pH和溶解性有机质影响下黑碳吸附农药行为的研究
摘要
黑碳是化石燃料和生物质不完全燃烧生成的具有高度芳香化结构的高聚物,它在环境(大气圈、水圈、生物圈、土壤和岩石)中无处不在。黑碳具有多孔性和高比表面积,对有机化合物有较高的亲和力,对生物利用和自然系统中污染物的迁移有着重要的影响。作为潜在的环境污染物载体,黑碳可能会引发一些土壤效应,导致增加农药的使用风险。在自然条件下,天然有机质的存在会对黑碳吸附农药污染物的行为产生重要的协同影响,pH值的变化也会改变黑碳和农药的性质,从而影响了黑碳对农药污染物的吸附行为。为了揭示黑碳对农药的吸附规律及pH值和溶解性有机质对黑碳吸附农药行为的影响,本论文以秸秆为原料制备了较高比表面积的黑碳(吸附剂),选择四类农药为目标吸附质,采用单宁酸和没食子酸为不同分子大小的代表性溶解性有机质(DOM)(预载吸附质),以DOM预载方式研究pH值和DOM对黑碳吸附农药的影响。
本论文研究了黑碳及预载化黑碳对弱酸性农药苯氧乙酸类除草剂的吸附行为。结果表明:在低pH条件下,吸附剂对农药吸附效果较好,且2.4-二氯苯氧乙酸的吸附量都明显高于苯氧乙酸。无论在何种pH值下,单宁酸对黑碳吸附酸性农药的行为都是明显的抑制作用,没食子酸对吸附行为是略有抑制,且都遵循预载量300μmol/g的抑制效果大于预载量10μmol/g的规律,最主要的原因是由于溶解性有机质的预载,导致产生了孔堵效应和竞争吸附。吸附机理主要依靠微孔填充、静电作用和范德华力等方式。影响吸附的主要因素是吸附质的溶解度、表面官能团含量、农药的pKa值及电离性质等。
弱碱性农药扑灭通在黑碳上的吸附行为表明,在pH=5.90条件下的吸附效果优于pH=1.25,且在这两种pH条件下吸附量差异非常明显。这主要与扑灭通的溶解度及其三氮苯骨架的结构有关。预载化黑碳对碱性农药的吸附规律和酸性农药相同,在相同的条件下,单宁酸和没食子酸对碱性农药的吸附行为同样是抑制作用,单宁酸的抑制效果显著,没食子酸的抑制作用微弱,且都随着溶解性有机质预载量的增加抑制效果增强,其原因主要还是孔堵效应和竞争吸附的影响。
中性农药敌稗在黑碳上的吸附规律表现为吸附量较高,无pH依赖性,主要原因是敌稗溶解度较低,有利于吸附剂对敌稗的吸附,且由于敌稗分子没有pKa,在两个pH条件下基本都以分子态形式存在,不发生解离,此外pH对吸附剂表面电荷性质影响不大,从而导致敌稗的吸附行为不受pH值影响。敌稗在预载化黑碳上的吸附规律和碱性农药相同。
两性农药毒莠定在黑碳及预载化黑碳上的吸附具有明显的pH依赖性,吸附量随pH值的增加先升后降,pH=5.90条件下吸附量最低,pH=3.00时吸附量最高,当pH=1.25时又有所下降,但还是明显高pH=5.90的条件下的吸附量。说明酸性条件下有利于吸附,且当pH值接近毒莠定的pKa时有很大吸附。pH值影响吸附剂吸附农药的行为主要是通过引起毒莠定分子形态和吸附剂表面电荷变化决定的。本实验研究表明,范德华力是黑碳吸附毒莠定的主要机理。单宁酸预载对毒莠定吸附行为的影响与其他农药相似,对毒莠定的吸附行为抑制作用明显,而没食子酸对毒莠定的吸附行为是明显增溶作用,并遵循预载量100μmol/g的促进作用大于预载量300μmol/g的规律。
采用Langmuir和Freundlich方程对所有吸附数据进行拟合,相关系数基本上均大于0.97,表明Langmuir和Freundlich模型能较好地用于描述上述吸附过程。
上述讨论较全面地研究了pH和溶解性有机质对黑碳吸附农药影响的作用规律和机理,将为今后研究高含碳土壤的吸附与修复研究提供理论的研究积累。
Black carbon (BC) is defined as the highly aromatic polymeric materials produced from incomplete combustion of fossil fuel and biomass. It exists in all the environmental compartments including atmosphere, hydrosphere, biosphere, soil and rock. With a porous structure and high surface areas, BC has a high affinity for organic compounds and plays an important role in the bioavailability and migration of pollutants in natural systems. As a potential carrier of environmental pollutants, BC may bring about certain soil effects and result in an increased risk associated with pesticide use. Under natural conditions, natural organic matter may have an important synergistic effect on the sorption of pesticides by BC. The variation in pH value may also alter the properties of both BC and pesticides, thereby influencing the adsorption of pesticides by BC. To elucidate the adsorption of pesticides on BC as influenced by dissolved organic matter (DOM), BCs of high surface areas were prepared from rice straws and used as the absorbents for four pesticides. The pesticides were weakly acidic, weakly basic, neutral or amphoteric in terms of their dissociating properties. Tannic acid and gallic acid, differing substantially in molecular size, were used as model DOM to evaluate the effects of pH and DOM preloading on the adsorption.
