期刊
CHEMCATCHEM
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202200577
关键词
DRIFTS; Fisher-Tropsch; Iron; Operando spectroscopy; Raman
资金
- Deutsche Forschungsgemeinschaft (DFG) [SPP 2080 (PN 406695057)]
- Projekt DEAL
Hematite can be used as a precursor for catalytically active iron (oxide) phases in CO2 Fischer-Tropsch synthesis. The transformation from alpha-Fe2O3 to Fe3O4 is faster than further reduction to Fe (metallic iron) in a hydrogen atmosphere, with the rate depending on temperature. Surface formate species are formed at elevated temperatures in a CO2/H2 gas mixture, while exposure to CO2 and CO leads to surface carbonate-carboxylate species. Reduced samples with varying Fe3O4 and Fe contents did not show observable adsorbates under reaction conditions. Carbonaceous species, indicating carbidation, were observed for a catalyst with medium reduction degree.
Hematite is a suitable precursor to obtain catalytically active iron (oxide) phases for CO2 Fischer-Tropsch synthesis after a reductive pretreatment. As concluded from in situ Raman spectroscopy, in hydrogen atmosphere the transformation from alpha-Fe2O3 to Fe3O4 is faster than the further reduction from Fe3O4 to Fe (metallic iron). The rate of these steps highly depends on the temperature. Starting from pure hematite, surface formate species are formed at a CO2/H-2 gas mixture at elevated temperatures, observable by DRIFT-spectroscopy. The exposure to CO2 and CO led to surface carbonate-carboxylate surface species. Reduced samples with varying contents of Fe3O4 and Fe did not show any observable adsorbates at reaction conditions. The same behavior was found during the dosage of the single gases CO2 and CO to these reduced catalysts. The formation of carbonaceous species, detected by Raman spectroscopy, could indirectly hint to the occurrence of carbidation and was especially observed for a good performing catalyst with a medium reduction degree.
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