4.8 Article

ZnO-POM Cluster Sub-1 nm Nanosheets as Robust Catalysts for the Oxidation of Thioethers at Room Temperature

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 39, Pages 16217-16225

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c07477

Keywords

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Funding

  1. National Key R&D Program of China [2017YFA0700101]
  2. NSFC [22035004]
  3. China National Postdoctoral Program for Innovative Talents [BX20200182]
  4. China Postdoctoral Science Foundation [2020M680509]
  5. Shuimu Tsinghua Scholar Program

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A versatile strategy was developed to prepare ZnO-POM-based 2D hybrid sub-1 nm nanosheets by incorporating three kinds of molybdenum-based POM clusters into the zinc oxide system. Molecular dynamics simulation results showed that the POM clusters interacted with ZnO/Zn(OH)(2) molecules to form stable 2D nanostructures. These materials exhibited excellent catalytic performance due to their large specific surface areas and the synergistic effect of multiple components.
Two-dimensional (2D) zinc oxides have attracted more and more research interests due to their unique properties. Yet, it remains a great challenge to limit the thickness to the sub-1 nm scale and further combine with other components to obtain 2D hybrid zinc oxide (ZnO)-based sub-1 nm materials. Herein, a versatile strategy was successfully developed to realize the controllable preparation of ZnO-polyoxometalate (POM)-based 2D hybrid sub-1 nm nanosheet (HSNS) superstructures by incorporating three kinds of molybdenum-based POM clusters into the zinc oxide system. Molecular dynamics simulation results demonstrated that POM clusters interact with ZnO/Zn(OH)(2) molecules and coassembled into stable 2D HSNSs. Significantly, theses materials as robust catalysts showed excellent catalytic activity, selectivity, and stability in the oxidation of thioethers at room temperature, which partly can be attributed to the special 2D sub-1 nm nanostructures with large specific areas leading to the full exposure of active sites. Meanwhile, the synergetic effect of multiple components also played an important role during the catalytic process. Thus, this work would pave the way for the precise synthesis of multicomponent 2D hybrid sub-1 nm materials for widespread applications.

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