Efficient groundwater defluorination over a wide concentration gradient through capacitive deionization with a three-layer structured membrane coating electrode

Fluoride (F − ) pollution in groundwater is an important environmental issue and capacitive deionization (CDI) holds promise for defluorination at moderate concentrations (e.g., 200 −1000 mg L −1 ). However, existing electrodes suffer from the overlap of electrical-double-layer (EDL) and severe co-ion effects at low (e.g., <200 mg L −1 ) and high sodium fluoride (NaF) concentrations (e.g., >1000 mg L −1 ), respectively, exhibiting poor salt adsorption capacity (SAC). Hence, a three-layer structured electrode, “membrane/carbon nanotube (CNT)/activated carbon (AC)” (CNT-MCE), was prepared through electrospinning CNT onto AC, followed by a polymer membrane coating. Compared to AC and membrane coated electrode, CNT-MCE with mesopore-dominated structure prevented EDL overlap, achieving a higher SAC of 40.8 mg g −1 at 100 mg L −1 NaF. At 1500 mg L −1 NaF, the positively charged CNT-MCE exhibited an improved SAC of 58.8 mg g −1 by inhibiting co-ion effects. Meanwhile, CNT-MCE consistently demonstrated superb SACs at 200 − 800 mg L −1 NaF and maintained excellent stability over a wide concentration gradient by inhibiting severe oxidation. Notably, CNT-MCE successfully decreased the F − concentration in simulated groundwater from 3.4 to 1.1 mg L −1 . Overall, our work provides an efficient strategy of electrode design to broaden the applicability of CDI for groundwater defluorination over a wide concentration gradient.