In-situ characterization technologies and theoretical calculations in carbon dioxide reduction: In-depth understanding of reaction mechanisms and rational design of electrocatalysts

Abstract

The electrochemical reduction of carbon dioxide (CO₂RR) enables the transformation of CO₂ into valuable chemicals and fuels using renewable electricity, offering a crucial pathway toward addressing the global energy crisis and achieving carbon neutrality. Traditional theories of catalyst stability and activity can be complicated by the dynamic reorganization of catalysts under operating circumstances, which is a significant issue in this subject. To address this, advanced in-situ technologies and theoretical calculations reveal the dynamic evolution of catalysts and intermediates during CO₂RR. In this review, we systematically analyze the integration of in-situ characterization technologies with theoretical calculations which underscores their critical role in understanding the mechanisms of CO₂RR and facilitating the design of efficient catalysts. Subsequently, we systematically summarize the recent advances in-situ studies and theoretical calculations on probing the reaction mechanisms during the CO₂RR. In this perspective, we can deepen our understanding of reaction mechanisms by combining advanced real-time monitoring and theoretical calculation approaches that relate the dynamic evolution of variable response environments to theoretical evolutionary models. Finally, this review seeks to enhance the understanding of reaction mechanisms and provide guidance for the rational design of efficient catalysts through the integration of in-situ characterization techniques and theoretical calculations.