School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, China.
Kunshan Hexin Mass Spectrometry Technology Co., Ltd., Kunshan, 215311, China.
Environ Sci Pollut Res Int. 2019 Mar;26(7):6773-6781. doi: 10.1007/s11356-019-04127-z. Epub 2019 Jan 10.
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.
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。