The obvious advantage of amino-functionalized metal-organic frameworks: As a persulfate activator for bisphenol F degradation

过硫酸盐 催化作用 化学 电子顺磁共振 双酚A 羟基化 金属有机骨架 激进的 密度泛函理论 光化学 降级(电信) 双酚 有机化学 物理化学 计算化学 环氧树脂 计算机科学 吸附 物理 电信 核磁共振
作者
Zhen Liu,Ruidian Su,Xun Sun,Weizhi Zhou,Baoyu Gao,Qinyan Yue,Qian Li
出处
期刊:Science of The Total Environment [Elsevier BV]
卷期号:741: 140464-140464 被引量:72
标识
DOI:10.1016/j.scitotenv.2020.140464
摘要

In this study, two iron-based metal-organic framework compounds (MOFs), were used and compared as catalysts for persulfate (PS) activation to degrade bisphenol F (BPF). The outstanding advantage of using amino-functionalized MOFs in the catalytic system was verified under different reaction conditions, and the mechanism was explored. The results indicated that NH2-MIL-101(Fe)/PS system not only had a wide pH application range, but also possessed an excellent catalytic performance towards interference from the coexisting anions and humic acid. Density functional theory (DFT) calculations showed that, compared with MIL-101(Fe), the -NH2 modification could significantly improve the electronic conductivity of NH2-MIL-101(Fe) by enhancing its Fermi level (-4.28 eV) and binding energy to PS (-1.19 eV). The free radical quenching experiments were combined with electron paramagnetic resonance (EPR) confirmed that free radicals (SO4-, OH, O2-) worked together with the non-radical (1O2) reaction to remove 91% BPF within 40 min in the NH2-MIL-101(Fe)/PS system. The two proposed BPF degradation pathway were related to hydroxylation, oxidation and ring cracking. The toxicity of the BPF degradation intermediates as well as its final products were also evaluated.
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