抗坏血酸/过硫酸盐氧化去除土壤中阿特拉津的效率及机理

杜宇; 孙淑晴; 戴雯; 曹梦华; 涂书新; 熊双莲

doi:10.13205/j.hjgc.202406017

抗坏血酸/过硫酸盐氧化去除土壤中阿特拉津的效率及机理

doi: 10.13205/j.hjgc.202406017

华中农业大学, 武汉 430070

基金项目:

湖北省自然科学基金(2022CFD003)

国家自然科学基金(21976065)

详细信息

作者简介:
杜宇(1995-),女,硕士研究生,主要研究方向为环境污染与修复。884511916@qq.com

通讯作者:
曹梦华(1985-),男,副教授,主要研究方向为土壤污染与修复。caomenghua@mail.hzau.edu.cn

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- 文章访问数: 59
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- 被引次数: 0
出版历程
- 收稿日期: 2023-09-21
- 网络出版日期: 2024-07-11

REMOVAL EFFICIENCY AND MECHANISM OF ATRAZINE FROM CONTAMINATED SOIL BY PERSULFATE AND ASCORBIC ACID

Huazhong Agricultural University, Wuhan 430070, China

摘要

摘要: 研究了抗坏血酸/过硫酸盐去除土壤中阿特拉津的效率、影响因素及机理。当抗坏血酸和过硫酸盐浓度分别为10,30 mmol/L,初始pH为3.0时,土壤中阿特拉津降解率达到92.4%。共存的无机阴离子(Cl^-和HCO^-₃)会抑制阿特拉津的降解。低浓度溶解态有机质(0~2.5 mg/L)能促进阿特拉津的氧化降解,高浓度溶解态有机质(>5 mg/L)会抑制阿特拉津的氧化降解。抗坏血酸一方面直接诱导过硫酸盐活化产生硫酸根自由基(SO^-₄·)和羟基自由基(·OH),另一方面促进土壤释放铁离子和Fe²⁺/Fe³⁺的循环,从而间接增强过硫酸盐的活化性能。此外,抗坏血酸增强了土壤中阿特拉津的解吸,降低了阿特拉津与氧化性自由基的传质阻力,有利于提升阿特拉津的氧化降解效率。抗坏血酸/过硫酸盐体系降解阿特拉津主要包括脱烷基氧化、脱氯和羟基化3种途径。
- 抗坏血酸 /
- 过硫酸盐 /
- 阿特拉津 /
- 土壤修复 /
- 氧化降解
Abstract: The efficiency, influencing factors, and mechanism of removing atrazine from soil by ascorbic acid/persulfate were studied. When the concentrations of ascorbic acid and persulfate were 10 and 30 mmol/L, respectively, the degradation ratio of atrazine in soil achieved 92.4% at a pH of 3.0. The co-existing inorganic anions (Cl^- and HCO^-₃) could inhibit the degradation of atrazine. Low concentrations of dissolved organic matter (0 to 2.5 mg/L) could promote the degradation of atrazine, while high concentrations of dissolved organic matter (>5 mg/L) could inhibit the oxidation of atrazine. On the one hand, ascorbic acid could directly activate persulfate to generate sulfate radicals and hydroxyl radicals. On the other hand, ascorbic acid could promote the release of iron ions from the soil and the cycle of Fe²⁺/Fe³⁺, which indirectly enhances the activation of persulfate. In addition, ascorbic acid could enhance the desorption of atrazine from the soil and reduce the mass transfer resistance between atrazine and oxidative radicals, which was beneficial for promoting atrazine oxidation. The degradation pathways of atrazine in the ascorbic acid/persulfate system mainly involved dealkylation oxidation, dechlorination, and hydroxylation.
- ascorbic acid /
- persulfate /
- atrazine /
- soil remediation /
- oxidation

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参考文献(28)

