Zong Yichen, Jacob Rohit J, Li Shuiqing, Zachariah Michael R
Department of Chemical and Biomolecular Engineering, Department of Chemistry and Biochemistry, University of Maryland, College Park, Maryland 20706, United States.
J Phys Chem A. 2015 Jun 18;119(24):6171-8. doi: 10.1021/acs.jpca.5b02590. Epub 2015 May 28.
While ultrafine metal particles offer the possibility of very high energy density fuels, there is considerable uncertainty in the mechanism by which metal nanoparticles burn, and few studies that have examined the size dependence to their kinetics at the nanoscale. In this work we quantify the size dependence to the burning rate of titanium and zirconium nanoparticles. Nanoparticles in the range of 20-150 nm were produced via pulsed laser ablation, and then in-flight size-selected using differential electrical mobility. The size-selected oxide free metal particles were directly injected into the post flame region of a laminar flame to create a high temperature (1700-2500 K) oxidizing environment. The reaction was monitored using high-speed videography by tracking the emission from individual nanoparticles. We find that sintering occurs prior to significant reaction, and that once sintering is accounted for, the rate of combustion follows a near nearly (diameter)(1) power-law dependence. Additionally, Arrhenius parameters for the combustion of these nanoparticles were evaluated by measuring the burn times at different ambient temperatures. The optical emission from combustion was also used to model the oxidation process, which we find can be reasonably described with a kinetically controlled shrinking core model.
虽然超细金属颗粒提供了极高能量密度燃料的可能性,但金属纳米颗粒燃烧的机制仍存在相当大的不确定性,并且很少有研究在纳米尺度上考察其动力学的尺寸依赖性。在这项工作中,我们量化了钛和锆纳米颗粒燃烧速率的尺寸依赖性。通过脉冲激光烧蚀制备了20 - 150 nm范围内的纳米颗粒,然后利用差分电迁移率在飞行中进行尺寸选择。将尺寸选择后的无氧化物金属颗粒直接注入层流火焰的火焰后区域,以创建高温(1700 - 2500 K)氧化环境。通过跟踪单个纳米颗粒的发射,利用高速摄像监测反应。我们发现烧结在显著反应之前就会发生,并且一旦考虑到烧结,燃烧速率遵循近乎(直径)(1) 的幂律依赖性。此外,通过测量不同环境温度下的燃烧时间,评估了这些纳米颗粒燃烧的阿累尼乌斯参数。燃烧产生的光发射也被用于模拟氧化过程,我们发现可以用动力学控制的收缩核模型合理地描述该过程。