文献类型：期刊文献

英文题名：Embedding Single Pd Atoms on NiGa Intermetallic Surfaces for Efficient and Selective Alkyne Hydrogenation

作者：Ge, Xiaohu[1];Jing, Yundao[1];Fei, Nina[1];Yan, Kelin[1];Liang, Yijing[1];Cao, Yueqiang[1];Zhang, Jing[1];Qian, Gang[1];Li, Lina[2];Jiang, Hao[3];Zhou, Xinggui[1];Yuan, Weikang[1];Duan, Xuezhi[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[3]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China

年份：2024

卷号：63

期号：43

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20243416917215);WOS:【SCI-EXPANDED(收录号:WOS:001295259000001)】；

基金：This work was financially supported by the National Key R&D Program of China (2022YFA1503804), the Natural Science Foundation of China (22332003, 22008067 and 22178100), Shanghai Rising-star Program (23QA1401900), the Shanghai Science and Technology Innovation Action Plan (22JC1403800), the Program of Shanghai Academic/Technology Research Leader (21XD1421000), Young Elite Scientists Sponsorship Program by CAST (2023QNRC001), the Fundamental Research Funds for the Central Universities, and the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20240222. This work was also supported by BL14W1, 13SSW and User Experiment Assist System of SSRF. This study is dedicated to Prof. Weikang Yuan (ECUST) on the occasion of his 90th birthday.

语种：英文

外文关键词：Alkyne semi-hydrogenation; Selectivity; Ni-based catalyst; Ensemble site; Hydrogen dissociation

摘要：Catalytic removal of alkynes is essential in industry for producing polymer-grade alkenes from steam cracking processes. Non-noble Ni-based catalysts hold promise as effective alternatives to industrial Pd-based catalysts but suffer from low activity. Here we report embedding of single-atom Pd onto the NiGa intermetallic surface with replacing Ga atoms via a well-defined synthesis strategy to design Pd-1-NiGa catalyst for alkyne semi-hydrogenation. The fabricated Pd1Ni2Ga1 ensemble sites deliver remarkably higher specific mass activity under superb alkene selectivity of >96 % than the state-of-the-art catalysts under industry-relevant conditions. Integrated experimental and computational studies reveal that the single-atom Pd synergizes with the neighbouring Ni sites to facilitate the sigma-adsorption of alkyne and dissociation of hydrogen while suppress the alkene adsorption. Such synergistic effects confer the single-atom Pd on the NiGa intermetallic with a Midas touch for alkyne semi-hydrogenation, providing an effective strategy for stimulating low active Ni-based catalysts for other selective hydrogenations in industry.