Theory‐Guided Design of Non‐Precious Single‐Atom Catalyst for Electrocatalytic Chlorine Evolution

Abstract The chlorine evolution reaction (CER) is a crucial anodic process in the chlor‐alkali industry but relies heavily on dimensionally stable anodes (DSAs) containing high‐loadings of expensive noble metal oxides. To address this challenge, herein, a comprehensive big data analysis encompassing a broad set of the reported CER experiments to date, combined with catalytic volcano modeling is conducted using binding energy as a key descriptor. Leveraging these data‐driven and theoretical insights, highly efficient non‐precious single‐atom catalysts (SACs) is designed for CER. Among them, the predicted NiN 3 O‐O SAC exhibited remarkable catalytic activity and selectivity, as confirmed by subsequent proof‐of‐concept experiments. Under acidic conditions (1 M NaCl, pH 0.9), NiN 3 O‐O demonstrates a low overpotential of 75 mV at 10 mA cm −2 and an exceptional Cl 2 selectivity of 95.8%, surpassing commercial DSA electrodes. Mechanistic investigations further reveal that the on‐top oxygen (O ot ) in NiN 3 O‐O serves as the active center, with a strong preference for chloride ion adsorption over competing intermediates, which underlies its superior catalytic performance. This work establishes non‐precious SACs as highly effective CER catalysts, opening a promising avenue for the development of cost‐effective and efficient CER electrocatalysts.