Catalyst–electrolyte interface chemistry for electrochemical CO₂ reduction

Abstract

This review article provides the recent progress in the electrochemical CO2 reduction reaction by understanding and tuning catalyst–electrolyte interfaces.

Quasi-graphitic carbon shell-induced Cu confinement promotes electrocatalytic CO2 reduction toward C2+ products

“…To elucidate the increased C 2 H 4 selectivity of B-doped and N-doped Cu, the average adsorption energy of two CO molecules and the free energy changes of the C-C coupling reaction for pristine Cu, Cu (B), and Cu (N) were calculated. Since the dimerization of two CO* on the Cu surface to form OCCO* is the rate-determining step in the C 2 H 4 formation pathway [35][36][37][38][39] , the free energy change of CO* dimerization was used as the descriptor of C 2 H 4 productivity. Figure 5c shows the plot of CO* dimerization energy as a function of the average CO adsorption energy of pristine Cu, Cu (B), and Cu (N).…”

Effect of Electrolyte Composition and Concentration on Pulsed Potential Electrochemical CO2 Reduction

“…Recognizing that improvements in electrocatalytic processes rely on better control over the solid‐liquid interface, increasing efforts have been directed at understanding the ‘soft’ side of the solid‐electrolyte interface, namely the chemistry of adsorbed species and the electrolyte environment that exist near the catalytic active sites ( i. e ., the ‘hard’ side) [11–18] . Previous studies have illustrated that the concentration and composition of the electrolyte impacts the eCO 2 R pathways in two important ways [19] .…”

Manipulating Interfaces of Electrocatalysts Down to Atomic Scales: Fundamentals, Strategies, and Electrocatalytic Applications

“…In addition, interfaces also involve in servicing catalytic surfaces, where the atomic and electronic structures at the solid–liquid–gas interfaces govern the kinetics of binding and release of reactant molecules from surface atoms, although there are a relatively few studies, due to the huge difficulties on operando detecting and locating the absorbed gas molecules for studying the catalytic reaction mechanisms. [ 149,150 ] An environmental TEM was applied to image the adsorbed CO molecule on the surface of Au NP under CO/air. [ 151 ] It was observed that CO molecules render a transformation from a (100) surface facet to (100)‐hex facet on Au NPs.…”

“…The combination of experimental observations and computational studies indicated that CO molecule prefers to adsorb on the produced (100)‐hex facet and leads to a higher reaction rate. Since then, gas pressure, [ 152 ] local reactant concentration, and pH value, [ 150 ] electric double layer between catalyst surface and electrolyte, [ 153 ] production release/transportation [ 5 ] have demonstrated a non‐negligible impact on the overall catalytic activity, selectivity, and stability, although some of the conclusions are relatively empirical and suffer from insufficient evidences of direction observation. A careful selection and improvement of the in situ/operando techniques prior to experiments is crucial for illuminating the effects of the above factors in the multiphase interfaces on catalytic properties.…”