Abstract
Per- and polyfluoroalkyl substances (PFAS) are a class of man-made chemicals extensively employed in industrial processes, with their strong C-F bond energy conferring exceptional stability. However, this stability also leads to bioaccumulation and environmental persistence, posing threats to ecosystems and human health. Conventional physical separation technologies can only concentrate PFAS without completely destroying them. Against this backdrop, electrochemical technology has emerged as one of the most promising strategies for complete PFAS destruction, benefiting from its mild reaction conditions and controllable electron transfer. This review systematically summarizes the research progress on electrochemical PFAS degradation, comprehensively examining the degradation mechanisms and key influencing factors in electrochemical oxidation, reduction, and combined processes. It highlights the crucial roles of density functional theory (DFT) and molecular dynamics (MD) calculations in elucidating interfacial behaviors and atomic-scale C-F bond activation mechanisms. Addressing the bottlenecks of mass transfer limitations and incomplete defluorination encountered in practical applications, this paper prospectively points out the potential of microenvironmental regulation and the development of bifunctional materials for achieving in situ deep mineralization. Furthermore, it briefly explores the application prospects of artificial intelligence (AI)-enabled high-throughput screening technologies in accelerating the development of multi-objective electrode materials. Overall, this review constructs a comprehensive research framework spanning from fundamental bond cleavage mechanisms to macroscopic processes and data-driven optimization. It provides systematic strategies for the complete destruction of PFAS and offers theoretical references for the rational design of advanced environmental functional materials.