Abstract
Sustainable water purification requires simultaneous desalination and disinfection, yet integrated solutions remain challenging due to mutual interference between the two processes. Here, we report a synchronous capacitive desalination-sterilization (CDIS) system driven by a rationally engineered dual-functional anode of silver nanoclusters embedded in carbon nanofibers (Ag NCs@CNF). This electrode uniquely combines efficient chloride-ion storage with molecular-ike electrocatalytic activity, enabling concurrent high-capacity desalination (84.25 mgCl g-1) and complete sterilization ( > 4.0 log reduction, detection limit) via in situ reactive species (RS) generation. Beyond performance, we provide the unambiguous mechanistic insight into microbe-ion dynamics in capacitive systems. Contrary to the spatial-competition paradigm, we reveal that performance decay primarily stems from electrostatic shielding by live bacteria, while inactivated cells undergo a fragmentation-aggregation process that eliminates shielding. Remarkably, bacterial inactivation further enhances cycling stability by scavenging RS and mitigating anode oxidation. This work establishes an efficient integrated electrochemical purification platform and offers a theoretical framework for designing sustainable water-treatment technologies.