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Nano Research 2023, 16(4): 4643-4649 https://doi.org/10.1007/s12274-022-5097-5
Research Article | Issue | Published: 02 November 2022

Construction of highly dispersed Pt single sites and high-efficiency-heterocatalysis silylation of alcohols with silanes

Show Author's Information Qiulian Wei1,2,  Yunqiang Sun2( ),  Shan Wang1,2,  Zunfu Hu2,  Qingyun Liu1( ),  Xiuwen Zheng1,2( )
School of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266510, China
Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong, College of Chemistry and Chemical Engineering, Linyi University, Linyi 276000, China
Keywords:
heterogeneous catalysis, single-atom catalysis, high-dispersion, O-silylation
Topics:
Nanocatalysts
Cite this article:
Wei Q, Sun Y, Wang S, et al. Construction of highly dispersed Pt single sites and high-efficiency-heterocatalysis silylation of alcohols with silanes. Nano Research, 2023, 16(4): 4643-4649. https://doi.org/10.1007/s12274-022-5097-5
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Abstract Full text Electronic supplementary material About this article

The construction of silicon–oxygen bonds has been highlighted as an exciting achievement in organosilicon and green chemistry, but their synthetic efficiency has great improvement potential, so it is crucial to explore and achieve an effective approach for synthesizing such compounds. In this study, we successfully prepared the highly dispersed platinum single-atom catalyst (Pt SAC/N-C) through a coordination-assisted strategy with a mixture of ligands (H2bpdc and H2bpydc), which were used for the O-silylation of alcohols with silanes. The strong coordination between Pt2+ and the Pyridine N at the skeleton of UiO-67 plays a critical role in accessing the atomically isolated dispersion of Pt sites. Without the assistance of the H2bpydc ligands, the Pt/ UiO-67-bpdc precursor is prone to aggregation during the pyrolysis process, resulting in the formation of Pt nanoparticles. Aided by advanced characterization techniques of high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy, it has been demonstrated that atomically dispersed Pt was formed on the UiO-67 through a local structure of four-coordinated Pt-N4, exhibiting a high actual Pt loading content (0.6962 wt.%). In the oxidation of silanes, the Pt SAC/N-C catalyst showed a high turnover frequency (TOF) value (up to 9,920 h−1) when the catalyst loading decreased to 0.005%. Excellent performance was maintained during recycling experiments, indicating high stability of the catalyst.


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Electronic supplementary material
About this article

Construction of highly dispersed Pt single sites and high-efficiency-heterocatalysis silylation of alcohols with silanes

Show Author's information Qiulian Wei1,2, Yunqiang Sun2( ), Shan Wang1,2, Zunfu Hu2, Qingyun Liu1( ), Xiuwen Zheng1,2( )
School of Chemical and Biological Engineering, Shandong University of Science and Technology, Qingdao 266510, China
Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong, College of Chemistry and Chemical Engineering, Linyi University, Linyi 276000, China

Abstract

The construction of silicon–oxygen bonds has been highlighted as an exciting achievement in organosilicon and green chemistry, but their synthetic efficiency has great improvement potential, so it is crucial to explore and achieve an effective approach for synthesizing such compounds. In this study, we successfully prepared the highly dispersed platinum single-atom catalyst (Pt SAC/N-C) through a coordination-assisted strategy with a mixture of ligands (H2bpdc and H2bpydc), which were used for the O-silylation of alcohols with silanes. The strong coordination between Pt2+ and the Pyridine N at the skeleton of UiO-67 plays a critical role in accessing the atomically isolated dispersion of Pt sites. Without the assistance of the H2bpydc ligands, the Pt/ UiO-67-bpdc precursor is prone to aggregation during the pyrolysis process, resulting in the formation of Pt nanoparticles. Aided by advanced characterization techniques of high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption fine structure (XAFS) spectroscopy, it has been demonstrated that atomically dispersed Pt was formed on the UiO-67 through a local structure of four-coordinated Pt-N4, exhibiting a high actual Pt loading content (0.6962 wt.%). In the oxidation of silanes, the Pt SAC/N-C catalyst showed a high turnover frequency (TOF) value (up to 9,920 h−1) when the catalyst loading decreased to 0.005%. Excellent performance was maintained during recycling experiments, indicating high stability of the catalyst.

Keywords: heterogeneous catalysis, single-atom catalysis, high-dispersion, O-silylation

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Publication history
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Acknowledgements

Publication history

Received: 15 July 2022
Revised: 08 September 2022
Accepted: 22 September 2022
Published: 02 November 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22075122 and 21971152), the Natural Science Foundation of Shandong Province (Nos. ZR2019BB038, ZR2020QB170, and ZR2020MB003). We thank LetPub (www.letpub.com) for its linguistic assistance during the preparation of this manuscript.

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