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光助Fe/BiOCl活化过硫酸盐降解橙黄Ⅱ

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钟欣, 吴迪, 张凯欣, 谭紫茵, 黄伟. 光助Fe/BiOCl活化过硫酸盐降解橙黄Ⅱ[J]. 环境化学, 2019, (12): 2860-2868. doi: 10.7524/j.issn.0254-6108.2019070806
引用本文: 钟欣, 吴迪, 张凯欣, 谭紫茵, 黄伟.

光助Fe/BiOCl活化过硫酸盐降解橙黄Ⅱ

[J]. 环境化学, 2019, (12): 2860-2868. doi: 10.7524/j.issn.0254-6108.2019070806
shu
ZHONG Xin, WU Di, ZHANG Kaixin, TAN Ziyin, HUANG Wei. Photo-assisted activation of persulfate by using Fe/BiOCl for the degradation of azo dye Orange Ⅱ[J]. Environmental Chemistry, 2019, (12): 2860-2868. doi: 10.7524/j.issn.0254-6108.2019070806
Citation: ZHONG Xin, WU Di, ZHANG Kaixin, TAN Ziyin, HUANG Wei.

Photo-assisted activation of persulfate by using Fe/BiOCl for the degradation of azo dye Orange Ⅱ

[J]. Environmental Chemistry, 2019, (12): 2860-2868. doi: 10.7524/j.issn.0254-6108.2019070806
shu

光助Fe/BiOCl活化过硫酸盐降解橙黄Ⅱ

  • 环境科学与工程系, 北京师范大学珠海分校, 珠海, 519000

    • 通讯作者: 钟欣, E-mail: zhongxin@whu.edu.cn ; 
  • 基金项目:

    广东省2018年青年人才创新项目（201912017QX），北京师范大学珠海分校教师科研促进计划（201850001），北京师范大学珠海分校2018年质量工程-环境科学与工程专业虚拟仿真实验教学（201832）资助.

Photo-assisted activation of persulfate by using Fe/BiOCl for the degradation of azo dye Orange Ⅱ

  • Department of Environmental Science and Engineering, Beijing Normal University, Zhuhai, 519000, China

    • Corresponding author: ZHONG Xin, zhongxin@whu.edu.cn ; 
  • Fund Project: Supported by the Youth Innovative Foundation Guangdong Province of China (201912017QX), Science Promotion Project Funds (201850001) and Quality Engineering Project of Beijing Normal University, Zhuhai (201832).

  • 摘要:

    为研究Fe/BiOCl在光照下活化过硫酸盐（PS）产生硫酸根自由基（·SO4-）降解偶氮染料橙黄Ⅱ的催化效果，采用一步水热合成法制备铁掺杂BiOCl纳米催化剂，并用X射线衍射（XRD），扫描电子显微镜（SEM），透射电子显微镜（TEM），X射线光电子能谱（XPS）对其形貌与组成成分进行表征.结果显示，铁元素成功掺杂进入BiOCl的结构中，呈现出纳米盘状形貌结构.在光照辐射下，考察Fe/BiOCl活化PS降解橙黄Ⅱ过程中初始pH、底物浓度、Fe/BiOCl催化剂投加量和PS投加量等影响因素对橙黄Ⅱ降解处理效果的影响.结果显示，橙黄Ⅱ降解效率随着pH值的降低而升高，Fe/BiOCl和PS投加量的增加对橙黄Ⅱ的去除率出现先增加后降低的趋势.Fe/BiOCl催化剂投加量为0.5 g·L-1，PS的投加量为1 mmol·L-1的条件下时，溶液pH值为3.0，反应60 min后，橙黄Ⅱ降解的效果最佳，其降解速率符合拟一级反应动力学.通过对催化剂Fe/BiOCl稳定性研究，经5次连续循环使用后，脱色率仍然可以保持在79.6%，说明该催化剂具有良好的循环使用性能.通过投加叔丁醇（TBA），甲醇（MeOH），草酸铵（AO），对苯醌（BQ）等自由基猝灭剂，证明光助Fe/BiOCl/PS体系中具有光生空穴，硫酸根自由基，羟基自由基和超氧自由基，其中超氧自由基和光生空穴在反应体系中起重要作用.反应过程中橙黄Ⅱ的降解产物运用GC/MS进行检测，推导得出橙黄Ⅱ的降解路径.

