Accelerated kinetics of alkaline hydrogen evolution/oxidation reactions on dispersed ruthenium sites through N and S dual coordination

Zhang, Zhen1,2; Ni, Liwen2; Liu, Haijun3; Zhao, Zhi-Liang2; Yuan, Xiao-Zi4; Li, Hui2

2022

10.1007/s11426-021-1190-7

Science China-Chemistry   影响因子和分区

1674-7291

1869-1870

Efficient, robust and cost-effective electrocatalysts that catalyze hydrogen evolution/oxidation reaction (HER/HOR) in alkaline media are highly demanded. Recently, single-atom catalysts (SACs) have emerged as new promising candidates; however, the rational design of supports and the optimization of coordination environment between supports and metal atoms are challenging. In this work, we successfully fabricate atomically dispersed ruthenium (Ru) species, which are strongly coordinated by N and S dual heteroatoms on holey graphene (RuSA/NSG), as an excellent bifunctional catalyst for HER/HOR. In alkaline media, the developed catalyst exhibits high catalytic performance with a low overpotential of 57.3 mV to drive a current density of 10 mA cm(-1) for HER, and its mass activity is about 5.8 times higher than that of commercial Pt/C and Ru/C catalysts at an overpotential of 100 mV. Similarly, considerable HOR performance of RuSA/NSG is verified to be superior to Pt/C and Ru/C. Furthermore, X-ray-based spectroscopy measurements and density-functional theory calculations have confirmed that, compared with Ru-N-4, the tailored Ru-N-4-S-2 with nearby S dopants can act as more active centers to greatly accelerate the sluggish HER/HOR kinetics in alkaline media. The present work provides a new atomic-level engineering strategy to modulate catalytic activities of SACs via the coordination design using dual heteroatoms on the carbon support.

single-atom catalyst ruthenium hydrogen evolution reaction hydrogen oxidation reaction density-functional theory

SCI ; EI

英语

通讯

National Key Research and Development Program of China[2018YFB1502503] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001] ; Shenzhen Key Laboratory Project[ZDSYS201603311013489] ; Shenzhen Science and Technology Projects for Sustainable Development[KCXFZ202002011010317] ; Foundation Research Project of Shenzhen[JCYJ20200109141216566]

Chemistry

Chemistry, Multidisciplinary

WOS:000742611000001

SCIENCE PRESS

20220411499440

Atoms ; Catalyst activity ; Coordination reactions ; Cost effectiveness ; Electrocatalysts ; Hydrogen ; Reaction kinetics ; Ruthenium ; Ruthenium compounds

Precious Metals:547.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Industrial Economics:911.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

Web of Science

1.Harbin Inst Technol, Sch Mat Sci & Engn, Harbin 150001, Peoples R China
2.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen Key Lab Hydrogen Energy, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen 518055, Peoples R China
4.Natl Res Council Canada, Res Ctr Energy Min & Environm, 4250 Wesbrook Mall, Vancouver, BC V6T 1W5, Canada

Zhang, Zhen,Ni, Liwen,Liu, Haijun,et al. Accelerated kinetics of alkaline hydrogen evolution/oxidation reactions on dispersed ruthenium sites through N and S dual coordination[J]. Science China-Chemistry,2022,65:611-618.

Zhang, Zhen,Ni, Liwen,Liu, Haijun,Zhao, Zhi-Liang,Yuan, Xiao-Zi,&Li, Hui.(2022).Accelerated kinetics of alkaline hydrogen evolution/oxidation reactions on dispersed ruthenium sites through N and S dual coordination.Science China-Chemistry,65,611-618.

Zhang, Zhen,et al."Accelerated kinetics of alkaline hydrogen evolution/oxidation reactions on dispersed ruthenium sites through N and S dual coordination".Science China-Chemistry 65(2022):611-618.