Targeted accumulation and spatial confinement effect of Fe(II)-MOFs@MIP for efficiently removing low concentration dibutyl phthalate

邻苯二甲酸二丁酯 吸附 降级(电信) 激进的 化学 选择性 分子印迹 猝灭(荧光) 催化作用 化学工程 环境化学 有机化学 工程类 物理 荧光 电信 量子力学 计算机科学
作者
Haiyuan Chi,Chengjun Li,Mei Huang,Jinquan Wan,Xiaoxia Zhou,Bing Yan
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:424: 130367-130367 被引量:57
标识
DOI:10.1016/j.cej.2021.130367
摘要

• Fe(II)-MOFs@MIP with high-efficiency targeted removal of DBP was synthesized. • Selectivity coefficient for adsorption and degradation were 7.28 and 4.46 respectively. • Specific recognition performance was through hydrogen bonding and π-π interaction. • Targeted accumulation and spatial confinement effect of Fe(II)-MOFs@MIP were proved. Sulfate radicals-based advanced oxidation processes are regarded as effective methods for removing organic contaminants. However, current removal technologies are often unable to achieve satisfactory results due to the low concentrations and high stability that are frequently characteristics for many types of organic contaminants. To improve the efficacy of using sulfate radicals to remove organic contaminants, we designed metal–organic frameworks (Fe(II)-MOFs) modified with enrichment and specific recognition of molecular imprinting layer (Fe(II)-MOFs@MIP). Using dibutyl phthalate (DBP) as the model target contaminant, the selectivity coefficient towards DBP was 7.28 for adsorption and 4.46 for catalytic degradation of Fe(II)-MOFs@MIP, which is excellent for most of the imprinted material. Additionally, we achieved the accurate recognition (169.25 μg × g −1 ) and efficient degradation (0.071 min −1 ) of DBP reducing levels to 100 μg × L -1 . UV–vis analysis confirmed that specific recognition of DBP was mainly through hydrogen bonding and π-π interaction, while in-situ Raman and radical quenching experiments showed that the imprinting layer could accurately adsorb and produce the spatial confinement effects on target contaminants, thereby reducing the transfer distance of free radicals. As a result, we show that Fe(II)-MOFs@MIP can achieve efficient targeted degradation of DBP, opening up a new avenue for the removal of this and other highly stable organic contaminants present at low concentrations in environmental systems.
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