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Surface‐enhanced Raman spectroscopic investigation on surface plasmon resonance and electrochemical catalysis on surface coupling reaction of pyridine at Au/TiO2 junction electrodes
Journal of Raman Spectroscopy ( IF 2.4 ) Pub Date : 2020-09-02 , DOI: 10.1002/jrs.5982 Jing Zhao 1 , Chenjie Zhang 1 , Yanhua Lu 1 , Qian Wu 1 , Yaxian Yuan 1 , Minmin Xu 1 , Jianlin Yao 1
Journal of Raman Spectroscopy ( IF 2.4 ) Pub Date : 2020-09-02 , DOI: 10.1002/jrs.5982 Jing Zhao 1 , Chenjie Zhang 1 , Yanhua Lu 1 , Qian Wu 1 , Yaxian Yuan 1 , Minmin Xu 1 , Jianlin Yao 1
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Surface plasmon resonance (SPR) is proved to induce catalysis and generate surface‐enhanced Raman scattering (SERS) effect. However, it remained a significant challenge in developing the efficient approach to in situ monitor the surface reaction and extending the SPR catalysis as a general approach in surface organic synthesis, especially for the C–C coupling. Herein, SPR from the Au nanoparticles played the bifunctional roles to induce the surface catalysis reaction and enhance the surface Raman signal. The SPR and electrochemical potential became two necessary external fields for the surface coupling reaction to produce 2,2′‐bipyridine, which was explored by SERS. The adsorbed pyridine molecules underwent a dimerization to produce cis‐configuration 2,2′‐bipyridine at the −0.7 V by appropriate laser irradiation. It demonstrated that the surface dimerization efficiency was critically dependent on the laser, potential, the solution properties, and so on. It was improved significantly at the relative negative potential and by 638 nm laser. The solvent with oxygen facilitated the surface dimerization reaction. Pd nanoparticles played the assistant role to capture the hydrogen released from the pyridine to accelerate the breaking of C–H bond and C–C coupling reaction. The surface reaction mechanisms involved the electrons transfer from Au to TiO2 and injected electron delivery to α‐H of pyridine for activation and the formation of carbon free radicals and coupling together to produce 2,2′‐bipyridine. This strategy is expected to further provide an alternative approach to the C–C coupling reaction and to extend the SPR and electrochemical catalysis to a practical application in surface modification as well as organic synthesis, and SERS is anticipated to be a promising in situ technique for the surface chemical reaction.
中文翻译：
Au / TiO2结电极上吡啶的表面偶合反应的表面等离子体共振和电化学催化的表面增强拉曼光谱研究
已证明表面等离振子共振（SPR）可以诱导催化并产生表面增强拉曼散射（SERS）效应。然而，在开发一种有效的方法来原位监测表面反应和扩展SPR催化作为表面有机合成的通用方法（尤其是对于C–C偶联）时，仍然是一个重大挑战。在此，来自Au纳米颗粒的SPR起着双功能的作用，以诱导表面催化反应并增强表面拉曼信号。SERS探索了SPR和电化学势成为产生2,2'-联吡啶的表面偶联反应的两个必要的外部场。吸附的吡啶分子经过二聚化生成顺式通过适当的激光照射在-0.7 V下配置2,2'-联吡啶。结果表明，表面二聚化效率主要取决于激光，电势，溶液性质等。在638 nm激光下，在相对负电位下它得到了显着改善。带有氧的溶剂促进了表面二聚反应。钯纳米粒子起着辅助作用，捕获从吡啶释放的氢，以加速C–H键的断裂和C–C偶联反应。表面反应机理涉及电子从Au转移到TiO 2以及注入电子传递到α-H吡啶用于活化和形成碳自由基，并偶联在一起产生2,2'-联吡啶。预计该策略将进一步为CC偶联反应提供替代方法，并将SPR和电化学催化扩展到表面改性以及有机合成的实际应用中，并且SERS有望成为一种有前途的原位技术表面化学反应。
更新日期：2020-09-02
中文翻译：
Au / TiO2结电极上吡啶的表面偶合反应的表面等离子体共振和电化学催化的表面增强拉曼光谱研究
已证明表面等离振子共振（SPR）可以诱导催化并产生表面增强拉曼散射（SERS）效应。然而，在开发一种有效的方法来原位监测表面反应和扩展SPR催化作为表面有机合成的通用方法（尤其是对于C–C偶联）时，仍然是一个重大挑战。在此，来自Au纳米颗粒的SPR起着双功能的作用，以诱导表面催化反应并增强表面拉曼信号。SERS探索了SPR和电化学势成为产生2,2'-联吡啶的表面偶联反应的两个必要的外部场。吸附的吡啶分子经过二聚化生成顺式通过适当的激光照射在-0.7 V下配置2,2'-联吡啶。结果表明，表面二聚化效率主要取决于激光，电势，溶液性质等。在638 nm激光下，在相对负电位下它得到了显着改善。带有氧的溶剂促进了表面二聚反应。钯纳米粒子起着辅助作用，捕获从吡啶释放的氢，以加速C–H键的断裂和C–C偶联反应。表面反应机理涉及电子从Au转移到TiO 2以及注入电子传递到α-H吡啶用于活化和形成碳自由基，并偶联在一起产生2,2'-联吡啶。预计该策略将进一步为CC偶联反应提供替代方法，并将SPR和电化学催化扩展到表面改性以及有机合成的实际应用中，并且SERS有望成为一种有前途的原位技术表面化学反应。
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