Affiliation:
1. College of Environmental Science and Engineering Hunan University Changsha Hunan 410082 P. R. China
2. Key Laboratory of Environmental Biology and Pollution Control (Hunan University) Ministry of Education Changsha Hunan 410082 P. R. China
3. College of Materials Science and Engineering Hubei University of Technology Wuhan 430068 P. R. China
Abstract
AbstractTransition metal compounds (TMCs) have long been potential candidate catalysts in persulfate‐based advanced oxidation process (PS‐AOPs) due to their Fenton‐like catalyze ability for radical generation. However, the mechanism involved in TMCs‐catalyzed nonradical PS‐AOPs remains obscure. Herein, the growth of FeO on the Fe3O4/carbon precursor is regulated by restricted pyrolysis of MIL‐88A template to activate peroxymonosulfate (PMS) for tetracycline (TC) removal. The higher FeO incorporation conferred a 2.6 times higher degradation performance than that catalyzed by Fe3O4 and also a higher interference resistance to anions or natural organic matter. Unexpectedly, the quenching experiment, probe method, and electron paramagnetic resonance quantitatively revealed that the FeO reassigned high nonradical species (1O2 and FeIV═O) generation to replace original radical system created by Fe3O4. Density functional theory calculation interpreted that PMS molecular on strongly‐adsorbed (200) and (220) facets of FeO enjoyed unique polarized electronic reception for surface confinement effect, thus the retained peroxide bond energetically supported the production of 1O2 and FeIV═O. This work promotes the mechanism understanding of TMCs‐induced surface‐catalyzed persulfate activation and enables them better perform catalytic properties in wastewater treatment.
Funder
National Program for Support of Top-notch Young Professionals
National Natural Science Foundation of China