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农药被广泛应用于农作物生产当中,是保证农作物产量不可或缺的产品. 然而,施用的农药仅有不足1/3会发挥其作用,其余大部分则残留于土壤环境中,或通过蒸发、渗滤等多种途径迁移至地下水、地表水以及大气中,不仅对环境造成了严重的破坏,且可能通过食物链累积并最终对人类健康产生威胁[1]. 因此,土壤农药污染已经成为亟需解决的重要环境问题[2-3]. 新烟碱农药(neonicotinoid)是以烟碱结构为基础研发的一类高效内吸性杀虫剂,主要通过选择性控制昆虫中枢神经系统的烟碱型乙酰胆碱受体(nicotinic acetylcholine receptors,nAChRs),阻碍昆虫神经冲动的正常传导,进而造成昆虫的麻痹和死亡[4-5]. 根据新烟碱农药的主要结构可将其分为氯吡啶基(吡虫啉、噻虫啉、烯啶虫胺、啶虫脒)、氯噻唑基(噻虫嗪、噻虫胺)和四氢呋喃基(呋虫胺)农药. 同时,高水溶性的新烟碱农药,如烯啶虫胺(590 g·L−1)、呋虫胺(39.83 g·L−1)、噻虫嗪(4.1 g·L−1)和啶虫脒(2.95 g·L−1)更易迁移至地表水或地下水中,而低水溶性的新烟碱农药吡虫啉(0.51 g·L−1)、噻虫胺(0.327 g·L−1)和噻虫啉(0.185 g·L−1)则更容易与疏水性有机物发生相互作用而残留于土壤中[6-7]. 据统计,新烟碱农药在农药化学品市场中约占1/4的份额,同时由于其高效、低毒等特点,被120多个国家/地区注册和使用[8]. 然而,近年来有研究者发现新烟碱农药会对非靶标生物,如传粉昆虫、食虫鸟类和水生动物等产生不利影响[9]. 此外,由于其高水溶性和低挥发性,新烟碱农药被认为具有较高的浸出潜力,不仅可以被植物的根叶迅速吸收并运输至果实,而且极易迁移以致污染地表水与地下水[1, 10]. 因此,新烟碱农药在环境中的迁移转化行为与环境风险亟需进一步研究关注.
生物炭是生物质在限氧条件下热解得到的具有高吸附能力和高芳香性的富碳固体颗粒[11-12]. 作为一种具有高效修复能力并且原料易得的环境友好型材料,生物炭独特的理化性质使其在提高土壤肥力和污染物的固定化减量化等方面都具有不可忽视的作用和意义[13-14]. 将生物炭应用于土壤污染修复时,不仅可以通过改变土壤的理化性质,有利于新烟碱农药在生物炭-土壤上的吸附,并能促进新烟碱农药的化学降解和生物降解[15-18]. 因此,研究土壤体系中新烟碱农药与生物炭之间的相互作用对于控制新烟碱农药在土壤中的迁移转化等问题具有实际意义.
本文综述了生物炭添加到土壤中吸附新烟碱农药的作用和机理,如极性相互作用、氢键作用、阳离子-π/P(π)-π 电子供体-受体(electron donor-acceptor,EDA)相互作用和孔隙填充机制等,综合分析了生物炭的pH值、矿物灰分、持久性自由基(persistent free radicals,PFRs)对新烟碱农药化学降解作用的影响,以及生物炭通过调控酶活性、高丝氨酸内酯(acyl-homoserine lactone,AHL)传导和土壤养分组成等途径间接影响新烟碱农药的生物降解作用. 其中,生物炭阻碍AHL传导可能是导致微生物群落结构组成变化的关键因素,同时生物炭通过改变土壤养分组成对新烟碱农药代谢途径及其产物的影响还需进一步研究. 最后,本文对未来新烟碱农药污染的治理提出了合理的建议和展望,将生物炭改性和微生物接种相结合的方式可能是解决农药残留更有效的方法.