The results from the adsorption of 2,4-D (2,4-dichlorophenoxyacetic acid, a weakly acidic pesticide) on virgin BC and DOM-preloaded BC show that the adsorption of 2,4-D was higher at lower pH values. Compared to phenoxyacetic acid, the adsorption of 2.4-D was significantly higher. At any experimental pH value, tannic acid significantly inhibited the adsorption of 2,4-D, in comparison to an only slight inhibition by gallic acid. The degree of inhibition was consistently higher by a loading of 300μmol/g than by 100μmol/g. This was due to the pore blockage by. and the competitive adsorption of. tannic acid. The adsorption occurred via micropore filling, electrostatic interaction, and van der Waals forces. The main influential factors included the solubility. pKa and dissociating properties of pesticide and the surface properties of BCs.
The adsorption of prometon (a weakly basic pesticide) was substantially higher at pH 5.90 than at pH 1.25. This may be explained in terms of the solubility and three-N benzene ring structure of prometon. Similar to the adsorption of 2.4-D. the adsorption of prometon was inhibited by both tannic acid and gallic acid, the former acid being much more powerful than the latter in the degree of inhibition. The inhibition increased with increasing the DOM loading. The pore blockage and competitive adsorption were again considered to have contributed to the observed inhibitory effect of DOM.
The adsorption of propanil (a neutral pesticide) on BC was high and independent of pH. This was due to the low solubility and non-dissociating property of propanil. In addition, the surface charge of BCs was not clearly affected by pH. The adsorption of propanil on DOM-loaded BCs occurred in a manner similar to that of 2,4-D.
The adsorption of picloram (an amphoteric pesticide) on BC and DOM-loaded BC showed an obvious dependence on pH. The adsorption increased as pH increased from 1.25 and reached the maximum at pH 3.00. The adsorption then decreased with further increasing pH and reached the minimum at pH 5.90. In addition, the adsorption at pH 1.25 was higher than that at pH 5.90. All these results indicate that acidic conditions, in particular when pH was close to pKal of picloram, were in favor of adsorption. The speciation of picloram and the surface charge of BCs. both influenced by pH, together determined the adsorption of picloram, which occurred through the van der Waals forces. Similar to other pesticides tested, the adsorption of picloram was reduced by the preloading of tannic acid. The reduction of picloram adsorption of preloading gallic acid was due to its solubility enhancement of picloram, which was higher at a loading of 100μmol/g than 300μmol/g.
All the adsorption data were fitted to the Langmuir equation and the Freundlich equation. The correlation coefficients obtained are generally greater than 0.97, indicating that both adsorption models were adequate to describe the adsorption of tested pesticides on BCs.
This thesis thoroughly investigated the influence of pH and DOM preloading on the adsorption of multiple pesticides on BCs and the underlying mechanisms. The results will lay a solid foundation for future investigation on sorption of pollutants and remediation in carbon-containing soils.
本论文研究了黑碳及预载化黑碳对弱酸性农药苯氧乙酸类除草剂的吸附行为。结果表明:在低pH条件下,吸附剂对农药吸附效果较好,且2.4-二氯苯氧乙酸的吸附量都明显高于苯氧乙酸。无论在何种pH值下,单宁酸对黑碳吸附酸性农药的行为都是明显的抑制作用,没食子酸对吸附行为是略有抑制,且都遵循预载量300μmol/g的抑制效果大于预载量10μmol/g的规律,最主要的原因是由于溶解性有机质的预载,导致产生了孔堵效应和竞争吸附。吸附机理主要依靠微孔填充、静电作用和范德华力等方式。影响吸附的主要因素是吸附质的溶解度、表面官能团含量、农药的pKa值及电离性质等。
弱碱性农药扑灭通在黑碳上的吸附行为表明,在pH=5.90条件下的吸附效果优于pH=1.25,且在这两种pH条件下吸附量差异非常明显。这主要与扑灭通的溶解度及其三氮苯骨架的结构有关。预载化黑碳对碱性农药的吸附规律和酸性农药相同,在相同的条件下,单宁酸和没食子酸对碱性农药的吸附行为同样是抑制作用,单宁酸的抑制效果显著,没食子酸的抑制作用微弱,且都随着溶解性有机质预载量的增加抑制效果增强,其原因主要还是孔堵效应和竞争吸附的影响。
中性农药敌稗在黑碳上的吸附规律表现为吸附量较高,无pH依赖性,主要原因是敌稗溶解度较低,有利于吸附剂对敌稗的吸附,且由于敌稗分子没有pKa,在两个pH条件下基本都以分子态形式存在,不发生解离,此外pH对吸附剂表面电荷性质影响不大,从而导致敌稗的吸附行为不受pH值影响。敌稗在预载化黑碳上的吸附规律和碱性农药相同。
两性农药毒莠定在黑碳及预载化黑碳上的吸附具有明显的pH依赖性,吸附量随pH值的增加先升后降,pH=5.90条件下吸附量最低,pH=3.00时吸附量最高,当pH=1.25时又有所下降,但还是明显高pH=5.90的条件下的吸附量。说明酸性条件下有利于吸附,且当pH值接近毒莠定的pKa时有很大吸附。pH值影响吸附剂吸附农药的行为主要是通过引起毒莠定分子形态和吸附剂表面电荷变化决定的。本实验研究表明,范德华力是黑碳吸附毒莠定的主要机理。单宁酸预载对毒莠定吸附行为的影响与其他农药相似,对毒莠定的吸附行为抑制作用明显,而没食子酸对毒莠定的吸附行为是明显增溶作用,并遵循预载量100μmol/g的促进作用大于预载量300μmol/g的规律。
采用Langmuir和Freundlich方程对所有吸附数据进行拟合,相关系数基本上均大于0.97,表明Langmuir和Freundlich模型能较好地用于描述上述吸附过程。
上述讨论较全面地研究了pH和溶解性有机质对黑碳吸附农药影响的作用规律和机理,将为今后研究高含碳土壤的吸附与修复研究提供理论的研究积累。
