Revealing the Role of Binary Distortion in PMS Activation over Spinel toward Efficient New Pollutants Removal

Abstract Improving peroxymonosulfate (PMS) activation efficiency to enhance simultaneous generation of radicals and non‐radicals is essential for removing new pollutants (NPs) in complex waters. However, achieving this with standard lattice‐structured heterogeneous catalysts remains challenging due to inefficient electron transfer. Here, CuCo₂O₄ properties are successfully tuned by controlling lattice distortion, enabling simultaneous PMS oxidation and reduction. Unlike the slow rate of electron transfer in heterogeneous metal catalysts with standard lattice structures, the highly active binary lattice distortion in CuCo₂O₄ alters the structure and electron distribution, exposes more Cu and Co sites, lowers the PMS adsorption barriers, and realizes the synergistic production of SO₄^•−/•OH), and ¹O₂. The k‐value for ciprofloxacin is as high as 17.83 min⁻¹ M⁻¹, 29.42 times higher than that with non‐binary lattice distortion. Additionally, the developed intermittent reactor consistently maintains a removal rate above 95% over five cycles in actual wastewater treatment scenarios. This work provides a new avenue for achieving the removal of new pollutants in complex water bodies.