纺织学报 ›› 2024, Vol. 45 ›› Issue (06): 105-112.doi: 10.13475/j.fzxb.20230507301

• 染整工程 • 上一篇    下一篇

铁-三联吡啶配合物活化高碘酸盐体系构建及其对染色废水的催化降解机制

武守营1,2, 黄启超2, 张开封2, 张琳萍1,2,3, 钟毅1,2,3, 徐红1,2,3, 毛志平1,2,3()   

  1. 1.东华大学 化学与化工学院, 上海 201620
    2.东华大学 生态纺织教育部重点实验室, 上海 201620
    3.山东中康国创先进印染技术研究院有限公司 国家先进印染技术创新中心, 山东 泰安 271000
  • 收稿日期:2023-05-30 修回日期:2023-11-21 出版日期:2024-06-15 发布日期:2024-06-15
  • 通讯作者: 毛志平(1969—),男,研究员,博士。主要研究方向为纺织清洁印染加工及功能整理。E-mail:zhpmao@dhu.edu.cn。
  • 作者简介:武守营(1992—),女,博士生。主要研究方向为金属配合物的制备及其催化性能研究。
  • 基金资助:
    中央高校基本科研业务费专项资金资助项目(2232023G-04)

Construction of catalytic system by FeⅢ(tpy)Cl3 complexes-activated periodate and its catalytic degradation mechanism for dyeing wastewater

WU Shouying1,2, HUANG Qichao2, ZHANG Kaifeng2, ZHANG Linping1,2,3, ZHONG Yi1,2,3, XU Hong1,2,3, MAO Zhiping1,2,3()   

  1. 1. College of Chemistry and Chemical Engineering, Donghua University, Shanghai 201620, China
    2. Key Laboratory of Science and Technology of Eco-Textile, Ministry of Education, Donghua University, Shanghai 201620, China
    3. National Innovation Center of Advanced Dyeing & Finishing Technology, Shandong Zhongkang Guochuang Research Institute of Advanced Dyeing & Finishing Technology Co., Ltd., Taian, Shandong 271000, China
  • Received:2023-05-30 Revised:2023-11-21 Published:2024-06-15 Online:2024-06-15

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摘要：

为开发新型、高效的染色废水处理方法,通过铁-三联吡啶(FeⅢ(tpy)Cl3)配合物活化高碘酸盐(PI)构建了FeⅢ(tpy)Cl3/PI催化氧化体系。在此基础上,采用酸性红1(AR1)作为染色废水模型污染物测试了该体系的催化降解性能,并通过捕获和探针实验研究了FeⅢ(tpy)Cl3配合物活化PI降解酸性红1的机制。结果表明:FeⅢ(tpy)Cl3配合物能够高效活化PI实现酸性红1的快速降解,15 min内对AR1的去除率高达98%;FeⅢ(tpy)Cl3/PI体系对酸性红1的降解符合伪一级动力学模型,同时酸性红1的降解速率常数随FeⅢ(tpy)Cl3配合物和PI浓度的增加而呈线性增加;在FeⅢ(tpy)Cl3/PI体系中包含超氧自由基、单线态氧以及高价铁,这些活性物质共同促进酸性红1的降解;该体系不仅对多种有机物的降解表现出普适性,同时催化降解过程不受溶液pH值以及常见无机盐离子的干扰。

关键词: 配合物, 高碘酸盐, 染色废水, 降解, 催化机制, 废水处理, 铁-三联吡啶

Abstract:

Objective The dyeing wastewater poses a threat to the ecological environment. Advanced oxidation processes (AOPs) exhibit excellent oxidation efficiency in wastewater treatment. The solid-state and stability of periodate (PI) make it obtained wide attention. As a result, PI-based AOPs are gradually gaining research and being tried for the treatment of dyeing wastewater. However, current transition metal-based activators for PI often require larger doses to obtain the desired effect, which undoubtedly increases the cost of wastewater treatment. Metal coordination complexes are applied similarly to biological enzymes, with trace and efficient application effects. This study aimed to construct a novel catalytic system by activating PI by FeⅢ(tpy)Cl3 complex to investigate its application prospects in wastewater treatment and to elucidate the catalytic mechanism.

