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Functionalized Silicon Electrodes in Electrochemistry.
Annual Review of Analytical Chemistry ( IF 5.9 ) Pub Date : 2020-06-12 , DOI: 10.1146/annurev-anchem-091619-092506
Vinicius R Gonçales 1 , Jiaxin Lian 1 , Shreedhar Gautam 1 , Richard D Tilley 1 , J Justin Gooding 1
Affiliation  

Avoiding the growth of SiOx has been an enduring task for the use of silicon as an electrode material in dynamic electrochemistry. This is because electrochemical assays become unstable when the SiOx levels change during measurements. Moreover, the silicon electrode can be completely passivated for electron transfer if a thick layer of insulating SiOx grows on the surface. As such, the field of silicon electrochemistry was mainly developed by electron-transfer studies in nonaqueous electrolytes and by applications employing SiOx-passivated silicon-electrodes where no DC currents are required to cross the electrode/electrolyte interface. A solution to this challenge began by functionalizing Si–H electrodes with monolayers based on Si–O–Si linkages. These monolayers have proven very efficient to avoid SiOx formation but are not stable for a long-term operation in aqueous electrolytes due to hydrolysis. It was only with the development of self-assembled monolayers based on Si–C linkages that a reliable protection against SiOx formation was achieved, particularly with monolayers based on α,ω-dialkynes. This review discusses in detail how this surface chemistry achieves such protection, the electron-transfer behavior of these monolayer-modified silicon surfaces, and the new opportunities for electrochemical applications in aqueous solution.

中文翻译:


电化学中的功能化硅电极。

对于将硅用作动态电化学中的电极材料,避免SiO x的生长一直是一项艰巨的任务。这是因为当测量过程中SiO x含量变化时,电化学分析变得不稳定。而且,如果绝缘SiO x的厚层在表面上生长,则硅电极可以被完全钝化以进行电子转移。因此,硅电化学领域的发展主要是通过在非水电解质中进行电子转移研究以及通过使用SiO x的应用来进行的。钝化的硅电极,不需要直流电流穿过电极/电解质界面。解决这一挑战的方法是通过基于Si-O-Si键的单层功能化Si-H电极。已证明这些单层非常有效地避免了SiO x的形成,但是由于水解作用,在水性电解质中长期运行不稳定。只有基于Si–C键的自组装单分子膜的开发,才能可靠地保护SiO x尤其是基于α,ω-二炔的单层膜,可以实现形成。本文详细讨论了这种表面化学如何实现这种保护,这些单层改性的硅表面的电子转移行为以及水溶液中电化学应用的新机会。

更新日期:2020-06-12
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