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Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

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Chemical Research in Chinese Universities Aims and scope

Abstract

Multiple metal sites doped in metal-organic frameworks (MOFs) are essential for their promising application in cascade reactions. However, precision synthesis of tetrametallic MOFs with total coordination and regular shapes is challenging due to the different coordination abilities of four metal ions. Herein, a series of tetrametallic MOFs (t-MOFs) with four regular morphologies is successfully constructed by regulating the metal ratio, amount of morphologic modulating reagent or growth time. The t-MOFs can be flexibly oxidized to afford porous metal oxides (MxCo3O4, M=CuZnNi) under air or reduced to carbon-encapsulated CuCoNi under H2/Ar for different reactions to maximize the value-in-use of MOFs. In particular, the t-MOF@MxCo3O4 obtained upon the surface oxidation of t-MOF well integrates the Lewis-base sites from MOF core with photothermal oxidation activity from MxCo3O4 shell. The hybrid effectively catalyzes the cascade reaction of styrene oxidation coupling Knoevenagel condensation under visible light. Thus, the by-product, benzaldehyde, is successfully converted to easily separated benzylidene malononitrile to finally obtain pure styrene epoxide (SO). In MxCo3O4, Ni species afford good photothermal effect, Cu and Co species provide catalytic activity, and Zn species increase SO selectivity. The host-object coordination and the synergy among objects may greatly boost more complex reactions in the future.

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Acknowledgements

This work was supported by the Excellent Youth Foundation of Natural Science Foundation of Shandong Province, China (No. ZR2020YQ08) and the National Natural Science Foundation of China (No. 22275108).

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Authors and Affiliations

  1. Department of Chemistry, College of Chemistry and Chemical Engineering, Qingdao University of Science and Technology, Qingdao, 266071, P. R. China

    Yiwen Fan, Yang Wang, Yuzhen Chen & Zhibo Li

  2. Experimental Center of Engineering and Material Science, University of Science and Technology of China, Hefei, 230026, P. R. China

    Huijuan Wang

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  1. Yiwen Fan
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  2. Yang Wang
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  3. Huijuan Wang
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  4. Yuzhen Chen
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Correspondence to Yuzhen Chen or Zhibo Li.

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40242_2024_4044_MOESM1_ESM.pdf

Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis

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Fan, Y., Wang, Y., Wang, H. et al. Precise Fabrication of Tetrametallic Metal-Organic Frameworks and Multivariate Hybrids for Enhanced Photothermal Tandem Catalysis. Chem. Res. Chin. Univ. (2024). https://doi.org/10.1007/s40242-024-4044-2

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  • DOI: https://doi.org/10.1007/s40242-024-4044-2

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