N 0.000 description 1
- OZECDDHOAMNMQI-UHFFFAOYSA-H cerium(3+);trisulfate Chemical class [Ce+3].[Ce+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O OZECDDHOAMNMQI-UHFFFAOYSA-H 0.000 description 1
- ITZXULOAYIAYNU-UHFFFAOYSA-N cerium(4+) Chemical compound [Ce+4] ITZXULOAYIAYNU-UHFFFAOYSA-N 0.000 description 1
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- HTXDPTMKBJXEOW-UHFFFAOYSA-N dioxoiridium Chemical compound O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 description 1
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- PTISTKLWEJDJID-UHFFFAOYSA-N sulfanylidenemolybdenum Chemical compound [Mo]=S PTISTKLWEJDJID-UHFFFAOYSA-N 0.000 description 1
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- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
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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
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- 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
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- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Description
V3++e− → V2+(充電) (1a)
V2+ → V3++e−(放電) (lb)
アノードにおいて:
V4+ → V5++e−(充電) (2a)
V5+ +e− →V4+ (放電) (2b)
カソード電解質において:
V2+→V3++e−(触媒床の放電または化学的再生)・・・(3):
アノード電解質において:
V5++e−→V4+(触媒床の放電または化学的再生)・・・(4)
表1:いくつかのカソード性およびアノード性のメディエータおよびいくつかの化学種に対する標準的な還元電位。
アノード電解質において:
Ce3+→Ce4++e− (充電) (5a)
Ce4++e−→Ce3+ (触媒床における化学的再生または放電) (5b)
カソード電解質において:
V3++e―→V2+(充電) (6a)
V2+→V3++e(触媒床における化学的再生または放電) (6b)
2V2++2H+→2V3++H2 (Moベース触媒の存在下において) (7)
4Ce4+2H2O→4Ce3++O2+4H+
嫌気性条件の下でlhの間の磁気攪拌により、1MのH2SO4、20mmのV(II)、および3mgのシリカ支持−MoS2、または購入時のままの(as-bought)Mo2C粉を支えた(S1O2:MoS2モル比は、10:1である)を含む2mlの溶液から、水素ガスが成功裏に産生した。液体より上の雰囲気(ヘッドスペース)は、気密シリンジで採取され、GCに注入された。Mo2C(図2)に対する結果は、N2(ピーク22)の当初の存在と比較して、H2(ピーク21)の明確な存在を示す。
酸素ガス化学生成物水の酸化の生成は、以下の実験的な条件で明らかに観察された:中隔で密封されたガラスのバイアルにおいて、RFBで産生する1MのHNO3の中の100mmのセリウム硝酸アンモニウム(Ce(IV))の2mlの溶液は、嫌気性条件の下で、且つ、lhのためにかすかに動くことの下で3mgのIrO2/Si02の存在下、反応した。空気は気密シリンジを使用して吸ってみられて、GCに注入された。結果(図6)は、O2(ピーク61)とN2(ピーク62)(実験の背景ガス)の存在を示す。
Claims (14)
- 以下を含む、レドックスフロー電池システム:
a.以下を含むレドックスフロー電池:
i.正(positive)電解質と、該正電解質に少なくとも部分的に浸漬された電極とを含む第1のコンパートメント;負(negative)電解質と、該負電解質に少なくとも部分的に浸漬された電極とを含む第2のコンパートメント;および該第1および第2のコンパートメントを互いに分離する膜;を有する電気化学的セル;
ii.異なる電荷の状態で、それぞれ正および負の電解質を貯蔵するための第1および第2の貯蔵タンク;
iii.前記コンパートメントから貯蔵タンクへ、および、貯蔵タンクからコンパートメントへ、正および負の電解質をポンプ輸送するためのポンプ;および
iv.前記システムを脱酸素化して、チャージされた電解質を安定させるための不活性ガス源とインレット;
b.正電解質から化学種を酸化的に形成するため、およびレドックスフロー電池における再利用のために正電解質を再生するための第1の触媒床;
c.負電解質からのプロトンを分子状水素ガスへ還元するため、およびレドックスフロー電池における再利用のために負電解質を再生するための第2の触媒床;および
d.第1の触媒床に正電解質を導く(directing)ためのバルブ、および第2の触媒床に負電解質を導く(directing)ためのバルブ。 - 前記正電解質が、Ce4/Ce3+、V5+/V4+、MnO4−/Mn2+、Mn3+/Mn2+、Co3+/Co2+、およびBr/BrO3 −から選択されるレドックス対を含む請求項1に記載のシステム。
- 前記正電解質が、レドックス対の溶解性を増大させるための添加剤を含む請求項1または2のいずれか1項に記載のシステム。
- 前記レドックス対がCe4/Ce3+であるとき、前記添加剤がメタンスルホン酸である請求項3に記載のシステム。
- 前記負電解質が、V(III)/V(II)、Ti3+/Ti2+、Cr3+/Cr2+およびZn2+/Znから選択されるレドックス対を含む請求項1〜4のいずれか1項に記載のシステム。
- 前記膜が、イオン交換膜、またはナノフィルトレーション膜、またはアスベスト隔膜(diaphragm)である請求項1〜5のいずれか1項に記載のシステム。
- 前記電極が、金属電極、カーボン・フェルト電極、および他のカーボン電極から選択される、請求項1〜6のいずれか1項に記載のシステム。
- 前記電極が、ナノ粒子触媒によって修飾されたカーボン電極である請求項7に記載のシステム。
- 前記化学種が、O2である請求項1〜8のいずれか1項に記載のシステム。
- 前記第1の触媒床への通過の前に前記正電解質と、追加的な化合物とが混合される請求項1〜9のいずれか1項に記載のシステム。
- 前記追加的な化合物が、塩素を生成する塩化物、H2SO4を生成するSO2、またはCO2を生成する任意の有機化合物でもある請求項10に記載のシステム。
- 前記第1の触媒床が、水を酸素へ酸化するためのIrO2、RuO2、Mnおよび/又はCo酸化物を含む請求項1〜11のいずれか1項に記載のシステム。
- 前記第2の触媒床が、プロトンを水素に還元するための貴金属を含む請求項1〜12のいずれか1項に記載のシステム。
- 前記電気化学的セルが、電極のバイポーラスタックを含む求項1〜13のいずれか1項に記載のシステム。
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PCT/EP2013/054238 WO2013131838A1 (en) | 2012-03-05 | 2013-03-04 | Redox flow battery for hydrogen generation |
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