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超细碳颗粒上实验性与理论性非均相成核的比较

Comparison of Experimental and Theoretical Heterogeneous Nucleation on Ultrafine Carbon Particles.

作者信息

Lee Doh-Won, Hopke Philip K, Rasmussen Don H, Wang Hwa-Chi, Mavliev Rashid

机构信息

Clarkson University, Potsdam, New York, Illinois Institute of Technology, Chicago, Illinois, and Air Liquide, Chicago Research Center, Countryside, Illinois.

出版信息

J Phys Chem B. 2003 Dec 18;107(50):13813-22. doi: 10.1021/jp0278216.

Abstract

Using a modified turbulent mixing CNC, the heterogeneous nucleation of different compounds (working fluids) on nanometer sized carbon particles was examined. The working fluids were dibutyl phthalate, octadecane, octadecanol, and octadecanoic acid. Based on the particle size distributions measured with a scanning mobility particle sizer system, nucleation and consequent growth were examined with respect to different temperature and vapor pressure for each working fluid. Nucleation rates for all conditions were calculated from the fitted size distribution data by subtracting the residual nonactivated particle concentration for each condition. Experimental nucleation rates were compared to the calculated ones based on Fletcher's heterogeneous nucleation theory. This theory matches well with the experiments with octadecanol and octadecanoic acid, and at high supersaturation ratios for dibutyl phthalate. However, the theory shows discrepancies with the observed phenomena at low supersaturation for dibutyl phthalate, and especially for octadecane. Several possible hypotheses for the discrepancies and observed particle growth are discussed.

摘要

使用改良的湍流混合化学气相凝聚法,研究了不同化合物(工作流体)在纳米级碳颗粒上的异质成核现象。工作流体包括邻苯二甲酸二丁酯、十八烷、十八烷醇和十八烷酸。基于用扫描迁移率粒径谱仪系统测量的粒径分布,针对每种工作流体,研究了不同温度和蒸气压下的成核及随后的生长情况。通过从每种条件下拟合的粒径分布数据中减去残余未活化颗粒浓度,计算出所有条件下的成核速率。将实验成核速率与基于弗莱彻异质成核理论计算出的速率进行了比较。该理论与十八烷醇和十八烷酸的实验结果以及邻苯二甲酸二丁酯在高过饱和比下的实验结果吻合良好。然而,该理论在邻苯二甲酸二丁酯低过饱和时,尤其是十八烷的情况下,与观察到的现象存在差异。讨论了造成这些差异以及观察到的颗粒生长现象的几种可能假设。

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