文献类型：期刊文献

英文题名：Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

作者：Ge, Xiaohu[1];Dou, Mingying[1];Cao, Yueqiang[1];Xi Liu[2];Qiang Yuwen[1];Jing Zhang[1];Gang Qian[1];Gong, Xueqing[3,4];Zhou, Xinggui[1];Chen, Liwei[2];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, In Situ 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：13

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000857058900006)】；

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 Shanghai Science and Technology Innovation Action Plan (22JC1403800), 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 and BL14W1 XAFS beamline of Shanghai Synchrotron Radiation Facility (SSRF) for providing the beamtime.

语种：英文

摘要：Mechanism driven catalyst design with atomically uniform ensemble sites is an important yet challenging issue in heterogeneous catalysis associated with breaking the activity-selectivity trade-off. Herein, a trimer Ni1Sb2 site in NiSb intermetallic featuring superior selectivity is elaborated for acetylene semi-hydrogenation via a theoretical guidance with a precise synthesis strategy. The trimer Ni1Sb2 site in NiSb intermetallic is predicted to endow acetylene reactant with an adequately but not excessively strong sigma-adsorption mode while ethylene product with a weak pi-adsorption one, where such compromise delivers higher ethylene formation rate. An in-situ trapping of molten Sb by Ni strategy is developed to realize the construction of Ni1Sb2 site in the intermetallic P6(3)/mmc NiSb catalysts. Such catalyst exhibits ethylene selectivity up to 93.2% at 100% of acetylene conversion, significantly prevailing over the referred Ni catalyst. These insights shed new lights on rational catalyst design by taming active sites to energetically match targeted reaction pathway. Designing atomically uniform ensemble sites for matching targeted reaction pathway is important yet challenging in heterogeneous catalysis. Here, the authors fabricate a trimer Ni1Sb2 site featuring superior selectivity for acetylene semi-hydrogenation via a mechanism-driven design strategy.