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Curvature‐induced Zn 3d Electron Return on Zn−N4 Single‐atom Carbon Nanofibers for Boosting Electroreduction of CO2

The electrochemical CO2 reduction to desired chemical feedstocks is of importance, yet it is still challenging to obtain high production selectivity with low overpotential at a current density surpassing the industry benchmark of 100 mA cm−2. Herein, we constructed a low‐cost Zn single‐atom anchored on curved N‐doped carbon nanofibers (Zn SAs/N−C) by a facile noncovalent self‐assembly approach. At a low overpotential of only 330 mV, the Zn SAs/N−C exhibited simultaneously both a high current density up to 121.5 mA cm−2 and a CO FE of 94.7 %, superior to the previous reports. Experiments and DFT calculations revealed that the Zn atoms in Zn−N4 acted as the active sites, while adjacent pyridine‐N coupled with Zn−N4 could synergistically decrease the free energy barrier for intermediate *COOH formation. Importantly, the curvature of catalyst induced Zn 3d electrons that were bound to the Zn−N bonds to return to Zn atom, thereby leading to an increase in electron density of Zn and accelerating CO2 electroreduction to CO.