文献类型：期刊文献

英文题名：Hydrogen Spillover-Bridged Volmer/Tafel Processes EnablingAmpere-Level Current Density Alkaline Hydrogen EvolutionReaction under Low Overpotential

作者：Fu, Huai Qin[1];Zhou, Min[2,3];Liu, Peng Fei[4];Liu, Porun[1];Yin, Huajie[1];Sun, Kai Zhi[4];Yang, Hua Gui[4];Al-Mamun, Mohammad[1];Hu, Peijun[2,3,5];Wang, Hai-Feng[2,3];Zhao, Huijun[1]

机构：[1]Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Gold Coast, Qld 4222, Australia;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Sch Mat Sci & Engn, Shanghai Engn Res Ctr Hierarch Nanomat, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China;[5]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland

年份：2022

卷号：144

期号：13

起止页码：6028

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20221411881519);WOS:【SCI-EXPANDED(收录号:WOS:000789021900043)】；

基金：This work was financially supported by the Australian Research Council Discovery Project (DP200100965), National Natural Science Funds for Distinguished Young Scholars (51725201), International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), NSFC (21873028, 91945302, 92045303), and Shanghai Shu Guang project (17SG30). The authors thank the 1W1B station for XAFS measurements in the Beijing Synchrotron Radiation Facility (BSRF).

语种：英文

外文关键词：Electrolysis - Dissociation - Nickel compounds - Desorption - Hydrogen production - Chromium compounds - Electrolytes - Electrocatalysts - Potassium hydroxide

摘要：Water-alkaline electrolysis holds a great promise forindustry-scale hydrogen production but is hindered by the lack ofenabling hydrogen evolution reaction electrocatalysts to operate atampere-level current densities under low overpotentials. Here, wereport the use of hydrogen spillover-bridged water dissociation/hydrogen formation processes occurring at the synergisticallyhybridized Ni3S2/Cr2S3sites to incapacitate the inhibition effect ofhigh-current-density-induced high hydrogen coverage at the waterdissociation site and concurrently promote Volmer/Tafel pro-cesses. The mechanistic insights critically important to enableampere-level current density operation are depicted from theexperimental and theoretical studies. The Volmer process isdrastically boosted by the strong H2O adsorption at Cr5csites ofCr2S3, the efficient H2O*dissociationviaa heterolytic cleavage process (Cr5c-H2O*+S3c(#)-> Cr5c-OH*+S3c-H#) on the Cr5c/S3csites in Cr2S3, and the rapid desorption of OH*from Cr5csites of Cr2S3viaa new water-assisted desorption mechanism (Cr5c-OH*+H2O(aq)-> Cr5c-H2O*+OH-(aq)), while the efficient Tafel process is achieved through hydrogen spillover to rapidly transferH#from the synergistically located H-rich site (Cr2S3) to the H-deficient site (Ni3S2) with excellent hydrogen formation activity. Asa result, the hybridized Ni3S2/Cr2S3electrocatalyst can readily achieve a current density of 3.5 A cm-2under an overpotential of 251 +/- 3 mV in 1.0 M KOH electrolyte. The concept exemplified in this work provides a useful means to address the shortfalls of ampere-level current-density-tolerant Hydrogen evolution reaction (HER) electrocatalysts.