文献类型：期刊文献

英文题名：Histidine-Based "Transfer Stations" at Carbon-Immobilized Metal Particles Enable Rapid Hydrogen Transfer for Efficient Formic Acid Dehydrogenation

作者：Yang, Zhenyi[1];Hou, Guoyu[1];Gao, Nana[2];Li, Yicheng[1];Li, Xingqiu[1];Chen, Zitao[3];Jin, Haibao[4];Zhao, Ming[5];Wang, Dongyang[6];Chen, Ke[6];Antonietti, Markus[7];Liu, Tianxi[8];Tian, Zhihong[2];Zhang, Yu[1]

机构：[1]East China Univ Sci & Technol, Sch Mech & Power Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Henan Univ, Engn Res Ctr Nanomat, Kaifeng 475004, Peoples R China;[3]South China Normal Univ, South China Acad Adv Optoelect, Guangzhou 510006, Peoples R China;[4]East China Univ Sci & Technol, Sch Mat & Sci Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117575, Singapore;[6]Henan Univ, Ctr Phys Low Dimens Mat, Sch Phys & Elect, Sch Future Technol, Kaifeng 475004, Peoples R China;[7]Max Planck Inst Colloids & Interfaces, Dept Colloid Chem, Muhlenberg 1, D-14476 Potsdam, Germany;[8]Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi 214122, Peoples R China

年份：2025

卷号：64

期号：26

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20251918361453);WOS:【SCI-EXPANDED(收录号:WOS:001478776800001)】；

基金：This work was supported by the National Natural Science Foundation of China (Nos. 22479048, 52373205, 22109044, and 52373114), Natural Science Foundation of Shanghai, China (No. 22ZR1418500), start-up funds from the East China University of Science and Technology, Henan Center for Outstanding Overseas Scientists (No. GZS2022014), Natural Science Foundation of Henan Province (No. 252300421103) and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：Formic acid dehydrogenation; Heterogeneous catalysis; L-histidine modified; Local enrichment

摘要：The interaction of surface metal species with the solution plays a key role in engineering heterogeneous catalytic processes. Herein, we present the facile synthesis of L-histidine-coordinated PdAg nanoparticles (4.03 +/- 0.08 nm) anchored on pristine carbon supports (denoted as PdAg-NH2/C) and their use for formic acid dehydrogenation (FAD). Significant acceleration of FAD related to the histidine is observed, and the enhancement mechanism is experimentally and theoretically investigated. The presence of L-histidine at metal sites promotes rapid binding of formic acid molecules due to acid-base interactions. The local enrichment of both protons and formate at the metal-solution interfaces promotes the subsequent formate decomposition and hydride transfer to the metal surface. The as-generated surface H species are more concentrated compared to the previously reported catalyst where the metal is loaded on an amino modified support, this enabling a significantly enhanced H2 production. The optimal Pd1Ag1-NH2/C catalyst exhibits a high turnover frequency (TOF) of 6493.5 h-1 at 333 K based on the total amount of Pd, together with an H2 selectivity of 100%. This study emphasizes the critical role of optimizing local transport pathways near catalytic centers chemically and further provides insights into the rational development of heterogeneous catalysts for FAD technologies.