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High voltage operation is effective to improve salt adsorption capacity (SAC) of capacitive deionization (CDI), while this will cause performance loss during long-term operation. Herein, to address this issue, we report a simple approach to prepare novel membrane coating electrode (MCE) that polyvinyl alcohol/polyethyleneimine membrane was deposited onto activated carbon fiber (ACF) and glutaraldehyde (GA) was used for crosslinking. Compared with ACF (SAC: 13.2–20.9 mg/g, charge efficiency: 63.6%–43.9%), MCE with optimized 5 wt% GA concentration (MCE (5)) showed an improved SAC from 14.6 to 28.4 mg/g and stable charge efficiency at 80.2% when voltage increased from 0.8 V to high voltage of 1.8 V due to suppressed anode oxidation. After forty cycles experiments at 1.8 V, SAC retention of ACF declined to 71.6% caused by degradation of electrode properties, while SAC retention of MCE (5) increased to 124.7%. The deposited membrane was found to act as a barrier and inhibitor to restrict ACF oxidation, and conversions of N-containing groups and reduced charge transfer resistance of cycled MCE (5) led to superb long-term performance. It is reasonable to believe that our work provides new strategy for enhancing CDI performance by using newly developed MCE. [Display omitted] • A novel MCE was prepared firstly by depositing PVA/PEI membrane onto ACF. • MCE (5) exhibited a high SAC and improved SAC retention under a high voltage. • MCE (5) showed a stable E pzc and reduced charge transfer resistance during cycling. • PVA/PEI membrane acted as a barrier and inhibitor to suppress ACF oxidation. [ABSTRACT FROM AUTHOR]

• Novel E-CDI with catalytic electrodes was developed for phosphonate degradation. • C-MCE with outstanding ORR performance improved the self-generation of H 2 O 2. • A-MCE provided an ideal platform for the reaction between ·OH and phosphonate. • E-CDI exhibited higher degradation efficiency and lower cost than traditional AOPs. Phosphonate is becoming a global interest and concern owing to its environment risk and potential value. Degradation of phosphonate into phosphate followed by the recovery is regarded as a promising strategy to control phosphonate pollution, relieve phosphorus crisis, and promote phosphorus cycle. Given these objectives, an anion-membrane-coated-electrode (A-MCE) doped with Fe-Co based carbon catalyst and cation-membrane-coated-electrode (C-MCE) doped with carbon-based catalyst were prepared as catalytic electrodes, and a novel electrocatalytic capacitive deionization (E-CDI) was developed. During charging process, phosphonate was enriched around A-MCE surface based on electrostatic attraction, ligand exchange, and hydrogen bond. Meanwhile, Fe2+ and Co2+ were self-oxidized into Fe3+ and Co3+, forming a complex with enriched phosphonate and enabling an intramolecular electron transfer process for phosphonate degradation. Additionally, benefiting from the stable dissolved oxygen and high oxygen reduction reaction activity of C-MCE, hydrogen peroxide accumulated in E-CDI (158 μM) and thus hydroxyl radicals (·OH) were generated by activation. E-CDI provided an ideal platform for the effective reaction between ·OH and phosphonate, avoiding the loss of ·OH and triggering selective degradation of most phosphonate. After charging for 70 min, approximately 89.9% of phosphonate was degraded into phosphate, and phosphate was subsequently adsorbed by A-MCE. Results also showed that phosphonate degradation was highly dependent on solution pH and voltage, and was insignificantly affected by electrolyte concentration. Compared to traditional advanced oxidation processes, E-CDI exhibited a higher degradation efficiency, lower cost, and less sensitive to co-existed ions in treating simulated wastewaters. Self-enhanced and selective degradation of phosphonate, and in-situ phosphate adsorption were simultaneously achieved for the first time by a E-CDI system, showing high promise in treating organic-containing saline wastewaters. [Display omitted] [ABSTRACT FROM AUTHOR]

Capacitive deionization (CDI) holds great promise for phosphorus adsorption and recovery from wastewater, while current electrodes exhibit poor salt adsorption capacity (SAC) and selectivity due to co-ion effect and interference of co-existed ions with high concentration. Herein, to overcome these issues, a facile route was proposed to prepare a covalent organic framework-membrane coating electrode (COF-MCE) by depositing polyvinyl alcohol/polyethyleneimine membrane onto activated carbon fiber (ACF) followed by the in-situ growth of COF-LZU1. Compared to ACF and MCE, COF-MCE, with abundant functional groups and specific sites, facilitated electrical double layer (EDL)-based adsorption and induced hydrogen-bond interaction with phosphorus, contributing to a higher SAC of phosphorus (10.5 mg/g) in treating 1 mM NaH 2 PO 4. When treating different mixtures of NaH 2 PO 4 /NaCl, NaH 2 PO 4 /NaNO 3 , and NaH 2 PO 4 /Na 2 SO 4 with molar ratio of 1:5, COF-MCE exhibited the high phosphorus selectivity of 3.62, 5.98 and 7.01, respectively, which was attributed to the synergistic effects of EDL-based adsorption, hydrogen-bond and pseudocapacitance. Desorption experiments revealed that high reversal voltage and alkaline condition can weaken the hydrogen-bond interaction and strengthen the electrostatic repulsion between COF-MCE and phosphorus, thus improving the desorption and recovery of phosphorus. These findings confirmed the high potential of COF-MCE in the effective electrosorption and recovery of phosphorus from wastewater. • COF-MCE was prepared by casting followed by in-situ growth of COF powders. • Inhibited co-ion effect and enhanced EDL formation led to superb P adsorption. • Hydrogen-bond and redox-reaction interaction contributed to high selectivity for P. • A reversal voltage and high pH weakened the interaction and favored P recovery. [ABSTRACT FROM AUTHOR]

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. [Display omitted] • Three-layer structured membrane coating electrode was prepared for F- removal. • High F- adsorption capacities were obtained over the wide concentration gradient. • Mesopore-dominated structure overcame the overlapping of electrical double layer. • Positively charged polymer membrane inhibited the serious co-ion repulsion effect. [ABSTRACT FROM AUTHOR]