Mn2O3/γ-Al2O3 catalysts synergistic double dielectric barrier discharge (DDBD) degradation of toluene, ethyl-acetate and acetone
Mn2O3/γ-Al2O3 catalysts synergistic double dielectric barrier discharge (DDBD) degradation of toluene, ethyl-acetate and acetone
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DOI：
10.1016/j.chemosphere.2021.131299
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发表时间：
2021-06-28
期刊：
影响因子：
8.8
通讯作者：
Zhong, Fangchuan
中科院分区：
文献类型：
--
作者：
Liu, Xin;Liu, Jianqi;Zhong, Fangchuan
将Mn 2 O3/γ-Al 2 O3催化剂与双介质阻挡放电（DDBD）相结合，对丙酮、甲苯和乙酸乙酯进行降解。采用水热法合成了不同Mn含量的Mn 2 O3/γ-Al 2 O3催化剂。采用XRD、SEM、XPS和H-2-TPR等方法对催化剂进行了表征。在所制备的催化剂中，Mn负载量为5wt%的Mn 2 O3/γ-Al 2 O3催化剂对多组分VOCs的降解性能最好，去除率最高（丙酮58.8%，甲苯96.3%，乙酸乙酯85.8%），在比输入能量（SIE）为700 J L-1时，获得最佳的碳平衡（87.5%）和CO2选择性（51.9%）。Mn_2O_3/γ-Al_2O_3催化剂的引入明显抑制了臭氧的生成。较高的Mn 3 +/Mn比、较高的O-2/O-2-比和良好的低温还原性有利于VOCs的降解。γ-Al 2 O3表面高度分散的Mn 2 O3晶体也可能是改善VOC降解的一种解释。GC-MS分析结果表明，随着SIE的增加，有机副产物的种类逐渐减少，并对混合VOCs在等离子体中和催化剂表面的降解机理进行了探讨。
Mn2O3/gamma-Al2O3 catalysts was combined with double dielectric barrier discharge (DDBD) for degradation of acetone, toluene and ethyl acetate. Mn2O3/gamma-Al2O3 catalysts with different Mn loading were synthesized by hydrothermal method. XRD, SEM, XPS and H-2-TPR were applied to characterize the catalysts. Among the catalysts prepared, the Mn2O3/gamma-Al2O3 catalysts with 5 wt% Mn loading presented the best performance in multicomponent VOCs degradation, which the highest removal efficiency (58.8% for acetone, 96.3% for toluene and 85.8% for ethyl acetate), the best carbon balance (87.5%) and CO2 selectivity (51.9%) were obtained at a specific input energy (SIE) of 700 J L-1. The formation of ozone was obviously inhibited with the introduction of Mn2O3/gamma-Al2O3 catalysts. The higher Mn3+/Mn ratio, higher O-2/O-2-ratio and excellent low-temperature reducibility were beneficial for the VOCs degradation. Highly dispersed Mn2O3 crystals on the surface of gamma-Al2O3 also might be an explanation for the improvement of VOCs degradation. According to the result of GC-MS, the variety of organic by-products gradually decreased with the increase of SIE, and the degradation mechanism of the mixed VOCs in plasma and on catalyst surface was discussed.