Removal of toluene by sequential adsorption-plasma oxidation: Mixed support and catalyst deactivation

Removal of toluene by sequential adsorption-plasma oxidation: Mixed support and catalyst deactivation
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连续吸附-等离子体氧化去除甲苯:混合载体和催化剂失活

DOI:
10.1016/j.jhazmat.2017.03.046
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发表时间:
2017-07-15
影响因子:
13.6
通讯作者:
Dang, Xiaoqing
Dang, Xiaoqing
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Qin, Caihong;Huang, Xuemin;Dang, Xiaoqing

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采用γ-Al_2O_3、HZSM-5、γ-Al_2O_3和HZSM-5的混合物以及它们负载的Mn-Ag催化剂,在常压和室温下,采用顺序吸附-等离子体氧化系统对模拟干燥空气中的甲苯进行了去除。等离子体氧化120 min后,γ-Al 2 O3的碳平衡比HZSM-5好(接近75%),但CO2产率只有50%左右,甲苯有一定程度的脱附。当使用质量比为1/2的HZSM-5和γ-Al 2 O 3的混合物时,碳平衡高达90%,其中82%是CO2。为了使这种高考克斯产率合理化,测试了混合载体的吸附性能和放电特性。在连续吸附-等离子体氧化的七个循环之后,发生载体和Mn-Ag催化剂失活。采用SEM、BET法、XRD、XPS和GC-MS等手段对失活前后的载体和催化剂进行了表征,探讨了载体和催化剂的失活机理。O2程序升温氧化可回收97.6%的失活载体和76%的失活催化剂。(C)2017 Elsevier B. V.版权所有。
A sequential adsorption-plasma oxidation system was used to remove toluene from simulated dry air using gamma-Al2O3, HZSM-5, a mixture of the two materials or their supported Mn-Ag catalyst as adsorbents under atmospheric pressure and room temperature. After 120 min of plasma oxidation, gamma-Al2O3 had a better carbon balance (similar to 75%) than HZSM-5, but the CO2 yield of gamma-Al2O3 was only similar to 50%; and there was some desorption of toluene when gamma-Al2O3 was used. When a mixture of HZSM-5 and gamma-Al2O3 with a mass ratio of 1/2 was used, the carbon balance was up to 90% and 82% of this was CO2. The adsorption performance and electric discharge characteristics of the mixed supports were tested in order to rationalize this high COx yield. After seven cycles of sequential adsorption-plasma oxidation, support and Mn-Ag catalyst deactivation occurred. The support and catalyst were characterized before and after deactivation by SEM, a BET method, XRD, XPS and GC-MS in order to probe the mechanism of their deactivation. 97.6% of the deactivated supports and 76% of the deactivated catalysts could be recovered by O-2 temperature-programmed oxidation. (C) 2017 Elsevier B.V. All rights reserved.