[1]	HUANG M Y, ZHAO Q, DUAN R Y, et al. The effect of atrazine on intestinal histology, microbial community and short chain fatty acids in Pelophylax nigromaculatus tadpoles[J]. Environmental Pollution, 2021, 288: 117702.
[2]	BAYATI M, NUMAAN M, KADHEM A, et al. Adsorption of atrazine by laser induced graphitic material: an efficient, scalable and green alternative for pollution abatement[J]. Journal of Environmental Chemical Engineering, 2020, 8: 104407.
[3]	王万红, 王彦红, 王世成, 等. 辽北农田土壤除草剂和有机氯农药残留特征[J]. 土壤通报, 2010, 41(3): 716-722.
[4]	CHANG J N, FANG W, CHEN L, et al. Toxicological effects, environmental behaviors and remediation technologies of herbicide atrazine in soil and sediment: a comprehensive review[J]. Chemosphere, 2022, 307: 136006.
[5]	宋佳, 潘妍, 王皙玮, 等. 除草剂阿特拉津在土壤中降解方式的研究现状[J]. 中国农学通报, 2022, 38(25): 90-95.
[6]	LI X Y, JIE B R, LIN H D, et al. Application of sulfate radicals-based advanced oxidation technology in degradation of trace organic contaminants (TrOCs): recent advances and prospects[J]. Journal of Environment Management, 2022, 308: 114664.
[7]	肖鹏飞, 姜思佳. 活化过硫酸盐氧化法修复有机污染土壤的研究进展[J]. 化工进展, 2018, 37(12): 4862-4873.
[8]	HOU X J, HUANG X P, AI Z H, et al. Ascorbic acid induced atrazine degradation[J]. Journal of Hazardous Materials, 2017, 327: 71-78.
[9]	曹梦华, 涂书新, 张娥, 等. 抗坏血酸还原降解土壤中的阿特拉津[J]. 环境工程, 2019, 37(12): 207-211.
[10]	CAO M H, HOU Y Z, ZHANG E, et al. Ascorbic acid induced activation of persulfate for pentachlorophenol degradation[J]. Chemosphere, 2019, 229: 200-205.
[11]	郭梦卓, 徐佰青, 乔显亮, 等. 表面活性剂强化过硫酸钠氧化修复石油烃污染土壤[J]. 土壤, 2023, 55(1): 171-177.
[12]	HOU X J, HUANG X P, LI M L, et al. Fenton oxidation of organic contaminants with aquifer sediment activated by ascorbic acid[J]. Chemical Engineering Journal, 2018, 348: 255-262.
[13]	SUN H W, XIE G H, HE D, et al. Ascorbic acid promoted magnetite Fenton degradation of alachlor: mechanistic insights and kinetic modeling[J]. Applied Catalysis B: Environmental, 2020, 267: 118383.
[14]	黄凤莲, 邹璇, 陈灿, 等. 亚铁活化次氯酸钠降解土壤中阿特拉津[J]. 环境工程, 2021, 39(2): 160-165 , 172.
[15]	FANG G D, CHEN X R, WU W H, et al. Mechanisms of interaction between persulfate and soil constituents: activation, free radical formation, conversion, and identification[J]. Environmental Science and Technology, 2018, 52: 14352-14361.
[16]	CAO M H, TU S X, XIONG S L, et al. EDDS enhanced PCB degradation and heavy metals stabilization in co-contaminated soils by ZVI under aerobic condition[J]. Journal of Hazardous Materials, 2018, 358: 265-272.
[17]	WEI X, GAO N, LI C, et al. Zero-valent iron (ZVI) activation of persulfate (PS) for oxidation of bentazon in water[J]. Chemical Engineering Journal, 2016, 285: 660-670.
[18]	LI Y, WANG F, REN X Y, et al. Peroxymonosulfate activation for effective atrazine degradation over a 3D cobalt-MOF: performance and mechanism[J]. Journal of Environmental Chemical Engineering, 2023, 11: 109116.
[19]	YANG J, LI X K, WEI M F, et al. Base-activated persulfate strategy for ceramic membrane cleaning after treatment of natural surface water[J]. Chemical Engineering Research and Design, 2023, 194: 245-255.
[20]	GUAN Y H, MA J, REN Y M, et al. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Research, 2013, 47: 5431-5438.
[21]	ZHOU S Q, YU Y H, SUN J L, et al. Oxidation of microcystin-LR by copper (Ⅱ) coupled with ascorbic acid: kinetic modeling towards generation of H₂O₂[J]. Chemical Engineering Journal, 2018, 333: 443-450.
[22]	WANG Q, LU X, CAO Y, et al. Degradation of Bisphenol S by heat activated persulfate: kinetics study, transformation pathways and influences of co-existing chemicals[J]. Chemical Engineering Journal, 2017, 328: 236-245.
[23]	PENG J L, LU X H, JIANG X, et al. Degradation of atrazine by persulfate activation with copper sulfide (CuS): kinetics study, degradation pathways and mechanism[J]. Chemical Engineering Journal, 2018, 354: 740-752.
[24]	FANG G D, GAO J, DIONYSIOU D D, et al. Activation of persulfate by quinones: free radical reactions and implication for the degradation of PCBs[J]. Environment Science and Technology, 2013, 47: 4605-4611.
[25]	WU S H, HE H J, LI X, et al. Insights into atrazine degradation by persulfate activation using composite of nanoscale zero-valent iron and graphene: performances and mechanisms[J]. Chemical Engineering Journal, 2018, 341: 126-136.
[26]	LIU W, AI Z H, CAO M H, et al. Ferrous ions promoted aerobic simazine degradation with Fe@Fe₂O₃ core-shell nanowires[J]. Applied Catalysis B: Environment, 2014, 150/151: 1-11.
[27]	AN Y J, LI X W, LIU Z H, et al. Constant oxidation of atrazine in Fe(Ⅲ)/PDS system by enhancing Fe(Ⅲ)/Fe(Ⅱ) cycle with quinones: reaction mechanism, degradation pathway and DFT calculation[J]. Chemosphere, 2023, 317: 137883.
[28]	QU J H, LIU R X, BI X W, et al. Remediation of atrazine contaminated soil by microwave activated persulfate system: performance, mechanism and DFT calculation[J]. Journal of Cleaner Production, 2023, 399: 136546.