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

Abstract

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.