典型多溴联苯醚在土壤中的吸附及对其生物降解性的影响
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摘要
多溴联苯醚（Polybrominated diphenyl ethers, PBDEs）是斯德哥尔摩公约中新增的受控物质，在PBDEs作为阻燃剂长期使用的过程当中，其原料生产、产品添加和后处理过程都可能造成相关场地土壤介质的污染，而产生严重的环境风险。本研究系统地考察了PBDEs典型单体在土壤中的吸附作用，分析了该吸附过程对其后续生物可降解性的影响，研究结果对于准确评价PBDEs的环境风险和相关场地采取相应的管理手段有重要的意义。
选择典型单体2,2',4,4'-四溴联苯醚（2,2',4,4'-tetrabromodiphenyl ether, BDE-47）为研究对象，以土壤、典型矿物以及胡敏酸（humic acid, HA）和黑碳（black carbon,BC）组分为吸附剂，在对其表面/结构特性表征的基础上，开展了静态吸附/解吸试验，结合其吸附性能的差异，识别了土壤有机组分在影响BDE-47水土体系吸附行为中的关键作用，其中，BC组分体现出了更明显的吸附非线性和解吸滞后性特征，而不同样本的有机组分间都存在着有机碳归一化吸附系数的显著差异，说明有机组分的表面/结构特性会对其吸附能力产生影响。
采用pp-LFER理论对BDE-47在20种模式有机组分上的三个浓度区间的单点吸附系数Koc进行了多参数线性回归，显著性分析的结果识别出基于芳香环结构的表面吸附和基于微孔结构的微孔填充是影响有机组分吸附BDE-47的关键因素，通过双模式模型，对其各自的贡献进行了定量解析，表明在吸附初始阶段，微孔填充占主导地位，吸附进程中，微孔点位逐渐饱和，优势地位逐渐被表面吸附替代。
通过对照苯胺、苯酚、对羟基苯甲酸和环己醇、环己酮、1,5-己二烯-3-醇在模式有机组分上的吸附特性，排除了环状结构、氢键和不饱和双键作为核心作用位点的可能性，识别出芳香环结构是表面吸附的核心作用位点，采用紫外/红外光谱技术，解析了供电子基团（羟基）对于BDE-47与芳香环结构之间作用力强弱的影响，揭示了π-π电子供受体作用是影响有机组分吸附BDE-47的关键作用力。
基于降解速率和潜在可降解性两个指标，考察了不同吸附作用对于吸附质在土壤体系的生物降解的影响，发现BDE-47从土壤有机组分上解吸过程是影响其降解速率的关键环节，选择生物表面活性剂提供优化的促解吸环境，发现解吸进行完全后，依托表面吸附的吸附质分子几乎能够全部从有机组分上解吸下来而得以降解，而微孔填充的吸附质分子无法从微孔位点释放，难以被微生物降解。
Polybrominated diphenyl ethers (PBDEs) are included as persistent organicpollutants (POPs) by Stockholm Convention. Heavy soil contamination has beentriggered by PBDEs production, utilization and post-treatment, which could induceserious environmental risks. In this study, the mechanism of interactions betweenPBDEs and soil organic matter fractions and its impact on the biodegradability ofPBDEs were studied, which would pave a better way for further risk assessment andmanagement of PBDEs contaminated sites.
2,2',4,4'-Tetrabromodiphenyl Ether (BDE-47), one typical PBDEs congener whichis included in persistent organic pollutants (POPs) list and frequently detected in naturalenvironment at high concentration level, is selected as the model PBDEs to explore itsinteraction with the tested sorbents: bulk soils, inorganic minerals, and the isolatedorganic fractions (humic acid and black carbon). Based on the characterization ofsurface and structural properties, sorption/desorption experiments were conducted toexplore the sorption characteristics of each sorbent. It was shown that compared tominerals, the major contribution to soil behaviors with BDE-47was attributed to soilorganic matter among which black carbon fraction displayed more pronouncednonlinear sorption isotherm and desorption hysteresis. Even for the different samples ofone same soil organic fraction, pronounced sorption affinity differences were observed.
Based on pp-LFER model, the single-point adsorption equilibrium constant (Koc) atthree C_elevels (C_e=0.001S_w,0.005S_w,0.05S_w) was correlated with four majorparameters (surface functionalities, microporosity, aromaticity and hydrophobicity)using multiple parameter linear analysis accompanied by significance test. The resultsindicated that at low concentration, surface microporosity representing pore fillingcontributed significantly to this relationship, while as concentration increased to higherlevels, functionality related to surface adsorption began to take the dominant role, whichwas further confirmed by results of Polanyi-based modeling. Given to above, a dualmode model based on Dubinin-Radushkevich (DR) and de Boer-Zwikker equations wasadopted to quantitatively assess the changes of significance of surface adsorption aswell as that of pore filling with sorption process developed. In addition, UV andinfrared spectra of four typical aromatic compounds which represented the key structural fragments of biochars before and after interactions with BDE-47wereanalyzed and proposed π-π electron-donor-acceptor interaction to contribute greatly tosurface adsorption.
