Single-Product Faradaic Efficiency for Electrocatalytic of CO to CO at Current Density Larger than 1.2 A cm in Neutral Aqueous Solution by a Single-Atom Nanozyme.

Electroreduction of CO to CO is a promising approach for the cycling use of CO , while it still suffers from impractical current density and durability. Here we report a single-atom nanozyme (Ni-N -C) that achieves industrial-scale performance for CO -to-CO conversion with a Faradaic efficiency (FE) exceeded 97 % over -0.8--2.4 V vs. RHE. The current density at -2.4 V vs. RHE reached a maximum of 1.23 A cm (turnover frequency of 69.7 s ) with an FE of 99.6 %. No obvious degradation was observed over 100 hours of continuous operation. Compared with the planar Ni-N site, the square-pyramidal Ni-N site has an increase and a decrease in the and d orbital energy levels, respectively, as revealed by density functional theory calculations. Thus, the Ni-N catalytic site is more superior to activate CO molecule and reduce the energy barriers as well as promote the CO desorption, thus boosting the kinetic activation process and catalytic activity.