高级氧化技术处理1,4-二烷污染研究进展

doi:10.16085/j.issn.1000-6613.2021-0988

摘要/Abstract

摘要：

随着工业的发展，各种新兴有机污染物不断出现，1,4-二烷作为其中之一，广泛存在于地表水和氯代烃污染的地下水中。由于其稳定的杂环结构及高水溶性，常规的水处理技术很难完全去除1,4-二烷，高级氧化技术利用?OH、 $S O 4 ? -$ 等强氧化性自由基可有效地降解1,4-二烷。本文首先阐述了1,4-二烷的污染现状，重点概述了近年来国内外1,4-二烷降解的高级氧化技术，主要包括光催化氧化法、电化学氧化法和活化过硫酸盐氧化法等，深入分析了这些高级氧化技术对1,4-二烷的降解机理，并总结了这些技术用于处理1,4-二烷的降解效果及影响因素，最后提出了高级氧化技术处理1,4-二烷目前存在的问题及未来的研究和发展方向，以推动1,4-二烷污染处理技术的发展，为实际污染水体的治理奠定理论基础。

关键词: 高级氧化, 光催化氧化, 电化学, 活化过硫酸盐

Abstract:

With the development of industry, various emerging organic pollutants continue to appear, as an emerging organic pollutant, 1,4-dioxane is widely distributed in surface water and groundwater with chlorinated hydrocarbons contaminated sites. Due to its stable heterocyclic structure and high solubility, it is difficult to completely remove 1,4-dioxane with conventional water treatment technology. Advanced oxidation technology utilizes strong oxidizing free radicals such as OH and $S O 4 ? -$ to effectively degrade 1,4-dioxane. This paper describes the current status of 1,4-dioxane pollution, and focuses on the introduction of advanced oxidation technologies for the degradation of 1,4-dioxane at home and abroad in recent years, including photocatalytic oxidation, electrochemical oxidation and persulfate oxidation activation method, etc. Degradation mechanisms of these advanced oxidation technologies on 1,4-dioxane were deeply analyzed, and the degradation rates and its influencing factors for treating 1,4-dioxane were also summarized. Finally, the problems and development directions of advanced oxidation technologies for 1,4-dioxane pollution treatment were proposed, lay a theoretical foundation for the actual treatment of polluted water bodies.

Key words: advanced oxidation, photocatalytic oxidation, electrochemistry, activated persulfate

中图分类号:

X523

张轩, 宋小三, 赵珀, 董元华, 刘云. 高级氧化技术处理1,4-二烷污染研究进展[J]. 化工进展, 2021, 40(S2): 380-388.

ZHANG Xuan, SONG Xiaosan, ZHAO Po, DONG Yuanhua, LIU Yun. A critical review of advanced oxidation technology to treat 1,4-dioxane pollution[J]. Chemical Industry and Engineering Progress, 2021, 40(S2): 380-388.

图/表 9

图1 1,4-DX分子结构图

表1 1,4-DX理化性质

项目	数值
分子式	C₄H₈O₂
水溶性/mg·L^-1	4.31×10⁵
分子量	88.11
亨利系数/atm·m³·mol^-1	4.88×10^-6
辛醇-水分配系数	0.27
沸点/℃	101.3

表2 常见氧化剂氧化电位[1]

氧化剂种类	氧化电位/eV	相对强度（氯=1）
·OH	2.7	2
$S O 4 ? -$	2.6	1.8
O₃	2.2	1.5
$S 2 O 8 2 -$	2.1	1.5
H₂O₂	1.8	1.3
$M N O 4 -$	1.7	1.2
Cl^-	1.4	1
O₂	1.2	0.9

表2 常见氧化剂氧化电位[1]

氧化剂种类	氧化电位/eV	相对强度（氯=1）
·OH	2.7	2
$S O 4 ? -$	2.6	1.8
O₃	2.2	1.5
$S 2 O 8 2 -$	2.1	1.5
H₂O₂	1.8	1.3
$M N O 4 -$	1.7	1.2
Cl^-	1.4	1
O₂	1.2	0.9

图2 光催化氧化降解1,4-DX机理[28]

表3 紫外光氧化技术降解1,4-DX

氧化技术	处理条件	影响因素	降解效率	参考文献
UV/H₂O₂	［DX］₀=100μg·L^-1 H₂O₂=10mg·L^-1 UV=550MJ·cm^-2	天然有机物（NOM）pH、硝酸盐、铁	pH为5~7之间，1，4-DX在3.5min内降解率达到90%。高浓度硝酸盐使去除率降低约25%	［35］
真空紫外（VUV）	［DX］₀=100μg·L^-1 H₂O₂=1~5mg·L^-1 光催化剂由非晶态Si0₂纤维制成的无纺布片，表面层为TiO₂	紫外线、催化剂、pH	1，4-DX的分解速率：UV<UV/TiO₂<VUV<VUV/TiO₂，VUV和BAC或GAC组合处理可有效经济地去除1，4-DX	［36］
氯氨/UV/H₂O₂	［DX］₀=250μmol·L^-1 pH=5.8NH₂Cl=50mmol·L^-1 NHCl₂=25mmol·L^-1 UV=3500MJ·cm^-2	NH₂Cl、NHCl₂、	当氯氨处于低剂量时，NH₂Cl比NHCl₂对DX去除率高约60%~80%，NH₂Cl为2mmol·L^-1时降解速率最大	［26］
UV/H₂O₂、UV/氯氨UV/游离氯	［DX］₀=15μg·L^-1 低/高剂量：Cl₂=2.7mg·L^-1/6.8mg·L^-1 NH₂Cl=1.3mg·L^-1/4.6mg·L^-1 H₂O₂=3.1mg·L^-1/6.2mg·L^-1	催化剂种类	DX去除效率：UV> UV/H₂O₂> UV/氯氨；达到90%以上，是传统UV/H₂O₂理想的代替技术	［37］
UV/O₃	［DX］₀=150mg·L^-1 ［O₃］₀=36.7mg·L^-1 pH=6~8	pH、O₃、催化剂	1，4-DX被完全降解	［38］
UV/TiO₂膜反应器	UV=0.58W·L^-1 ［DX］₀=850μg·L^-1 催化剂：5g·L^-1	膜制备过程、污染程度、催化剂浓度、紫外线强度	1，4-DX被完全降解，通过定期反冲洗保持膜的渗透性良好	［39］

图3 微生物燃料电池装置图

图4 电解耦合臭氧技术

图5 过硫酸盐活化机理

图6 生物炭负载nFe3O4活化过硫酸盐原理图[21]

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