Black carbon (BC) is defined as the highly aromatic polymeric materials produced from incomplete combustion of fossil fuel and biomass. It exists in all the environmental compartments including atmosphere, hydrosphere, biosphere, soil and rock. With a porous structure and high surface areas, BC has a high affinity for organic compounds and plays an important role in the bioavailability and migration of pollutants in natural systems. As a potential carrier of environmental pollutants, BC may bring about certain soil effects and result in an increased risk associated with pesticide use. Under natural conditions, natural organic matter may have an important synergistic effect on the sorption of pesticides by BC. The variation in pH value may also alter the properties of both BC and pesticides, thereby influencing the adsorption of pesticides by BC. To elucidate the adsorption of pesticides on BC as influenced by dissolved organic matter (DOM), BCs of high surface areas were prepared from rice straws and used as the absorbents for four pesticides. The pesticides were weakly acidic, weakly basic, neutral or amphoteric in terms of their dissociating properties. Tannic acid and gallic acid, differing substantially in molecular size, were used as model DOM to evaluate the effects of pH and DOM preloading on the adsorption.
The results from the adsorption of 2,4-D (2,4-dichlorophenoxyacetic acid, a weakly acidic pesticide) on virgin BC and DOM-preloaded BC show that the adsorption of 2,4-D was higher at lower pH values. Compared to phenoxyacetic acid, the adsorption of 2.4-D was significantly higher. At any experimental pH value, tannic acid significantly inhibited the adsorption of 2,4-D, in comparison to an only slight inhibition by gallic acid. The degree of inhibition was consistently higher by a loading of 300μmol/g than by 100μmol/g. This was due to the pore blockage by. and the competitive adsorption of. tannic acid. The adsorption occurred via micropore filling, electrostatic interaction, and van der Waals forces. The main influential factors included the solubility. pKa and dissociating properties of pesticide and the surface properties of BCs.
The adsorption of prometon (a weakly basic pesticide) was substantially higher at pH 5.90 than at pH 1.25. This may be explained in terms of the solubility and three-N benzene ring structure of prometon. Similar to the adsorption of 2.4-D. the adsorption of prometon was inhibited by both tannic acid and gallic acid, the former acid being much more powerful than the latter in the degree of inhibition. The inhibition increased with increasing the DOM loading. The pore blockage and competitive adsorption were again considered to have contributed to the observed inhibitory effect of DOM.
The adsorption of propanil (a neutral pesticide) on BC was high and independent of pH. This was due to the low solubility and non-dissociating property of propanil. In addition, the surface charge of BCs was not clearly affected by pH. The adsorption of propanil on DOM-loaded BCs occurred in a manner similar to that of 2,4-D.
The adsorption of picloram (an amphoteric pesticide) on BC and DOM-loaded BC showed an obvious dependence on pH. The adsorption increased as pH increased from 1.25 and reached the maximum at pH 3.00. The adsorption then decreased with further increasing pH and reached the minimum at pH 5.90. In addition, the adsorption at pH 1.25 was higher than that at pH 5.90. All these results indicate that acidic conditions, in particular when pH was close to pKal of picloram, were in favor of adsorption. The speciation of picloram and the surface charge of BCs. both influenced by pH, together determined the adsorption of picloram, which occurred through the van der Waals forces. Similar to other pesticides tested, the adsorption of picloram was reduced by the preloading of tannic acid. The reduction of picloram adsorption of preloading gallic acid was due to its solubility enhancement of picloram, which was higher at a loading of 100μmol/g than 300μmol/g.
All the adsorption data were fitted to the Langmuir equation and the Freundlich equation. The correlation coefficients obtained are generally greater than 0.97, indicating that both adsorption models were adequate to describe the adsorption of tested pesticides on BCs.
This thesis thoroughly investigated the influence of pH and DOM preloading on the adsorption of multiple pesticides on BCs and the underlying mechanisms. The results will lay a solid foundation for future investigation on sorption of pollutants and remediation in carbon-containing soils.
引文
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