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The atomically dispersed catalysts often give rise to a different reaction pathway compared to that of widely used nanoparticle-based catalysts, leading to unusual selectivity and activity for many electrocatalytic reactions, including the oxygen reduction reaction, hydrogen evolution reaction and fuel oxidation reactions 37, 38, 39, 40. However, MMOs still exhibit low CER selectivity at low Cl − concentration and neutral pH 5, 12, 15.Ītomically dispersed catalysts 34, 35 or single-atom catalysts 36 have recently been actively pursued to maximise the utilisation efficiency of precious metals. As alternative strategies, doping of other metals into the MMOs 28, 29, structural modification of MMOs 30, 31, 32, and the use of new compositions 12, 33 have been exploited to promote activity as well as selectivity for the CER. Nevertheless, high amounts (approximately 30 at%) were required to maintain sufficient electronic conductivity for the CER 5. To mitigate O 2 generation in the condition of the chlor-alkali process, the contents of precious metals were reduced. The oxidative water activation and concomitant surface oxidation on MMOs 25, 26, 27 are, therefore, unavoidable, leading to a decrease in active site density for the CER 25. This relationship suggests that two reactions are catalysed on a similar active site of the MMOs or form a common surface intermediate species 20, 21, 22, 23, 24. However, computational and experimental works revealed that MMO catalysts are also highly active for the OER, exhibiting a scaling relationship between the CER and OER 13, 17, 18, 19, 20. Mixed metal oxides (MMOs) based on precious metals (Ru and Ir), such as a dimensionally stable anode (DSA), have been predominantly used as CER catalysts irrespective of the pH of the solution 5, 6, 7, 8. Moreover, under the AC-generating conditions, the Cl − concentration is below 1 M, which makes the CER thermodynamically and kinetically more challenging than that in the chlor-alkali process 5, 14, 15, 16. Where R, T and F represent the universal gas constant, the temperature, and the Faraday constant, respectively. On the potential scale of reversible hydrogen electrode (RHE), the CER and OER occur via the following reactions and their standard reversible electrode potentials ( E 0). AC generation is typically conducted in neutral pH, where the oxygen evolution reaction (OER), the side reaction of CER, shows much lower overpotential than that in acidic pH 13, 14, leading to low CER selectivity. The CER is also important for generating active chlorine (AC) as a disinfectant for wastewater and ship ballast water treatments on account of its effectiveness in removing harmful organisms or invasive aquatic species with a long residual time 9, 10, 11, 12. To ensure high efficiency in the chlor-alkali system and the production of high purity Cl 2 gas, CER should be operated in acidic pH saturated with Cl − (ref. The current Cl 2 production is prevalently dependent on the chlor-alkali process 4, 5, for which the electrochemical chlorine evolution reaction (CER) plays a pivotal role as the anodic reaction 5, 6, 7, 8. It is used as a key chemical in the production of polymers and pharmaceuticals, pulp and paper industries, and water treatments 2, 3, 4. Density functional theory calculations suggest the PtN 4C 12 site as the most plausible active site structure for the CER.Ĭhlorine (Cl 2) is one of the most important industrial chemicals with an annual production of approximately 75 million tons worldwide 1. In situ electrochemical X-ray absorption spectroscopy reveals the direct adsorption of Cl − on Pt−N 4 sites during the CER. 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. The Pt 1/CNT catalyst shows superior CER activity to a Pt nanoparticle-based catalyst and a commercial Ru/Ir-based MMO catalyst. 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. 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. Chlorine evolution reaction (CER) is a critical anode reaction in chlor-alkali electrolysis.
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