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在可见光照射下,CeO/g-CN 复合材料对 2,4-二氯苯酚的高效降解:详细反应途径和机制。

Highly efficient degradation of 2,4-dichlorophenol over CeO/g-CN composites under visible-light irradiation: Detailed reaction pathway and mechanism.

机构信息

Engineering Research Center for Functional Ceramics of the Ministry of Education, School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan, 430074, PR China.

Department of Chemistry, Abdul Wali Khan University Mardan, 23200, KP, Pakistan.

出版信息

J Hazard Mater. 2019 Feb 15;364:635-644. doi: 10.1016/j.jhazmat.2018.10.088. Epub 2018 Oct 31.

Abstract

Herein, we report for the first time the highly efficient degradation of 2,4-dichlorophenol (2,4-DCP) over CeO/g-CN composites (xCeO/CN) prepared via wet-chemical solution method. It is shown that the resultant nanocomposites with a proper mass ratio percentage (15%) of CeO coupled exhibit greatly enhanced visible-light activity for 2,4-dichlorophenol (2,4-DCP) degradation compared to the bare g-CN. From photoluminescence (PL) and Fluorescence (FL) results, it is suggested that enhanced photo-degradation is attributed to the significantly improved charge separation and transfer as a result of the proper band alignments between g-CN and CeO components. Further, from radical trapping experiments, it is confirmed that hydroxyl radicals (OH) are the predominant oxidants involved in the degradation of 2,4-DCP over CeO/CN composites. Furthermore, a possible reaction pathway and detailed photocatalytic mechanism for 2,4-DCP degradation is proposed mainly based on the detected liquid chromatography tandem mass spectrometry (LC-MS) intermediate products, that readily transform into CO and HO. This work would help researchers to deeply understand the reaction mechanism of 2,4-DCP and would provide feasible routes to fabricate g-CN-based highly efficient photocatalysts for environmental remediation.

摘要

在此,我们首次报道了通过湿化学溶液法制备的 CeO/g-CN 复合材料(xCeO/CN)对 2,4-二氯苯酚(2,4-DCP)的高效降解。结果表明,与纯 g-CN 相比,具有适当质量比百分比(15%)CeO 结合的所得纳米复合材料对 2,4-二氯苯酚(2,4-DCP)的降解表现出大大增强的可见光活性。从光致发光(PL)和荧光(FL)结果可以看出,增强的光降解归因于 g-CN 和 CeO 组分之间的适当能带排列导致的电荷分离和转移的显著改善。此外,通过自由基捕获实验,证实了羟基自由基(OH)是 CeO/CN 复合材料降解 2,4-DCP 中涉及的主要氧化剂。此外,主要基于检测到的液相色谱串联质谱(LC-MS)中间产物,提出了 2,4-DCP 降解的可能反应途径和详细的光催化机制,这些中间产物很容易转化为 CO 和 HO。这项工作将有助于研究人员深入了解 2,4-DCP 的反应机制,并为制备基于 g-CN 的高效光催化剂用于环境修复提供可行途径。

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