Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 44, Pages 18153-18156Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja306499n
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Funding
- Exploratory Research for Advanced Technology (ERATO) program of the Japan Science and Technology Agency (JST)
- Ministry of Education, Culture, Sports, Science, Technology (MEXT) of the Japanese Government [21750186]
- Canon Foundation
- Research Fellowships of the Japan Society for Promotion of Science (PPS) for Young Scientists [21circle9161]
- Grants-in-Aid for Scientific Research [24655167, 21750186] Funding Source: KAKEN
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The development of Mn-oxide electrocatalysts for the oxidation of H2O to O-2 has been the subject of intensive researches not only for their importance as Components of artificial photosynthetic systems, but also as O-2-evolving centers in photosystem II. However, limited knowledge of the mechanisms underlying this oxidation reaction hampers the ability to rationally design effective catalysts. Herein, using in situ spectroelectrochemical techniques, we demonstrate that the stabilization of surface-associated intermediate Mn3+ species relative to charge disproportionation is an effective strategy to lower the overpotential for water oxidation by MnO2. The formation of N-Mn bonds via the coordination of amine groups of poly(allylamine hydrochloride) to the surface Mn sites of MnO2 electrodes effectively stabilized the Mn3+ species, resulting in an similar to 500-mV negative shift of the onset potential for the O-2 evolution reaction at neutral pH.
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