Selective photodegradation of tetracycline by molecularly imprinted ZnO@NH2-UiO-66 composites
Selective photodegradation of tetracycline by molecularly imprinted ZnO@NH2-UiO-66 composites
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DOI：
10.1016/j.cej.2020.124614
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发表时间：
2020-06
影响因子：
15.1
通讯作者：
Qiu-zheng Du;Pu Wu;Yiyang Sun;Jingyi Zhang;Hua He
中科院分区：
文献类型：
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作者：
Qiu-zheng Du;Pu Wu;Yiyang Sun;Jingyi Zhang;Hua He
以四环素（TC）为模板分子，采用合成后修饰法合成了一种结构简单、可重复使用的印迹催化复合物（ZnO@NH2-UiO-66，ZUM）。制备了一系列具有从0.1至0.7g的不同NH 2-UiO-66掺杂剂的ZUM-n复合材料并进行了比较。表征结果表明，ZUM-1具有粒径均匀、比表面积大、吸收光谱宽等优点。进一步的研究结果表明，ZUM-1复合材料具有选择性吸附能力，对TC具有较高的光催化降解效率，且无二次污染。在可见光照射下，ZUM-1在30 min内可降解61.9%的TC，这可能与复合材料对电子-空穴复合的抑制作用有关。通过比较ZUM-1对四环素、盐酸四环素和环丙沙星的降解效果，考察了ZUM-1对四环素、盐酸四环素和环丙沙星的降解选择性。在真实的样品中也证实了ZUM-1的高降解效率和选择性。稳定性实验表明，ZUM-1在光催化降解过程中具有良好的可回收性和稳定性，回收过程对环境友好。通过紫外-可见光谱、光电化学和自由基清除实验研究了ZUM-1光降解TC的机理。该方法为制备具有高特异性和光催化活性的可见光响应分子印迹复合材料提供了一种简便可行的方法。
A simple and recyclable imprinted catalytic composite (ZnO@NH2-UiO-66, ZUM) was synthesized by postsynthetic modification method with tetracycline (TC) as molecular template. A series of ZUM-n composites with different NH2-UiO-66 dopants from 0.1 to 0.7 g had been prepared and compared. The characterization results showed that ZUM-1 possessed the advantages of uniform size, high surface area and wide absorption spectrum. Further research results indicated that ZUM-1 composite has the ability of selective adsorption and the higher photocatalytic degradation efficiency to TC without secondary pollution. Under visible light irradiation, the ZUM-1 could degrade 61.9% of TC within 30 min, which may relate to the inhibition effect of composite materials on electron-hole recombination. The degradation selectivity of ZUM-1 was investigated by comparing the degradation efficiency of TC, tetracycline hydrochloride and ciprofloxacin. The high degradation efficiency and selectivity of ZUM-1 were also confirmed in real samples. The stability experiments showed that the ZUM-1 possessed excellent recyclability and stability in the photocatalytic degradation process, and the recycled process was environmentally friendly. The mechanism of TC photodegradation by ZUM-1 was investigated by UV–vis spectra, photoelectrochemical and radical scavenger experiment. And the possible degradation products were analyzed by HPLC-MS. All in all, this method provided a simple and promising perspective for preparing visible-light-responsive molecular imprinting composites with high specificity and photocatalytic activity.