    Abstract:

    In order to study the effect of sulfate radical (·SO4-) on the degradation of azo dye Orange Ⅱ by Fe/BiOCl catalyst activated persulfate (PS) under light irradiation, Fe doped BiOCl nanoparticles was successfully synthesized via a facile hydrothermal approach. The catalyst was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS), which clearly showed that the iron was successfully introduced into the framework of BiOCl structure with a nanoplate stracture. The effect of Fe/BiOCl dosage, PS concentration, initial pH value and initial Orange Ⅱ concentration on the degradation of Orange Ⅱ in the photo-assisted Fe/BiOCl/PS system was investigated. The results showed that Orange Ⅱ degradation efficiency was better under the acidic condition, and the degradation rate firstly increased with increased catalyst dose and PS concentrations, but decreased when the concentrations were overdosed. When pH value was 3.0, the catalyst addition was 0.5 g·L-1, PS concentration was 1 mmol·L-1, the degradation efficiency was the highest after 60 min reaction, and the degradation rate accorded with the pseudo first order reaction kinetics. The Orange Ⅱ degradation efficiency was still above 79.6% when Fe/BiOCl was used for 5 continuous cycles in the photo-assisted Fe/BiOCl/PS system, which indicates that the catalyst had a good recycling performance. Different quenching agents (tert-butyl alcohol (TBA), methanol (MeOH), ammonium oxalate (AO) and p-benzoquinone (BQ)) were added to the system for the Orange Ⅱ degradation, and the results confirmed the presence of active species (h+,·SO4-,·OH- and·O2-), and revealed the great contribution of·O2- and photo-generated holes (h+). The intermediates produced in the degradation system were also detected by GC/MS and a degradation pathway of Orange Ⅱ was proposed.

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出版历程
  • 收稿日期:  2019-07-08
  • 刊出日期:  2019-12-10

光助Fe/BiOCl活化过硫酸盐降解橙黄Ⅱ

    通讯作者: 钟欣, E-mail: zhongxin@whu.edu.cn ; 
  • 环境科学与工程系, 北京师范大学珠海分校, 珠海, 519000
  • 收稿日期:  2019-07-08
  • 网络出版日期:  2019-12-10
基金项目:

广东省2018年青年人才创新项目（201912017QX），北京师范大学珠海分校教师科研促进计划（201850001），北京师范大学珠海分校2018年质量工程-环境科学与工程专业虚拟仿真实验教学（201832）资助.

摘要: 

为研究Fe/BiOCl在光照下活化过硫酸盐（PS）产生硫酸根自由基（·SO4-）降解偶氮染料橙黄Ⅱ的催化效果，采用一步水热合成法制备铁掺杂BiOCl纳米催化剂，并用X射线衍射（XRD），扫描电子显微镜（SEM），透射电子显微镜（TEM），X射线光电子能谱（XPS）对其形貌与组成成分进行表征.结果显示，铁元素成功掺杂进入BiOCl的结构中，呈现出纳米盘状形貌结构.在光照辐射下，考察Fe/BiOCl活化PS降解橙黄Ⅱ过程中初始pH、底物浓度、Fe/BiOCl催化剂投加量和PS投加量等影响因素对橙黄Ⅱ降解处理效果的影响.结果显示，橙黄Ⅱ降解效率随着pH值的降低而升高，Fe/BiOCl和PS投加量的增加对橙黄Ⅱ的去除率出现先增加后降低的趋势.Fe/BiOCl催化剂投加量为0.5 g·L-1，PS的投加量为1 mmol·L-1的条件下时，溶液pH值为3.0，反应60 min后，橙黄Ⅱ降解的效果最佳，其降解速率符合拟一级反应动力学.通过对催化剂Fe/BiOCl稳定性研究，经5次连续循环使用后，脱色率仍然可以保持在79.6%，说明该催化剂具有良好的循环使用性能.通过投加叔丁醇（TBA），甲醇（MeOH），草酸铵（AO），对苯醌（BQ）等自由基猝灭剂，证明光助Fe/BiOCl/PS体系中具有光生空穴，硫酸根自由基，羟基自由基和超氧自由基，其中超氧自由基和光生空穴在反应体系中起重要作用.反应过程中橙黄Ⅱ的降解产物运用GC/MS进行检测，推导得出橙黄Ⅱ的降解路径.

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