Enhanced Catalytic Probe Design for Mapping Radical Density in the Plasma Afterglow.

IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry A Pub Date : 2024-11-11 DOI:10.1021/acs.jpca.4c06195
Anja Herrmann, Patrick M Krebaum, Susanta Bera, Mihalis N Tsampas, Mauritius C M van de Sanden
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Abstract

The electrification of chemical processes using plasma generates an increasing demand for sensors, monitoring concentrations of plasma-activated species such as radicals. Radical probes are a low-cost in situ method for spatially resolved quantification of the radical density in a plasma afterglow using the heat from the exothermal recombination of radicals on a catalytic surface. However, distinguishing recombination heating from other heat fluxes in the system is challenging. In this study, we present a heat flux analysis based on probe measurements inside the reactor, with simultaneous IR imaging monitoring of the temperature of the reactor wall. The impact of radiation heat on a single thermocouple as well as the advantage of a dual thermocouple setup (using a catalytic unit together with a reference thermocouple) is shown. We add a heat sink with a monitored temperature to the dual thermocouple setup, allowing the determination of conductive and radiative heat fluxes. The heat sink gives more information on the measurement and reduces ambiguities in the evaluation used by others. The probe was tested by mapping N atom densities throughout the plasma afterglow of our reactor, enabling evaluation of the recombination kinetics of the radicals in the gas phase. Three-body recombination was shown to be the main pathway of recombination, with a recombination rate of krec = (2.0 ± 0.9)·10-44 m6/s, which is in line with the known literature findings, demonstrating that the measured species are N radicals and the probe did not influence the plasma or recombination reactions in the afterglow.

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用于绘制等离子体余辉中自由基密度的增强型催化探针设计。
利用等离子体实现化学过程的电气化,对传感器的需求与日俱增,以监测等离子体活化物种(如自由基)的浓度。自由基探针是一种低成本的原位方法,利用催化表面自由基放热重组产生的热量,对等离子体余辉中的自由基密度进行空间分辨量化。然而,将重组加热与系统中的其他热通量区分开来具有挑战性。在本研究中,我们提出了一种基于反应器内探针测量的热通量分析方法,并同时对反应器壁的温度进行了红外成像监测。研究显示了辐射热对单个热电偶的影响以及双热电偶设置(使用催化装置和参考热电偶)的优势。我们在双热电偶装置中添加了一个可监测温度的散热器,从而可以确定传导热通量和辐射热通量。散热器提供了更多的测量信息,减少了他人评估中的模糊性。通过绘制反应器等离子体余辉中的 N 原子密度图,对探针进行了测试,从而评估了气相中自由基的重组动力学。结果表明,三体重组是重组的主要途径,重组率为 krec = (2.0 ± 0.9)-10-44 m6/s,这与已知的文献研究结果一致,表明测量到的物种是 N 自由基,探针不会影响余辉中的等离子体或重组反应。
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来源期刊
The Journal of Physical Chemistry A
The Journal of Physical Chemistry A 化学-物理:原子、分子和化学物理
CiteScore
5.20
自引率
10.30%
发文量
922
审稿时长
1.3 months
期刊介绍: The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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