Rational design of highly efficient carbon-based materials for electrochemical CO2 reduction reaction

The rational design of nanostructured carbon-based materials has emerged as a crucial research area due to their significant impact on the electrochemical CO2 reduction reaction (CO2RR). This process converts carbon dioxide gas into value-added chemical products, such as formate, CO, or other fuels. A variety of carbon-based electrocatalysts, including non-metallic doped carbon materials (e.g., N-doped carbon nanofibers, N-doped diamonds), metal-macroring materials (e.g., metal-porphyrins, metal-phthalocyanines, and metal-corroles), and M−N−C typical materials (Fe-N-C, Co-N-C, and Ni-N-C), have exhibited promising results as efficient catalysts for CO2RR. In this review, we discuss recent advances in the rational design of nanostructured carbon-based materials for CO2RR using both experimental and theoretical approaches. These include the design and synthesis of morphology-tunable carbon-based materials and heteroatom doping. Furthermore, we delve into the catalytic mechanisms of CO2 electrochemical reduction on carbon-based materials, encompassing surface reactions, geometric effects, and electronic effects. These findings contribute to the development of intrinsic descriptors for establishing the volcano relationship with catalytic performance. Finally, we highlight the challenges and future directions in the field of CO2RR, stressing the importance of gaining a better understanding of the complex structure–function relationships in carbon-based materials and the development of efficient and sustainable CO2RR processes for industrial applications.