SERS spectral evolution of azo-reactions mediated by plasmonic Au@Ag core-shell nanorods.
SERS spectral evolution of azo-reactions mediated by plasmonic Au@Ag core-shell nanorods.
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DOI：
10.1039/d2na00486k
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发表时间：
2022-11-08
影响因子：
4.7
通讯作者：
中科院分区：
文献类型：
--
作者：
局域表面等离子体激元共振光催化反应的机理和应用一直是人们关注的问题。在这项工作中，我们使用Au@Ag核壳纳米棒作为平台的等离子体激元驱动的拉曼光谱，这是原位研究的表面增强拉曼散射（Sers）光谱。吸附在纳米棒上的对氨基苯硫酚（PATP）和对硝基苯硫酚（PNTP）分别用不同的激发波长进行辐照（633 nm，785 nm），并转化为4，4 ′-二巯基偶氮苯（DMAB），如在1142 cm-1、1390 cm-1、1440 cm-1和1477 cm-1处出现的拉曼峰所证明的，对应于热载流子主导的PATP氧化和PNTP还原。通过比较1440 cm−1（NN的DMAB伸缩）和1080 cm−1（PATP和PNTP的C-S伸缩）处的Sers峰的相对强度比，进行初步的偶氮反应动力学和原位Sers测量。这些结果表明，催化效率是由激发波长以及纳米棒的等离子体激元带和激发线之间的共振条件。作为概念验证，将Au@Ag核壳纳米棒用于催化4-硝基苯酚分子，并通过原位Sers光谱和理论预测证实产物为4-羟基偶氮苯分子，显示出等离子体驱动催化降解有机分子的潜力。等离子体激元驱动的光催化效应产生偶氮反应。
The mechanism and application of localized surface plasmon resonance induced photocatalytic reactions remain an issue of interest. In this work, we used Au@Ag core–shell nanorods as a platform for plasmon-driven photocatalysis, which was in situ investigated by surface-enhanced Raman scattering (SERS) spectroscopy. The para-aminothiophenol (PATP) and para-nitrothiophenol (PNTP) adsorbed on the nanorods were irradiated with different excitation wavelengths (633 nm, 785 nm) and transformed into 4,4′-dimercaptoazobenzene (DMAB) as evidenced by the emerging Raman peaks at 1142 cm−1, 1390 cm−1, 1440 cm−1, and 1477 cm−1, corresponding to hot carrier dominated oxidation of PATP and reduction of PNTP. Preliminary azo-reaction kinetics and in situ SERS measurements were conducted by comparing the relative intensity ratio of SERS peaks at 1440 cm−1 (DMAB stretching of NN) and 1080 cm−1 (C–S stretching of PATP and PNTP). These results indicate that the catalytic efficiency was dominated by the excitation wavelength as well as the resonance condition between the plasmon band of the nanorods and the excitation line. As a proof of concept, the Au@Ag core–shell nanorods were used to catalyze 4-nitrophenol molecules, and 4-hydroxyazobenzene molecules as the product were confirmed by in situ SERS spectra as well theoretical predictions, showing potential in plasmon driven catalysis and degradation of organic molecules. Plasmon-driven photocatalytic effects generate azo reactions.
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