4.5 Article

Intercalation-Driven Defect-Engineering of MoS2 for Catalytic Transfer Hydrogenation

期刊

ADVANCED MATERIALS INTERFACES
卷 9, 期 16, 页码 -

出版社

WILEY
DOI: 10.1002/admi.202200505

关键词

catalytic transfer hydrogenation; coordinatively unsaturated sites; intercalation-driven defect-engineering; molybdenum disulfides; nitroarenes

资金

  1. National Major Research and Development Plan [2018YFA0209402]
  2. National Natural Science Foundation of China [22175077, 22088101]
  3. Natural Science Foundation of Guangdong Province [2021A1515012351]

向作者/读者索取更多资源

A new route of in situ intercalation is introduced to engineer defects on MoS2, which can be tuned to improve the catalytic performance of the material in the transfer hydrogenation reaction. The intercalation-induced defects enhance the reactivity of MoS2, demonstrating the promise of the defect-engineering strategy for designing TMDs-based catalysts.
Crystal defects are pivotal to boosting catalytic performance and an in-depth understanding of the working mechanism of transition-metal chalcogenides (TMDs), but their facile and controllable engineering are yet challenging. Herein, a new route is introduced to engineer defects on MoS2 via in situ intercalation during its hydrothermal preparation, accomplishing the efficient catalytic transfer hydrogenation (CTH) of nitroarenes. The combination of multiple structural characterizations demonstrates that the density of S defects can be tuned by the intercalation of ammonium and dimethylamine cations due to lattice strain/distortion and ligand substitution. As a proof of concept, the defect-dependent catalytic performance is evidenced in the CTH of nitrobenzene with isopropanol, highlighting the significance of coordinatively unsaturated Mo sites in generating reactive chemisorbed H for subsequent hydrogenation. The good efficiency of defective MoS2 within a broad substrate scope further verifies the promise of the intercalation-driven defect-engineering strategy for designing TMDs-based catalysts.

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