Super-exchange interaction enables Fe2−xMnxO3 perovskite with excellent catalytic oxidation activity toward hexabromocyclododecane under humidity

Although enhancing the catalytic oxidation activity is a hotspot in thermal-driven catalytic disposal of persistent organic pollutants, few studies have managed to improve catalysts' water-resistance properties. Herein, we developed Fe2−xMnxO3 perovskite to boost the catalytic oxidation of hexa...

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Veröffentlicht in:Journal of hazardous materials 2024-11, Vol.479, p.135691, Article 135691
Hauptverfasser: Wu, Mingge, Chen, Cheng, Duo, Jia, Li, Qianqian, Song, Maoyong, Sun, Bohua, Su, Guijin
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Sprache:eng
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Zusammenfassung:Although enhancing the catalytic oxidation activity is a hotspot in thermal-driven catalytic disposal of persistent organic pollutants, few studies have managed to improve catalysts' water-resistance properties. Herein, we developed Fe2−xMnxO3 perovskite to boost the catalytic oxidation of hexabromocyclododecane under humidity by modulating its super-exchange interaction (SEI, Fe3+ + Mn3+ → Fe2+ + Mn4+). Fe0.4Mn1.6O3, with the strongest SEI, exhibits the biggest oxidation rate-constant, which is 3 times higher than that of commonly used Fe2O3 without SEI. Notably, unlike Fe2O3 which deactivates at a relative humidity of 5 %. Fe0.4Mn1.6O3 maintains its activity and is even boosted by 22 % compared to dry conditions. Mechanistic insights reveal that SEI between Fe and Mn enhances the reactivity of Mn4+- linked Olatt by lowering the reductive temperature from Mn4+ to Mn3+. Meanwhile, SEI promotes the adsorption of the associatively adsorbed H2O (HOH-type water) by reducing adsorption energy, thereby facilitating the formation of hydroxyl species, which are crucial for the oxidation process under humidity. [Display omitted] •The synthetic Fe2-xMnxO3 feature an unusual super-exchange interaction (SEI).•SEI boost the catalytic oxidation activity of Fe2-xMnxO3 toward HBCD under humidity.•SEI enhance the reactivity of Olatt by facilitating the reduction of Mn4+to Mn3+.•SEI promote the adsorption of HOH-type water and facilitate the formation of hydroxyl.•Olatt and hydroxyl species are crucial for the oxidation process of HBCD.
ISSN:0304-3894
1873-3336
1873-3336
DOI:10.1016/j.jhazmat.2024.135691