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应用生态学报 ›› 2020, Vol. 31 ›› Issue (1): 333-339.doi: 10.13287/j.1001-9332.202001.035

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黑磷纳米片光催化甲基橙降解机理

韩雅琦1,2, 雷蕾1,2, 杨晨3, 张思玉1*, 赵青1, 张雪娇1   

  1. 1中国科学院沈阳应用生态研究所, 沈阳 110016;
    2中国科学院大学, 北京 100049;
    3东北大学资源与土木工程学院, 沈阳 110004
  • 收稿日期:2019-05-01 出版日期:2020-01-15 发布日期:2020-01-15
  • 通讯作者: E-mail: syzhang@iae.ac.cn
  • 作者简介:韩雅琦, 男, 1993年生, 硕士研究生。主要从事环境过程与环境毒理研究。E-mail: a512037441@qq.com
  • 基金资助:
    国家自然科学基金项目(21607165,41603120,41703107,418773891)、国家重点研发计划项目(2016YFD0800305)、沈阳市中青年科技创新人才团队支持计划项目(RC170020)和中国科学院青年创新促进会项目(2017242)

Mechanism underlying photocatalyzed degradation of methyl orange by layered black phosphorus

HAN Ya-qi1,2, LEI Lei1,2, YANG Chen3, ZHANG Si-yu1*, ZHAO Qing1, ZHANG Xue-jiao1   

  1. 1Institute of Applied Ecology, Chinese Academy of Sciences, Shenyang 110016, China;
    2 University of Chinese Academy of Sciences, Beijing 100049, China;
    3School of Resources and Civil Engineering, Northeastern University, Shenyang 110004, China
  • Received:2019-05-01 Online:2020-01-15 Published:2020-01-15
  • Contact: E-mail: syzhang@iae.ac.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21607165, 41603120,41703107,418773891), the National Key Research and Development Program of China (2016YFD0800305), the Youth and Middle-aged Science and Technology Innovation Talent Team of Shenyang (RC170020) and the Youth Innovation Promotion Association of China (2017242).

摘要: 偶氮废水大量排放到环境中会对生态系统和人类健康造成严重威胁,发展偶氮染料废水的高效处理技术具有实际意义。光催化法由于工艺简单、处理彻底等优点具有应用前景。本研究利用液相剥离法制备黑磷纳米片(LBP),以甲基橙(MO)为例,考察LBP对偶氮染料的光催化能力;利用淬灭及荧光探针试验判断体系中参与反应的主要瞬态物种;结合液相色谱-质谱的产物鉴定结果,阐明光催化降解机理。结果表明: MO在酸性(pH=3.0)和碱性(pH=11.0)条件下的降解速率(kobs)高于中性条件下(pH=7.0)。LBP光照下产生羟基自由基(·OH)进攻偶氮键使双键断裂生成中间产物,后者被·OH继续氧化,生成主要降解产物N,N-二甲基-4-(2-对苯甲基肼)苯胺、2-二甲胺基-5-((4-(二甲胺基)苯基)二氮基)苯酚和N,N-二甲基-4-硝基苯胺。

Abstract: A large amount of azo dye wastewater is discharged into the environment, with serious risks to ecosystems and human health. Therefore, the development of treatment technology of azo dye wastewater was of practical significance. Photocatalytic methods showed promising application prospects due to easy to implement and effective. In this study, layered black phosphorus nanosheet (LBP) was used as a catalyst through liquid phase exfoliation method. Methyl orange (MO) was employed as a model azo dye to investigate the catalytic mechanism of LBP. The dominant transient species involved in the photocatalytic reaction was probed by quenching and fluorescence probe experiments. Degradation pathways of MO were proposed according to degradation products identified by the liquid chromatography-mass spectrometry. The results showed that degradation rate (kobs) of MO at acidic condition (pH=3.0) or alkaline condition (pH=11.0) was higher than that at neutral condition (pH=7.0). Degradation pathways of MO included that the azo bond was attacked by hydroxyl radicals (·OH) photogenerated by the LBP, and the intermediate products were further oxidized by ·OH to produce N, N-dimethyl-4-(2-p-phenylmethylhydrazine) aniline, 2-(dimethylamino)-5-((4(dimethylamino) phenyl) diazenyl) phenol and N, N-dimethyl-4-nitroaniline.