Photocatalytic degradation of microcystin-LR with a nanostructured photocatalyst based on upconversion nanoparticles@TiO(2) composite under simulated solar lights.

Photocatalytic degradation of microcystin-LR with a nanostructured photocatalyst based on upconversion nanoparticles@TiO(2) composite under simulated solar lights.
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模拟太阳光下基于上转换纳米粒子@TiO2复合材料的纳米结构光催化剂光催化降解微囊藻毒素-LR

DOI:
10.1038/s41598-017-14746-6
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发表时间:
2017-10-31
期刊:
影响因子:
4.6
通讯作者:
Wang Z
Wang Z
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Wu S;Lv J;Wang F;Duan N;Li Q;Wang Z

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在这项工作中,我们制备了包覆TiO2光催化剂(NaYF4:Yb,Tm@TiO2)的先进上转换纳米颗粒,不仅利用了紫外能量,而且利用了大部分近红外能量,以提高太阳能灯的利用效率。当NaYF4:Yb浓度为Tm@TiO2 0.4 mg/mL,初始pH值为4时,30 min内MC-LR (10 μg/mL)的降解率接近100%,而在模拟太阳光照下,纯TiO2 (P25)的降解率为61%。研究了反应过程,拟合了一级动力学模型。高活性的羟基自由基(•OH)是主要的活性物质。同时,采用液相色谱/质谱法对MC-LR的7种降解中间体进行了检测,并对降解机理进行了分析。根据中间体的分子量,提出了主要的降解途径,反应机理为二烯键羟基化和Adda的芳环羟基化。根据中间体的结构对产物进行了无毒评价。该研究表明,除了紫外外,近红外能量可以作为光催化的驱动源,近红外响应的光催化具有高效和降解MC-LR的潜力。
In this work, we prepared advanced upconversion nanoparticle coated with TiO2 photocatalysts (NaYF4:Yb,Tm@TiO2) to utilize not only UV energy but also the large portion of NIR energy in order to improve the utilization efficiency of solar lights. The MC-LR (10 μg/mL) degradation rate can be approached 100% within 30 min at the concentration of NaYF4:Yb,Tm@TiO2 0.4 mg/mL and initial pH value 4, while 61%, using pure TiO2 (P25) under simulated solar lights. The reaction processes were studied and fitted with the pseudo-first-order kinetic model. Highly reactive hydroxyl radicals (•OH) were found to be the major reactive species. Meanwhile, seven degradation intermediates of MC-LR were examined by liquid chromatography/mass spectrometry and the degradation mechanism was analyzed. The main degradation pathways were proposed based on the molecular weight of the intermediates and the reaction mechanism are hydroxylation on the diene bonds and the aromatic ring of Adda. The products were evaluated to be nontoxic based on the construction of the intermediates. This study demonstrated that the NIR energy can be used as the driving source for photocatalysis besides the UV and the NIR-responsed photocatalysis had a high-efficiency and potential for MC-LR degradation.
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