MXene-induced electronic structure modulation of Fe-Al-LDH to boost the Fenton-like Reaction: Singlet oxygen evolution and electron-transfer mechanisms
Journal of Materials Science & Technology(2024)
摘要
Layered double hydroxide (LDH) based heterogonous peroxymonosulfate (PMS) activation degradation of pollutants has attracted extensive attention. The challenge is to selectively regulate the traditional free radical dominant degradation pathway into a nonradical degradation pathway. Herein, an interface architecture of Ti3C2Tx-MXene (MXene) loading on the Fe-Al LDH scaffold was developed, which showed excellent stability and robust resistance against harsh conditions. Significantly, the rate constant for tetracycline hydrochloride (TC) degradation in the MXene-LDH/PMS process was 0.421 min−1, which was ten times faster than the rate constant for pure Fe-Al LDH (0.042 min−1). Specifically, more reactive Fe with the closer d-band center to the Fermi level results in higher electron transfer efficiency. The occupations of Fe-3d orbitals in Mxene/Fe-Al LDH are pushed above the Fermi level to generate, which results in higher PMS adsorption and inhibition of the release of oxygen-containing active species intermediates, leading to the enhanced 1O2 generation. Additionally, the built-in electric field in the heterojunction was driven by the charge redistribution between MXene and Fe-Al LDH, resulting in a mediated-electron transfer mechanism, differentiating it from the Fe-Al LDH/PMS system. It was fascinating that MXene/Fe-Al LDH achieved satisfactory treatment efficiency in continuous column reactor and real landfill leachate.
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关键词
Interface engineering,Density functional theory,Layered double hydroxides,Peroxymonosulfate,Electron transfer
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