Highly Efficient Hydrosilylation of Ethyne over Pt/ZrO2 Catalysts with Size-Dependent Metal–Support Interactions

Tengfei Zhang; Mingyan Li; Peng Zheng; Jing Li; Jiajian Gao; Hongyan He; Fangna Gu; Wenxing Chen; Yongjun Ji; Ziyi Zhong; Dingrong Bai; Guangwen Xu; Fabing Su

doi:10.1021/acs.iecr.2c03553

Highly Efficient Hydrosilylation of Ethyne over Pt/ZrO₂ Catalysts with Size-Dependent Metal–Support Interactions

Tengfei Zhang, Mingyan Li, Peng Zheng, Jing Li, Jiajian Gao, Hongyan He, Fangna Gu, Wenxing Chen, Yongjun Ji, Ziyi Zhong, Dingrong Bai, Guangwen Xu, Fabing Su

Chemical Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

Replacing homogeneous noble-metal catalysts with supported catalysts in hydrosilylation reactions can overcome the difficulties of catalyst recovery and regeneration. Here, we report the scalable synthesis of heterogeneous Pt/ZrO2 catalysts with 1–5 wt % Pt supported on commercial ZrO2 nanocrystals. Pt/ZrO2 can effectively catalyze the hydrosilylation of triethoxysilane (TES) with ethyne to high-value triethoxyvinylsilane, even superior to the common homogeneous catalyst (H2PtCl6). Intensive characterizations indicate that the coating of ZrOx on Pt greatly depends on the size of Pt, with more ZrOx overlayers on smaller Pt metal particles. Among all the catalysts, 2Pt/ZrO2 exhibits the highest activity, optimal selectivity, and reusability toward hydrosilylation of TES with ethyne. The unusual catalytic properties of 2Pt/ZrO2 can be attributed to its more abundant surface PtOx species and the electron transfer between Pt and ZrO2. This change in local electronic properties promotes catalytic activity, which is also supported by the corresponding theoretical calculation. This work advances the understanding of metal–support interactions and provides a powerful approach to designing environmentally friendly heterogeneous catalysts for the industrially important hydrosilylation process.

Original language	English
Pages (from-to)	18703–18711
Journal	Industrial and Engineering Chemistry Research
Volume	61
Issue number	51
DOIs	https://doi.org/10.1021/acs.iecr.2c03553
State	Published - 16 Dec 2022

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10.1021/acs.iecr.2c03553

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@article{8eb3eb03778d4f27819ddea7e481f21f,

title = "Highly Efficient Hydrosilylation of Ethyne over Pt/ZrO2 Catalysts with Size-Dependent Metal–Support Interactions",

abstract = "Replacing homogeneous noble-metal catalysts with supported catalysts in hydrosilylation reactions can overcome the difficulties of catalyst recovery and regeneration. Here, we report the scalable synthesis of heterogeneous Pt/ZrO2 catalysts with 1–5 wt % Pt supported on commercial ZrO2 nanocrystals. Pt/ZrO2 can effectively catalyze the hydrosilylation of triethoxysilane (TES) with ethyne to high-value triethoxyvinylsilane, even superior to the common homogeneous catalyst (H2PtCl6). Intensive characterizations indicate that the coating of ZrOx on Pt greatly depends on the size of Pt, with more ZrOx overlayers on smaller Pt metal particles. Among all the catalysts, 2Pt/ZrO2 exhibits the highest activity, optimal selectivity, and reusability toward hydrosilylation of TES with ethyne. The unusual catalytic properties of 2Pt/ZrO2 can be attributed to its more abundant surface PtOx species and the electron transfer between Pt and ZrO2. This change in local electronic properties promotes catalytic activity, which is also supported by the corresponding theoretical calculation. This work advances the understanding of metal–support interactions and provides a powerful approach to designing environmentally friendly heterogeneous catalysts for the industrially important hydrosilylation process.",

author = "Tengfei Zhang and Mingyan Li and Peng Zheng and Jing Li and Jiajian Gao and Hongyan He and Fangna Gu and Wenxing Chen and Yongjun Ji and Ziyi Zhong and Dingrong Bai and Guangwen Xu and Fabing Su",

year = "2022",

month = dec,

day = "16",

doi = "10.1021/acs.iecr.2c03553",

language = "英语",

volume = "61",

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journal = "Industrial and Engineering Chemistry Research",

