Simultaneous Achieving of High Faradaic Efficiency and CO Partial Current Density for CO2 Reduction via Robust, Noble‐Metal‐Free Zn Nanosheets with Favorable Adsorption Energy

Abstract Electrocatalytic CO 2 reduction to fuels is considered a promising strategy for the sustainable carbon cycle. However, the improvement of the catalytic performance of CO 2 electrocatalysts still poses many challenges, especially achieving the large partial current density of product and high faradaic efficiency simultaneously, which are essential for future applications of the electrochemical CO 2 reduction reaction. In response, herein, an in situ porous Zn catalyst is prepared and exhibits high faradaic efficiency and large CO partial current density at the same time, benefiting from the porous architecture with increased exposure and accessibility of active sites. Furthermore, density functional theory calculations demonstrate that the high faradaic efficiency is attributed to the favorable adsorption energy of the key intermediate, which promotes CO 2 electroreduction to CO.