催化臭氧化处理酚类化合物的研究进展与机理解析

doi:10.16085/j.issn.1000-6613.2022-0725

化工进展 ›› 2022, Vol. 41 ›› Issue (S1): 545-555.DOI: 10.16085/j.issn.1000-6613.2022-0725

催化臭氧化处理酚类化合物的研究进展与机理解析

朱昊¹^,²(), 刘汉飞¹, 季雨凡¹, 李双涛¹, 黄益平¹, 高源¹, 魏振浩¹, 主凯¹, 韩卫清², 魏卡佳²

^1.中建安装集团有限公司，江苏南京 210046
^2.南京理工大学环境与生物工程学院，江苏南京 210094

收稿日期:2022-04-22 修回日期:2022-06-23 出版日期:2022-10-20 发布日期:2022-11-10
通讯作者: 朱昊
作者简介:朱昊（1992—），男，博士，研究方向化工废水处理及资源化利用。E-mail: zhu-hao@cscec.com。
基金资助:
中建安装2020年度科技研发计划(AZ-2020-05);中国建筑股份有限公司2022年度科技研发课题(CSCEC-2022-Z-60);南京市建设系统科技计划(Ks2116)

Research advance and mechanism analysis of catalytic ozonation of phenolic compounds

ZHU Hao¹^,²(), LIU Hanfei¹, JI Yufan¹, LI Shuangtao¹, HUANG Yiping¹, GAO Yuan¹, WEI Zhenhao¹, ZHU Kai¹, HAN Weiqing², WEI Kajia²

^1.China Construction Industrial & Energy Engineering Group Co. , Ltd. , Nanjing 210000, Jiangsu, China
^2.School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, Jiangsu, China

Received:2022-04-22 Revised:2022-06-23 Online:2022-10-20 Published:2022-11-10
Contact: ZHU Hao

摘要/Abstract

摘要：

催化臭氧化技术具有操作简单、氧化效率高、二次污染小等特点，在水中酚类化合物的去除方面具有较大的技术优势。本文以酚类化合物的催化臭氧化处理为切入点，介绍了均相催化臭氧化（二价铁离子）和非均相催化臭氧化（金属型、硅基负载型、碳基负载型、铝基负载型）处理不同浓度梯度酚类化合物的研究进展。然后，基于上述研究进展，根据污染物氧化过程的探针实验结果、催化剂表征特性和有机物转化规律，阐述了苯酚等酚类化合物的催化臭氧化机理。最后，从新型催化剂的再开发、酚类化合物的广谱催化和催化氧化机理的进一步探讨方面对催化臭氧化处理酚类化合物进行了展望。

关键词: 臭氧, 氧化, 催化剂, 酚类化合物, 废水

Abstract:

Catalytic ozonation technology showed the advantages of simple operation, high oxidation efficiency and little secondary pollution in the removal of phenolic compounds. This review focused on the treatment of phenolic compounds by catalytic ozonation. The advances in homogeneous (ferrous ion) and heterogeneous (metal catalyst, silicon-based loaded catalyst, carbon-based loaded catalyst, aluminum-based loaded catalyst) catalytic ozonation of phenolic compounds in solutions of different concentrations were presented. Then, the catalytic ozonation mechanism was described according to the results of probe tests, catalyst characterizations and the transformation rules of organic matters in the pollutants oxidation process. Finally, the treatment of phenolic compounds by catalytic ozonation was prospected from the aspects of catalyst redevelopment, broad-spectrum catalytic ozonation of phenolic compounds, and further study on the catalytic ozonation mechanism.

Key words: ozone, oxidation, catalyst, phenolic compounds, wastewater

中图分类号:

TU992.3

朱昊, 刘汉飞, 季雨凡, 李双涛, 黄益平, 高源, 魏振浩, 主凯, 韩卫清, 魏卡佳. 催化臭氧化处理酚类化合物的研究进展与机理解析[J]. 化工进展, 2022, 41(S1): 545-555.

