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

被引:101
作者
Yuan, Cheng-Zong [1 ,2 ]
Wang, Shuo [1 ]
San Hui, Kwan [5 ]
Wang, Kaixi [1 ]
Li, Junfeng [1 ]
Gao, Haixing [1 ]
Zha, Chenyang [1 ]
Zhang, Xiaomeng [2 ]
Dinh, Duc Anh [3 ]
Wu, Xi-Lin [4 ]
Tang, Zikang [1 ]
Wan, Jiawei [6 ]
Shao, Zongping [7 ]
Hui, Kwun Nam [1 ]
机构
[1] Univ Macau, Inst Appl Phys & Mat Engn, Minist Educ, Joint Key Lab, Taipa 999078, Macau, Peoples R China
[2] Chinese Acad Sci, Ganjiang Innovat Acad, Jiangxi Prov Key Lab Cleaner Prod Rare Earths, Ganzhou 341119, Peoples R China
[3] Nguyen Tat Thanh Univ, NTT Hitech Inst, VKTech Res Ctr, Ho Chi Minh City 700000, Vietnam
[4] Zhejiang Normal Univ, Coll Geog & Environm Sci, Jinhua 321004, Peoples R China
[5] Univ East Anglia, Fac Sci, Sch Engn, Norwich NR4 7TJ, Norfolk, England
[6] Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China
[7] Curtin Univ, WA Sch Mines Minerals Energy & Chem Engn WASM MECE, Perth, WA 6845, Australia
基金
中国国家自然科学基金;
关键词
defect-induced; in situ deposition strategy; oxygen vacancy defects; single-atom doping; electron decentralization; oxygen evolution reaction; ELECTROCATALYTIC ACTIVITY; NANOSHEETS; GROWTH; NANOPARTICLES; OPTIMIZATION; CATALYSTS; VACANCIES;
D O I
10.1021/acscatal.2c04946
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 coex-istence 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.
引用
收藏
页码:2462 / 2471
页数:10
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