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TY - JOUR

T1 - Highly Efficient Hydrosilylation of Ethyne over Pt/ZrO2 Catalysts with Size-Dependent Metal–Support Interactions

AU - Zhang, Tengfei

AU - Li, Mingyan

AU - Zheng, Peng

AU - Li, Jing

AU - Gao, Jiajian

AU - He, Hongyan

AU - Gu, Fangna

AU - Chen, Wenxing

AU - Ji, Yongjun

AU - Zhong, Ziyi

AU - Bai, Dingrong

AU - Xu, Guangwen

AU - Su, Fabing

PY - 2022/12/16

Y1 - 2022/12/16

N2 - Replacing homogeneous noble-metal catalysts with supported catalysts in hydrosilylation reactions can overcome the difficulties of catalyst recovery and regeneration. Here, we report the scalable synthesis of heterogeneous Pt/ZrO2 catalysts with 1–5 wt % Pt supported on commercial ZrO2 nanocrystals. Pt/ZrO2 can effectively catalyze the hydrosilylation of triethoxysilane (TES) with ethyne to high-value triethoxyvinylsilane, even superior to the common homogeneous catalyst (H2PtCl6). Intensive characterizations indicate that the coating of ZrOx on Pt greatly depends on the size of Pt, with more ZrOx overlayers on smaller Pt metal particles. Among all the catalysts, 2Pt/ZrO2 exhibits the highest activity, optimal selectivity, and reusability toward hydrosilylation of TES with ethyne. The unusual catalytic properties of 2Pt/ZrO2 can be attributed to its more abundant surface PtOx species and the electron transfer between Pt and ZrO2. This change in local electronic properties promotes catalytic activity, which is also supported by the corresponding theoretical calculation. This work advances the understanding of metal–support interactions and provides a powerful approach to designing environmentally friendly heterogeneous catalysts for the industrially important hydrosilylation process.

AB - Replacing homogeneous noble-metal catalysts with supported catalysts in hydrosilylation reactions can overcome the difficulties of catalyst recovery and regeneration. Here, we report the scalable synthesis of heterogeneous Pt/ZrO2 catalysts with 1–5 wt % Pt supported on commercial ZrO2 nanocrystals. Pt/ZrO2 can effectively catalyze the hydrosilylation of triethoxysilane (TES) with ethyne to high-value triethoxyvinylsilane, even superior to the common homogeneous catalyst (H2PtCl6). Intensive characterizations indicate that the coating of ZrOx on Pt greatly depends on the size of Pt, with more ZrOx overlayers on smaller Pt metal particles. Among all the catalysts, 2Pt/ZrO2 exhibits the highest activity, optimal selectivity, and reusability toward hydrosilylation of TES with ethyne. The unusual catalytic properties of 2Pt/ZrO2 can be attributed to its more abundant surface PtOx species and the electron transfer between Pt and ZrO2. This change in local electronic properties promotes catalytic activity, which is also supported by the corresponding theoretical calculation. This work advances the understanding of metal–support interactions and provides a powerful approach to designing environmentally friendly heterogeneous catalysts for the industrially important hydrosilylation process.

U2 - 10.1021/acs.iecr.2c03553

DO - 10.1021/acs.iecr.2c03553

M3 - 文章

SN - 0888-5885

VL - 61

SP - 18703

EP - 18711

JO - Industrial and Engineering Chemistry Research

JF - Industrial and Engineering Chemistry Research

IS - 51

ER -

Highly Efficient Hydrosilylation of Ethyne over Pt/ZrO2 Catalysts with Size-Dependent Metal–Support Interactions

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Highly Efficient Hydrosilylation of Ethyne over Pt/ZrO₂ Catalysts with Size-Dependent Metal–Support Interactions