The unique Co2Mn1N8 structure enhances peroxymonosulfate activation and singlet oxygen generation through a localized electric field

• A cobalt-manganese bimetallic catalyst with a unique structure (Co 2 Mn 1 N 8 ) was prepared. • The catalytic performance of CoMn-NC exceeds the reported PMS catalysts of the same type. • The synergistic effect between Co and Mn sites enhanced the adsorption of PMS and the generation of 1 O 2 . • The Co2Mn1N8 configuration creates an intrinsic electric polarization that boosts electron transfer efficiency during PMS activation. Atomically dispersed multi-metallic site catalysts have been extensively studied and utilized for the removal of various emerging pollutants. The combination of multiple atomic sites endows them with high catalytic performance. However, determining the atomic configuration and elucidating their true active sites remain challenging tasks. This study designed and synthesized a novel Co-Mn bimetallic carbon-based catalyst using Co and Mn-doped Zn-zeolitic imidazolate framework (ZIF-8) as a template, achieving efficient purification of organic pollutants. The structural characteristics of CoMn-NC (Co 2 Mn 1 N 8 ) were elucidated by integrating X-ray absorption spectroscopy with density functional theory (DFT) calculations. DFT computations also demonstrated that Co atoms in the Co 2 Mn 1 N 8 structure are the main active sites. Moreover, the collaborative interaction between Mn and Co sites fine-tunes the d-band center, significantly enhancing the activation of PMS, which in turn accelerates the removal of organic pollutants (removal rate of nearly 100 % within 10 min.). Overall, this study systematically elucidates the structure and advantages of the catalytic system, providing novel perspectives on the mechanisms underlying the activation of PMS by multi-metallic catalysts and potentially offering new strategies to advance Fenton-like water pollution control.