P-Block Aluminum Single-Atom Catalyst for Electrocatalytic CO Reduction with High Intrinsic Activity.

Atomically dispersed transition metal sites on nitrogen-doped carbon catalysts hold great potential for the electrochemical CO reduction reaction (CORR) to CO due to their encouraging selectivity. However, their intrinsic activity is restricted by the hurdle of the high energy barrier of either *COOH formation or *CO desorption due to the scaling relationship. Herein, we discover a p-block aluminum single-atom catalyst (Al-NC) featuring an Al-N site that enables disentangling this hurdle, which endows a moderate reaction kinetic barrier for *COOH formation and *CO desorption, as validated by in situ attenuated total reflection infrared spectroscopy and theoretical simulations.