ZHU Hao, LIU Hanfei, JI Yufan, LI Shuangtao, HUANG Yiping, GAO Yuan, WEI Zhenhao, ZHU Kai, HAN Weiqing, WEI Kajia. Research advance and mechanism analysis of catalytic ozonation of phenolic compounds[J]. Chemical Industry and Engineering Progress, 2022, 41(S1): 545-555.

图/表 7

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催化剂类型	技术指标	去除率/%	规律	参考文献
Al₂O₃	双酚A对应的TOC	90.0	同颗粒态相比，粉末态Al₂O₃使系统的TOC去除率由44.0%提高至90.0%	［12］
β-MnO₂	苯酚	91.6	4种MnO₂按苯酚去除率从大到小排列顺序：β-MnO₂>δ-MnO₂>γ-MnO₂>α-MnO₂	［13］
α-MnO₂	对硝基苯酚	98.4	优化制备条件：溴化十六烷基三甲铵的摩尔浓度0.02mol/L，焙烧温度500℃，焙烧时间3h	［14］
FeOOH	苯酚	66.5	当反应时间为30min时，催化臭氧化系统苯酚质量浓度降低值为66.5 mg/L，高于臭氧氧化系统的49.5mg/L	［15］
α-Fe₂O₃	苯酚对应的COD	97	当反应时间为30min时，催化臭氧化系统苯酚COD去除率达到97%以上	［16］
零价铁	COD	79	催化剂连续使用5次后，废水COD去除率仍达70%以上	［17］
ZnO	苯酚	—	当反应时间为60min时，催化臭氧化系统苯酚质量浓度剩余值为10.5 mg/L，低于臭氧氧化系统的27.7mg/L	［18］
MgO	苯酚	—	MgO催化臭氧化处理苯酚的表观反应速率常数与MgO投量、臭氧投量、溶液pH值和温度呈正相关，与苯酚初始质量浓度呈负相关	［19］
MgO	对氯苯酚	89.8	当反应时间为15min时，MgO催化臭氧化系统中对氯苯酚去除率最高为89.8%	［20］
MgO	苯酚	—	NaCl含量对MgO催化臭氧化处理苯酚没有负面影响	［21］

催化剂类型	技术指标	去除率/%	规律	参考文献
Al₂O₃	双酚A对应的TOC	90.0	同颗粒态相比，粉末态Al₂O₃使系统的TOC去除率由44.0%提高至90.0%	［12］
β-MnO₂	苯酚	91.6	4种MnO₂按苯酚去除率从大到小排列顺序：β-MnO₂>δ-MnO₂>γ-MnO₂>α-MnO₂	［13］
α-MnO₂	对硝基苯酚	98.4	优化制备条件：溴化十六烷基三甲铵的摩尔浓度0.02mol/L，焙烧温度500℃，焙烧时间3h	［14］
FeOOH	苯酚	66.5	当反应时间为30min时，催化臭氧化系统苯酚质量浓度降低值为66.5 mg/L，高于臭氧氧化系统的49.5mg/L	［15］
α-Fe₂O₃	苯酚对应的COD	97	当反应时间为30min时，催化臭氧化系统苯酚COD去除率达到97%以上	［16］
零价铁	COD	79	催化剂连续使用5次后，废水COD去除率仍达70%以上	［17］
ZnO	苯酚	—	当反应时间为60min时，催化臭氧化系统苯酚质量浓度剩余值为10.5 mg/L，低于臭氧氧化系统的27.7mg/L	［18］
MgO	苯酚	—	MgO催化臭氧化处理苯酚的表观反应速率常数与MgO投量、臭氧投量、溶液pH值和温度呈正相关，与苯酚初始质量浓度呈负相关	［19］
MgO	对氯苯酚	89.8	当反应时间为15min时，MgO催化臭氧化系统中对氯苯酚去除率最高为89.8%	［20］
MgO	苯酚	—	NaCl含量对MgO催化臭氧化处理苯酚没有负面影响	［21］

