High‐Performing Atomic Electrocatalyst for Chlorine Evolution Reaction

Abstract Electrocatalysts facilitating chlorine evolution reaction (ClER) play a vital role in chlor–alkali industries. Owing to a huge amount of chlorine consumed worldwide, inexpensive high‐performing catalysts for Cl2 production are highly demanded. Here, a superb ClER catalyst fabricated through uniform dispersion of Pt single atoms (SAs) in C2N2 moieties of N‐doped graphene (denoted as Pt‐1) is presented, which demonstrates near 100% exclusive ClER selectivity, long‐term durability, extraordinary Cl2 production rate (3500 mmol h−1 gPt−1), and >140 000‐fold increased mass activity over industrial electrodes in acidic medium. Excitingly, at the typical chlor–alkali industries’ operating temperature (80 °C), Pt‐1 supported on carbon paper electrode requires a near thermoneutral ultralow overpotential of 5 mV at 1 mA cm−2 current density to initiate the ClER, consistent with the predicted density functional theory (DFT) calculations. Altogether these results show the promising electrocatalyst of Pt‐1 toward ClER.