Efficient electroreduction of CO₂to C₂₊products on CeO₂modified CuO

Abstract

Electrocatalytic reduction of CO₂ into multicarbon (C₂₊) products powered by renewable electricity offers one promising method for CO₂ utilization and promotes the storage of renewable energy under an ambient environment. However, there is still a dilemma in the manufacture of valuable C₂₊ products between balancing selectivity and activity. In this work, cerium oxides were combined with CuO (CeO₂/CuO) and showed an outstanding catalytic performance for C₂₊ products. The faradaic efficiency of the C₂₊ products could reach 75.2% with a current density of 1.21 A cm^-2. <i>In situ</i> experiments and density functional theory (DFT) calculations demonstrated that the interface between CeO₂ and Cu and the subsurface Cu₂O coexisted in CeO₂/CuO during CO₂RR and two competing pathways for C-C coupling were promoted separately, of which hydrogenation of *CO to *CHO is energetically favoured. In addition, the introduction of CeO₂ also enhanced water activation, which could accelerate the formation rate of *CHO. Thus, the selectivity and activity for C₂₊ products over CeO₂/CuO can be improved simultaneously.