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Abstract Renewable‐electricity‐powered electrocatalytic CO 2 reduction reactions (CO 2 RR) have been identified as an emerging technology to address the issue of rising CO 2 emissions in the atmosphere. While the CO 2 RR has been demonstrated to be technically feasible, further improvements in catalyst performance through active sites engineering are a prerequisite to accelerate its commercial feasibility for utilization in large CO 2 ‐emitting industrial sources. Over the years, the improved understanding of the interaction of CO 2 with the active sites has allowed superior catalyst design and subsequent attainment of prominent CO 2 RR activity in literature. This review tracks the evolution of the understanding of CO 2 RR active sites on different electrocatalysts such as metals, metal‐oxides, single atoms, metal‐carbon, and subsequently metal‐free carbon‐based catalysts. Despite the tremendous research efforts in the field, many scientific questions on the role of various active sites in governing CO 2 RR activity, selectivity, stability, and pathways are still unanswered. These gaps in knowledge are highlighted and a discussion is set forth on the merits of utilizing advanced in‐situ and operando characterization techniques and machine learning (ML). Using this technique, the underlying mechanisms can be discerned, and as a result new strategies for designing active sites may be uncovered. Finally, this review advocates an interdisciplinary approach to discover and design CO 2 RR active sites (rather than focusing merely on catalyst activity) in a bid to stimulate practical research for industrial application.
Daiyan et al. (Wed,) studied this question.