Atomic-level regulation of peroxymonosulfate activation on coal gangue: Toward controllable catalytic pathways and enhanced environmental resilience

Upcycling coal gangue (CG) requires addressing the persistent bottlenecks of conventional heterogeneous catalysts, namely active site aggregation and poor selectivity in complex wastewater. This review critically assesses recent advances in constructing atomically precise catalytic systems on CG for targeted peroxymonosulfate (PMS) activation. We consolidate existing studies to propose a tripartite framework: (1) stabilizing metal atoms within oxygen vacancies to maximize atomic exposure, (2) modulating reaction pathways via nitrogen coordination (graphitic-N for singlet oxygen, pyridinic-N for radicals), and (3) establishing dual-metal pairs to accelerate interfacial electron transfer. Key findings from density functional theory (DFT) and machine learning (ML) studies are analyzed to elucidate structure-activity relationships. This review substantiates that the structural disorder of solid waste can be strategically harnessed for atomic-level precision, providing a viable pathway for developing high-performance environmental catalysts.