Unraveling an Overlooked Role of High‐Valent Ru Steered Electro‐Polymerization for Efficient Bisphenol A Removal in Single‐Atom Catalyst

Abstract Redirecting the pathways of pollutant removal from mineralization to polymerization in advanced oxidation processes is critical for simultaneously achieving low‐carbon contamination abatement and chemical energy recovery, yet the regulating strategy remains an obstacle. Herein, single‐atom catalysts are constructed through an inherent oxide anchoring strategy for directionally inducing the polymerization removal of bisphenol A (BPA). An appropriate amount of Ru single atoms (Ru‐SA) on Ti 4 O 7 support is conducive to the formation of high‐valent metal species (Ru(IV)), with its corresponding steady‐state concentration three orders of magnitude higher than that of Ti 4 O 7 , while excessive Ru‐SA inevitably leads to mutual quenching of Ru(IV) due to the significantly reduced interatomic distances. Ru(IV) beneficially induced the generation of phenoxyl‐like radicals through electron transfer, thereby triggering BPA removal via electro‐polymerization transfer. As a result, Ru 0.1 ‐Ti 4 O 7 achieves higher activity with the normalized K obs of 8.33 × 10 −7 m·s −1 , the current efficiency of 63%, and the energy consumption of 37.5 kWh·kg −1 for the electro‐polymerization removal of BPA, outperforming the conventional mineralization strategy. This work presents an adaptive paradigm to regulate the inter‐distance of single‐atom catalysts to promote the generation of high‐valent metal species and optimize pollutant removal from wastewater via polymerization.