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Catalytic oxidation of 1,2-dichloroethane over three-dimensional ordered meso-macroporous Co 3 O 4 /La 0.7 Sr 0.3 Fe 0.5 Co 0.5 O 3 : destruction route and mechanism

Tian, Mingjiao, He, Chi, Yu, Yanke, Pan, Hua, Smith, Louise, Jiang, Zeyu, Gao, Ningbo, Jian, Yanfei, Hao, Zhengping and Zhu, Qing 2018. Catalytic oxidation of 1,2-dichloroethane over three-dimensional ordered meso-macroporous Co 3 O 4 /La 0.7 Sr 0.3 Fe 0.5 Co 0.5 O 3 : destruction route and mechanism. Applied Catalysis A: General 553 (5) , pp. 1-14. 10.1016/j.apcata.2018.01.013

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Abstract

Three-dimensional ordered meso-macroporous La0.7Sr0.3Fe0.5Co0.5O3 (3DOM LSFCO)-supported Co3O4 catalysts were designed and prepared via a PMMA-templating strategy for the total oxidation of 1,2-dichloroethane (1,2-DCE). The physicochemical properties of all synthesized samples were characterized by XRD, FE-SEM, TEM, HAADF-STEM, low-temperature N2 sorption, XPS, H2-TPR, and in situ FT-IR. The introduction of Co3O4 increases the generation rate of oxygen vacancy, playing a crucial role in adsorption and activation of oxygen species. The special 3DOM structure of perovskite-type oxide promotes 1,2-DCE molecules to effectively and intimately contact with the surface adsorbed oxygen over supported catalysts and further accelerates the redox process. Compared with pure LSFCO, all the Co3O4 supported catalysts show superior catalytic performance with reaction rate increases from 5.53 × 10−12 to 2.29 × 10−11 mol g−1 s−1 and Ea decreases from 74.7 to 22.6 KJ mol−1. Amongst, the 10Co3O4/3DOM LSFCO catalyst exhibits the best catalytic activity, highest resistance to chlorine poisoning and lowest by-products concentration because of the largest amount of surface adsorbed oxygen. CO2, CO, HCl, and Cl2 are the main oxidation productions, while some typical reaction intermediates such as vinyl chloride, 1,1,2-trichloroethane and trichloroethylene are also observed, especially over the 3DOM LSFCO sample. Furthermore, the reaction mechanism of 1,2-DCE oxidation over obtained catalysts was proposed based on the results of gas chromatography, in situ FT-IR, and on-line MS. It is believed that the Co3O4/3DOM LSFCO are promising catalysts for the total removal of chlorinated volatile organic compounds.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Publisher: Elsevier
ISSN: 0926-860X
Date of First Compliant Deposit: 22 February 2018
Date of Acceptance: 13 January 2018
Last Modified: 12 Jun 2019 03:07
URI: http://orca.cf.ac.uk/id/eprint/109382

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