Degradation of sulfamerazine by a novel CuxO@C composite derived from Cu-MOFs under air aeration
Degradation of sulfamerazine by a novel CuxO@C composite derived from Cu-MOFs under air aeration
复制标题
空气曝气下由 Cu-MOF 衍生的新型 CuxO@C 复合材料降解磺胺甲基嘧啶
DOI：
10.1016/j.chemosphere.2021.130678
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发表时间：
2021
期刊：
影响因子：
8.8
通讯作者：
Liu Yong
中科院分区：
文献类型：
--
作者：
Chen Yong;Zhao Junfeng;Hu Lu;Tian Jing;Liu Yong
大多数金属有机骨架（MOFs）都是由羧酸盐和金属前驱体通过水热法合成的，这将消耗大量的溶剂和羧酸盐。为了解决这一问题，提出了一种制备铜基MOFs的新方法，即以天然高分子材料单宁酸为前驱体，通过高能球磨实现单宁酸和硫酸铜的自组装，制备铜基MOFs。在此基础上，通过高温烧结制备了一种新型铜基MOFs衍生物（CuxO@C复合物），并将其用于氧气活化去除磺胺甲基嘧啶（SMR）。CuxO @ C复合材料的BET比表面积和平均孔径分别为110.34 m2 g − 1和21.06 nm，对SMR的最大吸附容量（Qmax）为104.65 mg g− 1，有利于SMR的后续降解。XRD和XPS分析结果表明，CuxO@C复合材料中含有大量的Cu 0和Cu 2 O，其粒径分别为76.6 nm和9.8 nm，具有较高的氧活化性能。在初始pH为4.0、空气流量为100 mL min−1、CuxO @C投加量为1 g L− 1、反应时间为30 min的条件下，CuxO @C/空气体系中SMR和TOC的去除率分别达到100%和90.2%。在CuxO@C/air体系中检测到H2 O2、dotOH自由基和O2自由基等活性物种，其中dotOH自由基和O2自由基是SMR降解的主要原因.
Most metal-organic frameworks (MOFs) are synthesized from carboxylate and metal precursors by hydrothermal process, which will consume a large amount of solvent and carboxylate. To address this issue, a new strategy for Cu-based MOFs was developed, in which the Cu-based MOFs was obtained by using abundant natural polymer (tannic acid) as one of the precursors and using high-energy ball milling to achieve a self-assembly of tannic acid and copper sulfate. Based on this strategy, a novel Cu-based MOFs derivative (CuxO@C composite) was synthesized by high-temperature sintering of Cu-based MOFs and used for sulfamerazine (SMR) removal via O2activation. The BET specific surface area and average pore size of CuxO@C composite were 110.34 m2g−1and 21.06 nm, respectively, which made CuxO@C composite had the maximum adsorption capacity (Qmax) for SMR of 104.65 mg g−1and favored the subsequent degradation of SMR. The results from XRD and XPS indicated that CuxO@C composite contained a lot of Cu0and Cu2O with the sizes of 76.6 nm and 9.8 nm, respectively, which led to its high performance of O2activation. The removal efficiency of SMR and 90.2% TOC achieved 100% and 90.2%, respectively in the CuxO@C/air system at initial pH of 4.0, air flow rate of 100 mL min−1, CuxO@C dosage of 1 g L−1and reaction time of 30 min. Reactive species, including H2O2, radical dotOH and O2radical dot-radicals were detected in the CuxO@C/air system, and radical dotOH and O2radical dot-were mainly responsible for the degradation of SMR.