Layer-Stacked Zn with Abundant Corners for Selective CO₂ Electroreduction to CO

Electric-driven CO₂ reduction offers a promising strategy for CO₂ conversion into valuable chemicals and fuels. However, developing low cost and efficient catalysts is still a challenge. Although earth-abundant Zn with the capability of converting CO₂ to CO is considered to be one of the promising materials, the low selectivity and stability of Zn catalyst limit its practical applications in CO₂ reduction. Herein, we report a highly selective and stable layer-stacked Zn catalyst prepared by an efficient and facile electrochemical method for CO₂ reduction to CO. The layer-stacked Zn can produce CO with more than 90% Faradaic efficiency at an overpotential of 0.9 V. Notably, the layer-stacked Zn maintained ∼90% CO selectivity in CO₂ electrolysis for more than 70 h, which significantly surpasses the durability of the reported Zn-based catalysts to date. In addition, after prolonged CO₂ reduction, the robust catalytic performance of layer-stacked Zn can be recovered repeatedly by the simple electrochemical method, which may be linked to the maintained layer-stacked structure even after multiple reactivations. Further analysis suggests that while abundant low-coordinated sites (corners and edges) can be created on layer-stacked Zn, the enhanced catalytic performance in CO₂ reduction is mainly correlated with the created corners instead of edges, owing to that corners not only improve the intrinsic CO₂ reduction activity but also inhibit H₂ evolution simultaneously.