Litcius/Paper detail

Superoxide radicals mediated by high-spin Fe catalysis for organic wastewater treatment

Yanxiao Li, Dongpeng Zhang, Pengfei Wang, Jinyong Qu, Sihui Zhan

2024Proceedings of the National Academy of Sciences57 citationsDOIOpen Access PDF

Abstract

Water resources are indispensable basic resources and important environmental carriers; the presence of organic contaminants in wastewater poses considerable risks to the health of both humans and ecosystems. Although the Fenton-like reactions using H 2 O 2 as the oxidant to destroy organic pollutants are attractive, there are still challenges in improving reaction activity under neutral or even alkaline conditions. Herein, we designed a H 2 O 2 activation pathway with O 2 •− as the main active species and elucidated that the spin interaction between Fe sites and coordinated O atoms effectively promotes the generation of the key intermediate Fe–*OOH. Furthermore, we successfully captured and analyzed the Fe–*OOH intermediate by in situ Raman spectroscopy. When applying FBOB to a continuous-flow reactor, CIP removal efficiency remained at around 90% within 600 min of continuous operation, achieving excellent efficiency, stability, and pH tolerance in removing pollutants.

Topics & Concepts

RadicalCatalysisSuperoxideWastewaterPhotochemistryChemistryEnvironmental scienceOrganic chemistryEnvironmental engineeringEnzymeAdvanced oxidation water treatmentElectrocatalysts for Energy ConversionEnvironmental remediation with nanomaterials