文献类型：期刊文献

英文题名：Carburization induced phase transition of Ni3In to Ni3InC0.5 intermetallic carbide for acetylene semihydrogenation

作者：Ge, Xiaohu[1];Fei, Nina[1];Cao, Yueqiang[1];Jiang, Hao[2];Zhang, Jing[1];Qian, Gang[1];Zhou, Xinggui[1];Duan, Xuezhi[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Ultrafine Mat, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn,Minist Educ, Shanghai, Peoples R China

年份：2025

卷号：71

期号：7

外文期刊名：AICHE JOURNAL

收录：;EI(收录号：20251518204666);WOS:【SCI-EXPANDED(收录号:WOS:001458133000001)】；

基金：This work was financially supported by the National Key R&D Program of China (2022YFA1503804), the Natural Science Foundation of China (22332003, 22478106, and 22408097), 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, the China Postdoctoral Science Foundation (2024 M760912), and the Postdoctoral Fellowship Program of CPSF under Grant Number GZB20240222. This work was also supported by BL16U1, BL13SSW, and User Experiment Assist System of SSRF.

语种：英文

外文关键词：acetylene semihydrogenation; adsorption behavior; ethylene selectivity; interstitial carbon; Ni-In intermetallic

摘要：In this work, we develop a carburization strategy to transform hexagonal Ni3In into face-centered cubic Ni3InC0.5 intermetallic carbide, leveraging partially isolated Ni sites for improved acetylene semihydrogenation. The catalyst synthesized via carburization of Ni3In intermetallic compound derived from Ni/In/Mg/Al layered double hydroxides in a C2H2/H-2 atmosphere is evidenced to show Ni3InC0.5 intermetallic carbide phase through detailed characterizations, including high-resolution transmission electron microscopy and X-ray absorption spectroscopy. Catalytic tests reveal that the Ni3InC0.5 catalyst achieves 92.0% ethylene selectivity at full acetylene conversion, outperforming the Ni and Ni3In catalysts. Both experimental and theoretical evidence demonstrate that interstitial carbon atoms in Ni3InC0.5 synergize with neighboring In atoms to modify the electronic structure of surface Ni sites via significant hybridization between Ni 3d, In 5p, and C 2p orbitals. These unique features enable higher kinetic favorability of ethylene desorption over its further hydrogenation on the Ni3InC0.5 catalyst and thus contribute to the enhanced semihydrogenation.