期刊
JOURNAL OF CATALYSIS
卷 388, 期 -, 页码 52-65出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2020.05.004
关键词
Ethylene production; Oxidative dehydrogenation; Ethane; CO2 utilization; FeOx-based catalysts; Carbon deposition
资金
- Hellenic Foundation Research & Innovation (II-CUDET project) [HFRI-FM17-1899]
Ethylene is a very important raw material for chemical industry, which can be produced from the underutilized ethane, originating from shale gas, through the oxidative ethane dehydrogenation (EDH) using CO2 as a mild oxidant. Two 5 wt%Fe-based catalysts, supported on mixed MgO-ZrO2 and NiO-MgO-ZrO2 oxides, prepared by auto-combustion sol-gel method, were investigated for CO2-EDH. The crystallographic structure of the catalysts was examined by X-ray diffraction (XRD), while the surface composition and oxidation state were identified using X-ray photoelectron spectroscopy (XPS). The effect of catalyst pre-treatment, reduction by H-2, on catalytic activity, selectivity and carbon-resistance was evaluated for the studied samples. Both catalysts provided high ethylene selectivity and activity during CO2-oxidative dehydrogenation of C2H6 at 873 K, atmospheric pressure and equimolar CO2/C2H6 ratio. The addition of NiO in the support material had a promoting effect, since it resulted in a catalyst with a twofold higher activity. Similarly, the selectivity towards C2H4 remained at high levels, above 70%, slightly increased, as it was exemplified during an iso-conversion experiment. The best candidate lost 25% of its initial activity during the first 3 h of a stability test, while it remained unchanged from 3 to 17 h. Deposited carbon was negligible, whereas sintering was identified as the main deactivation reason. Systematic XPS analysis revealed that deposition of Fe on NiO-MgO-ZrO2 support significantly affected the local environment of Ni, contributing to the enhanced catalytic performance. Increased Fe2+ concentration was found for the used Fe-catalyst supported on NiO-MgO-ZrO2, compared to the as-prepared, implying partial reduction of Fe during CO2-EDH reaction, as it was also observed by HRTEM. (C) 2020 Elsevier Inc. All rights reserved.
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