Defect and interface engineering for promoting electrocatalytic N-integrated CO2 co-reduction

Current industrial manufacturing producing chemicals and fertilizers usually requires harsh conditions with high energy consumption, and is thus a major contributor to global carbon dioxide (CO2) emissions. With the increasing demand for sustainability, the scientific researchers are endeavoring to develop efficient carbon-neutral and nitrogen-cycle strategies that utilize sustainable energy storage and conversion technologies. In this context, electrocatalytic coupling of CO2 and nitrogenous species (such as nitrogen, ammonia, nitrate, and nitrite) to high-value-added chemicals and fuels with rationally designed electrocatalysts is a promising strategy to restore the imbalanced carbon neutrality and nitrogen cycle. However, despite considerable breakthrough in recent years, the electrocatalytic N-integrated CO2 co-reduction still suffers from the unsatisfactory activity and selectivity, as well as the ambiguous C-N coupling mechanisms. In this review, we summarize the recent progress on defect and interface engineering strategies to design highly efficient electrocatalysts for electrochemical C-N coupling. Especially, the structure-activity relationships between defect/interface engineering and electrochemical performance are systematically illustrated using representative experimental data and theoretical calculations. Moreover, the major challenge and future development direction of defect and interface engineering are also proposed. It is hoped that this work can provide guidance and enlightenment for the development of electrochemical C-N coupling technology. (c) 2024, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.