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.