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Regulating the surface plasmon resonance (SPR) of metallic nanostructures is of great interests for optical and catalytic applications, however, it is still a great challenge for tuning SPR features of small metallic nanoparticles (< 10 nm). In this work, we design a unique dielectric support—urchin-like mesoporous silica nanoparticles (U-SiO2) with ordered long spikes on its surface, which can well enhance the SPR properties of ~ 3 nm gold nanocrystals (AuNCs). The U-SiO2 not only realizes the uniform self-assembly of AuNCs, but also prevents their aggregation due to the unique confinement effect. The finite-difference time-domain simulations show that the AuNCs on U-SiO2 can generate plasmonic hot spots with highly enhanced electromagnetic field. Moreover, the hot electrons can be effectively and rapidly transferred through the interface junction to TiO2. Thus, a high visible-light-driven photocatalytic activity can be observed, which is 3.8 times higher than that of smooth photocatalysts. The concept of dielectric supports engineering provides a new strategy for tuning SPR of small metallic nanocrystals towards the development of advanced plasmon-based applications.


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Hot spots engineering by dielectric support for enhanced photocatalytic redox reactions

Show Author's information Yan Yu1,2Yujun Xie2Pengfei Zhang1Wei Zhang1,3Wenxing Wang1( )Shuyu Zhang2( )Qiongrong Ou2Wei Li1( )
Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Lab of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, China
Institute for Electric Light Sources, School of Information Science and Technology, Fudan University, Shanghai 200433, China
Zhuhai Fudan Innovation Institute, Guangdong-Macao In-Depth Cooperation Zone in Hengqin, Zhuhai 519000, China

Abstract

Regulating the surface plasmon resonance (SPR) of metallic nanostructures is of great interests for optical and catalytic applications, however, it is still a great challenge for tuning SPR features of small metallic nanoparticles (< 10 nm). In this work, we design a unique dielectric support—urchin-like mesoporous silica nanoparticles (U-SiO2) with ordered long spikes on its surface, which can well enhance the SPR properties of ~ 3 nm gold nanocrystals (AuNCs). The U-SiO2 not only realizes the uniform self-assembly of AuNCs, but also prevents their aggregation due to the unique confinement effect. The finite-difference time-domain simulations show that the AuNCs on U-SiO2 can generate plasmonic hot spots with highly enhanced electromagnetic field. Moreover, the hot electrons can be effectively and rapidly transferred through the interface junction to TiO2. Thus, a high visible-light-driven photocatalytic activity can be observed, which is 3.8 times higher than that of smooth photocatalysts. The concept of dielectric supports engineering provides a new strategy for tuning SPR of small metallic nanocrystals towards the development of advanced plasmon-based applications.

Keywords: photocatalysis, TiO2, surface plasmon resonance, hot spots, urchin-like silica nanoparticles, core–shell structures

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Publication history
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Acknowledgements

Publication history

Received: 01 June 2022
Revised: 26 June 2022
Accepted: 27 June 2022
Published: 12 August 2022
Issue date: January 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Key Research and Development Program of China (No. 2018YFE0201701), the National Natural Science Foundation of China (Nos. 21975050, 21905052, 11975081, and 22105041), Science and Technology Commission of Shanghai Municipality (No. 21ZR1408800), Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 19JC1410700), the Program of Shanghai Academic Research Leader (No. 21XD1420800), and Guangdong Basic and Applied Basic Research Foundation (No. 2021A1515010108).

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