Catalytic processes are implicated in everyday applications related to energy production, agriculture, medicine, and various other fields. Many catalytic processes are sufficiently complex, meaning experimental measurements cannot be used to accurately quantify various details of the reaction pathways and kinetics. Sophisticated computational models of chemical catalysis are therefore necessary to both understand and predict the outcomes of these reactions, and to inform future catalyst development. One such example of catalysis can be found in the reduction of carbon dioxide into useful two-carbon chemicals using copper electrodes as the catalyst. This system is of interest as a potential target for efficient production of energy and chemical feedstocks which also provide a viable pathway to carbon recycling. We investigate the myriad scientific difficulties posed by this system while developing computational tools which can also be transferred to the study other catalytic systems of chemical and societal interest.