厌氧环境中硫化亚铁还原降解噻虫嗪的机制研究
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1.三峡大学生物与制药学院;2.中国科学院南京土壤研究所;3.三峡库区生态环境教育部工程研究中心三峡大学;4.复旦大学环境科学与工程系

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中图分类号:

X592

基金项目:

国家自然科学基金(42177030和U21A20293)和中国科学院南京土壤研究所“十四五”自主部署项目(ISSAS2422)资助。*通讯作者(wangxh@issas.ac.cn;juangao@issas.ac.cn)


The mechanism of reductive degradation of thiamethoxam by ferrous sulfide under anaerobic environment
Author:
Affiliation:

1.College of Biological and Pharmaceutical Sciences,China Three Gorges University;2.Hubei,China;3.Institute of Soil Science,Chinese Academy of Sciences;4.China;5.Engineering Research Center of Eco-environment in Three Gorges Reservoir Region,Ministry of Education,China Three Gorges University;6.Department of Environmental Science and Engineering, Fudan University

Fund Project:

the National Natural Science Foundation of China (42177030,U21A20293) and The 14th Five-Year Plan Independent Deployment Project of Nanjing Institute of Soil Science, Chinese Academy of Sciences (ISSAS2422).

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    摘要:

    新烟碱类杀虫剂进入环境后容易发生生物或非生物转化,而目前关于厌氧环境下非生物还原降解过程研究较少。本文探讨了噻虫嗪(THI)在模拟厌氧环境中硫化亚铁(FeS)介导的还原降解过程与机制。实验发现,FeS在厌氧环境中能有效促使THI发生还原降解,FeS浓度、pH值及环境中共存无机离子和腐殖酸等是主要影响因素。THI在酸性条件下的降解率显著高于碱性环境,无机离子中Al3?和NO??离子则表现出抑制作用,其它常规无机离子Cl-、NO3-、CO32-、K+、Ca2+、Na+、Mg2+、Fe2+、Mn2+、NH4+等和有机组分腐殖酸均无明显影响。通过机制研究表明,Fe(Ⅱ)和硫空位是主要的还原活性位点,首先硫空位与THI分子的硝基官能团相互作用发生电子传递过程,从而促使Fe(II)将电子传递给THI发生还原作用。鉴定FeS还原THI的降解产物,并提出THI的还原脱硝和还原脱氯降解途径。研究结果为理解和优化土壤及地下水中新烟碱类农药的自然降解过程提供了新视角,并为相关环境修复策略的制定提供了理论依据。

    Abstract:

    Neonicotinoid insecticides are prone to biotic or abiotic transformation processes after entering the environment, and there are few studies on the abiotic reduction and degradation process in anaerobic environment. In this paper, we discussed the process and mechanism of ferrous sulfide (FeS)-mediated reductive degradation of thiamethoxam (THI) in a simulated anaerobic environment. The results showed that FeS could effectively promote the degradation of THI in an anaerobic environment, and the effects of FeS concentrations, pH levels, and the coexistence of inorganic ions and humic acid were also investigated in the environment. Under acidic conditions, the degradation rate of THI was significantly higher than that in alkaline environment, and the presence of inorganic Al3? and NO?? ions significantly inhibited the THI degradation, while no obvious effect on THI degradation was observed in the presence of Cl-、NO3-、CO32-、K+、Ca2+、Na+、Mg2+、Fe2+、Mn2+、NH4+and humic acid. Mechanistic studies have shown that Fe(Ⅱ) and sulfur vacancies are the main reductive active sites, in which sulfur vacancies could interact with the oxygen in nitro functional groups of THI molecules to promote the electron transfer between Fe(Ⅱ) and THI. In addition, the degradation products of THI by FeS were identified, and the reduction and dechlorination degradation pathways of THI were proposed. The results of this study provide a new perspective for understanding and optimizing the natural degradation process of neonicotinoid pesticides in soil and groundwater, and provide a theoretical basis for the formulation of related environmental remediation strategies.

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  • 收稿日期:2024-09-14
  • 最后修改日期:2024-10-05
  • 录用日期:2024-10-11
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