Elahi, A; (2014) Plasma electrochemistry: electron transfer at the solid/gas interface. Doctoral thesis , UCL (University College London).

Abstract

The ability to control redox reactions at the solid/gas interface is demonstrated for the first time, by considering gaseous flame plasma as an electrolyte. An innovative method to perform potentio-dynamic experiments in a liquid-free electrochemical system using flame plasma is described. This novel approach can help apply the well-established foundations of electrochemistry developed almost exclusively in liquids, to the new context of gas plasma. There are limited examples using plasmas as media to study redox reactions but no examples of voltammetry in the gas phase at true solid/gas interfaces. Successful electrochemical measurements are illustrated by doping the flame plasma with both inorganic and organic species, and recording distinct faradaic peaks at defined potentials in cyclic voltammograms. The sensitivity of the system is highlighted by the ability to distinguish between several amino acids, pinpointing specific functional groups. The most significant innovation responsible for these measurements is the development of a reference electrode able to function at temperatures over 1300 K. Extensive assessment of several materials has enabled the development and optimisation of a reference electrode, allowing an extension of the potential window to 10 V; an unprecedented value in electrochemistry. After careful experimentation and appropriate control experiments, the features observed are confirmed as specific reduction processes at the solid/gas interface. Undoubtedly, and perhaps expectedly, there are significant departures from the analogous process in condensed phases. The physical origin of these electrochemical signals is discussed and a framework of interpretation upon which a full mechanistic understanding can be based is provided. The scope of commercial and academic impact is extensive. Liquid-free electrochemistry presents access to a plethora of redox reactions, which lie outside potential limits defined by liquids. The prospect of new redox chemistries will enable new technological applications such as electrodeposition and electroanalysis, which have significant economic and environmental benefits.

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