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介质阻挡放电辅助苯氧化中的可变产物。

Variable products in dielectric-barrier discharge assisted benzene oxidation.

机构信息

Radiation & Photochemistry Division, Bhabha Atomic Research Centre, Trombay, Mumbai 400085, India.

出版信息

J Hazard Mater. 2010 Jun 15;178(1-3):693-8. doi: 10.1016/j.jhazmat.2010.01.143. Epub 2010 Feb 4.

DOI:10.1016/j.jhazmat.2010.01.143
PMID:20188466
Abstract

Atmospheric-pressure dielectric-barrier discharge (DBD) assisted control of benzene((g)) oxidation into different classes of products is presented in this study. The gas-phase products were directly analyzed online by GC-FID and GC-MS. In addition, a solid yellowish surface deposit also formed, which was dissolved in 10 mL ethanol after each 10 min DBD cycle for GC analyses. One of the gas-phase products, phenol was also separately collected and estimated by Folin-Ciocalteu's wet-colorimetric method. In the gas phase only phenol and biphenyl were detected at maximum total conversion of approximately 3%, while in the ethanolic solution furthermore 1,2- and 1,4-dihydroxybenzene, 2,2'-biphenol, 2- and 4-phenylphenol and 4-phenoxyphenol were estimated at microM to mM level, and reveal approximately 30% total conversion. Products' types hint at the phenyl radical as the primary precursor. However, with the use of mesoporous molecular sieve 10X packing in unison with DBD, while the concentrations of such phenolic products decreased drastically, a number of open chain and non-aromatic ethers, aldehydes and esters, and also naphthalene and biphenylene were formed. In addition to high DBD process efficiency, the latter results suggest modification of discharge characteristics, and also strong physicochemical effects of cavity size and surface property on the intermediate reactions therein. Thus, use of such packing highlights a novel and practical methodology for control of chemical reactions towards useful product types, vis-à-vis pollutant mitigation.

摘要

本研究提出了大气压介质阻挡放电(DBD)辅助控制苯(g)氧化为不同类别的产物。通过气相色谱-氢火焰离子化检测器(GC-FID)和气相色谱-质谱联用仪(GC-MS)在线直接分析气相产物。此外,还形成了一种黄色的固体沉积物,在每次 10 分钟 DBD 循环后,将其溶解在 10 mL 乙醇中进行 GC 分析。气相产物之一苯酚也通过 Folin-Ciocalteu 的湿比色法进行了单独收集和估计。在气相中,仅在最大总转化率约为 3%时检测到苯酚和联苯,而在乙醇溶液中,还估计到微摩尔至毫摩尔水平的 1,2-和 1,4-二羟基苯、2,2'-联苯、2-和 4-苯苯酚和 4-苯氧苯酚,总转化率约为 30%。产物类型表明苯基自由基是主要的前体。然而,使用介孔分子筛 10X 与 DBD 一起包装,虽然酚类产物的浓度急剧下降,但形成了许多开链和非芳烃醚、醛和酯,以及萘和联苯。除了具有高的 DBD 工艺效率外,后者的结果表明了放电特性的修饰,以及空腔尺寸和表面特性对其中间反应的强烈物理化学影响。因此,这种包装的使用突出了一种新颖而实用的方法,用于控制化学反应以获得有用的产物类型,同时减轻污染物的排放。

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