Engineering Organic Molecule–Copper Interfaces for Selective C2+ Production in CO2 Electroreduction

The electrochemical carbon dioxide reduction reaction (CO2RR) serves as a crucial bridge linking CO2 utilization, renewable electricity, and chemical production. Driven by intermittent clean energy sources such as wind and solar power, it can convert CO2 into high-value chemicals and fuels under ambient temperature and pressure and is therefore regarded as a promising route for artificial carbon recycling and sustainable manufacturing of chemicals. Copper (Cu) is currently the only metal capable of deep CO2 reduction to multicarbon (C2+) products in aqueous electrolytes. However, the product selectivity and catalytic stability of Cu-based catalysts still demand further improvement. In recent years, organic molecule modification strategies have emerged as an effective approach to optimizing Cu-based CO2RR catalysts and have attracted increasing attention. Organic molecules can form favorable organic-inorganic interfaces with the Cu surface through various interactions, promoting the formation of C2+ products via multiple mechanisms. This review summarizes the recent advances in constructing efficient Cu-based catalysts for CO2RR through organic molecule modification strategy. By reviewing the fundamentals for C2+ formation over Cu-based catalysts, this paper first sorts out the interfacial structures and interactions between the organic molecules and Cu surfaces. Then, the underlying mechanisms of the well-defined organic molecule–Cu interfaces for enhanced CO2RR performance are discussed, including the modulation of surface charge and oxidation state of Cu, the tuning of the local microenvironments, and the synergies for activating CO2 or stabilizing key intermediates. Furthermore, current research challenges and future prospects associated with the engineering of organic molecule–Cu interfaces are outlined, aiming to provide insights for the rational design of Cu-based catalysts for CO2RR.