In Situ/Operando Characterization Techniques of Electrochemical CO2 Reduction

Electrocatalytic conversion of carbon dioxide to valuable chemicals and fuels driven by renewable energy plays a crucial role in achieving netzero carbon emissions. Understanding the structure-activity relationship and the reaction mechanism is significant for tuning electrocatalyst selectivity. Therefore, characterizing catalyst dynamic evolution and reaction intermediates under reaction conditions is necessary but still challenging. We first summarize the most recent progress in mechanistic understanding of heterogeneousCO(2)/CO reduction using in situ/operando techniques, including surface-enhanced vibrational spectroscopies, X-ray- and electronbased techniques, and mass spectroscopy, along with discussing remaining limitations.We then offer insights and perspectives to accelerate the future development of in situ/operando techniques.

Automated summary

Electrocatalytic conversion of carbon dioxide to valuable chemicals and fuels driven by renewable energy is vital for achieving net-zero carbon emissions. Understanding the structure-activity relationship and reaction mechanism is crucial for improving electrocatalyst selectivity. However, characterizing catalyst dynamic evolution and reaction intermediates under reaction conditions remains challenging. This article provides a summary of recent progress in mechanistic understanding of heterogeneous CO(2)/CO reduction using in situ/operando techniques, along with insights and perspectives to accelerate future development of these techniques.