Facile synthesis of precious-metal single-site catalysts using organic solvents

Abstract

Single-site catalysts can demonstrate high activity and selectivity in many catalytic reactions. The synthesis of these materials by impregnation from strongly oxidizing aqueous solutions or pH-controlled deposition often leads to low metal loadings or a range of metal species. Here, we demonstrate that simple impregnation of the metal precursors onto activated carbon from a low-boiling-point, low-polarity solvent, such as acetone, results in catalysts with an atomic dispersion of cationic metal species. We show the generality of this method by producing single-site Au, Pd, Ru and Pt catalysts supported on carbon in a facile manner. Single-site Au/C catalysts have previously been validated commercially to produce vinyl chloride, and here we show that this facile synthesis method can produce effective catalysts for acetylene hydrochlorination in the absence of the highly oxidizing acidic solvents previously used.

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Fig. 1: Characterization of Ru/C, Pd/C, Pt/C and Au/C catalysts prepared by impregnation of metal precursors from acetone.
Fig. 2: Characterization and testing of a series of Au/C catalysts prepared by impregnation of the metal precursor from different solvents.
Fig. 3: Au L3-edge XAS characterization of the Au/C-acetone catalyst.
Fig. 4: Catalytic performance of the Au/C-acetone catalyst.
Fig. 5: Characterization and testing of Ru/C, Pd/C, Pt/C and Au/C catalysts prepared by impregnation of metal precursors from acetone.

Data availability

Data supporting the results presented here, including how to access them, can be found in the Cardiff University data catalogue at https://doi.org/10.17035/d.2020.0098831512.

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Acknowledgements

The authors thank Cardiff University for financial support. X.S. thanks the China Scholarship Council (CSC) for his scholarship. S.J.F. acknowledges the Ser Cymru II Fellowship scheme part-funded by the European Regional Development Fund. C.J.K. acknowledges funding from the National Science Foundation Major Research Instrumentation program (GR MRI/DMR-1040229). We thank Diamond Light Source for access and support in the use of the Electron Physical Science Imaging Centre (ePSIC Instrument E01 with proposal numbers MG22766-1 and EM20643-2 (with R. Wang, University College London)). We acknowledge Diamond Light Source for time on Beamline B18 under proposals SP19580-1, SP19850-2 and SP19580-3.

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Catalysts were prepared, tested and characterized by X.S., S.R.D., T.E.P. and G.M. under the supervision of S.A.K., S.J.F. and G.J.H. Microscopy was carried out by T.E.D., Q.H. and L.L. under the supervision of C.J.K. XPS was carried out by D.J.M and T.E.P., and testing under industrial conditions was carried out by N.C. and P.J. The manuscript was written by S.J.F., S.A.K., G.M. and G.J.H. with input from all authors.

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Correspondence to Graham J. Hutchings.

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Supplementary Tables 1–6 and Figs. 1–16.

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Sun, X., Dawson, S.R., Parmentier, T.E. et al. Facile synthesis of precious-metal single-site catalysts using organic solvents. Nat. Chem. 12, 560–567 (2020). https://doi.org/10.1038/s41557-020-0446-z

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