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One-pot synthesis of monolithic Mn-Ce-Zr ternary mixed oxides catalyst for the catalytic combustion of chlorobenzene
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2018-07-18 , DOI: 10.1016/j.cej.2018.07.091
Gaoyuan Long , Mengxia Chen , Yajun Li , Jiafeng Ding , Runze Sun , Yanfang Zhou , Xiuying Huang , Gaorui Han , Weirong Zhao

Mn-based catalysts have been widely investigated for the disposal of chlorinated volatile organic compounds (CVOCs), due to their excellent catalytic performances. In this study, Ce-Zr co-modified monolithic Mn-based oxide catalysts were synthesized by one-pot solution combustion method. All the samples were tested with chlorobenzene (CB), as a model molecule of CVOCs. The Mn-Ce-Zr catalyst retained high surface area, small particle size and high redox properties, and exhibited superior catalytic activity with T90% at 390 °C. The superior catalytic activity of Mn-Ce-Zr catalyst originated from the larger specific surface area, the higher Mn4+ cation and surface oxygen contents, as well as the greater oxygen mobility and manganese reducibility. The catalytic activity declined slightly during the life test and the reduced activity could be partially regenerated by introducing water vapor. H2-TPR results indicated that the blockage of active sites by strongly adsorbed chlorine species contributed to the deactivation. By-products generated during CB oxidation included phenol, 2-butene, 2-butenal, acetone, trichloromethane, etc., no highly toxic polychlorinated aromatic compounds were detected. CB oxidation was initiated by CCl bond cleavage followed with ring-open reactions. This work developed a monolithic Mn-Ce-Zr ternary mixed oxides catalyst with striking activity and stability and provided some insightful understandings for designing industrial catalysts.



中文翻译:

一锅法合成整体式Mn-Ce-Zr三元混合氧化物催化剂用于催化燃烧氯苯

锰基催化剂因其出色的催化性能而被广泛研究用于处理氯化挥发性有机化合物(CVOC)。本研究采用一锅法溶液燃烧法合成了Ce-Zr共修饰的整体式锰基氧化物催化剂。所有样品均用氯苯(CB)作为CVOC的模型分子进行了测试。Mn-Ce-Zr催化剂保留了较高的表面积,较小的粒径和较高的氧化还原特性,并在390°C时具有90%的T表现出优异的催化活性。Mn-Ce-Zr催化剂的优异催化活性源自较大的比表面积,较高的Mn 4+阳离子和表面氧含量,以及更高的氧迁移率和锰还原性。在寿命试验中,催化活性略有下降,而降低的活性可以通过引入水蒸气而部分再生。H 2 -TPR结果表明,强烈吸附的氯物种对活性位点的阻塞导致了失活。在CB氧化过程中产生的副产物包括苯酚,2-丁烯,2-丁烯醛,丙酮,三氯甲烷等,未检测到高毒性的多氯芳族化合物。C引发的CB氧化Cl键裂解后发生开环反应。这项工作开发了具有显着活性和稳定性的整体式Mn-Ce-Zr三元混合氧化物催化剂,并为工业催化剂的设计提供了一些深刻的认识。

更新日期:2018-07-18
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