4.8 Article

Facile Synthesis of Single Iron Atoms over MoS2 Nanosheets via Spontaneous Reduction for Highly Efficient Selective Oxidation of Alcohols

Journal

SMALL
Volume 18, Issue 19, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202201092

Keywords

catalytic activity; iron; molybdenum sulfide; oxidation of alcohols; single atom catalysis

Funding

  1. China Postdoctoral Science Foundation [2019M661247, 2020T130091]
  2. Postdoctoral Science Foundation of Heilongjiang Province [LBH-Z19047]
  3. Scientific Research Foundation for Returned Scholars of Heilongjiang Province of China [719900091]
  4. Heilongjiang Touyan Innovation Team Program
  5. National Natural Science Foundation of China [51902052]

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This study presents an efficient spontaneous reduction approach to create atomically dispersed iron atoms supported over MoS2 nanosheets for the selective oxidation of benzyl alcohol. The single-atom catalyst shows exceptional catalytic efficiency and recyclability.
The facile creation of high-performance single-atom catalysts (SACs) is intriguing in heterogeneous catalysis, especially on 2D transition-metal dichalcogenides. An efficient spontaneous reduction approach to access atomically dispersed iron atoms supported over defect-containing MoS2 nanosheets is herein reported. Advanced characterization methods demonstrate that the isolated iron atoms situate atop of molybdenum atoms and coordinate with three neighboring sulfur atoms. This Fe SAC delivers exceptional catalytic efficiency (1 atm O-2 @ 120 degrees C) in the selective oxidation of benzyl alcohol to benzaldehyde, with 99% selectivity under almost 100% conversion. The turnover frequency is calculated to be as high as 2105 h(-1). Moreover, it shows admirable recyclability, storage stability, and substrate tolerance. Density functional theory calculations reveal that the high catalytic activity stems from the optimized electronic structure of single iron atoms over the MoS2 support.

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