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dc.contributor.authorSun, Yuanmiaoen_US
dc.contributor.authorLiao, Hanbinen_US
dc.contributor.authorWang, Jiaruien_US
dc.contributor.authorChen, Boen_US
dc.contributor.authorSun, Shengnanen_US
dc.contributor.authorOng, Samuel Jun Hoongen_US
dc.contributor.authorXi, Shiboen_US
dc.contributor.authorDiao, Caozhengen_US
dc.contributor.authorDu, Yonghuaen_US
dc.contributor.authorWang, Jia-Ouen_US
dc.contributor.authorBreese, Mark B. H.en_US
dc.contributor.authorLi, Shuzhouen_US
dc.contributor.authorZhang, Huaen_US
dc.contributor.authorXu, Jason Zhichuanen_US
dc.identifier.citationSun, Y., Liao, H., Wang, J., Chen, B., Sun, S., Ong, S. J. H., Xi, S., Diao, C., Du, Y., Wang, J., Breese, M. B. H., Li, S., Zhang, H. & Xu, J. Z. (2020). Covalency competition dominates the water oxidation structure-activity relationship on spinel oxides. Nature Catalysis, 3, 554-563.
dc.description.abstractSpinel oxides have attracted growing interest over the years for catalysing the oxygen evolution reaction (OER) due to their efficiency and cost-effectiveness, but fundamental understanding of their structure–property relationships remains elusive. Here we demonstrate that the OER activity on spinel oxides is intrinsically dominated by the covalency competition between tetrahedral and octahedral sites. The competition fabricates an asymmetric MT−O−MO backbone where the bond with weaker metal–oxygen covalency determines the exposure of cation sites and therefore the activity. Driven by this finding, a dataset with more than 300 spinel oxides is computed and used to train a machine-learning model for screening the covalency competition in spinel oxides, with a mean absolute error of 0.05 eV. [Mn]T[Al0.5Mn1.5]OO4 is predicted to be a highly active OER catalyst and subsequent experimental results confirm its superior activity. This work sets mechanistic principles of spinel oxides for water oxidation, which may be extendable to other applications.en_US
dc.description.sponsorshipMinistry of Education (MOE)en_US
dc.description.sponsorshipNational Research Foundation (NRF)en_US
dc.relation.ispartofNature Catalysisen_US
dc.rights© 2020 The Author(s), under exclusive licence to Springer Nature Limited. All rights reserved. This paper was published in Nature Catalysis and is made available with permission of The Author(s).en_US
dc.titleCovalency competition dominates the water oxidation structure-activity relationship on spinel oxidesen_US
dc.typeJournal Articleen
dc.contributor.schoolSchool of Materials Science and Engineeringen_US
dc.contributor.organizationThe Cambridge Centre for Advanced Research and Education in Sinpagore, Sinpagpreen_US
dc.contributor.organizationSingapore–HUJ Alliance for Research and Enterprise (SHARE), Nanomaterials for Energy and Energy–Water Nexus (NEW), Campus for Research Excellence and Technological Enterprise (CREATE), Singapore, Singaporeen_US
dc.contributor.organizationInstitute of Chemical and Engineering Science A*Star, Singaporeen_US
dc.contributor.organizationSingapore Synchrotron Light Source (SSLS), National University of Singapore, Singaporeen_US
dc.contributor.organizationBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, Chinaen_US
dc.contributor.organizationDepartment of Chemistry, City University of Hong Kong, Hong Kong, Chinaen_US
dc.contributor.organizationHong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Hong Kong, Chinaen_US
dc.contributor.organizationBeijing Key Laboratory for Magnetoelectric Materials and Devices (BKLMMD), Beijing Innovation Center for Engineering Science and Advanced Technology (BIC-ESAT), Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing, China.en_US
dc.contributor.organizationNational Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, USAen_US
dc.contributor.researchEnergy Research Institute @ NTU (ERI@N)en_US
dc.contributor.researchSolar Fuels Laboratoryen_US
dc.description.versionAccepted versionen_US
dc.subject.keywordsWater Oxidationen_US
dc.subject.keywordsSpinel Oxidesen_US
dc.subject.keywordsCovalency Competitionen_US
dc.description.acknowledgementThis work was supported by Singapore Ministry of Education Tier 2 Grant (MOE2018-T2-2-027) and the Singapore National Research Foundation under its Campus for Research Excellence And Technological Enterprise (CREATE) programme. We thank the Facility for Analysis, Characterization, Testing, and Simulation (FACTS) in Nanyang Technological University. This research used resources of the National Synchrotron Light Source II, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704. We also appreciate the XAS measurements from SSLS, soft X-ray and ultraviolet beamline. Y.S. and Z.X. thank A. Lapkin (University of Cambridge) for helpful discussion on machine-learning concepts and thank L. Zeng (Southern University of Science and Technology) for helpful discussion on catalyst performance. H.Z. gives thanks for the support from ITC via the Hong Kong Branch of National Precious Metals Material (NPMM) Engineering Research Center, and the start-up grant (project no. 9380100) and grants (project no. 9610478 and 1886921) in City University of Hong Kongen_US
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