Shifting Oxygen Charge Towards Octahedral Metal: A Way to Promote Water Oxidation on Cobalt Spinel Oxides
| Autor: | Bicheng Huang, Yuanmiao Sun, Zhichuan J. Xu, Shibo Xi, Yonghua Du, Xiao Ren, Ye Zhou, Hanbin Liao, Luyuan Paul Wang, Shengnan Sun |
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| Přispěvatelé: | School of Materials Science and Engineering, Interdisciplinary Graduate School (IGS), Campus for Research Excellence and TechnologicalEnterprise (CREATE), Energy Research Institute @ NTU (ERI@N) |
| Rok vydání: | 2019 |
| Předmět: |
Materials science
Materials [Engineering] Spinel Oxide Oxygen evolution chemistry.chemical_element General Medicine General Chemistry engineering.material Oxygen Catalysis Metal-oxygen Covalency Metal chemistry.chemical_compound Crystallography Transition metal chemistry visual_art visual_art.visual_art_medium engineering Cobalt Geometry Effects |
| Zdroj: | Angewandte Chemie International Edition. 58:6042-6047 |
| ISSN: | 1521-3773 1433-7851 |
| DOI: | 10.1002/anie.201902114 |
| Popis: | Cobalt spinel oxides are a class of promising transition metal (TM) oxides for catalyzing oxygen evolution reaction (OER). Their catalytic activity depends on the electronic structure. In a spinel oxide lattice, each oxygen anion is shared amongst its four nearest transition metal cations, of which one is located within the tetrahedral interstices and the remaining three cations are in the octahedral interstices. This work uncovered the influence of oxygen anion charge distribution on the electronic structure of the redox-active building block Co-O. The charge of oxygen anion tends to shift toward the octahedral-occupied Co instead of tetrahedral-occupied Co, which hence produces strong orbital interaction between octahedral Co and O. Thus, the OER activity can be promoted by pushing more Co into the octahedral site or shifting the oxygen charge towards the redox-active metal center in CoOmetal-oxygen covalency octahedra. Ministry of Education (MOE) National Research Foundation (NRF) This work was supported by the Singapore Ministry of Education Tier 1 Grant (RG3/18 (S)), Tier 2 Grant (MOE2018-T2-2–027) and the Singapore National Research Foundation under its Campus for Research Excellence And Technological Enterprise (CREATE) programme. Authors thank the Facility for Analysis, Characterization, Testing, and Simulation (FACTS) in Nanyang Technological University and appreciate the XAFCA beamline of the Singapore Synchrotron Light Source for XAFS characterization. The authors would like to acknowledge the SUV beamline of Singapore Synchrotron Light Source (SSLS) for providing the facility necessary for conducting the research. The Laboratory is a National Research Infrastructure under the National Research Foundation Singapore. |
| Databáze: | OpenAIRE |
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