文献类型：期刊文献

英文题名：Enhanced acetylene semi-hydrogenation on a subsurface carbon tailored Ni-Ga intermetallic catalyst

作者：Ge, Xiaohu[1];Ren, Zhouhong[2];Cao, Yueqiang[1];Liu, Xi[2];Zhang, Jing[1];Qian, Gang[1];Gong, Xueqing[3,4];Chen, Liwei[2];Zhou, Xinggui[1];Yuan, Weikang[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]Shanghai Jiao Tong Univ, Insitu Ctr Phys Sci, Frontiers Sci Ctr Transformat Mol, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2022

卷号：10

期号：37

起止页码：19722

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20222412230598);WOS:【SCI-EXPANDED(收录号:WOS:000808109500001)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803, 22008067, 22072090 and 22178100), the Innovation Program of Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (21XD1421000), the China Postdoctoral Science Foundation (2020M681202 and 2021T140204), and National Key R&D Plan (2021YFA1500300 and 2021YFA1500303). We thank the BL11B XAFS beamline of Shanghai Synchrotron Radiation Facility (SSRF) for providing the beam time.

语种：英文

外文关键词：Acetylene - Atoms - Binary alloys - Carbon - Catalyst selectivity - Electronic structure - Ethylene - Intermetallics - Lighting - Nickel - X ray absorption spectroscopy

摘要：Tailoring the active sites to promote the formation of the target product is of great importance for selective hydrogenations catalyzed by non-noble metals but remains challenging. Herein, we propose to employ carbon atoms to be incorporated into the Ni3Ga intermetallic with partially isolated Ni sites aiming to enhance the catalytic performances for acetylene semi-hydrogenation. The incorporation of carbon atoms into the lattice of the Ni3Ga intermetallic is achieved by thermal processing of the Ni3Ga intermetallic catalyst in an acetylene atmosphere. The processed catalyst is proven to show the typical Ni3GaC0.5 phase by multiple characterization techniques including atomic-resolution electron microscopy and X-ray absorption spectroscopy. The presence of subsurface carbon in the Ni3GaC0.5 catalyst is experimentally and theoretically demonstrated to synergize with Ga sites for modifying the electronic structures of Ni via obvious hybridization of Ni 3d with Ga 2p and C 2p orbitals. The performance tests show that the Ni3GaC0.5 catalyst delivers high ethylene selectivity, up to ca. 90% at full conversion of acetylene, which outperforms the referred Ni and Ni3Ga catalysts. The excellent selectivity to ethylene is rationalized by theoretical calculations, which point out that the desorption of ethylene from the Ni3GaC0.5 catalyst is kinetically more favourable than its hydrogenation to ethane. In addition, the stability of the Ni3GaC0.5 catalyst is also enhanced against the Ni and Ni3Ga catalysts due to the suppressed formation of C-4 products.