In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co3O4 for Efficient Oxygen Evolution

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...

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Veröffentlicht in:ACS catalysis 2023-02, Vol.13 (4), p.2462-2471
Hauptverfasser: Yuan, Cheng-Zong, Wang, Shuo, San Hui, Kwan, Wang, Kaixi, Li, Junfeng, Gao, Haixing, Zha, Chenyang, Zhang, Xiaomeng, Dinh, Duc Anh, Wu, Xi-Lin, Tang, Zikang, Wan, Jiawei, Shao, Zongping, Hui, Kwun Nam
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container_issue 4
container_start_page 2462
container_title ACS catalysis
container_volume 13
creator Yuan, Cheng-Zong
Wang, Shuo
San Hui, Kwan
Wang, Kaixi
Li, Junfeng
Gao, Haixing
Zha, Chenyang
Zhang, Xiaomeng
Dinh, Duc Anh
Wu, Xi-Lin
Tang, Zikang
Wan, Jiawei
Shao, Zongping
Hui, Kwun Nam
description 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.
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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. 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