Eliminating refractory organic pollutants in water using advanced oxidation processes (AOPs) often consumes lots of energy, which greatly hindered its large scale application. Most of the organic pollutants possess very high chemical energy, but the energies of these reactant have not been effectively utilized for water purification. Herein, chemical conjuncted Fe0-FeyCz/Fex, graphited ZIF-8 and rGO (Fe0-FeyCz/Fex-GZIF-8-rGO) is first prepared via a surface growth process for destructing these organic pollutants in air-saturated aqueous suspension without additional energy. According to the characterization, Fe–O–C, Fe–N–C and C–O–Zn–N chemical coordination bonds were formed in the interface of the three phases, which induced the strong (Fe or Zn)-π interactions occur on the composite surface, causing the surface potential energy ~ 310.97 to 663.96 kJ/mol. The electron paramagnetic resonance (EPR), adsorption isotherms and gas chromatography-mass spectroscopy (GC-MS) analysis as well as density functional theory (DFT) calculations revealed that the electrons for the adsorbed group of pollutants are found to delocalize to around the iron species and could be trapped by O2 in aqueous suspension during this process, producing hydroxyl radical (●OH), H and adsorbed organic cation radicals, which are hydrolyzed or hydrogenated to intermediate. The target pollutants undergo surface cleavage, and convert H2O to ●OH, consuming chemical adsorption energy (~2.852 - 9.793 kJ/mol), much lower than that of AOPs. Our findings provide a novel technology for water purification and bring new insights into pollutant oxidation chemistry.

Cation–π induced surface cleavage of organic pollutants with ●OH formation from H2O for water treatment

ACS Spring 2022

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