Charge-Enhanced Separation of Organic Pollutants in Water by Anionic Covalent Organic Frameworks

[Image: see text] The effective removal of organic pollutants in wastewater is a key environmental challenge. In this work, an anionic covalent organic framework (named TpPa-SO(3)Na) was synthesized through a green two-in-one synthesis strategy with autocatalytic imine formation. The slowly generated acetic acid as a catalyst is favorable to sustain the reversibility of the covalent organic framework (COF) formation reaction and improve the crystallinity of TpPa-SO(3)Na. TpPa-SO(3)Na consists of a homogeneous distribution of sulfonate groups to produce negatively charged regular channels. The strong electrostatic and hydrogen-bonding interactions between the sulfonate groups anchored in the nanochannels and the amine groups in organic pollutants improve the adsorption selectivity and capacity. These structures allow a high degree of control over adsorption processes to boost the adsorption kinetics and improve selective separation. TpPa-SO(3)Na exhibits ultrafast adsorption (<1 min) of cationic antibiotics and dyes (average over 95%). Furthermore, TpPa-SO(3)Na exhibits high selectivity for the uptake of dye molecules on the basis of the differences in charge and molecular size. This work explored functional designs and green manufacturing of anionic COFs for removal of hydrophilic organic pollutants.