Boosting multi-carbon products selectivity of carbon dioxide reduction via bifunctional cyclodextrin-modification on...

Electrochemical carbon dioxide reduction to multi-carbon (C₂₊) products presents a significant opportunity for converting greenhouse gases into valuable fuels and feedstocks. The development of highly active and stable catalysts remains a critical challenge. In this study, we report the design and synthesis of cyclodextrin-modified Cu/Cu₂O electrocatalysts, which exhibit remarkable efficiency in driving the CO₂ electroreduction process towards C₂₊ products. Our optimized catalyst achieves a C₂₊ Faradaic efficiency exceeding 50 % at a high current density of over 200 mA cm^-2. Experimental findings, supported by density functional theory (DFT) calculations, reveal that cyclodextrin plays a dual role in stabilizing Cu⁺ and increasing the surface density of hydroxyl radicals. This dual function greatly benefits for enhancing *CO intermediate adsorption and promotes *CHO formation, thereby facilitating the crucial dimerization step for the formation of C₂₊ products. This work provides valuable insights into the development of highly active and selective electrocatalysts by carefully tuning the local catalytic environment, potentially opening new avenues for functionalizing electrocatalysts for future research in this area.