Sorption of sulfonamide pharmaceutical antibiotics on whole soils and particle-size fractions
Sorption of sulfonamide pharmaceutical antibiotics on whole soils and particle-size fractions
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DOI：
10.2134/jeq2004.1331
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发表时间：
2004-07-01
影响因子：
2.4
通讯作者：
Leinweber, P
中科院分区：
文献类型：
--
作者：
Thiele-Bruhn, S;Seibicke, T;Leinweber, P
药物抗生素的残留物存在于环境中，其命运和影响取决于吸附作用。因此，对氨基苯甲酸和五种磺胺类抗生素（磺胺，磺胺二甲嘧啶，磺胺嘧啶，磺胺二甲氧嘧啶，磺胺吡啶）的土壤吸附的程度和机制进行了研究，使用施肥和未施肥的土壤表层及其有机矿物颗粒大小的部分。Freundlich吸附系数（K-f）范围为0.5至6.5。吸附增加的芳香性和电负性的功能基团连接到磺酰基苯胺核心。吸附到土壤和粒度级的顺序增加：粗粉砂<全土<中粉砂<砂<粘土<细粉砂，并受pH值的影响。吸附非线性（1/n：0.76）表示特定的相互作用与土壤有机质（SOM）的功能基团。酚和羧基，N-杂环化合物，和木质素分解产物被暂定为首选的结合位点，使用热解质谱和吸附系数的统计分析。磺胺类药物对矿物土壤胶体的吸附较弱，导致从粘土粒度组分中的解吸较强。此外，粘土级分中有机-矿物复合物的空间可及性显著降低。采用定量结构-性质相关（QSPR）模型，结合有机碳浓度、磺胺类药物的色谱容量因子（k '）和非解离态浓度（CFa），估算了分配系数（K-d），交叉验证回归系数Q（2）= 0.71。模拟和分子力学计算表明，吸附剂-SOM复合物通过氢键和货车范德华相互作用表现出较好的位点特异性吸附。不同的化学结构特性，如芳香性和货车范德华体积，与吸附数据。
Residues of pharmaceutical antibiotics are found in the environment, whose fate and effects are governed by sorption. Thus, the extent and mechanisms of the soil sorption of p-aminobenzoic acid and five sulfonamide antibiotics (sulfanilamide, sulfadimidine, sulfadiazine, sulfadimethoxine, and sulfapyridine) were investigated using top-soils of fertilized and unfertilized Chernozem and their organic-mineral particle-size fractions. Freundlich adsorption coefficients (K-f) ranged from 0.5 to 6.5. Adsorption increased with aromaticity and electronegativity of functional groups attached to the sulfonyl-phenylamine core. Adsorption to soil and particle-size fractions increased in the sequence: coarse silt < whole soil < medium silt < sand < clay < fine silt and was influenced by pH. Sorption nonlinearity (1/n : 0.76) indicated specific interactions with functional groups of soil organic matter (SOM). Phenolic and carboxylic groups, N-heterocyclic compounds, and lignin decomposition products were tentatively assigned as preferred binding sites using statistical analysis of pyrolysis-mass spectra and adsorption coefficients. Adsorption of sulfonamides to mineral soil colloids was weaker and resulted in a stronger desorption from clay-size fractions. Moreover, steric accessibility of organic-mineral complexes in clay-size fractions was significantly reduced. With a quantitative structure-property relationship (QSPR) model, combining the organic carbon concentration, the sulfonamides' chromatographic capacity factor (k'), and nondissociated species concentration (CFa), distribution coefficients (K-d) were estimated with a cross-validated regression coefficient Q(2) = 0.71. Modeling and molecular mechanics calculations of antibiotic-SOM complexes showed preferred site-specific sorption via hydrogen bonds and van der Waals interactions. Distinct chemical structural properties, such as aromaticity and van der Waals volumes, correlated with the sorption data.