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 similar to 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.