Effective electrosorption and recovery of phosphorus by capacitive deionization with a covalent organic framework-membrane coating electrode

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 NaH₂PO₄. When treating different mixtures of NaH₂PO₄/NaCl, NaH₂PO₄/NaNO₃, and NaH₂PO₄/Na₂SO₄ 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.