零价铁激活过硫酸盐降解水中铬黑T特性

张饮江, 相元泉, 鲁仙, 张亚峰, 张伯仑, 高乃云

中国环境科学 ›› 2020, Vol. 40 ›› Issue (2) : 653-660.

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中国环境科学 ›› 2020, Vol. 40 ›› Issue (2) : 653-660.
水污染与控制

零价铁激活过硫酸盐降解水中铬黑T特性

  • 张饮江1, 相元泉1, 鲁仙1,2, 张亚峰2, 张伯仑3, 高乃云2
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Characteristics on the Eriochrome black T (EBT) degradation in aquatics by Fe/persulfate system

  • ZHANG Yin-jiang1, XIANG Yuan-quan1, LU Xian1,2, ZHANG Ya-feng2, ZHANG Bo-lun3, GAO Nai-yun2
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摘要

采用零价铁/过硫酸盐(Fe0/PS)高级氧化工艺降解水中有机染料铬黑T(EBT),考察了不同体系(PS、Fe0、Fe0/PS)、PS与Fe0物质的量之比、无机阴离子(NO3-,CO32-,Cl-)、溶液初始pH值、温度以及天然有机物对EBT降解的影响.结果表明,Fe0/PS工艺降解EBT符合准一级反应动力学模型(R2>0.87);和Fe0以及单独PS处理EBT相比,Fe0/PS能够高效降解水中的EBT,20min时EBT的去除率高达96.21%.PS/Fe0降解EBT的最佳物质的量之比为1:1.5.溶液中存在的NO3-,CO32-以及天然有机物均对EBT降解有不同程度的抑制作用.EBT的降解速率随溶液初始pH值的增加逐渐减小.随着温度的增加,EBT降解速率满足先增加后减小的规律,其反应活化能(Ea)为43.98kJ/mol.EBT在实际水体中的去除率仍能够保持较高的水平.使用GC-MS识别出10种中间产物,并据此提出反应路径.ECOSAR模型分析表明EBT降解产物中小分子有机物的生态毒性高于其大分子有机物.

Abstract

Zero-valent iron (Fe0) activated persulfate (PS) advance oxidation process was applied to degrade organic Eriochrome black T (EBT) dye in water. The effects of different system (PS oxidation alone, Fe0 and Fe0/PS, PS/Fe0 molar ratio, inorganic ions(NO3-, CO32-, Cl-), initial solution pH value, temperature and natural organic matter on the EBT degradation was investigated. The experiment result indicated EBT degradation followed well with the pseudo-first-order kinetic model (R2>0.87). Compared with the Fe0 and PS oxidation alone, EBT can be removed efficiently by Fe0/PS system, the removal percentage of EBT can be reached to 96. 21%. The optimum molar ratio of PS/Fe0 for EBT degradation was 1:1.5. Inorganic ions (NO3-, CO32-) and natural organic matter had negative influence on degradation of EBT to a certain extent. The degradation rate of EBT decreased with the increase of initial solution pH. With the increase of temperature from 303K to 318K, the degradation rate increased at the beginning and then decreased slowly, meanwhile the reaction activation energy (Ea) was 43. 98kJ/mol. The removal efficiencies of EBT in real water still kept a high level. Based on the analysis result of GC-MS, ten intermediates were identified and the degradation pathway was proposed. The evaluation results of ECOSAR model showed that the ecotoxicity of small molecular organic matter from EBT degradation products was higher than that of macromolecular organic matter.

关键词

毒性评价 / 过硫酸盐 / 降解机理 / 零价铁

Key words

degradation mechanism / persulfate / toxicity assessment / zero-valent iron

引用本文

导出引用
张饮江, 相元泉, 鲁仙, 张亚峰, 张伯仑, 高乃云. 零价铁激活过硫酸盐降解水中铬黑T特性[J]. 中国环境科学. 2020, 40(2): 653-660
ZHANG Yin-jiang, XIANG Yuan-quan, LU Xian, ZHANG Ya-feng, ZHANG Bo-lun, GAO Nai-yun. Characteristics on the Eriochrome black T (EBT) degradation in aquatics by Fe/persulfate system[J]. China Environmental Science. 2020, 40(2): 653-660
中图分类号: X52   

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基金

中国博士后科学基金资助项目(2018M641983);上海市青年科技英才扬帆计划资助项目(2019YF1990)


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