Adsorption and degradation of multiple micropollutants with trace concentrations by porous Zr-porphyrin metal-organic frameworks with missing linker defects in water
Adsorption and degradation of multiple micropollutants with trace concentrations by porous Zr-porphyrin metal-organic frameworks with missing linker defects in water
复制标题
水中缺失连接缺陷的多孔Zr-卟啉金属有机框架对多种微量浓度微污染物的吸附和降解
DOI：
10.1016/j.micromeso.2023.112444
复制
发表时间：
2023
影响因子：
5.2
通讯作者：
Bo Wang
中科院分区：
文献类型：
--
作者：
Xianyi Gan;Xiang Li;Bo Wang
金属-有机骨架材料（MOFs）是一种高效的光催化剂，具有高比表面积和优异的可见光吸收性能。本研究制备了一种锆卟啉（PCN-134）及其衍生物PCN-134（Fe）和PCN-134（Cu），用于去除6种结构不同的极低浓度（100 μg/L）微污染物。PCN-134（Cu）对5种药物（安替比林（AT）、磺胺二甲氧嘧啶（SSM）、氯贝酸（CA）、双氯芬酸（DF）和布洛芬（IBU））的初始吸附速率为174.5 μ g/（g·min）~ 2256.5 μg/（g · min），是PCN-134的1.2-2.5倍。一系列的光学和光电性能进行了研究，使用莫特-肖特基图，紫外-可见漫反射光谱（UV-DRS），瞬态光电流强度分析。PCN-134（Fe）成功地扩展了750 nm附近的可见光吸收边。PCN-134和PCN-134（Fe）有利于产生·O2−，通过Mott−Schottky图和UV-Vis漫反射光谱（UV-DRS）计算出ECB值分别为-1.04 eV和-0.55 eV。金属的掺入增强了PCN-134的电荷分离性能。PCN-134（Fe）的瞬态光电流强度是PCN-134（Cu）的3.1倍。结果表明，PCN-134（Fe）对萘普生（NPX）、安替比林（AT）和氯贝酸（CA）的降解效率分别是未处理PCN-134的2.4倍和11.3倍。·O2-和1 O2可能是产生的主要ROS，通过淬灭实验和电子顺磁共振（EPR）技术证实。该研究为改进现有净水材料提供了有益的指导。
Metal-organic frameworks (MOFs) are effective photocatalysts with high surface area and excellent visible light absorption. In this study, a kind of Zr-porphyrin (PCN-134) and its derivatives PCN-134(Fe) and PCN-134 (Cu) were prepared for removing six structurally diverse micropollutants with extremely low concentrations (100 μg/L). The initial adsorption rates for five selected pharmaceuticals (antipyrine (AT), sulfadimethoxypyrimidine (SSM), clofibric acid (CA), diclofenac (DF), and ibuprofen (IBU)) ranged from 174.5 μg/(g • min) to 2256.5 μg/(g • min) over PCN-134 (Cu), which is 1.2–2.5 times higher than those of PCN-134. A series of optical and photoelectric properties were studied using Mott−Schottky plots, UV–Vis diffuse reflectance spectrum (UV-DRS), and transient photocurrent intensity analysis. PCN-134 (Fe) successfully extended the visible-light absorption edges at around 750 nm. PCN-134 and PCN-134 (Fe) were favorable for generating •O2−with ECBvalues calculated at −1.04 eV and - 0.55 eV by Mott−Schottky plots and UV–Vis diffuse reflectance spectrum (UV-DRS). The incorporation of metals enhanced the charge separation properties of PCN-134. The transient photocurrent intensity of PCN-134 (Fe) was 3.1 times higher than that of PCN-134 (Cu). The degradation efficiency for naproxen (NPX) over PCN-134 (Fe) for antipyrine (AT) and clofibric acid (CA) was 2.4 times and 11.3 times higher than those over the pristine PCN-134. •O2−and1O2could be the major ROS produced, confirmed by quenching experiments and electron paramagnetic resonance (EPR) technologies. This study offers useful guidance to improve the current materials for water purification.