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Chlorine evolution reaction (CER) is a critical anode reaction in chlor-alkali electrolysis. Although precious metal-based mixed metal oxides (MMOs) have been widely used as CER catalysts, they suffer from the concomitant generation of oxygen during the CER. Herein, we demonstrate that atomically dispersed Pt−N
4
sites doped on a carbon nanotube (Pt
1
/CNT) can catalyse the CER with excellent activity and selectivity. The Pt
1
/CNT catalyst shows superior CER activity to a Pt nanoparticle-based catalyst and a commercial Ru/Ir-based MMO catalyst. Notably, Pt
1
/CNT exhibits near 100% CER selectivity even in acidic media, with low Cl
−
concentrations (0.1 M), as well as in neutral media, whereas the MMO catalyst shows substantially lower CER selectivity. In situ electrochemical X-ray absorption spectroscopy reveals the direct adsorption of Cl
−
on Pt−N
4
sites during the CER. Density functional theory calculations suggest the PtN
4
C
12
site as the most plausible active site structure for the CER.
Chlorine evolution reaction (CER) is a key electrochemical reaction for chemical, pulp, and paper industries, and water treatments. Here, the authors report that an atomically dispersed Pt−N
4
site can catalyse CER with high activity and selectivity under a wide range of Cl
–
concentrations and pH.