Abstract
Electrochemical chlorine evolution reaction (CER) is one of the most important electrochemical reactions due to importance of Cl2 as an industrial chemical. However, electrochemical CER is bridled with parallel oxygen evolution reaction (OER) reducing the performance of anodic CER In this context, guiding principles behind enhancing the selectivity of CER is investigated experimentally and computationally in RuO2 doped with earth-abundant first-row-transition-metals (i.e. Ti, Fe, Mn, Co, Ni, Cu, Zn). Computational studies suggest that doping of metals having higher d-electrons than Ru in RuO2 tend to lower the binding strength of OER intermediates thereby increasing its overpotential. However, doping has less effect on the binding strength of monovalent CER intermediates resulting in higher CER selectivity. Computational studies suggest that Cu (d9)-doped RuO2 would show maximum CER selectivity and this is corroborated by experiments in acidic medium with electrodeposited Cu-doped RuO2 where 95% selectivity was obtained at a dopant concentration of 2%.
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