Method The catalytic degradation performance of the FeⅢ(tpy)Cl3/PI system was tested using the dye Acid Red 1 (AR1) as the target pollutant. The effects of catalyst and oxidant dosage, pH, and temperature on the catalytic performance of this system were explored. Meanwhile, the catalytic mechanism of the system was investigated by capture and probe experiments. Moreover, the practical application prospects of the system were evaluated by testing the degradation efficiency of various organics and the resistance to inorganic salt ions.

Results The result showed that the FeⅢ(tpy)Cl3 complexes have excellent activation effects on PI, which could remove 98% of AR1 within 15 min. More importantly, the performance of the FeⅢ(tpy)Cl3/PI system is much higher than that of the previously reported FeⅢ(tpy)Cl3/H2O2 system. Meanwhile, the test results show that the concentration of FeⅢ(tpy)Cl3 and PI has a great influence on the performance of the FeⅢ(tpy)Cl3/PI system. In detail, the degradation of AR1 in the FeⅢ(tpy)Cl3/PI system is following the pseudo-first-order kinetic model, while the rate constant of AR1 degradation increase linearly with the increase of FeⅢ(tpy)Cl3 and PI dose. Moreover, the results show that the catalytic performance of FeⅢ(tpy)Cl3/PI system is almost independent of pH and could achieve efficient degradation of the dye over a wide pH range (3-9). Also, the increase in temperature could increase the catalytic activity of the FeⅢ(tpy)Cl3/PI system and accelerate the degradation of AR1. In addition, the active species in this system were investigated using methanol, benzoquinone, and furfuryl alcohol as hydroxyl radical, superoxide radical, and singlet oxygen trapping agents, respectively, and PMSO as a probe for high-valent metal-oxo. The results of mechanism studies show that FeⅢ(tpy)Cl3/PI system includes superoxide radicals, singlet oxygen, and high-valent metal-oxo, and these active species together promote the degradation of AR1. The removal rates of sulfamethoxazole, 2,4-dichlorophenol, 2,4,6-trichlorophenol, and rhodamine B in the FeⅢ(tpy)Cl3/PI system are 100%, 81%, 89%, and 89%, respectively, indicating that the FeⅢ(tpy)Cl3/PI system is well suited for the removal of most organics. Inorganic salt ions are usually included in the actual organic wastewater. The results show that the catalytic system is not disturbed by common inorganic salt ions for the degradation of organic matter and has good prospects for practical application.

Conclusion FeⅢ(tpy)Cl3 has excellent activation performance for PI, and the removal rate of AR1 is up to 98% within 15 min, which is much higher than the conventional FeⅢ(tpy)Cl3/H2O2 system. Compared with other iron-based catalysts, FeⅢ(tpy)Cl3 complexes are simple to prepare and require only minute doses to achieve efficient degradation of organic matter, which helps to reduce the economic cost of wastewater treatment. In addition, the system shows universality for the degradation of various organics, and the catalytic degradation process do not interfere with the solution pH and common inorganic salt ions, which makes this system excellent prospect for practical wastewater treatment applications. Overall, this study provides a novel PI activator and also provides an efficient method for dyeing wastewater treatment.

Key words: coordination complex, periodate, dyeing wastewater, degradation, catalytic mechanism, wastewater treatment, FeⅢ (tpy) Cl3

中图分类号: 

  • TS190.3

图1

不同体系对AR1的降解情况对比"

图2

FeⅢ(tpy)Cl3和PI浓度对FeⅢ(tpy)Cl3/PI体系催化性能的影响"

图3

pH值和温度对FeⅢ(tpy)Cl3/PI体系催化性能的影响"

图4

FeⅢ(tpy)Cl3/PI体系中活性物质的鉴定结果"

图5

FeⅢ(tpy)Cl3/PI体系的应用性能"

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