Combined Experimental and Multi-Scale Modeling Approach to the Development of Electrocatalysts with Improved CO_2 Reduction Activity Towards C_(2+) Alcohols

摘要

The development of high performance catalysts for the production of fuels and chemical in electrochemical reactors call for a profound understanding of the processes occurring at multiple scales and emphasizes the importance of broadening catalyst design principles beyond the transition state theory to include fundamentals of mass and charge transport. The selective production of C_(2+) alcohols on cooper electrodes requires that multiple thermo-chemical and electro-chemical steps occur at the electrode-electrolyte interface at rates faster than those for the competing hydrogen and hydrocarbon evolution reactions. At the same time, the rates of most of these reactions are not only dependent on the intrinsic activity of copper, but are highly affected by the local environments that determine the rate of regeneration of reaction intermediates, the availability of proton sources for proton-electron coupled steps and the extend of the thermodynamic driving force for the formation of each of the multiple products.