Abstract

Electrosorption holds extraordinary promise for uranium (U(VI)) capture but is still limited by the finite accessible active sites of electrode materials, poor surface wettability and its intrinsic co-ion repulsion effect. Here we originally designed KOH-etched porous graphitic carbon nitride (g-C3N4) as active material, and multi-functional crosslinked xanthan gum-polyacrylic acid (XG-PAA) as binder to fabricate g-C3N4-X electrode for U(VI) capture. The abundant in-plane nanopores on 2D g-C3N4 lamellar, rich O- and N-containing active sites, and 3D tough interconnected conductive architecture, endowed g-C3N4-X electrode with fast electron/ion transport channels, alleviated co-ions exclusion, superior electrochemical properties, and hydrophilicity. These unique structure characteristics enabled U(VI) ions to form micro electric-field attraction with negatively charged COO- groups in advance to alleviate co-ion repulsion, then to electro-migrate towards and coordinate with active sites, and eventually to be electrocatalytic reduced into U(IV) deposits. Consequently, the g-C3N4-X electrode exhibited a 1.87 times faster adsorption kinetics, a much higher removal ratio of 98.1% within 70 min than traditional PVDF-bound electrode. Meanwhile, the cumulative adsorption capacity of g-C3N4-X electrode after six cycles was up to 1459.1 mg g−1. This efficient, scalable, and cost-effective g-C3N4-X electrode represents a significant step forward toward the practical applications of U(VI) electrosorption.

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