In situ SERS Investigation of SPR-driven Catalytic Reactions on Au Nanoparticles Monolayer Film

doi:10.6023/A17050198

Acta Chim. Sinica ›› 2017, Vol. 75 ›› Issue (9): 860-865.DOI: 10.6023/A17050198 Previous Articles Next Articles

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金纳米粒子单层膜表面SPR催化反应的原位SERS研究

张晨杰, 张婧, 林洁茹, 金琦, 徐敏敏, 姚建林

苏州大学材料与化学化工学部苏州 215123

投稿日期:2017-05-07 发布日期:2017-09-04
通讯作者: 姚建林 E-mail:jlyao@suda.edu.cn
基金资助:
国家自然科学基金（Nos.21473128，21673152）、国家仪器计划（No.2011YQ031240402）和江苏高校优势学科建设工程资助.

In situ SERS Investigation of SPR-driven Catalytic Reactions on Au Nanoparticles Monolayer Film

Zhang Chenjie, Zhang Jing, Lin Jieru, Jin Qi, Xu Minmin, Yao Jianlin

College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123

Received:2017-05-07 Published:2017-09-04
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 21473128, 21673152), the National Instrumentation Program (No. 2011YQ031240402) and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

The activity and uniformity of surface-enhanced Raman scattering (SERS) effect has been already become the critical role for fundamental research and practical application. Herein, Au nanoparticle monolayer films (Au MLF) were fabricated based on the self-assembly of nanoparticles at the air/water interface by introduction of polyvinylpyrrolidone (PVP) as additional agent. The change of assembly duration allowed the formation of Au MLFs with different density. Due to the excitation mode and intensity of localized surface plasmon resonance (LSPR) varying with the nanoparticle density, the activity and uniformity of SERS substrate could not be taken into account at the same time. For example, loose Au MLF exhibited excellent SERS and catalytic performance but poor uniformity, while compact Au MLF held excellent uniformity and reasonable SERS and catalytic performance. It demonstrated that the intensity of SERS signal was not only relevant to the activity but also to the number of "hot spots", while the conversion rate of surface plasmon resonance (SPR) induced catalysis was only associated with the activity of "hot spots". By using the compact film with relative standard deviation of SERS intensity and SPR catalytic efficiency less than 5% and 6% as the SERS substrate, the influence of the external environment on the SPR catalytic reaction was clarified. In this paper, the effect of laser power on the efficiency and reaction rate of SPR induced catalytic reaction was investigated according to the coupling reaction of para-aminothiophenol (PATP) and decarboxylation process of 4-mercaptobenzoic acid (MBA). It was found that the increase of laser power not only improved the efficiency of SPR catalytic reaction, but also accelerated the reaction rate from the perspective of reaction kinetics due to the heat effect and hot electrons generated by SPR. The results indicated that the rate of the SPR catalytic reaction was linear with the reciprocal of the square of the laser power. It provided a new approach for the determination of the kinetic parameters of the related surface processes.

Key words: surface-enhanced Raman scattering (SERS), Au monolayer film, plasmon catalyzed surface reaction, laser power, decarboxylation reaction

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Zhang Chenjie, Zhang Jing, Lin Jieru, Jin Qi, Xu Minmin, Yao Jianlin. In situ SERS Investigation of SPR-driven Catalytic Reactions on Au Nanoparticles Monolayer Film[J]. Acta Chim. Sinica, 2017, 75(9): 860-865.

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金纳米粒子单层膜表面SPR催化反应的原位SERS研究

In situ SERS Investigation of SPR-driven Catalytic Reactions on Au Nanoparticles Monolayer Film

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