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Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin
Low overpotential water oxidation under mild conditions is required for new energy conversion technologies with potential application prospects. Extensive studies on molecular catalysis have been performed to gain fundamental knowledge for the rational designing of cheap, efficient and robust cataly...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Royal Society of Chemistry
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6419937/ https://www.ncbi.nlm.nih.gov/pubmed/30996977 http://dx.doi.org/10.1039/c8sc04529a |
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author | Liu, Yanju Han, Yongzhen Zhang, Zongyao Zhang, Wei Lai, Wenzhen Wang, Yong Cao, Rui |
author_facet | Liu, Yanju Han, Yongzhen Zhang, Zongyao Zhang, Wei Lai, Wenzhen Wang, Yong Cao, Rui |
author_sort | Liu, Yanju |
collection | PubMed |
description | Low overpotential water oxidation under mild conditions is required for new energy conversion technologies with potential application prospects. Extensive studies on molecular catalysis have been performed to gain fundamental knowledge for the rational designing of cheap, efficient and robust catalysts. We herein report a water-soluble Cu(II) complex of tetrakis(4-N-methylpyridyl)porphyrin (1), which catalyzes the oxygen evolution reaction (OER) in neutral aqueous solutions with small overpotentials: the onset potential of the catalytic water oxidation wave measured at current density j = 0.10 mA cm(–2) is 1.13 V versus a normal hydrogen electrode (NHE), which corresponds to an onset overpotential of 310 mV. Constant potential electrolysis of 1 at neutral pH and at 1.30 V versus NHE displayed a substantial and stable current for O(2) evolution with a faradaic efficiency of >93%. More importantly, in addition to the 4e water oxidation to O(2) at neutral pH, 1 can catalyze the 2e water oxidation to H(2)O(2) in acidic solutions. The produced H(2)O(2) is detected by rotating ring–disk electrode measurements and by the sodium iodide method after bulk electrolysis at pH 3.0. This work presents an efficient and robust Cu-based catalyst for water oxidation in both neutral and acidic solutions. The observation of H(2)O(2) during water oxidation catalysis is rare and will provide new insights into the water oxidation mechanism. |
format | Online Article Text |
id | pubmed-6419937 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-64199372019-04-17 Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin Liu, Yanju Han, Yongzhen Zhang, Zongyao Zhang, Wei Lai, Wenzhen Wang, Yong Cao, Rui Chem Sci Chemistry Low overpotential water oxidation under mild conditions is required for new energy conversion technologies with potential application prospects. Extensive studies on molecular catalysis have been performed to gain fundamental knowledge for the rational designing of cheap, efficient and robust catalysts. We herein report a water-soluble Cu(II) complex of tetrakis(4-N-methylpyridyl)porphyrin (1), which catalyzes the oxygen evolution reaction (OER) in neutral aqueous solutions with small overpotentials: the onset potential of the catalytic water oxidation wave measured at current density j = 0.10 mA cm(–2) is 1.13 V versus a normal hydrogen electrode (NHE), which corresponds to an onset overpotential of 310 mV. Constant potential electrolysis of 1 at neutral pH and at 1.30 V versus NHE displayed a substantial and stable current for O(2) evolution with a faradaic efficiency of >93%. More importantly, in addition to the 4e water oxidation to O(2) at neutral pH, 1 can catalyze the 2e water oxidation to H(2)O(2) in acidic solutions. The produced H(2)O(2) is detected by rotating ring–disk electrode measurements and by the sodium iodide method after bulk electrolysis at pH 3.0. This work presents an efficient and robust Cu-based catalyst for water oxidation in both neutral and acidic solutions. The observation of H(2)O(2) during water oxidation catalysis is rare and will provide new insights into the water oxidation mechanism. Royal Society of Chemistry 2019-01-07 /pmc/articles/PMC6419937/ /pubmed/30996977 http://dx.doi.org/10.1039/c8sc04529a Text en This journal is © The Royal Society of Chemistry 2019 http://creativecommons.org/licenses/by/3.0/ This article is freely available. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0) |
spellingShingle | Chemistry Liu, Yanju Han, Yongzhen Zhang, Zongyao Zhang, Wei Lai, Wenzhen Wang, Yong Cao, Rui Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin |
title | Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin
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title_full | Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin
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title_fullStr | Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin
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title_full_unstemmed | Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin
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title_short | Low overpotential water oxidation at neutral pH catalyzed by a copper(ii) porphyrin
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title_sort | low overpotential water oxidation at neutral ph catalyzed by a copper(ii) porphyrin |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6419937/ https://www.ncbi.nlm.nih.gov/pubmed/30996977 http://dx.doi.org/10.1039/c8sc04529a |
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