The effects of soil organic matter-BDE-47interactions on the biodegradability ofBDE-47by Pseudomonas putida TZ-1were examined. The presence of all tested modelsoil organic fractions decreased the biodegradation rate as the degradation of solid phaseBDE-47was slower than that of liquid phase BDE-47for the desorption hysteresis fromsoil organic fractions. In terms of potential biodegradability, the microporous soilorganic fractions contributed to a significant negative impact, while the effects ofnon-porous soil organic fractions were negligible, as BDE-47sorbed within deepmicropores would be resistant to rigorous chemical extraction and long-term desorption.
选择典型单体2,2',4,4'-四溴联苯醚（2,2',4,4'-tetrabromodiphenyl ether, BDE-47）为研究对象，以土壤、典型矿物以及胡敏酸（humic acid, HA）和黑碳（black carbon,BC）组分为吸附剂，在对其表面/结构特性表征的基础上，开展了静态吸附/解吸试验，结合其吸附性能的差异，识别了土壤有机组分在影响BDE-47水土体系吸附行为中的关键作用，其中，BC组分体现出了更明显的吸附非线性和解吸滞后性特征，而不同样本的有机组分间都存在着有机碳归一化吸附系数的显著差异，说明有机组分的表面/结构特性会对其吸附能力产生影响。
采用pp-LFER理论对BDE-47在20种模式有机组分上的三个浓度区间的单点吸附系数Koc进行了多参数线性回归，显著性分析的结果识别出基于芳香环结构的表面吸附和基于微孔结构的微孔填充是影响有机组分吸附BDE-47的关键因素，通过双模式模型，对其各自的贡献进行了定量解析，表明在吸附初始阶段，微孔填充占主导地位，吸附进程中，微孔点位逐渐饱和，优势地位逐渐被表面吸附替代。
通过对照苯胺、苯酚、对羟基苯甲酸和环己醇、环己酮、1,5-己二烯-3-醇在模式有机组分上的吸附特性，排除了环状结构、氢键和不饱和双键作为核心作用位点的可能性，识别出芳香环结构是表面吸附的核心作用位点，采用紫外/红外光谱技术，解析了供电子基团（羟基）对于BDE-47与芳香环结构之间作用力强弱的影响，揭示了π-π电子供受体作用是影响有机组分吸附BDE-47的关键作用力。
基于降解速率和潜在可降解性两个指标，考察了不同吸附作用对于吸附质在土壤体系的生物降解的影响，发现BDE-47从土壤有机组分上解吸过程是影响其降解速率的关键环节，选择生物表面活性剂提供优化的促解吸环境，发现解吸进行完全后，依托表面吸附的吸附质分子几乎能够全部从有机组分上解吸下来而得以降解，而微孔填充的吸附质分子无法从微孔位点释放，难以被微生物降解。
Polybrominated diphenyl ethers (PBDEs) are included as persistent organicpollutants (POPs) by Stockholm Convention. Heavy soil contamination has beentriggered by PBDEs production, utilization and post-treatment, which could induceserious environmental risks. In this study, the mechanism of interactions betweenPBDEs and soil organic matter fractions and its impact on the biodegradability ofPBDEs were studied, which would pave a better way for further risk assessment andmanagement of PBDEs contaminated sites.
2,2',4,4'-Tetrabromodiphenyl Ether (BDE-47), one typical PBDEs congener whichis included in persistent organic pollutants (POPs) list and frequently detected in naturalenvironment at high concentration level, is selected as the model PBDEs to explore itsinteraction with the tested sorbents: bulk soils, inorganic minerals, and the isolatedorganic fractions (humic acid and black carbon). Based on the characterization ofsurface and structural properties, sorption/desorption experiments were conducted toexplore the sorption characteristics of each sorbent. It was shown that compared tominerals, the major contribution to soil behaviors with BDE-47was attributed to soilorganic matter among which black carbon fraction displayed more pronouncednonlinear sorption isotherm and desorption hysteresis. Even for the different samples ofone same soil organic fraction, pronounced sorption affinity differences were observed.
Based on pp-LFER model, the single-point adsorption equilibrium constant (Koc) atthree C_elevels (C_e=0.001S_w,0.005S_w,0.05S_w) was correlated with four majorparameters (surface functionalities, microporosity, aromaticity and hydrophobicity)using multiple parameter linear analysis accompanied by significance test. The resultsindicated that at low concentration, surface microporosity representing pore fillingcontributed significantly to this relationship, while as concentration increased to higherlevels, functionality related to surface adsorption began to take the dominant role, whichwas further confirmed by results of Polanyi-based modeling. Given to above, a dualmode model based on Dubinin-Radushkevich (DR) and de Boer-Zwikker equations wasadopted to quantitatively assess the changes of significance of surface adsorption aswell as that of pore filling with sorption process developed. In addition, UV andinfrared spectra of four typical aromatic compounds which represented the key structural fragments of biochars before and after interactions with BDE-47wereanalyzed and proposed π-π electron-donor-acceptor interaction to contribute greatly tosurface adsorption.
The effects of soil organic matter-BDE-47interactions on the biodegradability ofBDE-47by Pseudomonas putida TZ-1were examined. The presence of all tested modelsoil organic fractions decreased the biodegradation rate as the degradation of solid phaseBDE-47was slower than that of liquid phase BDE-47for the desorption hysteresis fromsoil organic fractions. In terms of potential biodegradability, the microporous soilorganic fractions contributed to a significant negative impact, while the effects ofnon-porous soil organic fractions were negligible, as BDE-47sorbed within deepmicropores would be resistant to rigorous chemical extraction and long-term desorption.
引文
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