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使用基于O2的纯转动相干反斯托克斯拉曼散射对火焰喷雾热解过程的液相和颗粒相进行气相温度测量。

Gas phase temperature measurements in the liquid and particle regime of a flame spray pyrolysis process using O2-based pure rotational coherent anti-Stokes Raman scattering.

作者信息

Engel Sascha R, Koegler Andreas F, Gao Yi, Kilian Daniel, Voigt Michael, Seeger Thomas, Peukert Wolfgang, Leipertz Alfred

机构信息

Institute of Engineering Thermodynamics, University of Erlangen-Nuremberg, Erlangen 91058, Germany.

出版信息

Appl Opt. 2012 Sep 1;51(25):6063-75. doi: 10.1364/AO.51.006063.

DOI:10.1364/AO.51.006063
PMID:22945152
Abstract

For the production of oxide nanoparticles at a commercial scale, flame spray processes are frequently used where mostly oxygen is fed to the flame if high combustion temperatures and thus small primary particle sizes are desired. To improve the understanding of these complex processes in situ, noninvasive optical measurement techniques were applied to characterize the extremely turbulent and unsteady combustion field at those positions where the particles are formed from precursor containing organic solvent droplets. This particle-forming regime was identified by laser-induced breakdown detection. The gas phase temperatures in the surrounding of droplets and particles were measured with O(2)-based pure rotational coherent anti-Stokes Raman scattering (CARS). Pure rotational CARS measurements benefit from a polarization filtering technique that is essential in particle and droplet environments for acquiring CARS spectra suitable for temperature fitting. Due to different signal disturbing processes only the minority of the collected signals could be used for temperature evaluation. The selection of these suitable signals is one of the major problems to be solved for a reliable evaluation process. Applying these filtering and signal selection steps temperature measurements have successfully been conducted. Time-resolved, single-pulse measurements exhibit temperatures between near-room and combustion temperatures due to the strongly fluctuating and flickering behavior of the particle-generating flame. The mean flame temperatures determined from the single-pulse data are decreasing with increasing particle concentrations. They indicate the dissipation of large amounts of energy from the surrounding gas phase in the presence of particles.

摘要

对于商业规模的氧化物纳米颗粒生产,常采用火焰喷雾工艺,若希望达到高燃烧温度从而获得小的一次粒径,则大多向火焰中通入氧气。为深入了解这些复杂的原位过程,应用了非侵入式光学测量技术来表征在由含前驱体的有机溶剂液滴形成颗粒的位置处极其湍流且不稳定的燃烧场。通过激光诱导击穿检测确定了这种颗粒形成状态。利用基于O(2)的纯转动相干反斯托克斯拉曼散射(CARS)测量液滴和颗粒周围的气相温度。纯转动CARS测量受益于一种偏振滤波技术,该技术在颗粒和液滴环境中对于获取适合温度拟合的CARS光谱至关重要。由于不同的信号干扰过程,只有少数采集到的信号可用于温度评估。选择这些合适的信号是可靠评估过程中要解决的主要问题之一。应用这些滤波和信号选择步骤已成功进行了温度测量。由于产生颗粒的火焰强烈波动和闪烁,时间分辨的单脉冲测量显示温度介于近室温与燃烧温度之间。从单脉冲数据确定的平均火焰温度随颗粒浓度增加而降低。它们表明在有颗粒存在的情况下,大量能量从周围气相耗散。

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