In situ Deposition of ‘Naked’ Gold Nanoparticles Supported on Silica Spheres as Recyclable Catalysts in Styrene Epoxidation

doi:10.1007/s40242-019-9127-0

高等学校化学研究 ›› 2019, Vol. 35 ›› Issue (5): 854-859.doi: 10.1007/s40242-019-9127-0

In situ Deposition of ‘Naked’ Gold Nanoparticles Supported on Silica Spheres as Recyclable Catalysts in Styrene Epoxidation

SHEN Qihui, ZHOU Xinyu, LYU Yang, LI Miao, LIU Yan

Department of Chemistry and Pharmaceutical Engineering, Jilin Institute of Chemical Technology, Jilin 132022, P. R. China

收稿日期:2019-05-06 出版日期:2019-10-01 发布日期:2019-09-24
通讯作者: LIU Yan E-mail:ly@jlict.edu.cn
基金资助:
Supported by the National Natural Science Foundation of China(No.21805107) and the National Program on Key Research & Development Program Sub-project, China(No.2016YFC0800905-Z03).

In situ Deposition of ‘Naked’ Gold Nanoparticles Supported on Silica Spheres as Recyclable Catalysts in Styrene Epoxidation

SHEN Qihui, ZHOU Xinyu, LYU Yang, LI Miao, LIU Yan

Department of Chemistry and Pharmaceutical Engineering, Jilin Institute of Chemical Technology, Jilin 132022, P. R. China

Received:2019-05-06 Online:2019-10-01 Published:2019-09-24
Contact: LIU Yan E-mail:ly@jlict.edu.cn
Supported by:
Supported by the National Natural Science Foundation of China(No.21805107) and the National Program on Key Research & Development Program Sub-project, China(No.2016YFC0800905-Z03).

摘要/Abstract

摘要： The rational designs of particle size, morphology and surface states of the Au nanoparticles(AuNPs) are crucial for Au nanocatalyst. We herein report a method to synthesize the silica microspheres supported AuNPs(ca. 1 nm) and their application in controlling the reaction conversion and selectivity in styrene epoxidation. Surfactant-free AuNPs deposited on silica microspheres were in situ fabricated with aid of the Ag nanoparticles (AgNPs) as sacrificial template by galvanic replacement reaction, leading to AuNPs/SiO₂ catalyst directly without any post-treatment to expose crystal facets. A high conversion of 46.7% and selectivity of 91.7% to styrene oxide was achieved with H₂O₂ as oxidant in ethanol. The solid catalyst could be reused at least 10 reaction cycles without significant decrease in activity and selectivity. This study not only supplies an active, recoverable catalyst for styrene oxidation with green oxidant and solvent, but also demonstrates that the silica microspheres functionalized with thiol groups have a superior ability in stabilizing noble metal nanoparticles even without any surfactant.

关键词: Au nanoparticles, Styrene epoxidation, Galvanic replacement

Abstract: The rational designs of particle size, morphology and surface states of the Au nanoparticles(AuNPs) are crucial for Au nanocatalyst. We herein report a method to synthesize the silica microspheres supported AuNPs(ca. 1 nm) and their application in controlling the reaction conversion and selectivity in styrene epoxidation. Surfactant-free AuNPs deposited on silica microspheres were in situ fabricated with aid of the Ag nanoparticles (AgNPs) as sacrificial template by galvanic replacement reaction, leading to AuNPs/SiO₂ catalyst directly without any post-treatment to expose crystal facets. A high conversion of 46.7% and selectivity of 91.7% to styrene oxide was achieved with H₂O₂ as oxidant in ethanol. The solid catalyst could be reused at least 10 reaction cycles without significant decrease in activity and selectivity. This study not only supplies an active, recoverable catalyst for styrene oxidation with green oxidant and solvent, but also demonstrates that the silica microspheres functionalized with thiol groups have a superior ability in stabilizing noble metal nanoparticles even without any surfactant.

Key words: Au nanoparticles, Styrene epoxidation, Galvanic replacement

SHEN Qihui, ZHOU Xinyu, LYU Yang, LI Miao, LIU Yan. In situ Deposition of ‘Naked’ Gold Nanoparticles Supported on Silica Spheres as Recyclable Catalysts in Styrene Epoxidation[J]. 高等学校化学研究, 2019, 35(5): 854-859.

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In situ Deposition of ‘Naked’ Gold Nanoparticles Supported on Silica Spheres as Recyclable Catalysts in Styrene Epoxidation

In situ Deposition of ‘Naked’ Gold Nanoparticles Supported on Silica Spheres as Recyclable Catalysts in Styrene Epoxidation

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