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highly desirable. Ideally, these techniques would be compatible with industrially relevant reaction conditions (high current densities, high pH, light illumination, gas-diffusion electrode). These techniques would not only shed light on questions related to the reaction mech- anism through the identification of reaction intermediates such as those illustrated in Figure 2.5, but they would also provide a route to correlate activity and selectivity with material structure and com- position [8–10]. Figure 2.5: Key reaction mechanism questions in CO2RR. Reproduced with permission from [5]. Simultaneously, fundamental understanding of the CO2RR under relevant process conditions will be aided by the design of well-defined and well-characterized electrode architectures (e.g. pre- pared by colloidal or solvothermal routes, electrochemistry or nano-lithography) for optimal control over the interplay between surface electrocatalysis and chemical potential gradients existing in the electrolyte. 2.3.3 Advancing fundamental understanding of CO2RR: theoretical methods A core cross-cutting goal is the advancement of existing theo- retical methods in concert with the in situ and operando ex- perimental techniques described above. Advances are needed in the realistic ab initio modeling of electrode-electrolyte interfaces (including explicit solvent, electrolyte ions, and electrolyte-driven surface reconstructions) as well as in the coupling of atomic-scale mechanistic insights to reaction ki- netics and mass transport phenomena at longer length scales with the ultimate goal of elucidating critical activity and selectivity descriptors for high-value products (Figure 2.6). Mass and heat transport phenomena and water management should be explored with larger-scale, continuum models of porous electrodes and full cell and stack-level models. Validation of theoret- ical models will crucially depend on high-quality experimental data on well-characterized systems 23 Figure 2.6: Descriptor-based approach to cat- alyst discovery. Adapted with permission from [11].PDF Image | sustainable production of fuels and chemicals
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