文献类型：期刊文献

英文题名：Operando Stable Palladium Hydride Nanoclusters Anchored on Tungsten Carbides Mediate Reverse Hydrogen Spillover for Hydrogen Evolution

作者：Fan, Hao[1];Yang, Qian Qian[1];Fang, Song Ru[1];Xu, Yi Ning[1];Lv, Yao[2,3];Lin, Hao Yang[1];Lin, Miao Yu[1];Liu, Ji Kai[1];Wu, Yi Xiao[1];Yuan, Hai Yang[1];Dai, Sheng[2,3];Liu, Peng Fei[1];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Inst Fine Chem, Key Lab Adv Mat, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2024

卷号：63

期号：51

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20244417276648);WOS:【SCI-EXPANDED(收录号:WOS:001342189800001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (22239001, 51920105003, 22376062 and 22379043), the Shanghai Pilot Program for Basic Research (22TQ1400100-12), and the Science and Technology Commission of Shanghai Municipality (23520710700, 21DZ1207101 and 22ZR1415700), and the Fundamental Research Funds for the Central Universities. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF), and the 1W1B beamline of Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses.

语种：英文

外文关键词：Operando Hydrogen Intercalation; Pd Hydrides; PEM Electrolysis; Reverse Hydrogen Spillover; Tungsten Carbides

摘要：Proton exchange membrane (PEM) electrolysis holds great promise for green hydrogen production, but suffering from high loading of platinum-group metals (PGM) for large-scale deployment. Anchoring PGM-based materials on supports can not only improve the atomic utilization of active sites but also enhance the intrinsic activity. However, in practical PEM electrolysis, it is still challenging to mediate hydrogen adsorption/desorption pathways with high coverage of hydrogen intermediates over catalyst surface. Here, operando generated stable palladium (Pd) hydride nanoclusters anchored on tungsten carbide (WCx) supports were constructed for hydrogen evolution in PEM electrolysis. Under PEM operando conditions, hydrogen intercalation induces formation of Pd hydrides (PdHx) featuring weakened hydrogen binding energy (HBE), thus triggering reverse hydrogen spillover from WCx (strong HBE) supports to PdHx sites, which have been evidenced by operando characterizations, electrochemical results and theoretical studies. This PdHx-WCx material can be directly utilized as cathode electrocatalysts in PEM electrolysis with ultralow Pd loading of 0.022 mg cm(-2), delivering the current density of 1 A cm(-2) at the cell voltage of similar to 1.66 V and continuously running for 200 hours without obvious degradation. This innovative strategy via tuning the operando characteristics to mediate reverse hydrogen spillover provide new insights for designing high-performance supported PGM-based electrocatalysts.