Electrocatalysis for alcohol oxidation, ammonia oxidation and organic transformations. From catalyst development to unified organic electrocatalysis

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Already during the 1st funding period of the research unit "UNODE", we proposed to replace the commonly used oxygen evolution reaction in electrolyzers with oxidation reactions in which an available substance is converted to a value-added product. The overall objective will remain the investigation of electrocatalyst-modified electrodes for unusual anode reactions. However, the investigated reactions will be extended from glycerol and HMF oxidation to strategies and mechanisms to convert organic reactants to value-added chemicals of industrial relevance with emphasis on selectivity as the most critical parameter of performance. The ultimate goal is a paradigm shift from exchanging electrons at an inert electrode interface with organic reactions invoking chemical follow-up reactions in the solution to specific adsorption of organic molecules on catalyst surfaces and electron transfer in the adsorbed state. In case of success, this approach will allow tuning selectivity not only with the applied potential/current, the electrolyte, and concentrations but also by the interaction with catalyst materials. This concept will be of utmost importance for the electrification of organic synthesis processes. Additionally, the electrooxidation of NH3 to NO, nitride, and nitrate in aqueous solution, a new field of supposedly significant impact, will be explored. Synthesis strategies for new catalyst materials, specifically multinary elements complex solid solutions (high-entropy materials), will be developed keeping scalability in mind. The obtained electrocatalysts will be immobilized on stable electrode substrates like Ni foam or carbon cloth and will be evaluated regarding activity, stability and selectivity in the previously developed small flow-through electrolyzer cell for glycerol oxidation, organo-electrosynthesis and NH3 oxidation. The catalyst-modified electrodes will be used by the partners in the consortium and the obtained results will be supported by mechanistic insights from ATR-FTIR spectroelectrochemistry.