除草剂苄嘧磺隆在几种粘粒矿物与地带性土壤表面的吸附研究
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摘要
为了探讨不同土壤和粘粒矿物吸附除草剂苄嘧磺隆的机理与卤素阴离子配体对吸附行为及活性的影响,以了解施入不同土壤中的苄嘧磺隆的残留、活性、迁移和对地下水污染的差异,为苄嘧磺隆的合理施用提供科学资料和依据,本文用平衡吸附法、傅立叶变换红外光谱(FT-IR)以及X-射线衍射(XRD)较系统研究了中南地区几种有代表性的地带性土壤和粘土矿物、粘粒氧化物对苄嘧磺隆的吸附行为及其影响因素;探讨了供试粘土矿物和粘粒氧化物吸附苄嘧磺隆的可能机制。研究结果对揭示土壤不同组分与其相互作用机理,阐明土壤吸附除草剂活性的有关影响因素,与苄嘧磺隆在不同酸碱性水稻土中的迁移转化与残留规律,对合理使用苄嘧磺隆及可能出现的不良影响提出防治措施、建立其环境安全性评价及指导农业生产有重要的理论和实际意义。取得的主要进展和结果有:
1、用碱溶法提纯精制出绿磺隆、苄嘧磺隆的样品,与标样的熔点、折光率、红外光谱图一致,纯度相近,可用作一般残留分析与商检的标准物质。
2、中南地区几种代表性的地带性土壤对苄嘧磺隆的吸附都能较好地用Langmuir方程描述,部分结果能用Fruendlich方程描述。pH5.0时,供试土壤对苄嘧磺隆最大吸附量(μg·g~(-1))的顺序为:海南砖红壤(18.68)>郴县红壤(15.00)>贺胜桥棕红壤(13.69)>孝感黄棕壤(13.11)>枣阳黄褐土(12.76)。
3、供试土壤对苄嘧磺隆的吸附率与土壤的pH值呈显著的负相关,海南砖红壤、郴县红壤、贺胜桥棕红壤、孝感黄棕壤、枣阳黄褐土对苄嘧磺隆的吸附率分别由pH=4时的17.13%、11.01%、15.12%、9.28%、1.50%下降至pH=8时的1.03%、1.45%、2.01%、1.19%、0.06%。土壤的有机质、铁铝氧化物和粘粒含量及电荷零点与苄嘧磺隆的吸附呈显著正相关。
4、供试粘土矿物与粘粒氧化物对苄嘧磺隆的吸附都能较好地符合Langmuir方程,部分还能较好地用Fruendlich方程描述。pH5.5时的最大吸附量(μg·g~(-1))顺序为:膨润土BM(184.3)>膨润土HM(167.41)>针铁矿(44.65)>非晶形氧化铝(39.85)>水铁矿(31.32)>高岭土(19.49)>水钠锰矿(10.67),其它pH值时,最大吸附量的顺序与此大体一致。
5、供试粘土矿物及粘粒氧化物对苄嘧磺隆的吸附率随体系pH值的上升呈显著下降的趋势。从pH4.0提高到pH5.5时,膨润土BM、膨润土HM、针铁矿、非晶形氧化铝、水铁矿、高岭土、水钠锰矿对苄嘧磺隆的最大吸附量分别降低:36.4、67.0、24.48、6.53、1.43、0.06、3.35μg·g~(-1),降低程度分别为:16.49%、28.58%、35.41%、14.08%、0.04%、0.003%、23.89%;提高到pH8.0时分别降低:151.56、170.98、44.48、23.99、8.16、13.34、5.68μg·g~(-1),降低程度分别为:68.67%、72.94%、63.34%、51.72%、24.92%、68.37%、40.53%。
6、供试粘土矿物及粘粒氧化物对节嚓磺隆的吸附量与它们的表面电荷和比表面呈
显著正相关,并随体系中卤素离子(F一、Cl一)浓度的增加而降低,其中非晶形氢氧化铝
和针铁矿的降幅较大,表明吸附过程存在专性吸附机制。
7、供试粘土矿物及粘粒氧化物吸附节嚓磺隆的红外光谱和X一射线衍射分析表明:
针铁矿、水铁矿及非晶形氧化铝等带正电荷的氧化物表面是电荷一偶极键形式。在蒙脱
石为主的有机膨润土表面吸附程度较高,并能进入蒙脱石的层间与其中的水化交换性阳
离子形成氢键。
A study of adsorption processes and mechanisms of a relatively new sulfonyluera herbicide, bensulfuron-methyl on 4 oxides (goethite, ferrihydrite, amorphous alumina ,birnessite), 3 clay minerals (kaolinite, montorillonite HM, montorillonite BM ) and 5 soils (Hainan latosol, Chenxian red earth, Heshengqiao brown red earth, Xiaogan yellow Brown earth, Zaoyang tan earth) in middle-south area of China has been carried out through a batch of equilibrium methods , FT-IR and X diffraction.
1. The chlorsulfuron and bensulfuron-methyl were purified from industrial product as standard samples and were indentified and titrated. The content of chlorsulfuron and bensulfuron-methyl of purified samples, which can be used as the standard sample of commodity inspection and the analysis of residue, are almost the same as that of standard samples.
2. The adsorption of bensulfuron-methyl by each soils can be described though Langmuir 's equation, relatively only a few of these adsorptions fit Fruendlich 's equation . pH5.0,the The maximum absorbing capacities ( g g-1) were according to : Hainan latosol (18.68) > Chenxian red earth (15.00) > Heshengqiao brown red earth (13.69) > Xiaogan yellow Brown earth (13.11) > Zaoyang tan earth (12.76).
3. Multivariate linear regression analysis of the adsorptions of bensulfuron-methyl by each soils shows that were interrelated to the physical and chemical characteristics of the soils. The pH of the systems shows evidently negative correlation, the content of organic matter, the content of oxides of iron and alumina, the content of clay and the point of zero charge show significant positive correlation.
4. The adsorption of bensulfuron-methyl by each oxides and clay minerals can be described though Langmuir's equation ( H type or L type ). The maximum absorbing capacities ( g g-1 ) were that Bentonite BM (184.3)>Bentonite HM (167.4)>amorphous alumina (44.65)> goethite (39.85) > ferrihydrite (31.32)> kaolinite (19.49)> birnessite (10.67). Otherwise, only a few of these adsorptions fit Fruendlich 's equation .
5. The adsorption of bensulfuron-methyl by each oxides and clay minerals was controlled by the pH of each system. The adsorption percentage was independent of the amount of bensulfuron-methyl added, and markedly decreased with the increasing pH.
6. The effects of F-1 ,C1-1 to each adsorption were also examined. The results indicated that the absorbing capacities were decrease by the concentrations of F-1 and CI-1 increase, especially in amorphous alumina and goethite systems.
7. A FT-IR study on bensulfuron-methyl adsorption by goethite has been carried out. The results showed that: The adsorption was occurred through the carbonyl group, sulfonyl group of bensulfuron-methyl with the hydrate hydroxyl groups (-OH2+) on the surface of the oxides of iron and alumina, and a possible mechanism was that the adsorption was conducted by means of charge-dipole interaction though hydrogen bond.
8. The strong adsorption of bensulfuron-methyl by the bentonite (main component is montmorillonite) has been analysis by x-ray diffraction. The results showed that bensulfuron-methyl can go into the interlayer of the montmorillonite and bond with the exchangeable cation through hydrogen bond.
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