Interfacial water engineering boosts neutral water reduction

Kaian Sun; Xueyan Wu; Zewen Zhuang; Leyu Liu; Jinjie Fang; Lingyou Zeng; Junguo Ma; Shoujie Liu; Jiazhan Li; Ruoyun Dai; Xin Tan; Ke Yu; Di Liu; Weng-Chon Cheong; Aijian Huang; Yunqi Liu; Yuan Pan; Hai Xiao; Chen Chen

doi:10.1038/s41467-022-33984-5

Interfacial water engineering boosts neutral water reduction

Nat Commun. 2022 Oct 21;13(1):6260. doi: 10.1038/s41467-022-33984-5.

Authors

Kaian Sun¹, Xueyan Wu², Zewen Zhuang^{1

3}, Leyu Liu¹, Jinjie Fang⁴, Lingyou Zeng⁵, Junguo Ma¹, Shoujie Liu¹, Jiazhan Li¹, Ruoyun Dai¹, Xin Tan¹, Ke Yu¹, Di Liu¹, Weng-Chon Cheong¹, Aijian Huang⁶, Yunqi Liu⁵, Yuan Pan⁵, Hai Xiao¹, Chen Chen⁷

Affiliations

¹ Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, 100084, Beijing, China.
² State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, 830017, Urumqi, China. Wuxy90@xju.edu.cn.
³ College of Materials Science and Engineering, Fuzhou University, 350108, Fuzhou, China.
⁴ Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, 100029, Beijing, China.
⁵ State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), 266580, Qingdao, China.
⁶ School of Electronics Science and Engineering, Center for Public Security Technology, University of Electronic Science and Technology of China, 610054, Chengdu, China.
⁷ Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, 100084, Beijing, China. cchen@tsinghua.edu.cn.

Abstract

Hydrogen evolution reaction (HER) in neutral media is of great practical importance for sustainable hydrogen production, but generally suffers from low activities, the cause of which has been a puzzle yet to be solved. Herein, by investigating the synergy between Ru single atoms (RuNC) and RuSe_x cluster compounds (RuSe_x) for HER using ab initio molecular dynamics, operando X-ray absorption spectroscopy, and operando surface-enhanced infrared absorption spectroscopy, we establish that the interfacial water governs neutral HER. The rigid interfacial water layer in neutral media would inhibit the transport of H₂O*/OH* at the electrode/electrolyte interface of RuNC, but the RuSe_x can promote H₂O*/OH* transport to increase the number of available H₂O* on RuNC by disordering the interfacial water network. With the synergy of RuSe_x and RuNC, the resulting neutral HER performance in terms of mass-specific activity is 6.7 times higher than that of 20 wt.% Pt/C at overpotential of 100 mV.

Abstract

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