In situ immobilizing atomically dispersed Ru on oxygen-defective Co3O4 for efficient oxygen evolution

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Yuan, Cheng-Zong, Wang, Shuo, San Hui, Kwan ORCID: https://orcid.org/0000-0001-7089-7587, Wang, Kaixi, Li, Junfeng, Gao, Haixing, Zha, Chenyang, Zhang, Xiaomeng, Dinh, Duc Anh, Wu, Xi-Lin, Tang, Zikang, Wan, Jiawei, Shao, Zongping and Hui, Kwun Nam (2023) In situ immobilizing atomically dispersed Ru on oxygen-defective Co3O4 for efficient oxygen evolution. ACS Catalysis, 13 (4). pp. 2462-2471. ISSN 2155-5435

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Abstract

The synergistic regulation of the electronic structures of transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their oxygen evolution reaction (OER) performance, which remains challenging due to complex synthetic procedures. Herein, a facile defect-induced in situ single-atom deposition strategy is developed to anchor atomically dispersed Ru single-atom onto oxygen vacancy-rich cobalt oxides (Ru/Co3O4–x) based on the spontaneous redox reaction between Ru3+ ions and nonstoichiometric Co3O4–x. Accordingly, the as-prepared Ru/Co3O4–x electrocatalyst with the coexistence of oxygen vacancies and Ru atoms exhibits excellent performances toward OER with a low overpotential of 280 mV at 10 mA cm–2, a small Tafel slope value of 86.9 mV dec–1, and good long-term stability in alkaline media. Furthermore, density functional theory calculations uncover that oxygen vacancy and atomically dispersed Ru could synergistically tailor electron decentralization and d-band center of Co atoms, further optimizing the adsorption of oxygen-based intermediates (*OH, *O, and *OOH) and reducing the reaction barriers of OER. This work proposes an available strategy for constructing electrocatalysts with abundant oxygen vacancies and atomically dispersed noble metal and presents a deep understanding of synergistic electronic engineering of transition-metal-based catalysts to boost oxygen evolution.

Item Type: Article
Additional Information: Funding Information: This work was funded by the Science and Technology Development Fund, Macau SAR (File no. 0191/2017/A3, 0041/2019/A1, 0046/2019/AFJ, 0021/2019/AIR, and 0007/2021/AGJ), University of Macau (File no. MYRG2018-00192-IAPME, MYRG2020-00187-IAPME, and MYRG2022-00223-IAPME), UEA fund, National Key R&D Program (2022YFB3504302, 2021YFB3500801, 2019YFC1908405, and 2019YFC1907304), and Open Funding Project of the Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths (E03MYB0309). C.Z. Yuan acknowledges the UM Macao Postdoctoral Fellowship and Associateship. This work was financially supported by the National Natural Science Foundation of China (grant no. 52022097), Foundation of the Youth Innovation Promotion Association of CAS (2020048). The DFT calculations are performed at High Performance Computing Cluster (HPCC) of Information and Communication Technology Office (ICTO) at the University of Macau.
Uncontrolled Keywords: defect-induced,electron decentralization,in situ deposition strategy,oxygen evolution reaction,oxygen vacancy defects,single-atom doping,catalysis,chemistry(all) ,/dk/atira/pure/subjectarea/asjc/1500/1503
Faculty \ School: Faculty of Science > School of Engineering
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Depositing User: LivePure Connector
Date Deposited: 09 May 2024 11:30
Last Modified: 09 May 2024 11:30
URI: https://ueaeprints.uea.ac.uk/id/eprint/95108
DOI: 10.1021/acscatal.2c04946

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