Aggregation Kinetics of Higher-Order Fullerene Clusters in Aquatic Systems

被引:39
作者
Aich, Nirupam [1 ,3 ]
Boateng, Linkel K. [2 ,4 ]
Sabaraya, Indu Venu [1 ]
Das, Dipesh [1 ]
Flora, Joseph R. V. [2 ]
Saleh, Navid B. [1 ]
机构
[1] Univ Texas Austin, Dept Civil Architectural & Environm Engn, Austin, TX 78712 USA
[2] Univ S Carolina, Dept Civil & Environm Engn, Columbia, SC 29208 USA
[3] SUNY Buffalo, Dept Civil Struct & Environm Engn, Buffalo, NY 14260 USA
[4] Clemson Univ, Dept Chem & Biomol Engn, Clemson, SC 29634 USA
关键词
NATURAL ORGANIC-MATTER; C-60; FULLERENE; AQUEOUS C-60; COLLOIDAL PROPERTIES; GOLD NANOPARTICLES; CARBON NANOTUBES; HUMIC-ACID; WATER; METALLOFULLERENES; RELAXIVITY;
D O I
10.1021/acs.est.5b05447
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The aggregation kinetics of nC(60) and higher order fullerene (HOF) clusters, i.e., nC(70), nC(76), and nC(84), was systematically studied under a wide range of mono- (NaCl) and divalent (CaCl2) electrolytes and using time-resolved dynamic light scattering. Suwanee River Humic Acid (SRHA) was also used to determine the effect of natural macromolecules on nHOF aggregation. An increase in electrolyte concentration resulted in electrical double-layer compression of the negatively charged fullerene clusters, and the nC(60)s and nHOFs alike displayed classical Derjaguin Landau Verwey Overbeek (DLVO) type interaction. The critical coagulation concentration (CCC) displayed a strong negative correlation with the carbon number in fullerenes and was estimated as 220, 150, 100, and 70 mM NaCl and 10, 12, 6, and 7.5 mM CaCl2 for nC(60), nC(70), nC(76), and nC(84), respectively. The aggregation mechanisiin. (i.e., van der Waals interaction domination) was enumerated via molecular dynamics simulation and modified DLVO model. The presence of SRHA. (2.5 mg TOC/L) profoundly influenced the aggregation behavior by stabilizing all fullerene clusters, even at a 100 mM NaCl concentration. The results from this study can be utilized to predict aggregation kinetics of nHOF clusters other than the ones studied here. The scaling factor for van der Waals interaction can also be used to model nHOF duster interaction.
引用
收藏
页码:3562 / 3571
页数:10
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