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多晶金表面上单巯基十一烷酸自组装单层。

Self-Assembled Monolayer of Monomercaptoundecahydro--dodecaborate on a Polycrystalline Gold Surface.

机构信息

Centro de Investigación y Desarrollo Tecnológico en Electroquímica S.C, Parque Tecnológico Querétaro, Querétaro 76703, Mexico.

División de Química y Energías Renovables, Universidad Tecnológica de San Juan del Río, Avenida La Palma No. 125 Vista Hermosa, Querétaro 76800, Mexico.

出版信息

Molecules. 2022 Apr 12;27(8):2496. doi: 10.3390/molecules27082496.

DOI:10.3390/molecules27082496
PMID:35458692
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9026543/
Abstract

In this work, we present an electrochemical study of the boron cage monomercaptoundecahydro--dodecaborate [BHSH] in solution and in a self-assembled monolayer over a polycrystalline gold electrode. Cyclic voltammetry of the anion [BHSH] in solution showed a shift in the peak potentials related to the redox processes of gold hydroxides, which evidences the interaction between the boron cage and the gold surface. For an Au electrode modified with the anion [BHSH], cyclic voltammetry response of the probe Fe(CN)/Fe(CN) showed a ΔEp value typical for a surface modification. Electrochemical impedance spectroscopy presented and C values related to the formation of a self-assembled monolayer (SAM). A comparison of electrochemical responses of a modified electrode with thioglycolic acid (TGA) reveals that the boron cage [BHSH] diminishes the actives sites over the Au surface due to the steric effects. Differential capacitance measurements for bare gold electrode and those modified with [BHSH] and (TGA), indicate that bulky thiols enhance charge accumulation at the electrode-solution interface. In addition to electrochemical experiments, DFT calculations and surface plasmon resonance measurements (SPR) were carried out to obtain quantum chemical descriptors and to evaluate the molecular length and the dielectric constant of the Boron cage. From SPR experiments, the adsorption kinetics of [BHSH] were studied. The data fit for a Langmuir kinetic equation, typical for the formation of a monolayer.

摘要

在这项工作中，我们对硼笼单巯基十一氢-十二硼酸盐 [BHSH] 在溶液中和在多晶金电极上自组装单层中的电化学行为进行了研究。阴离子 [BHSH] 在溶液中的循环伏安法显示出与金氢氧化物氧化还原过程相关的峰电位的移动，这证明了硼笼与金表面之间的相互作用。对于用阴离子 [BHSH] 修饰的 Au 电极，探针 Fe(CN)/Fe(CN) 的循环伏安响应显示出典型的表面修饰的ΔEp 值。电化学阻抗谱呈现出与自组装单层（SAM）形成相关的 和 C 值。修饰电极与巯基乙酸（TGA）的电化学响应的比较表明，由于空间位阻效应，硼笼 [BHSH] 减少了 Au 表面上的活性位点。对于裸金电极和用 [BHSH] 和 (TGA) 修饰的电极的差分电容测量表明，体积庞大的硫醇增强了在电极-溶液界面处的电荷积累。除了电化学实验外，还进行了密度泛函理论计算和表面等离子体共振测量（SPR），以获得量子化学描述符，并评估硼笼的分子长度和介电常数。从 SPR 实验中，研究了 [BHSH] 的吸附动力学。数据适合 Langmuir 动力学方程，这是单层形成的典型特征。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d29fea88eb84/molecules-27-02496-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/9559df44f551/molecules-27-02496-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/ac3222b9e458/molecules-27-02496-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/be1ebbf6f82a/molecules-27-02496-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d647704a0cfe/molecules-27-02496-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/22d25ae29ba1/molecules-27-02496-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/ef90d4e301e7/molecules-27-02496-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/117a9cad6da0/molecules-27-02496-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d9df9a744072/molecules-27-02496-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/548b6d47c367/molecules-27-02496-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d29fea88eb84/molecules-27-02496-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/9559df44f551/molecules-27-02496-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/ac3222b9e458/molecules-27-02496-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/be1ebbf6f82a/molecules-27-02496-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d647704a0cfe/molecules-27-02496-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/22d25ae29ba1/molecules-27-02496-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/ef90d4e301e7/molecules-27-02496-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/117a9cad6da0/molecules-27-02496-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d9df9a744072/molecules-27-02496-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/548b6d47c367/molecules-27-02496-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d7e1/9026543/d29fea88eb84/molecules-27-02496-g007.jpg

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