Mechanism driven design of trimer Ni1Sb2 site delivering superior hydrogenation selectivity to ethylene

Xiaohu Ge; Mingying Dou; Yueqiang Cao; Xi Liu; Qiang Yuwen; Jing Zhang; Gang Qian; Xueqing Gong; Xinggui Zhou; Liwei Chen; Weikang Yuan; Xuezhi Duan

doi:10.1038/s41467-022-33250-8

Mechanism driven design of trimer Ni₁Sb₂ site delivering superior hydrogenation selectivity to ethylene

Nat Commun. 2022 Sep 21;13(1):5534. doi: 10.1038/s41467-022-33250-8.

Authors

Xiaohu Ge¹, Mingying Dou¹, Yueqiang Cao², Xi Liu³, Qiang Yuwen¹, Jing Zhang¹, Gang Qian¹, Xueqing Gong⁴, Xinggui Zhou¹, Liwei Chen⁵, Weikang Yuan¹, Xuezhi Duan⁶

Affiliations

¹ State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
² State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China. yqcao@ecust.edu.cn.
³ School of Chemistry and Chemical Engineering, In-situ Center for Physical Sciences, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China. liuxi@sjtu.edu.cn.
⁴ Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
⁵ School of Chemistry and Chemical Engineering, In-situ Center for Physical Sciences, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China.
⁶ State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China. xzduan@ecust.edu.cn.

Abstract

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 σ-adsorption mode while ethylene product with a weak π-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 P6₃/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.

Abstract

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