[ACIE] Pd单原子嵌入NiGa金属间化合物表面实现高效选择性炔烃半氢化

文摘   2024-07-07 08:05   江西  

Abstract

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 Pd1-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 located synergizes with the neighbouring Ni sites to facilitate the σ-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.

X. Ge, Y. Jing, N. Fei, K. Yan, Y. Liang, Y. Cao, J. Zhang, G. Qian, L. Li, H. Jiang, X. Zhou, W. Yuan, X. Duan, Embedding Single Pd Atoms on NiGa Intermetallic Surfaces for Efficient and Selective Alkyne Semi-hydrogenation, Angewandte Chemie International Edition, n/a (2024) e202410979. DOI: 10.1002/anie.202410979.


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