过渡金属活化过硫酸盐降解有机废水技术研究进展

doi:10.16085/j.issn.1000-6613.2020-1469

化工进展 ›› 2021, Vol. 40 ›› Issue (6): 3480-3488.DOI: 10.16085/j.issn.1000-6613.2020-1469

过渡金属活化过硫酸盐降解有机废水技术研究进展

田婷婷¹^,²(), 李朝阳¹^,², 王召东², 陆慧², 李新冬¹(), 毛艳丽², 宋忠贤², 朱新锋²()

^1.江西理工大学土木与测绘工程学院，江西赣州 341000
^2.河南城建学院市政与环境工程学院，河南平顶山 467000

收稿日期:2020-07-29 修回日期:2020-10-19 出版日期:2021-06-06 发布日期:2021-06-22
通讯作者: 李新冬,朱新锋
作者简介:田婷婷（1996—），女，硕士研究生，研究方向为污水处理技术。E-mail：723341434@qq.com。
基金资助:
国家自然科学基金(51864017);江西省教育厅科技项目(GJJ160619);国家级大学生创新创业训练项目(201910407009);河南省科技厅项目(182102311016)

Research progress of transition metal activated persulfate to degrade organic wastewater

TIAN Tingting¹^,²(), LI Chaoyang¹^,², WANG Shaodong², LU Hui², LI Xindong¹(), MAO Yanli², SONG Zhongxian², ZHU Xinfeng²()

^1.School of Civil and Surveying Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, Jiangxi, China
^2.Faculty of Environmental and Municipal Engineering, Henan University of Urban Construction, Pingdingshan, 467000, Henan, China

Received:2020-07-29 Revised:2020-10-19 Online:2021-06-06 Published:2021-06-22
Contact: LI Xindong,ZHU Xinfeng

摘要/Abstract

摘要：

活化过硫酸盐高级氧化技术用于降解水体中有机污染物备受关注，其中采用过渡金属活化过硫酸盐降解有机污染物的研究越来越多，也取得了良好的效果。本文综述了近几年来国内外利用以过渡金属为基础的催化剂活化过硫酸盐降解污染物的应用研究；阐述了贵金属催化剂、单金属催化剂、复合金属催化剂（尖晶石结构催化剂、纳米核壳结构催化剂、三维纳米结构催化剂）在水体中降解有机污染物的研究进展；探讨了过渡金属催化剂的优缺点和研究现状，最后提出了该活化体系目前面临的问题，期望为过渡金属活化过硫酸盐降解污染物技术的应用提供参考。

关键词: 废水, 活化, 催化剂, 过渡金属, 过硫酸盐

Abstract:

The use of activated persulfate advanced oxidation technology to degrade organic pollutants in water has attracted much attention. Among them, more and more researches focused on that transition metals activate persulfate to degrade organic pollutants exhibited the excellent performance. In this paper, the application research of degrading pollutants by transition metal-based catalysts via activate persulfate in recent years was reviewed. Furthermore, precious metal, single metal and composite metal catalysts (nano-spinel structure catalysts, nano-cores shell structure catalysts and three-dimensional nano-structured catalysts) in the degradation of organic pollutants were investigated. Besides, the advantages and disadvantages of transition metal catalysts were discussed, as well as the current research status. Finally, the problems facing the activation system were proposed. It is expected to provide a reference for the application of transition metal activated persulfate degradation technology.

Key words: waste water, activation, catalyst, transition metal, persulfate

中图分类号:

田婷婷, 李朝阳, 王召东, 陆慧, 李新冬, 毛艳丽, 宋忠贤, 朱新锋. 过渡金属活化过硫酸盐降解有机废水技术研究进展[J]. 化工进展, 2021, 40(6): 3480-3488.

TIAN Tingting, LI Chaoyang, WANG Shaodong, LU Hui, LI Xindong, MAO Yanli, SONG Zhongxian, ZHU Xinfeng. Research progress of transition metal activated persulfate to degrade organic wastewater[J]. Chemical Industry and Engineering Progress, 2021, 40(6): 3480-3488.

