Highly Selective and Stable Isolated Non-Noble Metal Atom Catalysts for Selective Hydrogenation of Acetylene

Baoai Fu, Alan McCue, Yanan Liu* (Corresponding Author), Shaoxia Weng, Yuanfei Song, Yufei He, Junting Feng, Dianqing Li* (Corresponding Author)

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

A strategy to fabricate a stable and site-isolated Ni catalyst is reported. Specifically, Mo3S4 clusters allowed individual Ni atoms to bond with Mo and S to create a type of active site. A site-isolated Ni1MoS/Al2O3 sample exhibited high performance in the selective hydrogenation of acetylene. Concretely, 90% ethylene selectivity was achievable at full acetylene conversion under relatively mild reaction conditions without any obvious decay in performance observed during longer testing periods. In contrast, a reference catalyst with Ni ensembles exhibited poor selectivity and stability. Density functional theory (DFT) calculations suggested that H2 molecules were activated by a heterolytic route over Ni1MoS/Al2O3, which enhanced the reaction rate. Improved selectivity originated from the unique isolated Niδ+ structure induced by Mo and S, which facilitated product desorption as opposed to overhydrogenation or oligomerization. This work provides a feasible way to construct site-isolated catalysts with higher active metal loadings and opens up an opportunity for selective hydrogenation.

Original languageEnglish
Pages (from-to)607-615
Number of pages9
JournalACS Catalysis
Early online date22 Dec 2021
DOIs
Publication statusPublished - 7 Jan 2022

Keywords

  • Non-noble Ni catalysts
  • Isolated Niδ
  • structure
  • Selective hydrogenation
  • Mo3S4 cluster
  • Confinement strategy

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