催化剂类型	技术指标	去除率/%	规律	参考文献
Fe₂O₃/SBA-15	苯酚对应的COD	65.0	催化剂连续使用500h，含酚废水COD去除率保持65%以上，催化剂活性不低于83%	［22］
MnO₂/SBA-15	苯酚对应的TOC	35.0	高比表面积的有序纳米棒有助于催化剂表面的传质和活性位暴露，从而提高催化效率	［23］
CeO _x /SBA-16	双酚A对应的TOC	60.9	介孔催化剂比表面积大，孔分布均匀，有利于催化剂的表面传质	［24］
Ce/ZSM-5	苯酚对应的COD	85.7	Ce/ZSM-5催化臭氧化处理苯酚活性较高，稳定性较强	［25］
Co-Fe/ZSM-5	苯酚	92.9	碱改性的ZSM-5作为Co和Fe的载体，催化臭氧化处理苯酚效果显著	［26］
Cu/沸石	COD	72.4	Cu/沸石催化臭氧化处理煤化工废水效果良好，对应的COD去除率为72.4%	［27］
MnO _x /泡沫陶瓷	苯酚	89.6	当Mn(NO₃)₂的摩尔浓度为0.5 mol/L时，制备的催化剂稳定性最佳	［28］
CoAl₂O₄/蜂窝陶瓷	对苯二酚	81.2	采用涂覆法制备的催化剂呈尖晶石结构，比表面积、孔径和孔容较大	［29］
Mn-Co/蜂窝陶瓷	对苯二酚	78.0	采用涂覆盖制备的催化剂主要活性组分为Mn₃O₄和CoO	［30］

催化剂类型	技术指标	去除率/%	规律	参考文献
Fe₂O₃/SBA-15	苯酚对应的COD	65.0	催化剂连续使用500h，含酚废水COD去除率保持65%以上，催化剂活性不低于83%	［22］
MnO₂/SBA-15	苯酚对应的TOC	35.0	高比表面积的有序纳米棒有助于催化剂表面的传质和活性位暴露，从而提高催化效率	［23］
CeO _x /SBA-16	双酚A对应的TOC	60.9	介孔催化剂比表面积大，孔分布均匀，有利于催化剂的表面传质	［24］
Ce/ZSM-5	苯酚对应的COD	85.7	Ce/ZSM-5催化臭氧化处理苯酚活性较高，稳定性较强	［25］
Co-Fe/ZSM-5	苯酚	92.9	碱改性的ZSM-5作为Co和Fe的载体，催化臭氧化处理苯酚效果显著	［26］
Cu/沸石	COD	72.4	Cu/沸石催化臭氧化处理煤化工废水效果良好，对应的COD去除率为72.4%	［27］
MnO _x /泡沫陶瓷	苯酚	89.6	当Mn(NO₃)₂的摩尔浓度为0.5 mol/L时，制备的催化剂稳定性最佳	［28］
CoAl₂O₄/蜂窝陶瓷	对苯二酚	81.2	采用涂覆法制备的催化剂呈尖晶石结构，比表面积、孔径和孔容较大	［29］
Mn-Co/蜂窝陶瓷	对苯二酚	78.0	采用涂覆盖制备的催化剂主要活性组分为Mn₃O₄和CoO	［30］

催化剂类型	技术指标	去除率/%	规律发现	参考文献
Mn/Al₂O₃	苯酚	82.7	当Al₂O₃表面负载4%的Mn时，苯酚的催化臭氧化效率最高	［39］
Mn/Al₂O₃	苯酚	76.3	Mn/Al₂O₃优化制备条件为：Mn负载量10%，焙烧温度500℃，焙烧时间5h	［40］
Ce/Al₂O₃	苯酚	98.3	Ce/Al₂O₃优化制备条件为：Ce负载量1%，焙烧温度500℃，焙烧时间1h	［41］
Cu/Al₂O₃	COD	50.0	Cu/Al₂O₃晶型良好，比表面积大，中孔结构丰富	［42］
Ni/Al₂O₃	对苯二酚	78.0	Ni/Al₂O₃优化制备条件为：50%硝酸盐浸渍载体8h，焙烧温度600℃，焙烧时间3h	［43］
Mn-Fe-Ce/Al₂O₃	苯酚	88.0	催化剂循环使用5次后仍具有较高的催化活性	［44］

催化臭氧化处理酚类化合物的研究进展与机理解析

Research advance and mechanism analysis of catalytic ozonation of phenolic compounds

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