碳纳米管及其与DOM复合体系对阿特拉津的吸附
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摘要
本文采用振荡平衡法研究了阿特拉津(AT)在单壁碳纳米管(SWNTs)和多壁碳纳米管(MWNTs)上的吸附/解吸行为,同时还研究了离子强度、pH值等介质条件对吸附的影响。表面活性剂和天然有机物(NOM)与碳纳米管(CNTs)的结合不仅可以增加CNTs的迁移性,而且可以成为持久性有机物(POPs)潜在的载体,使得POPs迁移、转化和毒性效应变得更加复杂。用不同来源的腐殖酸(HA)和不同离子类型的表面活性剂对SWNTs和MWNTs进行改性,研究了经表面活性剂和HA改性后的CNTs对AT的吸附过程,并研究了改性后CNTs的分散稳定性。结合吸附剂和吸附质的理化性质探究吸附作用机理,为CNTs的安全性评价提供科学依据,并为探讨有机污染物在天然环境中的行为和归宿提供理论基础。
实验结果表明,离子强度对AT在SWNTs和MWNTs上的吸附没有显著影响,但随着pH值的增大,AT在2种碳纳米材料上的吸附量显著增加;这表明,AT在溶液中的存在状态是吸附的主要影响因素。在本实验的研究条件下,AT从SWNTs和MWNTs上的解吸行为不存在明显的滞后效应。CNTs对AT较高的吸附容量和吸附的可逆性表明,CNTs的大规模应用将可能带来一定的环境和健康风险。经表面活性剂和HA改性后的CNTs对AT的吸附实验结果表明,表面活性剂和HA明显的抑制了CNTs对AT的吸附,泥炭腐殖酸(PHA)的抑制作用大于土壤腐殖酸(SHA)的抑制作用,而两种表面活性剂的抑制作用相似。表面活性剂浓度不同时其在溶液中的存在形式不同,探究了表面活性剂投加量对吸附的影响。结果表明,在表面活性剂浓度低于0.5CMC(临界胶束浓度)时AT的吸附受到明显抑制,当表面活性剂浓度大于0.5CMC时对AT吸附的抑制达到相对平衡状态。MWNTs经腐殖酸和表面活性剂表面改性后可以很好的分散,但是SWNTs不能被腐殖酸和表面活性剂有效分散。
In this paper, the sorption and desorption behaviors of atrazine (AT) onto single-walled carbon nanotubes (SWNTs) and multi-walled carbon nanotubes (MWNTs) were studied. The effect of ionic strength and pH were also elucidated. The association of surfactant and natural organic matters (NOM) with carbon nano-tubes (CNTs) not only could increase the mobility of CNTs, but also become a potential carrier for persistent organic pollutants (POPs) and thus make the transport, fate and toxicological effects of POPs more complicated. In this study, MWNTs and SWNTs were modified by humic acids (HA) from different sources and surfactants with different ionic types. The adsorption of atrazine by modified CNTs was investigated and the dispersion stability of modified CNTs was also observed. Physical and chemical properties of different sorbents were analyzed for interpreting sorption mechanisms.
Results showed that the ionic strength had no significant influence on the adsorption of AT onto SWNTs and MWNTs. With the increase of pH, the adsorption of AT onto the two nanomaterials increased obviously, which indicated the speciation change of atrazine was the dominant factor controlling the adsorption capacity. The adsorption-desorption curves revealed that no significant desorption hysteresis existed under the condition of this study. High adsorption capacity and adsorption reversibility of atrazine on CNTs implied that CNTs could result in health and environmental risks when applied in large scale. The inhibition effect of peat humic acid (PHA) was relatively stronger than that of soil humic acid (SHA), but the two surfactants had much similar impact on the atrazine adsorption by two CNTs. With the increase of surfactant concentration in solution, the adsorption of atrazine by CNTs decreased rapidly when the surfactant concentration was less than 0.5CMC (Critical Micelle Concentration). Surface modification by humic acid and surfactant could effectively separate MWNTs into well dispersed suspensions, but the SWNTs could not be appreciably dispersed by humic acids and surfactants.
实验结果表明,离子强度对AT在SWNTs和MWNTs上的吸附没有显著影响,但随着pH值的增大,AT在2种碳纳米材料上的吸附量显著增加;这表明,AT在溶液中的存在状态是吸附的主要影响因素。在本实验的研究条件下,AT从SWNTs和MWNTs上的解吸行为不存在明显的滞后效应。CNTs对AT较高的吸附容量和吸附的可逆性表明,CNTs的大规模应用将可能带来一定的环境和健康风险。经表面活性剂和HA改性后的CNTs对AT的吸附实验结果表明,表面活性剂和HA明显的抑制了CNTs对AT的吸附,泥炭腐殖酸(PHA)的抑制作用大于土壤腐殖酸(SHA)的抑制作用,而两种表面活性剂的抑制作用相似。表面活性剂浓度不同时其在溶液中的存在形式不同,探究了表面活性剂投加量对吸附的影响。结果表明,在表面活性剂浓度低于0.5CMC(临界胶束浓度)时AT的吸附受到明显抑制,当表面活性剂浓度大于0.5CMC时对AT吸附的抑制达到相对平衡状态。MWNTs经腐殖酸和表面活性剂表面改性后可以很好的分散,但是SWNTs不能被腐殖酸和表面活性剂有效分散。
In this paper, the sorption and desorption behaviors of atrazine (AT) onto single-walled carbon nanotubes (SWNTs) and multi-walled carbon nanotubes (MWNTs) were studied. The effect of ionic strength and pH were also elucidated. The association of surfactant and natural organic matters (NOM) with carbon nano-tubes (CNTs) not only could increase the mobility of CNTs, but also become a potential carrier for persistent organic pollutants (POPs) and thus make the transport, fate and toxicological effects of POPs more complicated. In this study, MWNTs and SWNTs were modified by humic acids (HA) from different sources and surfactants with different ionic types. The adsorption of atrazine by modified CNTs was investigated and the dispersion stability of modified CNTs was also observed. Physical and chemical properties of different sorbents were analyzed for interpreting sorption mechanisms.
Results showed that the ionic strength had no significant influence on the adsorption of AT onto SWNTs and MWNTs. With the increase of pH, the adsorption of AT onto the two nanomaterials increased obviously, which indicated the speciation change of atrazine was the dominant factor controlling the adsorption capacity. The adsorption-desorption curves revealed that no significant desorption hysteresis existed under the condition of this study. High adsorption capacity and adsorption reversibility of atrazine on CNTs implied that CNTs could result in health and environmental risks when applied in large scale. The inhibition effect of peat humic acid (PHA) was relatively stronger than that of soil humic acid (SHA), but the two surfactants had much similar impact on the atrazine adsorption by two CNTs. With the increase of surfactant concentration in solution, the adsorption of atrazine by CNTs decreased rapidly when the surfactant concentration was less than 0.5CMC (Critical Micelle Concentration). Surface modification by humic acid and surfactant could effectively separate MWNTs into well dispersed suspensions, but the SWNTs could not be appreciably dispersed by humic acids and surfactants.
引文
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