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制备 MnO-CeO/堇青石催化剂,掺杂 FeO 和 CuO,以实现对氯苯的优先催化氧化。

Fabrication of MnO-CeO/cordierite catalysts doped with FeO and CuO for preferable catalytic oxidation of chlorobenzene.

机构信息

Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technologies, Jiangsu Key Laboratory of Atmospheric Environmental Monitoring & Pollution Control, School of Environmental Science & Engineering, Nanjing University of Information Science & Technology, Nanjing, People's Republic of China.

出版信息

Environ Technol. 2020 May;41(13):1664-1676. doi: 10.1080/09593330.2018.1543359. Epub 2018 Nov 8.

Abstract

A series of MnO-CeO catalysts with MO doping (M = Cu, Fe, Co and La) supported on cordierite were synthesized by the citric acid complex method, showing preferable catalytic oxidation of chlorobenzene. The distribution of active oxides, surface areas, as well as the structural morphology of M-MnO-CeO catalysts varied with the different Mn/Ce and M/Mn molar ratios. Meanwhile, physicochemical properties of these catalysts were characterized by XRD, BET, SEM, TEM, H-TPR and IR. More importantly, the catalytic oxidation routes were also investigated where the process was from chlorobenzene to CO, HO, HCl and other by-products for the FeO-MnO-CeO and CuO-MnO-CeO catalysts. The CuO-MnO-CeO catalysts showed a higher chlorobenzene conversion, and the measured light-off temperature was approximately 400°C. However, a large amount of chloropropane as main by-products was observed. For the FeO-MnO-CeO catalysts, more carbon monoxide could be found with inadequate oxidation. Comparative analyses of two catalysts indicated that the main cause of the oxidation activities and mechanisms were different in the oxidation capacity and water absorbability of FeO and CuO. Nevertheless, all of these catalysts did not exhibit any deactivation due to chloride with a high reaction temperature, with chloride transformed to form HCl in the off-gas stream.

摘要

一系列负载在堇青石上的具有 MO 掺杂(M=Cu、Fe、Co 和 La)的 MnO-CeO 催化剂通过柠檬酸络合法合成,表现出对氯苯的较好的催化氧化性能。不同的 Mn/Ce 和 M/Mn 摩尔比会导致 M-MnO-CeO 催化剂的活性氧化物分布、比表面积以及结构形态发生变化。同时,这些催化剂的物理化学性质通过 XRD、BET、SEM、TEM、H-TPR 和 IR 进行了表征。更重要的是,还研究了催化氧化途径,其中 FeO-MnO-CeO 和 CuO-MnO-CeO 催化剂的过程是从氯苯到 CO、HO、HCl 和其他副产物。CuO-MnO-CeO 催化剂表现出较高的氯苯转化率,测量的起燃温度约为 400°C。然而,观察到大量的氯丙烷作为主要副产物。对于 FeO-MnO-CeO 催化剂,由于 FeO 的氧化能力和水吸收能力不同,发现更多的一氧化碳,但氧化不足。对两种催化剂的比较分析表明,氧化活性和机制的主要原因是 FeO 和 CuO 的氧化能力和水吸收能力不同。然而,所有这些催化剂在高反应温度下都不会因氯化物而失活,氯化物在废气中转化为 HCl。

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