图/表 9

表1 各种活化方式的活化机理比较

活化方式	机理	主要的自由基种类	特点	参考文献
热活化	S₂O $8 2 -$ +heat $→$ SO $4 · -$ +SO $4 · -$ SO $4 · -$ +H₂O $→$ ·OH+SO $4 2 -$ +H⁺ SO $4 · -$ +OH^- $→$ ·OH+SO $4 2 -$	·OH和SO $4 · -$ 共同作用，·OH的作用大于SO $4 · -$	氧化性强，需要高温环境；在中性或碱性下反应速率高，污水中存在阴离子会影响污染物的降解	［18］
碱活化	2S₂O $8 2 -$ +2H₂O+OH^- $→$ 3SO $4 2 -$ +SO $4 · -$ +O $2 · -$ +4H⁺	还原剂（超氧化物）和SO $4 · -$	污染物在24h才能被完全降解，反应时间过长，且需要的过硫酸盐和碱的含量很大	［18］
UV活化	S₂O $8 2 -$ +hv $→$ SO $4 · -$ +SO $4 · -$	·OH和SO $4 · -$ 共同作用，SO $4 · -$ 的作用大于·OH	受pH的影响较大，会随着污水的成分不同产生不同的副产物，增加二次污染	［18］
以碳为基础的材料活化	利用以碳为基础的材料具有比表面积大、吸附性能高、化学稳定性好等特点将金属离子负载在其表面增加活性位点，提高污染物的降解率	SO $4 · -$ 、·OH、O $2 · -$	催化剂稳定性好，重复使用率高，适用pH范围广，可以降解的污染物种类多，但催化剂的制备过程复杂，制作成本高	［18］
电活化	在电流的作用下，水被电解产生·OH，附着在电极表面的表面活性剂得失电子，两者共同降解污染物	SO $4 · -$ 、·OH	受电流密度影响较大，阳极材料受限制，非活性阳极材料需要加入可以产生高活性物质的表面活性剂，成本高	［18］
超声活化	超声波产生的气蚀、高温高压促使过硫酸盐中的O—O键断裂，产生SO $4 · -$ ；超声波产生的能量增加了溶液中物质的传输速度，加快反应速率	SO $4 · -$ 、·OH	活化过程受超声功率、频率、pH、温度的影响较大；对处理大量的实际污水存在困难	［18］

表1 各种活化方式的活化机理比较

活化方式	机理	主要的自由基种类	特点	参考文献
热活化	S₂O $8 2 -$ +heat $→$ SO $4 · -$ +SO $4 · -$ SO $4 · -$ +H₂O $→$ ·OH+SO $4 2 -$ +H⁺ SO $4 · -$ +OH^- $→$ ·OH+SO $4 2 -$	·OH和SO $4 · -$ 共同作用，·OH的作用大于SO $4 · -$	氧化性强，需要高温环境；在中性或碱性下反应速率高，污水中存在阴离子会影响污染物的降解	［18］
碱活化	2S₂O $8 2 -$ +2H₂O+OH^- $→$ 3SO $4 2 -$ +SO $4 · -$ +O $2 · -$ +4H⁺	还原剂（超氧化物）和SO $4 · -$	污染物在24h才能被完全降解，反应时间过长，且需要的过硫酸盐和碱的含量很大	［18］
UV活化	S₂O $8 2 -$ +hv $→$ SO $4 · -$ +SO $4 · -$	·OH和SO $4 · -$ 共同作用，SO $4 · -$ 的作用大于·OH	受pH的影响较大，会随着污水的成分不同产生不同的副产物，增加二次污染	［18］
以碳为基础的材料活化	利用以碳为基础的材料具有比表面积大、吸附性能高、化学稳定性好等特点将金属离子负载在其表面增加活性位点，提高污染物的降解率	SO $4 · -$ 、·OH、O $2 · -$	催化剂稳定性好，重复使用率高，适用pH范围广，可以降解的污染物种类多，但催化剂的制备过程复杂，制作成本高	［18］
电活化	在电流的作用下，水被电解产生·OH，附着在电极表面的表面活性剂得失电子，两者共同降解污染物	SO $4 · -$ 、·OH	受电流密度影响较大，阳极材料受限制，非活性阳极材料需要加入可以产生高活性物质的表面活性剂，成本高	［18］
超声活化	超声波产生的气蚀、高温高压促使过硫酸盐中的O—O键断裂，产生SO $4 · -$ ；超声波产生的能量增加了溶液中物质的传输速度，加快反应速率	SO $4 · -$ 、·OH	活化过程受超声功率、频率、pH、温度的影响较大；对处理大量的实际污水存在困难	［18］

图1 Fe2+与Fe3+之间的转化

图2 Co2+与Co3+之间的转化

图3 Mn+与M(n+1)+之间的转化示意

图4 尖晶石结构催化剂活化原理

图5 纳米核壳结构活化原理

图6 海胆状催化剂

图7 三维中空管状催化剂

图8 三维介孔状催化剂

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过渡金属活化过硫酸盐降解有机废水技术研究进展

Research progress of transition metal activated persulfate to degrade organic wastewater

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