Dopants fixation of Ruthenium for boosting acidic oxygen evolution stability and activity

Shaoyun Hao; Min Liu; Junjie Pan; Xiangnan Liu; Xiaoli Tan; Nan Xu; Yi He; Lecheng Lei; Xingwang Zhang

doi:10.1038/s41467-020-19212-y

Dopants fixation of Ruthenium for boosting acidic oxygen evolution stability and activity

Nat Commun. 2020 Oct 23;11(1):5368. doi: 10.1038/s41467-020-19212-y.

Authors

Shaoyun Hao¹, Min Liu², Junjie Pan¹, Xiangnan Liu¹, Xiaoli Tan¹, Nan Xu¹, Yi He¹, Lecheng Lei^{1

3}, Xingwang Zhang^{4

5}

Affiliations

¹ Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, Zhejiang Province, China.
² School of Physics and Electronics, Central South University, 410083, Changsha, Hunan, China.
³ Institute of Zhejiang University-Quzhou, 78 Jiuhua Boulevard North, 324000, Quzhou, China.
⁴ Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 310027, Hangzhou, Zhejiang Province, China. xwzhang@zju.edu.cn.
⁵ Institute of Zhejiang University-Quzhou, 78 Jiuhua Boulevard North, 324000, Quzhou, China. xwzhang@zju.edu.cn.

Abstract

Designing highly durable and active electrocatalysts applied in polymer electrolyte membrane (PEM) electrolyzer for the oxygen evolution reaction remains a grand challenge due to the high dissolution of catalysts in acidic electrolyte. Hindering formation of oxygen vacancies by tuning the electronic structure of catalysts to improve the durability and activity in acidic electrolyte was theoretically effective but rarely reported. Herein we demonstrated rationally tuning electronic structure of RuO₂ with introducing W and Er, which significantly increased oxygen vacancy formation energy. The representative W_0.2Er_0.1Ru_0.7O_2-δ required a super-low overpotential of 168 mV (10 mA cm^-²) accompanied with a record stability of 500 h in acidic electrolyte. More remarkably, it could operate steadily for 120 h (100 mA cm^-²) in PEM device. Density functional theory calculations revealed co-doping of W and Er tuned electronic structure of RuO₂ by charge redistribution, which significantly prohibited formation of soluble Ru^x>4 and lowered adsorption energies for oxygen intermediates.