Atomically dispersed Pt–N4 sites as efficient and selective electrocatalysts for the chlorine evolution reaction

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Abstract
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−N4sites doped on a carbon nanotube (Pt1/CNT) can catalyse the CER with excellent activity and selectivity. The Pt1/CNT catalyst shows superior CER activity to a Pt nanoparticle-based catalyst and a commercial Ru/Ir-based MMO catalyst. Notably, Pt1/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−N4sites during the CER. Density functional theory calculations suggest the PtN4C12site as the most plausible active site structure for the CER.
Funding Information
  • National Research Foundation of Korea (NRF-2014R1A5A1009799, NRF-2017R1A2B2008464, NRF-2017R1A4A1015533)

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