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Electrocatalytic Water Oxidation by MnOx /C: In Situ Catalyst Formation, Carbon Substrate Variations, and Direct O2 /CO2 Monitoring by Membrane-Inlet Mass Spectrometry
Albert-Ludwigs-Universitat, Freiburg, Germany.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Umeå Universitet, Umeå, Sweden. (Molecular Biomimetics)ORCID iD: 0000-0002-9732-8867
Umeå Universitet, Umeå, Sweden.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. Umeå Universitet, Umeå, Sweden.
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2017 (English)In: ChemSusChem, ISSN 1864-5631, E-ISSN 1864-564X, Vol. 10, no 22, p. 4491-4502Article in journal (Refereed) Published
Abstract [en]

Layers of amorphous manganese oxides were directly formed on the surfaces of different carbon materials by exposing the carbon to aqueous solutions of permanganate (MnO4- ) followed by sintering at 100-400 °C. During electrochemical measurements in neutral aqueous buffer, nearly all of the MnOx /C electrodes show significant oxidation currents at potentials relevant for the oxygen evolution reaction (OER). However, by combining electrolysis with product detection by using mass spectrometry, it was found that these currents were only strictly linked to water oxidation if MnOx was deposited on graphitic carbon materials (faradaic O2 yields >90 %). On the contrary, supports containing sp3 -C were found to be unsuitable as the OER is accompanied by carbon corrosion to CO2 . Thus, choosing the "right" carbon material is crucial for the preparation of stable and efficient MnOx /C anodes for water oxidation catalysis. For MnOx on graphitic substrates, current densities of >1 mA cm-2 at η=540 mV could be maintained for at least 16 h of continuous operation at pH 7 (very good values for electrodes containing only abundant elements such as C, O, and Mn) and post-operando measurements proved the integrity of both the catalyst coating and the underlying carbon at OER conditions.

Place, publisher, year, edition, pages
2017. Vol. 10, no 22, p. 4491-4502
Keywords [en]
carbon materials, electrocatalysis, manganese, mass spectrometry, oxides
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-336243DOI: 10.1002/cssc.201701383ISI: 000416158500025PubMedID: 28869720OAI: oai:DiVA.org:uu-336243DiVA, id: diva2:1165474
Funder
Swedish Energy Agency, 36658-1Knut and Alice Wallenberg Foundation, KAW 2011.0055Available from: 2017-12-13 Created: 2017-12-13 Last updated: 2018-09-21Bibliographically approved

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Kwong, Wai LingMessinger, Johannes

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