Heterogeneous catalysts promoting efficient production of reactive species and dynamically stabilized electron transfer mechanisms for peroxomonosulfates (PMS) still lack systematic investigation. Herein, a more stable magnetic layered double oxides (CFLDO/N-C), was designed using self-polymerization and high temperature carbonization of dopamine. The CFLDO/N-C/PMS system effectively activated PMS to remove 99% (k = 0.737 min⁻¹) of tetracycline (TC) within 10 min. The CFLDO/N-C/PMS system exhibited favorable resistance to inorganic anions and natural organics, as well as satisfactory suitability for multiple pollutants. The magnetic properties of the catalyst facilitated the separation of catalysts from the liquid phase, resulting in excellent reproducibility and effectively reducing the leaching of metal ions. An electronic bridge was constructed between cobalt (the active platform of the catalyst) and PMS, inducing PMS to break the O–O bond to generate the active species. The combination of static analysis and dynamic evolution confirmed the effective adsorption of PMS on the catalyst surface as well as the strong radical-assisted electron transfer process. Eventually, we further identified the sites where the reactive species attacked the TC and evaluated the toxicity of the intermediates. These findings offer innovative insights into the rapid degradation of pollutants achieved by transition metals in SR-AOPs and its mechanistic elaboration.

Nickel oxide (NiO_X) has been established as a highly efficient and stable hole-transporting layer (HTL) in perovskite solar cells (PSCs). However, existing deposition methods for NiO_X have been restricted by high-vacuum processes and fail to address the energy level mismatch at the NiO_X/perovskite interface, which has impeded the development of PSCs. Accordingly, we explored the application of NiO_X as a hybrid HTL through a sol–gel process, where a NiO_X film was pre-doped with Ag ions, forming a p/p⁺ homojunction in the NiO_X-based inverted PSCs. This innovative approach offers two synergistic advantages, including the enlargement of the built-in electric field for facilitating charge separation, optimizing energy level alignment, and charge transfer efficiency at the interface between the perovskite and HTL. Incorporating this hybrid HTL featuring the p/p⁺ homojunction in the inverted PSCs resulted in a high-power conversion efficiency (PCE) of up to 19.25%, significantly narrowing the efficiency gap compared to traditional n-i-p devices. Furthermore, this innovative strategy for the HTL enhanced the environmental stability to 30 days, maintaining 90% of the initial efficiency.