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火焰中碱金属化合物的激光诱导光碎片荧光成像

Laser-Induced Photofragmentation Fluorescence Imaging of Alkali Compounds in Flames.

作者信息

Leffler Tomas, Brackmann Christian, Aldén Marcus, Li Zhongshan

机构信息

1 Division of Combustion Physics, Lund University, Lund, Sweden.

2 R&D, Strategic Development, Vattenfall AB, Älvkarleby, Sweden.

出版信息

Appl Spectrosc. 2017 Jun;71(6):1289-1299. doi: 10.1177/0003702816681010. Epub 2016 Jan 1.

DOI:10.1177/0003702816681010
PMID:28534679
Abstract

Laser-induced photofragmentation fluorescence has been investigated for the imaging of alkali compounds in premixed laminar methane-air flames. An ArF excimer laser, providing pulses of wavelength 193 nm, was used to photodissociate KCl, KOH, and NaCl molecules in the post-flame region and fluorescence from the excited atomic alkali fragment was detected. Fluorescence emission spectra showed distinct lines of the alkali atoms allowing for efficient background filtering. Temperature data from Rayleigh scattering measurements together with simulations of potassium chemistry presented in literature allowed for conclusions on the relative contributions of potassium species KOH and KCl to the detected signal. Experimental approaches for separate measurements of these components are discussed. Signal power dependence and calculated fractions of dissociated molecules indicate the saturation of the photolysis process, independent on absorption cross-section, under the experimental conditions. Quantitative KCl concentrations up to 30 parts per million (ppm) were evaluated from the fluorescence data and showed good agreement with results from ultraviolet absorption measurements. Detection limits for KCl photofragmentation fluorescence imaging of 0.5 and 1.0 ppm were determined for averaged and single-shot data, respectively. Moreover, simultaneous imaging of KCl and NaCl was demonstrated using a stereoscope with filters. The results indicate that the photofragmentation method can be employed for detailed studies of alkali chemistry in laboratory flames for validation of chemical kinetic mechanisms crucial for efficient biomass fuel utilization.

摘要

激光诱导光碎片荧光已被用于预混层流甲烷 - 空气火焰中碱金属化合物的成像研究。使用一台提供波长为193 nm脉冲的ArF准分子激光器,对火焰后区域中的KCl、KOH和NaCl分子进行光解离,并检测激发态碱金属原子碎片发出的荧光。荧光发射光谱显示出碱金属原子的明显谱线,便于进行有效的背景滤波。瑞利散射测量得到的温度数据以及文献中给出的钾化学模拟结果,有助于得出钾物种KOH和KCl对检测信号的相对贡献。讨论了单独测量这些成分的实验方法。信号功率依赖性和计算得到的解离分子分数表明,在实验条件下,光解过程达到饱和,与吸收截面无关。根据荧光数据评估出高达百万分之30(ppm)的KCl定量浓度,与紫外吸收测量结果吻合良好。对于平均数据和单次拍摄数据,KCl光碎片荧光成像的检测限分别确定为0.5 ppm和1.0 ppm。此外,使用带滤光片的立体显微镜实现了KCl和NaCl的同时成像。结果表明,光碎片方法可用于实验室火焰中碱金属化学的详细研究,以验证对高效生物质燃料利用至关重要的化学动力学机制。

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