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Intramolecular hydr...
Intramolecular hydroxyl nucleophilic attack pathway by a polymeric water oxidation catalyst with single cobalt sites
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- Yang, Hao (author)
- KTH,Organisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Li, Fusheng (author)
- KTH,Molekylär elektronik, CMD,Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian, Peoples R China.
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- Zhan, Shaoqi (author)
- KTH,Teoretisk kemi och biologi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Theoret Chem & Biol, Stockholm, Sweden
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- Liu, Yawen (author)
- Uppsala universitet,Fysikalisk kemi
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- Li, Wenlong (author)
- Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian, Peoples R China.
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- Meng, Qijun, 1990- (author)
- KTH,Organisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Kravchenko, Alexander (author)
- KTH,Organisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Liu, Tianqi (author)
- KTH,Organisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Yang, Yi (author)
- KTH,Tillämpad fysikalisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Fang, Yuan (author)
- KTH,Tillämpad fysikalisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Wang, Linqin (author)
- Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou, Peoples R China.;Westlake Univ, Sch Sci, Dept Chem, Hangzhou, Peoples R China.
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- Guan, Jiaqi (author)
- Westlake Univ, Instrumentat & Serv Ctr Phys Sci, Hangzhou, Peoples R China.
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- Furo, Istvan (author)
- KTH,Tillämpad fysikalisk kemi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden
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- Ahlquist, Mårten S. G., 1979- (author)
- KTH,Teoretisk kemi och biologi,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Theoret Chem & Biol, Stockholm, Sweden
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- Sun, Licheng, 1962- (author)
- KTH,Organisk kemi,Molekylär elektronik, CMD,KTH Royal Inst Technol, Sch Engn Sci Chem Biotechnol & Hlth, Dept Chem, Stockholm, Sweden.;Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, Inst Artificial Photosynth, State Key Lab Fine Chem, Dalian, Peoples R China.;Westlake Univ, Ctr Artificial Photosynth Solar Fuels, Sch Sci, Hangzhou, Peoples R China.;Westlake Univ, Sch Sci, Dept Chem, Hangzhou, Peoples R China
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(creator_code:org_t)
- 2022-05-25
- 2022
- English.
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In: Nature Catalysis. - : Springer Nature. - 2520-1158. ; 5:5, s. 414-429
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Abstract
Subject headings
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- Exploration of efficient water oxidation catalysts (WOCs) is the primary challenge in conversion of renewable energy into fuels. Here we report a molecularly well-defined heterogeneous WOC with Aza-fused, pi-conjugated, microporous polymer (Aza-CMP) coordinated single cobalt sites (Aza-CMP-Co). The single cobalt sites in Aza-CMP-Co exhibited superior activity under alkaline and near-neutral conditions. Moreover, the molecular nature of the isolated catalytic sites makes Aza-CMP-Co a reliable model for studying the heterogeneous water oxidation mechanism. By a combination of experimental and theoretical results, a pH-dependent nucleophilic attack pathway for O-O bond formation was proposed. Under alkaline conditions, the intramolecular hydroxyl nucleophilic attack (IHNA) process with which the adjacent -OH group nucleophilically attacks Co4+=O was identified as the rate-determining step. This process leads to lower activation energy and accelerated kinetics than those of the intermolecular water nucleophilic attack (WNA) pathway. This study provides significant insights into the crucial function of electrolyte pH in water oxidation catalysis and enhancement of water oxidation activity by regulation of the IHNA pathway.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
Publication and Content Type
- ref (subject category)
- art (subject category)
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- By the author/editor
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Yang, Hao
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Li, Fusheng
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Zhan, Shaoqi
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Liu, Yawen
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Li, Wenlong
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Meng, Qijun, 199 ...
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Kravchenko, Alex ...
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Liu, Tianqi
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Yang, Yi
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Fang, Yuan
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Wang, Linqin
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Guan, Jiaqi
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Furo, Istvan
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Ahlquist, Mårten ...
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Sun, Licheng, 19 ...
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- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Physical Chemist ...
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Chemical Science ...
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and Organic Chemistr ...
- Articles in the publication
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Nature Catalysis
- By the university
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Royal Institute of Technology
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Uppsala University