Catalytic oxidation of benzene with ozone over alumina-supported manganese oxides
Catalytic oxidation of benzene with ozone over alumina-supported manganese oxides
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DOI：
10.1016/j.jcat.2004.07.029
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发表时间：
2004-10-25
影响因子：
7.3
通讯作者：
Futamura, S
中科院分区：
文献类型：
--
作者：
Einaga, H;Futamura, S
以氧化铝负载的锰氧化物为催化剂，在室温(295K)下进行了臭氧催化氧化苯的反应，考察了苯氧化和环氧化合物的生成行为。臭氧和苯的分解速率之比为6，与臭氧浓度、反应时间和锰负载量无关。臭氧的分解量与COX的生成量呈线性相关，而臭氧的分解量与苯反应的量偏离线性关系。碳平衡在26-37%的范围内，这是由于形成了两种中间体，即弱结合化合物，包括甲酸和强结合表面甲酸盐和羧酸盐。在苯氧化过程中，由于中间体在催化剂表面的堆积，催化剂明显失活。在氧气流中573K的热处理可使弱结合化合物脱除。强结合的表面甲酸盐和羧酸盐通过进一步加热到723K被氧化成COX，失活的催化剂通过热处理再生。(C)2004 Elsevier Inc.保留所有权利。
Catalytic oxidation of benzene with ozone over alumina-supported manganese oxides was carried out at room temperature (295 K) to investigate the behavior of benzene oxidation and COx formation. The ratio of the decomposition rate for ozone to that for benzene was found to be 6, independent of ozone concentration, reaction times, and the amount of Mn loading. A linear correlation was observed for the amount of ozone decomposed and that of COx formed, whereas deviation from linearity was observed between the amount of ozone decomposed and that of benzene reacted. Carbon balance was in the range of 26-37% due to the formation of two types of intermediates, weakly bound compounds including formic acid and strongly bound surface formate and carboxylates. Catalyst was significantly deactivated due to the buildup of the intermediates on the catalyst surface during the course of benzene oxidation. The weakly bound compounds were removed by heat treatment at 573 K in the O-2 flow. The strongly bound surface formate and carboxylates were oxidized to COx by further heating up to 723 K. The deactivated catalyst was regenerated by the heat treatment. (C) 2004 Elsevier Inc. All rights reserved.