Amorphous Ruthenium-Sulfide with Isolated Catalytic Sites for Pt-Like Electrocatalytic Hydrogen Production Over Whole pH Range

Pengsong Li; Xinxuan Duan; Shiyuan Wang; Lirong Zheng; Yaping Li; Haohong Duan; Yun Kuang; Xiaoming Sun

doi:10.1002/smll.201904043

Amorphous Ruthenium-Sulfide with Isolated Catalytic Sites for Pt-Like Electrocatalytic Hydrogen Production Over Whole pH Range

Small. 2019 Nov;15(46):e1904043. doi: 10.1002/smll.201904043. Epub 2019 Sep 17.

Authors

Pengsong Li^{1

2}, Xinxuan Duan¹, Shiyuan Wang¹, Lirong Zheng³, Yaping Li¹, Haohong Duan⁴, Yun Kuang¹, Xiaoming Sun¹

Affiliations

¹ State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
² Department of Chemistry and Energy Sciences Institute, Yale University, West Haven, CT, 06516, USA.
³ Institute of High Energy Physics (IHEP) of the Chinese Academy of Sciences (CAS) Beijing, Beijing, 100049, China.
⁴ Department of Chemistry, Tsinghua University, 30 Shuangqing Rd, Haidian Qu, Beijing Shi, 100084, China.

PMID: 31529772
DOI: 10.1002/smll.201904043

Abstract

Electrocatalytic hydrogen evolution reaction (HER) is an efficient way to generate hydrogen fuel for the storage of renewable energy. Currently, the widely used Pt-based catalysts suffer from high costs and limited electrochemical stability; therefore, developing an efficient alternative catalyst is very urgent. Herein, one pot hydrothermal synthesis is reported of amorphous ruthenium-sulfide (RuS_x ) nanoparticles (NPs) supported on sulfur-doped graphene oxide (GO). The as-obtained composite serves as a Pt-like HER electrocatalyst. Achieving a current density of -10 mA cm^-2 only requires a small overpotential (-31, -46, and -58 mV in acidic, neutral, and alkaline electrolyte, respectively) with high durability. The isolated Ru active site inducing Volmer-Heyrovsky mechanism in the RuS_x NPs is demonstrated by the Tafel analysis and X-ray absorption spectroscopy characterization. Theoretical simulation indicates the isolated Ru site exhibits Pt-like Gibbs free energy of hydrogen adsorption (-0.21 eV) therefore generating high intrinsic HER activity. Moreover, the strong bonding between the RuS_x and S-GO, as well as pH tolerance of RuS_x are believed to contribute to the high stability. This work shows a new insight for amorphous materials and provides alternative opportunities in designing advanced electrocatalysts with low-cost for HER in the hydrogen economy.

Keywords: amorphous; electrocatalysts; hydrogen evolution reaction; ruthenium sulfide; whole pH range.

Abstract

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