The Faradaic-Induced hybrid capacitive engine enables high-performance selective defluorination via capacitive deionization.

[Display omitted] • A novel active unit Sb with electrically driven redox reaction with F- is reported. • The antimony active sites initiate the Faradaic-induced pseudocapacitive behavior. • The N-rich carbon laminar framework endows rapid ion diffusion and electron transfer. • The SNTPC2 electrode exhibit a superior F- removal capacity of 178.58 mg g−1. • This system performs excellent selectivity towards F- and outstanding recyclability. Fluoride (F-) contamination has become a pressing environmental concern owing to its extensive origins and severe toxicity. Capacitive deionization (CDI) emerges as a promising technique for efficient defluorination, with the development of electrode materials being pivotal to its efficiency. Herein, we present a novel design of Sb-decorated N-rich carbon composites (SNTPCs) for the formation of a hybrid capacitive engine that integrates Faradaic-induced pseudocapacitance and electrical double layer capacitance, enabling efficient F- electrosorption. This approach features a distinctive N-rich carbonaceous laminar framework that not only guarantees rapid ion diffusion and electron transfer but also provides a dense electrical double layer for F- storage. The Sb sites are electrically stimulated to release the intrinsic affinity with F-, forming the Faradaic Sb-F bonds. The SNTPC2 electrode exhibits the exceptional saturation removal capability and dynamic electrosorption capacity for defluorination, reaching 178.58 and 34.77 mg F/g at 1.2 V respectively, which exceeds most reported F- capture electrodes. It also demonstrates excellent selectivity towards F- in complex conditions and exhibits effectiveness across a wide range of pH values. Additionally, the utilized electrode performs outstanding regeneration performance after 20 consecutive cycles. This study provides innovative perspectives for the effective elimination of fluoride pollution in aquatic environments. [ABSTRACT FROM AUTHOR]