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Defective and "c-Disordered" Hortensia-like Layered MnOx as an Efficient Electrocatalyst for Water Oxidation at Neutral pH
KTH, School of Chemical Science and Engineering (CHE), Chemistry.
KTH, School of Chemical Science and Engineering (CHE), Chemistry.
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Organic Chemistry.
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2017 (English)In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 7, no 9, p. 6311-6322Article in journal (Refereed) Published
Abstract [en]

The development of a highly active manganese-based water oxidation catalyst in the design of an ideal artificial photosynthetic device operating under neutral pH conditions remains a great challenge, due to the instability of pivotal Mn3+ intermediates. We report here defective and "c-disordered" layered manganese oxides (MnOx-300) formed on a fluorine-doped tin oxide electrode by constant anodic potential deposition and subsequent annealing, with a catalytic onset (0.25 mA/cm(2)) at an overpotential (eta) of 280 mV and a benchmark catalytic current density of 1.0 mA/cm(2) at an overpotential (eta) of 330 mV under neutral pH (1 M potassium phosphate). Steady current density above 8.2 mA/cm(2) was obtained during the electrolysis at 1.4 V versus the normal hydrogen electrode for 20 h. Insightful studies showed that the main contributing factors for the observed high activity of MnOx-300 are (i) a defective and randomly stacked layered structure, (ii) an increased degree of Jahn-Teller distorted Mn3+ in the MnO6 octahedral sheets, (iii) effective stabilization of Mn3+, (iv) a high surface area, and (v) improved electrical conductivity. These results demonstrate that manganese oxides as structural and functional models of an oxygen-evolving complex (OEC) in photosystem II are promising catalysts for water oxidation in addition to Ni/Co-based oxides/hydroxides.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017. Vol. 7, no 9, p. 6311-6322
Keywords [en]
artificial photosynthesis, electrocatalyst, layered manganese oxide, oxygen evolution, solar fuel, water oxidation
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-215387DOI: 10.1021/acscatal.7b00420ISI: 000410005700085Scopus ID: 2-s2.0-85029142521OAI: oai:DiVA.org:kth-215387DiVA, id: diva2:1148249
Funder
Swedish Energy AgencyKnut and Alice Wallenberg FoundationSwedish Research Council
Note

QC 20171010

Available from: 2017-10-10 Created: 2017-10-10 Last updated: 2017-10-10Bibliographically approved

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