土壤体系中生物炭吸附降解新烟碱农药的研究进展
Advances in adsorption and degradation mechanism on neonicotinoids mediated by biochar in soil
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摘要: 作为一种有效的土壤修复材料,生物炭可以吸附土壤中的新烟碱农药,也可以通过直接或间接影响促进新烟碱农药的降解,从而减小其环境风险. 目前,新烟碱农药在生物炭上的吸附机制已被基本阐明,但由于生物炭、新烟碱农药、土壤环境以及微生物之间相互作用的复杂性,生物炭对土壤环境中新烟碱农药降解过程所产生的影响仍缺乏系统性研究. 本文简述了新烟碱农药在生物炭上的主要吸附机制,综合分析了生物炭的pH值、矿物灰分、氧化还原能力和持久性自由基(PFRs)对新烟碱农药化学降解的影响,以及生物炭通过调控酶活性、高丝氨酸内酯(AHL)传导和改变土壤养分组成等途径对新烟碱农药生物降解的影响. 值得注意的是,生物降解作用是土壤环境中新烟碱农药降解的主要途径,在土壤中添加生物炭,将导致微生物生境变化以及群落结构改变,进而影响酶的分泌、种类和活性并改变其生物降解作用. 最后,本文对未来新烟碱农药污染的治理提出了合理的建议和展望,将生物炭改性和微生物接种相结合的方式可能是解决农药残留更有效的方法.Abstract: As an effective soil amendment, biochar could be applied to adsorb neonicotinoids in soil, and promote the degradation of neonicotinoids by direct or indirect effect, thus reducing neonicotinoids’ environmental risks. The adsorption mechanism of neonicotinoids on biochar has attracted many research attentions. However, the interaction between biochar and neonicotinoids may be controlled by soil chemical and biological environment, it is necessary to further study neonicotinoids’ behavior mediated by biochar in this complex system to effectively control their environmental risks. This paper summarized the mechanisms of adsorption of neonicotinoids by biochar. The effects of pH value, mineral ash, and persistent free radicals (PFRs) relevant to biochar on chemical degradation of neonicotinoids were comprehensively analyzed. In addition, biochar could indirectly affect the biodegradation of neonicotinoids by regulating enzyme activity, Acyl-homoserine lactone (AHL) conduction, and soil nutrient composition. It is worth noting that the degradation of neonicotinoids in soil is mainly controlled by biodegradation. The changes in microbial habitat and community structure caused by the addition of biochar will eventually affect the secretion, species, and activity of enzymes. This paper also put further suggestions and prospects for the treatment of neonicotinoid pollution in the future. Concretely speaking, the combination of biochar modification and microorganism inoculation may be a more effective method to solve pesticide residues.
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Key words:
- insecticide /
- adsorption /
- degradation /
- enzyme /
- microorganism.
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表 1 新烟碱农药的微生物降解和代谢
Table 1. Degradation and metabolism of microorganisms on neonicotinoids
农药
Insecticide药效基团
Pharmacophore微生物属名
Name of microorganisms分类
Classification培养环境
Culture environment代谢方式
Metabolic mode底物类型
Zymolyte type降解酶
Degrading enzyme代谢产物
Degradation products杀虫活性
Insecticidal activity参考文献
Reference吡虫啉 硝基亚胺 (=N—NO2) 假单胞菌属Pseudomonas 革兰氏阴性菌 矿物盐培养基 共代谢 麦芽糖 CYP450 5-羟基吡虫啉 — [56] 柠檬酸 AOX 亚硝基吡虫啉 — 黄单胞菌属Xanthomonas LB培养基 共代谢 蔗糖 — 5-羟基吡虫啉 — [61] 琥珀酸 — 烯烃吡虫啉 增大19倍 假单胞菌属Pseudomonas LB培养基 共代谢 葡萄糖 — 尿素代谢物 — [62] 假黄单胞菌属Pseudoxanthomonas 矿物盐培养基 共代谢 乳糖 — 5-羟基吡虫啉 — [63] 丙酮酸 — 烯烃吡虫啉 — 假单胞菌属Pseudomonas 基本培养基 生长代谢 — — 尿素代谢物 降低5倍 [64] 啶虫脒 氰基亚胺 (=N—CN) 红酵母Rhodotorula 真菌 矿物盐培养基 共代谢 蔗糖 — 尿素代谢物 — [65] 嗜染料菌属Pigmentiphaga 革兰氏阴性菌 LB培养基 生长代谢 — — 尿素代谢物 — [66] 黄单胞菌属Xanthomonas LB培养基 共代谢 蔗糖 CYP450 去甲基代谢物 降低10倍 [67] 噻虫啉 氰基亚胺 (=N—CN) 红酵母Rhodotorula 真菌 矿物盐培养基 共代谢 蔗糖 — 酰胺代谢物 降低10倍 [65] 贪噬菌属Variovorax 革兰氏阴性菌 土壤 生长代谢 — NHase 酰胺代谢物 降低10倍 [68] 黄单胞菌属Xanthomonas LB培养基 共代谢 蔗糖 CYP450 4-羟基噻虫啉 降低156倍 [69] 根瘤菌属Rhizobium Frank 矿物盐培养基 共代谢 葡萄糖 NHase 酰胺代谢物 降低10倍 [70] 氯噻啉 硝基亚胺 (=N—NO2) 黄单胞菌属Xanthomonas 革兰氏阴性菌 LB培养基 共代谢 蔗糖 — 5-羟基氯噻啉
烯烃氯噻啉— [71] 注:中出“—”代表参考文献中对该内容并未提及.
Note: "—" the content is not mentioned in the reference. -
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