Coordination structure regulation of Pt-N_(x)O_(y)-S_(1)catalytic sites for promoting high-efficiency hydrogen evolution  

作　　者：Minmin Wang Chao Feng Xin Zhang Ping He Houyu Zhu Yunqi Liu Yuan Pan 

机构地区：[1]State Key Laboratory of Heavy Oil Processing,China University of Petroleum(East China),Qingdao 266580,Shandong,China [2]Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Songling Road 189,Laoshan District,Qingdao 266101,Shandong,China [3]School of Chemistry and Materials Science,Anhui Normal University,Wuhu 241002,Anhui,China

出　　处：《Journal of Energy Chemistry》2025年第3期661-669,共9页能源化学(英文版)

基　　金：supported by the National Natural Science Foundation of China(22108306,22478432 and 22406191);Taishan Scholars Program of Shandong Province(tsqn201909065);the Natural Science Foundation of Shandong Province(ZR2024JQ004,ZR2021YQ15)。

摘　　要：The development of atomically dispersed platinum-based catalysts with high performance and welldefined active site structures is crucial for the commercialization of water electrolysis for hydrogen production.Herein,we propose a coordination dual-shell synergistic regulation mechanism of coal pitchderived carbon-supported single atom Pt-N_(x)O_(y)-S_(1)catalytic sites by a self-assembly-pyrolysis strategy for promoting hydrogen evolution reaction(HER).The Pt-N_(3)O1-S_(1)sites exhibited the highest HER performance,with an overpotential of 92 mV at a current density of 400 mA cm^(-2).At 50 mV,the turnover frequency was 34.04 s^(-1)and the mass activity was 22.83 A mg_(Pt)^(-l),which is 63.4 times that of the 20%Pt/C catalyst.Theoretical calculations revealed that the coordination dual-shell impacts the electronic structure of the Pt atoms and the adsorption strength towards reactants synergistically.The S atoms in the second coordination shell weakened the strength of Pt-N first shell,resulting the more surface valence electrons around Pt atoms,exhibiting the most suitable adsorption free energy and enhancing the adsorption of H^(+)on Pt-N_(3)O_(1)-S_(1)sites,thus enhancing the electrocatalytic HER process by promoting Volmer step.This work reveals that coordination dual-shell synergistic regulation is an effective strategy for enhancing the electrocatalytic reaction process.

关 键 词：Single-atom catalysts Hydrogen evolution reaction Self-assembly pyrolysis strategy Coordinationen vironment Electronic structure 

分 类 号：O643.36[理学—物理化学]