臭氧微纳米气泡氧化降解典型紫外线过滤剂的效能和机理

姜民禹; 郭若男; 郭昌胜; 徐建

doi:10.12153/j.issn.1674-991X.20240039

臭氧微纳米气泡氧化降解典型紫外线过滤剂的效能和机理

doi: 10.12153/j.issn.1674-991X.20240039

姜民禹^{1, 2,},
郭若男^{1, 2},
郭昌胜^{1, 2},
徐建^{1, 2, ,}

1.
中国环境科学研究院环境健康风险评估与研究中心
2.
生态环境部化学品生态效应与风险评估重点实验室

基金项目: 国家杰出青年科学基金项目（42325706）

详细信息

作者简介:
姜民禹（1998— ），男，硕士研究生，主要从事水处理研究，16622720670@163.com

通讯作者:
徐建（1978—），男，研究员，主要从事新污染物风险和控制研究，xujian@craes.org.cn

中图分类号: X703
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- 被引次数: 0
出版历程
- 收稿日期: 2024-01-18
- 录用日期: 2024-04-23
- 修回日期: 2024-04-03

Efficiency and mechanism of oxidative degradation of typical UV filters by ozone micro-nano bubbles

JIANG Minyu^{1, 2
,},
GUO Ruonan^{1, 2},
GUO Changsheng^{1, 2},
XU Jian^{1, 2
, ,}

1.
Center for Environmental Health Risk Assessment and Research, Chinese Research Academy of Environmental Sciences
2.
State Environmental Protection Key Laboratory of Ecological Effect and Risk Assessment of Chemicals

摘要

摘要:
臭氧微纳米气泡具有高臭氧利用率和高臭氧传质速率的优势，采用臭氧微纳米气泡氧化降解紫外线过滤剂二乙氨基羟基苯甲酰基苯甲酸己酯（DHHB），通过改变不同溶气方式和液相臭氧浓度，考察了臭氧微纳米气泡的性能及对DHHB的降解机制，同时探讨了不同温度、pH、天然有机质和不同离子强度等因素对降解效果的影响。结果表明：臭氧微纳米气泡比臭氧传统气泡对污染物氧化性能有明显提升，体系内液相臭氧、羟基自由基浓度、羟基自由基产率与臭氧利用率显著增加，在室温（25 ℃）、气相臭氧浓度为10.22 mg/L、pH为11时，对DHHB的去除率在60 min内可达87.3%，去除率是臭氧传统气泡的2.02倍。天然有机质和碳酸氢根离子对DHHB降解过程有不同程度的抑制作用。通过淬灭试验分析，65.2%的DHHB降解由羟基自由基贡献，14.9%由超氧自由基贡献。研究证实了利用臭氧微纳米气泡体系处理水中DHHB的可行性，为该体系的实际应用提供了理论参考。
- 臭氧氧化 /
- 微纳米气泡 /
- 氧化机理 /
- 自由基 /
- 紫外线过滤剂
Abstract:
Ozone micro-nano bubbles are known for their beneficial traits, such as high ozone utilization and mass transfer rates. In this study, ozone micro-nano bubbles were utilized to degrade the ultraviolet filter, diethylamino hydroxybenzoyl hexyl benzoate (DHHB). The characteristics of ozone micro-nano bubbles and their degradation mechanism on DHHB were studied by varying dissolved gas modes and liquid-phase ozone concentrations, and the impacts of temperature, pH, natural organic matter and different ion strengths on the degradation efficiency were explored. The results indicated that the oxidation efficiency of ozone micro-nano bubbles exceeded that of conventional ozone bubbles. The concentration of liquid-phase ozone, hydroxyl radicals, hydroxyl radical yield, and ozone utilization rate in the system increased significantly. The DHHB removal rate achieved 87.3% within 60 min at 25 °C, with a gas-phase ozone concentration of 10.22 mg/L and pH of 11. The removal effectiveness was 2.02 times greater than that of traditional ozone bubbles. Natural organic matter and bicarbonate ions inhibited the degradation of DHHB to different extents. According to the quenching test, 65.2% of DHHB degradation was contributed by hydroxyl radicals and 14.9% by superoxide radicals. This study confirms the feasibility of utilizing an ozone micro-nano bubble system for treating DHHB in water, and offers a theoretical basis for the practical implementation of this system.
- ozonation /
- micro-nano bubbles /
- oxidation mechanism /
- free radical /
- UV filters

HTML全文

图 1 不同溶气方式试验装置

①—臭氧发生部分；②—微纳米气泡发生部分；③—反应与取样部分；④—废气处理部分。

Figure 1. Experimental setups with different dissolved gas methods

下载: 全尺寸图片幻灯片

图 2 反应体系内液相臭氧浓度与臭氧暴露量随时间的变化

注：图例中未标注传统气泡的均为臭氧微纳米气泡，全文同。

Figure 2. Variation of liquid-phase ozone concentration and ozone exposure in the reaction system with time

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图 3 反应体系内·OH的暴露量与产率

Figure 3. Amount of exposure and yield of hydroxyl radical in the reaction system

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图 4 不同影响因素下的臭氧利用率

Figure 4. Ozone utilization efficiency under different influencing factors

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图 5 不同外加条件对DHHB降解效果的影响

Figure 5. Effects of different external conditions on the degradation of DHHB

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图 6 不同化学参数对臭氧微纳米气泡降解DHHB的影响

Figure 6. Effect of chemical parameters on the degradation of DHHB by ozone micro-nano bubbles

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图 7 自由基淬灭剂对DHHB降解的影响

Figure 7. Effect of free radical quenchers on DHHB degradation

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表 1 不同外加条件下DHHB拟一级动力学分析

Table 1. Pseudo-first-order kinetic analysis of DHHB degradation under different external conditions

处理方式	外加条件	k_obs/min⁻¹	R²
溶气方式	臭氧微纳米气泡	0.039 7	0.971
	臭氧传统气泡	0.011 1	0.972
	氧气微纳米气泡	0.002 9	0.918
进气气相臭氧浓度/（mg/L）	2.89	0.020 4	0.963
	5.28	0.024 6	0.962
	10.22	0.038 7	0.979
温度/℃	20	0.0387	0.979
	30	0.0359	0.974
	40	0.0312	0.974
pH	3	0.019 9	0.975
	5	0.022 7	0.960
	7	0.028 0	0.976
	9	0.040 4	0.954
	11	0.043 7	0.926

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