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Balancing Activity and Stability in Spinel Cobalt Oxides through Geometrical Sites Occupation towards Efficient Electrocatalytic Oxygen Evolution |
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| Authors: | Prof. Li An Dr. Hong Zhang Jiamin Zhu Prof. Shibo Xi Prof. Bolong Huang Mingzi Sun Prof. Yong Peng Prof. Pinxian Xi Prof. Chun-Hua Yan |
| Affiliation: | 1. State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China;2. Electron Microscopy Centre of Lanzhou University, School of Materials and Energy, Key Laboratory of Magnetism and Magnetic Materials of Ministry of Education, School of Physical Science and Technology, Lanzhou University, Lanzhou, 730000 China These authors contributed equally to this work.;3. Institute of Chemical and Engineering Sciences, Agency for Science, Technology and Research (A*STAR), 1 Pesek Road, Singapore, 627833 Singapore;4. Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kow-loon, Hong Kong SAR, China;5. Electron Microscopy Centre of Lanzhou University, School of Materials and Energy, Key Laboratory of Magnetism and Magnetic Materials of Ministry of Education, School of Physical Science and Technology, Lanzhou University, Lanzhou, 730000 China;6. State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Frontiers Science Center for Rare Isotopes, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, 730000 P. R. China Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Rare Earth Materials Chemistry and Applications, PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871 China |
| Abstract: | Designing active and stable oxygen evolution reaction (OER) catalysts are vitally important to various energy conversion devices. Herein, we introduce elements Ni and Mn into (Co)tet(Co2)octO4 nanosheets (NSs) at fixed geometrical sites, including Mnoct, Nioct, and Nitet, to optimize the initial geometrical structure and modulate the CoCo2O4 surface from oxygen-excess to oxygen-deficiency. The pristine (Ni,Mn)-(Co)tet(Co2)octO4 NSs shows excellent OER activity with an overpotential of 281.6 mV at a current density of 10 mA cm−2. Moreover, without damaging their initial activity, the activated (Act)-(Ni,Mn)-(Co)tet(Co2)octO4 NSs after surface reconstruction exhibit long-term stability of 100 h under 10 mA cm−2, 50 mA cm−2, or even 100 mA cm−2. The optimal balance between electroactivity and stability leads to remarkable OER performances, providing a pivotal guideline for designing ideal electrocatalysts and inspiring more works to focus on the dynamic change of each occupation site component. |
| Keywords: | geometrical site occupation surface reconstruction decoupled proton-electron transfer OER well-balanced performance |