Quasi-Two-Dimensional Intermetallic Electride CeRuSi for Efficient Alkaline Hydrogen Evolution

Cai, Weizheng1; Zhou, Chuan1; Hu, Xinmeng1; Jiao, Tiwen1; Liu, Yijia1; Li, Lei1; Li, Jiang2; Kitano, Masaaki2; Hosono, Hideo2; Wu, Jiazhen1

2023-03-01

10.1021/acscatal.2c06382

ACS CATALYSIS   影响因子和分区

2155-5435

Electrides are emerging catalyst materials, in which excess electrons serve as periodic anions. Although they have been successfully used for various hydrogenation reactions, due to weak chemical stabilities, their applications in aqueous systems remain challenging. Herein, we develop a quasi-two-dimensional (2D) intermetallic electride CeRuSi as a high-performance alkaline hydrogen evolution electrocatalyst, realizing an ultralow over potential of 28 mV at a current density of 10 mA/cm(2 )and longterm stability in 1.0 M KOH. The rate-determining step is deduced to be the Tafel step with accelerated kinetics. We show that CeRuSi is so far the best electride-based electrocatalyst for hydrogen evolution. We further demonstrate that high activity is mainly ascribed to the unique electride features and the coordinatively unsaturated Ru sites, exposed and activated via selective chemical etching. Finally, we confirm the superior catalytic performance using density functional theory calculations and find an optimized H adsorption energy over the Ru active centers. This work will stimulate more electrocatalytic studies on electrides and provide guidance for the design of electrocatalysts.

electride intermetallic catalysts RTX compounds electrocatalysis hydrogen evolution

SCI ; EI

英语

第一 ; 通讯

Guangdong Basic and Applied Basic Research Foundation[2022A1515011295] ; National Natural Science Foundation of China[52173284] ; Shenzhen fundamental research funding[JCYJ20210324115809026] ; Shenzhen Key Laboratory Program[ZDSYS20210709112802010] ; China Postdoctoral Science Foundation[2022 M721455] ; JSPS Kakenhi[17H06153] ; JST-Mirai Program[JPMJMI21E9]

Chemistry

Chemistry, Physical

WOS:000960442400001

AMER CHEMICAL SOC

20231413840423

Alkalinity ; Catalyst activity ; Density functional theory ; Electrocatalysts ; Electrolysis ; Etching ; Hydrogenation ; Intermetallics ; Potassium hydroxide ; Ruthenium ; Ruthenium compounds ; Silicon compounds

Metallurgy:531.1 ; Precious Metals:547.1 ; Chemistry, General:801.1 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

Web of Science

1.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen Key Lab Micro Nanoporous Funct Mat, Shenzhen 518055, Peoples R China
2.Tokyo Inst Technol, MDX Res Ctr Element Strategy, Int Res Frontiers Initiat, Yokohama, Kanagawa 2268503, Japan

Cai, Weizheng,Zhou, Chuan,Hu, Xinmeng,et al. Quasi-Two-Dimensional Intermetallic Electride CeRuSi for Efficient Alkaline Hydrogen Evolution[J]. ACS CATALYSIS,2023,13(7):4752-4759.

Cai, Weizheng.,Zhou, Chuan.,Hu, Xinmeng.,Jiao, Tiwen.,Liu, Yijia.,...&Wu, Jiazhen.(2023).Quasi-Two-Dimensional Intermetallic Electride CeRuSi for Efficient Alkaline Hydrogen Evolution.ACS CATALYSIS,13(7),4752-4759.

Cai, Weizheng,et al."Quasi-Two-Dimensional Intermetallic Electride CeRuSi for Efficient Alkaline Hydrogen Evolution".ACS CATALYSIS 13.7(2023):4752-4759.