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离子强度和温度对多壁碳纳米管聚集和沉积的影响。

Effects of ionic strength and temperature on the aggregation and deposition of multi-walled carbon nanotubes.

机构信息

Environment Research Institute, Shandong University, Jinan 250100, China.

Environment Research Institute, Shandong University, Jinan 250100, China.

出版信息

J Environ Sci (China). 2017 Jan;51:248-255. doi: 10.1016/j.jes.2016.07.003. Epub 2016 Jul 25.

Abstract

The aggregation and deposition of carbon nanotubes (CNTs) determines their transport and fate in natural waters. Therefore, the aggregation kinetics of humic-acid treated multi-walled carbon nanotubes (HA-MWCNTs) was investigated by time-resolved dynamic light scattering in NaCl and CaCl electrolyte solutions. Increased ionic strength induced HA-MWCNT aggregation due to the less negative zeta potential and the reduced electrostatic repulsion. The critical coagulation concentration (CCC) values of HA-MWCNTs were 80mmol/L in NaCl and 1.3mmol/L in CaCl electrolyte, showing that Ca causes more serious aggregation than Na. The aggregation behavior of HA-MWCNTs was consistent with Derjaguin-Landau-Verwey-Overbeek theory. The deposition kinetics of HA-MWCNTs was measured by the optical absorbance at 800nm. The critical deposition concentrations for HA-MWCNT in NaCl and CaCl solutions were close to the CCC values, therefore the rate of deposition cannot be increased by changing the ionic strength in the diffusion-limited aggregation regime. The deposition process was correlated to the aggregation since larger aggregates increased gravitational deposition and decreased random Brownian diffusion. HA-MWCNTs hydrodynamic diameters were evaluated at 5, 15 and 25°C. Higher temperature caused faster aggregation due to the reduced electrostatic repulsion and increased random Brownian motion and collision frequency. HA-MWCNTs aggregate faster at higher temperature in either NaCl or CaCl electrolyte due to the decreased electrostatic repulsion and increased random Brownian motion. Our results suggest that CNT aggregation and deposition are two correlated processes governed by the electrolyte, and CNT transport is favored at low ionic strength and low temperature.

摘要

碳纳米管(CNTs)的聚集和沉积决定了它们在天然水中的迁移和归宿。因此,通过在 NaCl 和 CaCl 电解质溶液中使用时间分辨动态光散射研究了腐殖酸处理的多壁碳纳米管(HA-MWCNTs)的聚集动力学。由于zeta 电位变得不那么负和静电排斥减少,离子强度的增加导致 HA-MWCNT 聚集。HA-MWCNTs 的临界聚沉浓度(CCC)值在 NaCl 中为 80mmol/L,在 CaCl 电解质中为 1.3mmol/L,表明 Ca 比 Na 引起更严重的聚集。HA-MWCNTs 的聚集行为符合德加古林-兰德维厄-奥弗贝克理论。通过 800nm 的光吸收测量了 HA-MWCNTs 的沉积动力学。HA-MWCNT 在 NaCl 和 CaCl 溶液中的临界沉积浓度接近 CCC 值,因此在扩散限制聚集区,通过改变离子强度不能增加沉积速率。沉积过程与聚集相关,因为较大的聚集体增加了重力沉积并减少了随机布朗扩散。在 5、15 和 25°C 下评估了 HA-MWCNTs 的水动力直径。由于静电排斥减少和随机布朗运动和碰撞频率增加,较高的温度导致更快的聚集。在 NaCl 或 CaCl 电解质中,较高的温度使 HA-MWCNTs 更快地聚集,这是由于静电排斥减少和随机布朗运动增加。我们的结果表明,CNT 聚集和沉积是两个相互关联的过程,受电解质控制,CNT 输运在低离子强度和低温下更有利。

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