Enhanced Selectivity in PMS Activation via Non-Metal\nDoping for Efficient <sup>1</sup>O<sub>2</sub> Generation in Emerging\nOrganic Pollutants Degradation

The\nactivation of peroxymonosulfate (PMS) to generate singlet oxygen\n(<sup>1</sup>O<sub>2</sub>) for the removal of emerging organic pollutants\n(EOPs) from complex aqueous environments has garnered widespread attention.\nHowever, the low efficiency and selectivity of current PMS activation\nfor <sup>1</sup>O<sub>2</sub> generation result in suboptimal EOP\ndegradation. To enhance the selectivity of PMS activation and promote\nthe non-radical pathway, non-metal heteroatoms with varying electronegativities\nwere introduced to disrupt the symmetrical coordination structure\nof Fe active sites in Fe single-atom catalysts. The results showed\nthat, in the B-Fe<sub>1</sub>/GLCNs/PMS system, the pseudo-first-order\nkinetic rate for bisphenol A (BPA) degradation reached 4.435 min<sup>–1</sup>, which is 7.4 times higher than that of the unmodified\ncontrol group. Experimental and theoretical calculations demonstrated\nthat the doping of non-metal heteroatoms altered the electron density\nand distribution at the Fe active sites, thereby modulating the adsorption\nconfiguration of HSO<sub>5</sub><sup>–</sup> and increasing\nthe selectivity for PMS activation to generate <sup>1</sup>O<sub>2</sub>. Additionally, the degradation of EOPs by <sup>1</sup>O<sub>2</sub> produced intermediate products with lower biological toxicity, and <sup>1</sup>O<sub>2</sub> demonstrated strong anti-interference capability.\nThe change in HSO<sub>5</sub><sup>–</sup> morphology improved\nthe rate of <sup>1</sup>O<sub>2</sub> generation. This study provides\ndeep insights into designing high-performance PMS activation catalysts\nvia non-metal doping to regulate the electronic structure of active\nsites for a selective non-radical pathway.