2,3-Dimercaptosuccinic Acid Adsorbed on Silver Surface Using Electrochemical SERS and Reduction Method

LIU Wen-han; YUAN Rong-hui; TENG Yuan-jie

doi:10.3788/fgxb20143509.1124

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2,3-Dimercaptosuccinic Acid Adsorbed on Silver Surface Using Electrochemical SERS and Reduction Method

更新时间：2020-08-12

- 2,3-Dimercaptosuccinic Acid Adsorbed on Silver Surface Using Electrochemical SERS and Reduction Method
- Chinese Journal of Luminescence Vol. 35, Issue 9, Pages: 1124-1130(2014)
- 作者机构：
  
  浙江工业大学化学工程学院绿色化学合成技术国家重点实验室培育基地,浙江杭州,310032
- 作者简介：
- 基金信息：
- DOI：10.3788/fgxb20143509.1124
  CLC： O657
- Received：14 April 2014，
  
  Revised：08 July 2014，
  
  Published：03 September 2014
- 稿件说明：
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刘文涵, 袁荣辉, 滕渊洁. 2,3-二巯基丁二酸在银表面的电化学表面增强拉曼光谱及电还原特性[J]. 发光学报, 2014,35(9): 1124-1130

LIU Wen-han, YUAN Rong-hui, TENG Yuan-jie. 2,3-Dimercaptosuccinic Acid Adsorbed on Silver Surface Using Electrochemical SERS and Reduction Method[J]. Chinese Journal of Luminescence, 2014,35(9): 1124-1130
刘文涵, 袁荣辉, 滕渊洁. 2,3-二巯基丁二酸在银表面的电化学表面增强拉曼光谱及电还原特性[J]. 发光学报, 2014,35(9): 1124-1130 DOI： 10.3788/fgxb20143509.1124.

LIU Wen-han, YUAN Rong-hui, TENG Yuan-jie. 2,3-Dimercaptosuccinic Acid Adsorbed on Silver Surface Using Electrochemical SERS and Reduction Method[J]. Chinese Journal of Luminescence, 2014,35(9): 1124-1130 DOI： 10.3788/fgxb20143509.1124.

摘要

采用原位电化学表面增强拉曼光谱（EC-SERS）和电化学还原方法，研究了内消旋-2，3-二巯基丁二酸（DMSA）在活化的银电极上的吸附行为。通过模型分子DMSA进行结构优化的密度泛函理论计算，得到了理论拉曼光谱。在相同的DMSA自组装时间条件下，其在Ag电极表面的覆盖度倒数与溶液浓度倒数成线性关系，说明DMSA单分子层在活性Ag表面的化学吸附遵循Langmuir等温吸附模型。在酸性介质中，DMSA浸置自组装50 min后，SERS峰强趋于稳定，达到了该浓度下的动态吸附平衡。EC-SERS信号随施加电位的负移逐渐减弱至基本消失。通过计算探针分子DMSA在不同电位下的增强因子（EF），指出较负电位下存在着还原/脱附作用，使得Ag表面的拉曼活性降低，尤其在小于-0.4 V的还原电位时，增强因子显著减小。

Abstract

Meso-2

3-dimercaptosuccinic acid (DMSA) assembled on activated silver electrode was analyzed by

in-situ

electrochemical surface-enhanced Raman scattering (EC-SERS) and electro-reduction. Density functional theory calculations had been carried to obtain the molecular optimization structure and theoretical Raman spectra. The reduction peak of S-Ag derived from DMSA on activated Ag was at -0.4 V (

vs.

SCE). Under the same self-assembly time

a linear regression fit between the reciprocals of surface coverage and solution concentration was investigated by using linear sweep voltammetry (LSV)

which indicating that DMSA monolayer adsorbed on surfactivity Ag obeys the Langmuir isothermal adsorption equation. The maximum surface coverage of DMSA on Ag electrode from LSV was 5.4110

-10

molcm

-2

and the adsorption coefficient was 3.7410

Lmol

-1

. The stabilized SERS signals of target concentrations were detected after 50 min for an adsorption equilibrium at acid condition. It was found that EC-SERS intensities became weaker

and the peaks eventually disappeared when the potential was negatively shifted. A single molecule area for DMSA adsorbed on Ag substrates was 0.389 nm

and the effective depth of 785.18 nm laser beam irradiated to the ideal solution focusing surface was 3.461 m. Furthermore

the performance change of silver electrode was proposed by calculating enhancement factor (EF) at different potentials. As a result of reduction/desorption behavior of DMSA at relatively negative potentials

EF of probe molecule on silver was significantly reduced and the Raman enhanced activity was lost especially the potential value was less than -0.4 V.

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Keywords

references

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