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介质阻挡放电反应器中有机副产物的实时监测与定量及丙酮分解机理研究。

Real-time monitoring and quantification of organic by-products and mechanism study of acetone decomposition in a dielectric barrier discharge reactor.

机构信息

School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, China.

Kunshan Hexin Mass Spectrometry Technology Co., Ltd., Kunshan, 215311, China.

出版信息

Environ Sci Pollut Res Int. 2019 Mar;26(7):6773-6781. doi: 10.1007/s11356-019-04127-z. Epub 2019 Jan 10.

Abstract

Non-thermal plasma (NTP) degradation of low-concentration acetone was investigated in a cylindrical dielectric barrier discharge reactor. The effects of oxygen content and flow rate on the removal efficiency at various discharge powers were examined in real-time. The acetone removal efficiency decreases drastically and then remains stable or increases gradually as the O content increases from 0 to 25%, and further to 50%. The organic by-products were characterized and quantified using a real-time proton transfer reaction time-of-flight mass spectrometry (PTR-TOF-MS) instrument. The observed organic compounds, with concentrations about ppbv/ppmv by volume, were mainly formaldehyde, methanol, ketene, acetaldehyde, formic acid, acetone, and acetic acid. The discharge power was a critical factor affecting the concentration of the organic by-products and the selectivity toward CO. The mechanism study based on the by-product monitor in real-time showed that acetone firstly fragments into methyl radicals, acetyl radicals, and H; then, the methyl and acetyl radicals are oxidized by O or OH radicals into acetaldehyde, methanol, and other compounds. It seems that acetaldehyde could be an intermediate in acetone decomposition. Firstly, most of the acetone molecules were decomposed into acetaldehyde molecules; then, the acetaldehyde molecules continued to be decomposed and oxidized into other compounds, such as acetic acid and formaldehyde. These investigations not only proposed a detail decomposition mechanism for acetone in dielectric barrier discharge reactor, but also provided a potential way to analyze and evaluate the practicability of NTP removal of VOCs.

摘要

采用圆柱形介质阻挡放电反应器研究了低浓度丙酮在非热等离子体(NTP)中的降解情况。实时考察了不同放电功率下氧含量和流速对去除效率的影响。随着 O 含量从 0 增加到 25%,然后增加到 50%,丙酮去除效率急剧下降,然后保持稳定或逐渐增加。使用实时质子转移反应飞行时间质谱(PTR-TOF-MS)仪器对有机副产物进行了表征和定量分析。观察到的有机化合物浓度约为体积的 ppbv/ppmv,主要为甲醛、甲醇、烯酮、乙醛、甲酸、丙酮和乙酸。放电功率是影响有机副产物浓度和 CO 选择性的关键因素。基于实时副产物监测的机理研究表明,丙酮首先裂化成甲基自由基、乙酰基自由基和 H;然后,甲基和乙酰基自由基被 O 或 OH 自由基氧化成乙醛、甲醇和其他化合物。似乎乙醛是丙酮分解的中间产物。首先,大部分丙酮分子分解成乙醛分子;然后,乙醛分子继续分解和氧化成其他化合物,如乙酸和甲醛。这些研究不仅提出了介质阻挡放电反应器中丙酮的详细分解机理,而且为分析和评估 NTP 去除 VOCs 的实用性提供了一种潜在的方法。

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