文献类型：期刊文献

英文题名：Local Structure Insight into Hydrogen Evolution Reaction with Bimetal Nanocatalysts

作者：Li, Qiang[1];Zhu, He[1];Chen, Xiaoyu[2];Liu, Hui[1];Ren, Yang[3];Chen, Yanan[4];Ohara, Koji[5];Zhou, Lihui[6];Chen, Jun[1];Deng, Jinxia[1];Miao, Jun[1];Lin, Kun[1];Kuang, Xiaojun[7];Xing, Xianran[1]

机构：[1]Univ Sci & Technol Beijing, Beijing Adv Innovat Ctr Mat Genome Engn, Inst Solid State Chem, Beijing 100083, Peoples R China;[2]Shenzhen Univ, Coll Mat Sci & Engn, Shenzhen 518071, Peoples R China;[3]City Univ Hong Kong, Dept Phys, Kowloon, Hong Kong 999077, Peoples R China;[4]Tianjin Univ, Sch Mat Sci & Engn, Key Lab Adv Ceram & Machining Technol, Minist Educ,Tianjin Key Lab Composite & Funct Mat, Tianjin 300072, Peoples R China;[5]SPring 8, Japan Synchrotron Radiat Res Inst, Sayo, Hyogo 6795148, Japan;[6]East China Univ Sci & Technol, Key Lab Adv Mat & Joint Int Res Lab Precis Chem &, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[7]Guilin Univ Technol, Coll Chem & Bioengn, Guilin 541006, Peoples R China

年份：2022

卷号：144

期号：44

起止页码：20298

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20224613095308);WOS:【SCI-EXPANDED(收录号:WOS:000879071000001)】；

基金：y This research was supported by the National Key R&D Program of China (2020YFA0406202), the National Natural Science Foundation of China (22090042, 21731001 and 22175018), Guangxi BaGui Scholars Special Funding, the China Postdoctoral Science Foundation (2019 M660446) and the Program for Postdoctoral Innovative Talents (BX20190031). We are grateful for using the Beijing Synchrotron Radiation Facility (1W1B beamline) and thank Yuanpeng Zhang for their help in RMCprofile. The total scattering experiments were performed at the beamline BL08W of SPring-8 (Proposal No. 2018B1045, 2019B1311 and 2021A1060). Additional HAADF-STEM support was provided by the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology.

语种：英文

外文关键词：Atoms - Binary alloys - Chemical bonds - Coordination reactions - Distribution functions - Hydrogen - Iron alloys - Nanocatalysts - Platinum - Platinum alloys - Surface segregation

摘要：The revelation of the atomic 3D structure of sub-5 nm bimetal nanocatalysts challenges the limitations of conventional methods. Notably, the identification of the cooperative relationship between the active sites and nearby coordination environment during catalytic reactions depends on the stereo distribution of local phases and chemical composition within a short range. As a model nanocatalyst in our investigation, we studied the ordered PtFe bimetals in hydrogen evolution reactions (HER). By combining pair distribution functions with reverse Monte Carlo, local-range phase symmetry, chemical composition, and atom distribution were determined. The segregation of local phase segments as disordered Pt-rich A1 and Pt3Fe L1(2) phases can be attributed to the marked improvement of HER activity and stability in Pt56Fe44. Following the etching of the outermost-surface Fe, the remaining disordered segregation offered a large number of active Pt sites for discharge and electrochemical desorption reactions. It resulted in local-bonding Pt pairs that made it easier for adsorbed hydrogen atoms to recombine. The current research will provide structural insight into the local range for bimetal nanocatalysts and be valuable for the creation of new, low-cost nano catalysts.