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Kinetics of organic molecules in pulsed plasmas of nitrogen or N2/O2 mixtures at near atmospheric pressure

S Pasquiers, N Blin-Simiand, L Magne2013年Plasma Physics and Controlled FusionIF 2.2出版社

In plasmas of atmospheric gases, the kinetics of some aliphatic organic molecules belonging to the hydrocarbons (propene, propane), aldehydes (acetaldehyde) and ketones (acetone) families were studied using a photo-triggered discharge (homogeneous plasma). It was shown that quenchings of N2 metastable states, and the group of singlets , a 1Πg and w 1Δu, are important processes for the decomposition of such molecules. It plays a fundamental role in the nitrogen plasma, but it is also present in air. At low temperature, the oxidation reactions by the oxygen atom or by the hydroxyl radical are not always sufficiently effective to induce an increase of the molecule decomposition when oxygen is added to the nitrogen/organic mixture. For most cases, quenching processes appear purely dissociative. However, recent results obtained for propene lead to the conclusion that a non-dissociative exit route could exist. The quenching of the singlet states induces a break of the double bound C = O for the acetaldehyde and acetone molecules. Some kinetic analogies appear between filamentary and homogeneous plasmas, which could be very useful to get a comprehensive understanding of the physico-chemical processes in dielectric barriers or corona discharges used for various applications.

日本語訳

大気ガスのプラズマ中において、炭化水素(プロペン)、アルデヒド(アセトアルデヒド)、ケトン(アセトン)の各ファミリーに属するいくつかの脂肪族有機分子の動力学を、光誘起放電(均一プラズマ)を用いて研究した。N₂の準安定状態、すなわち一重項状態 A³Σu⁺、a'¹Σu⁻、および w¹Δu の消滅が、そのような分子の分解において重要なプロセスであることが示された。これは窒素プラズマにおいて基本的な役割を果たすが、空気中にも存在する。低温では、酸素原子または水酸基による酸化反応は、窒素/有機物混合物に酸素を添加した際に分子の分解を増加させるほど常に効果的であるとは限らない。ほとんどの場合、消滅プロセスは純粋に解離的であるように見える。しかしながら、プロペンについて得られた最近の結果は、非解離的な脱出経路が存在し得るという結論に導く。一重項状態の消滅は、アセトアルデヒドおよびアセトン分子の C=O 二重結合の切断を誘起する。フィラメント状プラズマと均一プラズマの間にはいくつかの速度論的類似性が現れており、これはさまざまな用途に使用される誘電体バリア放電やコロナ放電における物理化学的プロセスの包括的な理解を得るために非常に有用であり得る。

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