Advanced oxidation processes are widely utilized to eliminate persistent organic pollutants from water. However, their practical effectiveness is significantly constrained by irreversible catalyst deactivation and limited tunability of oxidant pathways. In peroxymonosulfate activation, a central challenge remains sustaining metal redox turnover while maintaining complementary reactive oxygen species under prolonged operation. Here we show that a FeS₂/MoS₂ heterointerface functions as an internal redox shuttle, driving a self-sustaining charge-circulation loop that autonomously regenerates dual active sites. A built-in electric field enforces directional electron transfer from Mo to Fe, thereby stabilizing continuous iron redox cycling for the production of radicals (•OH and SO₄^•−). Simultaneously, this architecture enables Mo-mediated generation of nonradical singlet oxygen, which mitigates catalyst deactivation and sustains oxidant output. As a result, the system achieves rapid removal of acetaminophen and retains 91.5% of its catalytic activity after 3000 min of continuous operation in various water matrices. These findings establish self-sustaining interfacial charge circulation as a broadly applicable and highly effective strategy for designing robust catalysts for sustainable water treatment.

The recycling of lithium-ion batteries (LIBs) is essential for promoting the closed-loop sustainable development of the LIB industry. However, progress in LIB recycling technologies is slow. There are significant gaps between academic research and industrial application, which hinder the industrialization of new technologies and the improvement of existing ones. Here we show a universal model for spent LIB-lithium recycling (SliRec) to evaluate the applicability and upgrading potential across various recycling technologies. Instead of modeling the entire recycling process, we focus on partial processes to enable a comparative analysis of environmental and economic impacts. We find a strong correlation between lithium concentration (LC) and the advancement of recycling technologies, where higher LC is associated with a reduced carbon footprint and increased economic benefits. The implementation of high-level recycling technology can result in an 85.91% reduction in carbon footprint and a 5.97-fold increase in economic returns. Additionally, we explore the effects of technological interventions through scenario analysis, demonstrating that while low-level recycling technology faces more substantial challenges in upgrading, it holds greater potential for reducing carbon emissions (−2.38 kg CO₂-eq mol⁻¹) and enhancing economic benefits (CNY 11.04 mol⁻¹). Our findings emphasize the significance of process modeling in evaluating the quality of spent LIB recycling technologies, and can provide comparative information for the application of emerging technologies or the upgrade of existing ones.