Formation of atomically dispersed zirconium through the utilization of nanoconfined environments

Abstract

Single-atom catalysts are highly effective in catalyzing a wide range of reactions owing to their capacity to have precise coordination patterns and fully leverage the potential of metal atoms. Although several techniques have been reported for the preparation of single-atom catalysts, adopting a convenient method to construct them still has a challenge. In this work, we report a convenient method for the preparation of Zr-based single-atom catalyst that takes advantage of the nanoconfined environments between the template and silica wall in template-occupied silica SBA-15. After introducing Zr-containing precursor into the nanoconfined environments of the template-occupied silica SBA-15 using solid-phase milling, Zr-based single-atom catalysts were produced via the following calcination step. Density functional theory calculations and experimental findings show that Zr atoms form Zr–O–Si structure in the silica walls. The Zr single-atom catalyst synthesized using the nanoconfined environments exhibited notably superior catalytic performance in the synthesis of benzyl acetate from the esterification reaction between acetic acid and benzyl alcohol (63.3% yield), outperforming the counterpart that synthesized without such nanoconfined environments (19.8% yield).

Graphical abstract

Keywords

single-atom catalysts / zirconium / nanoconfined environments / esterification

References

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Acknowledgements

We acknowledge the financial support of this work by the National Science Fund for Distinguished Young Scholars (Grant No. 22125804) and the National Natural Science Foundation of China (Grant No. 22078155). We are grateful to the High-Performance Computing Center of Nanjing Tech University for supporting the computational resources. We appreciate the XANES measurements provided by the BL11B beam station at the Shanghai Synchrotron Radiation Facility (SSRF).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-025-2524-7 and is accessible for authorized users.

Competing interests

The authors declare that they have no competing interests.

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