Heterogeneous Fe(IV)[dbnd]O mediated fenton-like process on Fe-Zr heterojunction for selective oxidation of organic pollutants at near neutral pH

Abstract

Remarkable heterogeneous Fe(IV)O (≡Fe(IV)O) mediated Fenton-like process on (1 1 0)-(1 0 0) heterojunction of Fe-Zr bimetallic oxide was proposed in this work for selective oxidation of organic pollutants under near-neutral conditions. The formation of heterojunction shortened the Fe-O bond length by 0.14 Å and increased the binding energy of Fe 2p3/2 orbital by 0.8 eV on Fe-Zr (1 1 0)-(1 0 0) interface, compared with that on Fe2O3 (1 1 0) facet. This will promote the cyclic complexes of Fe(II)-[OOH]+ formation on Fe-Zr (1 1 0)-(1 0 0) interface. Besides, energy barrier of Fe(II)-[OOH]+ on (1 1 0)-(1 0 0) heterojunction was 10.6 kJ mol−1 lower than that on Fe2O3 (1 1 0) facet. It will facilitate the inner two-electron transfer process to generate Fe(IV)O. And electrostatic repulsion and electrophilic addition enable Fe(IV)O to selectively oxidize target organic pollutants in the system containing ions and humic acids. This work provides a fundamental information toward the structure-performance relationship between heterojunction structure and Fe(IV)O formation, and it will enlighten the selective oxidation of pollutants in wastewater treatment.