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量子点和聚苯乙烯乳胶纳米颗粒在氧化铝上的沉积动力学:水化学和颗粒涂层的作用。

Deposition kinetics of quantum dots and polystyrene latex nanoparticles onto alumina: role of water chemistry and particle coating.

机构信息

Department of Chemical Engineering, McGill University , Montreal, Quebec H3A 2B2, Canada.

出版信息

Environ Sci Technol. 2013 Mar 5;47(5):2212-20. doi: 10.1021/es303392v. Epub 2013 Feb 20.

Abstract

A clear understanding of the factors controlling the deposition behavior of engineered nanoparticles (ENPs), such as quantum dots (QDs), is necessary for predicting their transport and fate in natural subsurface environments and in water filtration processes. A quartz crystal microbalance with dissipation monitoring (QCM-D) was used to study the effect of particle surface coatings and water chemistry on the deposition of commercial QDs onto Al2O3. Two carboxylated QDs (CdSe and CdTe) with different surface coatings were compared with two model nanoparticles: sulfate-functionalized (sPL) and carboxyl-modified (cPL) polystyrene latex. Deposition rates were assessed over a range of ionic strengths (IS) in simple electrolyte (KCl) and in electrolyte supplemented with two organic molecules found in natural waters; namely, humic acid and rhamnolipid. The Al2O3 collector used here is selected to be representative of oxide patches found on the surface of aquifer or filter grains. Deposition studies showed that ENP deposition rates on bare Al2O3 generally decreased with increasing salt concentration, with the exception of the polyacrylic-acid (PAA) coated CdTe QD which exhibited unique deposition behavior due to changes in the conformation of the PAA coating. QD deposition rates on bare Al2O3 were approximately 1 order of magnitude lower than those of the polystyrene latex nanoparticles, likely as a result of steric stabilization imparted by the QD surface coatings. Adsorption of humic acid or rhamnolipid on the Al2O3 surface resulted in charge reversal of the collector and subsequent reduction in the deposition rates of all ENPs. Moreover, the ratio of the two QCM-D output parameters, frequency and dissipation, revealed key structural information of the ENP-collector interface; namely, on bare Al2O3, the latex particles were rigidly attached as compared to the more loosely attached QDs. This study emphasizes the importance of considering the nature of ENP coatings as well as organic molecule adsorption onto particle and collector surfaces to avoid underestimating ENP mobility in natural and engineered aquatic environments.

摘要

要预测工程纳米颗粒(ENP),如量子点(QD)在自然地下环境和水过滤过程中的迁移和归宿,就必须清楚了解控制其沉积行为的因素。本研究采用石英晶体微天平(QCM-D)研究了颗粒表面涂层和水化学对商用 QD 在 Al2O3 上沉积的影响。比较了两种具有不同表面涂层的羧基化 QD(CdSe 和 CdTe)和两种模型纳米颗粒:硫酸化官能化(sPL)和羧基改性(cPL)聚苯乙烯乳胶。在简单电解质(KCl)和补充了两种天然水中存在的有机分子(即腐殖酸和鼠李糖脂)的电解质中,评估了一系列离子强度(IS)下的沉积速率。这里使用的 Al2O3 收集器被选择为代表含水层或过滤颗粒表面上氧化物斑块。沉积研究表明,ENP 在裸 Al2O3 上的沉积速率通常随盐浓度的增加而降低,除了聚丙稀酸(PAA)涂覆的 CdTe QD 外,由于 PAA 涂层构象的变化,CdTe QD 表现出独特的沉积行为。在裸 Al2O3 上的 QD 沉积速率比聚苯乙烯乳胶纳米颗粒低约 1 个数量级,这可能是由于 QD 表面涂层赋予的空间稳定作用。腐殖酸或鼠李糖脂在 Al2O3 表面的吸附导致收集器电荷反转,随后所有 ENP 的沉积速率降低。此外,两个 QCM-D 输出参数,即频率和耗散的比值,揭示了 ENP-收集器界面的关键结构信息;即在裸 Al2O3 上,乳胶颗粒刚性附着,而 QD 则附着较松。本研究强调了考虑 ENP 涂层的性质以及有机分子在颗粒和收集器表面上的吸附的重要性,以避免低估自然和工程水生环境中 ENP 的迁移性。

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