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      Preparative History vs Driving Force in Water Oxidation Catalysis: Parameter Space Studies of Cobalt Spinels

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          Abstract

          The development of efficient, stable, and economic water oxidation catalysts (WOCs) is a forefront topic of sustainable energy research. We newly present a comprehensive three-step approach to systematically investigate challenging relationships among preparative history, properties, and performance in heterogeneous WOCs. To this end, we studied (1) the influence of the preparative method on the material properties and (2) their correlation with the performance as (3) a function of the catalytic test method. Spinel-type Co 3O 4 was selected as a clear-cut model WOC and synthesized via nine different preparative routes. In search of the key material properties for high catalytic performance, these cobalt oxide samples were characterized with a wide range of analytical methods, including X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, powder X-ray diffraction, Raman spectroscopy, BET surface area analysis, and transmission electron microscopy. Next, the corresponding catalytic water oxidation activities were assessed with the three most widely applied protocols to date, namely, photocatalytic, electrocatalytic, and chemical oxidation. The activity of the Co 3O 4 samples was found to clearly depend on the applied test method. Increasing surface area and disorder as well as a decrease in oxidation states arising from low synthesis temperatures were identified as key parameters for high chemical oxidation activity. Surprisingly, no obvious property–performance correlations were found for photocatalytic water oxidation. In sharp contrast, all samples showed similar activity in electrochemical water oxidation. The substantial performance differences between the applied protocols demonstrate that control and comprehensive understanding of the preparative history are crucial for establishing reliable structure–performance relationships in WOC design.

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          Splitting Water with Cobalt

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            Recent Progress in Cobalt-Based Heterogeneous Catalysts for Electrochemical Water Splitting

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              Photophysics, photochemistry and solar energy conversion with tris(bipyridyl)ruthenium(II) and its analogues

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                Author and article information

                Journal
                ACS Omega
                ACS Omega
                ao
                acsodf
                ACS Omega
                American Chemical Society
                2470-1343
                13 September 2019
                24 September 2019
                : 4
                : 13
                : 15444-15456
                Affiliations
                []Department of Chemistry, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland
                []Empa—Swiss Federal Laboratories for Materials Science and Technology , Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
                Author notes
                Article
                10.1021/acsomega.9b01677
                6761687
                Copyright © 2019 American Chemical Society

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

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                ao9b01677
                ao-2019-01677s

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