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Nano Research 2023, 16(7): 8751-8756 https://doi.org/10.1007/s12274-023-5756-1
Communication | Issue | Published: 18 May 2023

Tunable hydrogen coverage on electron-deficient platinum nanoparticles for efficient hydrogenation reactions

Show Author's Information Lu-Han Sun1,  Qi-Yuan Li1,  Yu-Shuai Xu1,  Si-Yuan Xia1,  Dong Xu1,  Xiu Lin1,  Jingsan Xu2,  Jie-Sheng Chen1,  Guo-Dong Li3,  Xin-Hao Li1( )
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai 200240, China
School of Chemistry and Physics, Faculty of Science, Centre for Materials Science , Queensland University of Technology, Brisbane, QLD 4001, Australia
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
Keywords:
Schottky barrier, heterogeneous catalysis, hydrogenation, hydrogen coverage
Topics:
Catalysis
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Sun L-H, Li Q-Y, Xu Y-S, et al. Tunable hydrogen coverage on electron-deficient platinum nanoparticles for efficient hydrogenation reactions. Nano Research, 2023, 16(7): 8751-8756. https://doi.org/10.1007/s12274-023-5756-1
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Abstract Full text Electronic supplementary material About this article

Dissociation of active H species over the catalytic sites with the carbon-supported Pt metals as the mainstream catalysts is crucial to facilitate hydrogen donation and accelerate the hydrogen addition process in catalytic hydrogenation systems to produce polymers, pharmaceuticals, agrochemicals, fragrances, and biofuels at million-ton scale. Much attention has been paid to the design of the more active catalytic site to effectively adsorb and activate reactants and H2 molecules. At the same time, there is still a huge room to develop powerful strategies to accelerate the donation of acted H species to the reactants from the Pt surface further to boost the final catalytic efficiencies of Pt catalysts and depress the total Pt consumption. Herein, we present a new strategy for promoting the Pt–H bond dissociation by increasing surface hydrogen coverage on designed electron-deficient Pt nanoparticles. The electron deficiency of Pt nanoparticles has been successfully tuned by constructing a rectifying contact with an even “noble” boron-rich carbon support (Pt/BC). Theoretical and experimental results confirm the dominant role of the pronounced electron deficiencies of Pt nanoparticles in enhancing the H coverage for 2.3 times higher than that of neutral Pt nanoparticles, significantly boosting the Pt–H bond dissociation and thus the whole hydrogenation process as reflected by the extremely high turnover frequency (TOF) value of 388 h−1 at 30 °C and 10 bar H2 for phenol hydrogenation on the Pt/BC, outperforming the bench-marked catalysts by a factor of 9.


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Electronic supplementary material
About this article

Tunable hydrogen coverage on electron-deficient platinum nanoparticles for efficient hydrogenation reactions

Show Author's information Lu-Han Sun1, Qi-Yuan Li1, Yu-Shuai Xu1, Si-Yuan Xia1, Dong Xu1, Xiu Lin1, Jingsan Xu2, Jie-Sheng Chen1, Guo-Dong Li3, Xin-Hao Li1( )
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai 200240, China
School of Chemistry and Physics, Faculty of Science, Centre for Materials Science , Queensland University of Technology, Brisbane, QLD 4001, Australia
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China

Abstract

Dissociation of active H species over the catalytic sites with the carbon-supported Pt metals as the mainstream catalysts is crucial to facilitate hydrogen donation and accelerate the hydrogen addition process in catalytic hydrogenation systems to produce polymers, pharmaceuticals, agrochemicals, fragrances, and biofuels at million-ton scale. Much attention has been paid to the design of the more active catalytic site to effectively adsorb and activate reactants and H2 molecules. At the same time, there is still a huge room to develop powerful strategies to accelerate the donation of acted H species to the reactants from the Pt surface further to boost the final catalytic efficiencies of Pt catalysts and depress the total Pt consumption. Herein, we present a new strategy for promoting the Pt–H bond dissociation by increasing surface hydrogen coverage on designed electron-deficient Pt nanoparticles. The electron deficiency of Pt nanoparticles has been successfully tuned by constructing a rectifying contact with an even “noble” boron-rich carbon support (Pt/BC). Theoretical and experimental results confirm the dominant role of the pronounced electron deficiencies of Pt nanoparticles in enhancing the H coverage for 2.3 times higher than that of neutral Pt nanoparticles, significantly boosting the Pt–H bond dissociation and thus the whole hydrogenation process as reflected by the extremely high turnover frequency (TOF) value of 388 h−1 at 30 °C and 10 bar H2 for phenol hydrogenation on the Pt/BC, outperforming the bench-marked catalysts by a factor of 9.

Keywords: Schottky barrier, heterogeneous catalysis, hydrogenation, hydrogen coverage

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Publication history
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Acknowledgements

Publication history

Received: 04 March 2023
Revised: 30 March 2023
Accepted: 18 April 2023
Published: 18 May 2023
Issue date: July 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the Shanghai Science and Technology Committee (No. 20520711600), the National Natural Science Foundation of China (Nos. 22071146 and 21931005), the SJTU-MPI partner group, and the Open Research Fund of the State Key Laboratory of Inorganic Synthesis and Preparative Chemistry (Jilin University, China, No. 2021-1).

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