Journal
JOURNAL OF CATALYSIS
Volume 411, Issue -, Pages 97-108Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2022.05.006
Keywords
Cobalt; Fischer-Tropsch; High conversion; Manganese promoter; Water; Surface oxygen
Categories
Funding
- DSI-NRF centre of excellence in catalysis, c*change
- NRF [UID: 114606, 94878]
- Sasol Ltd
- LOreal for Women in Science
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The addition of manganese to cobalt-based Fischer-Tropsch catalysts improves their activity and liquid fuel yield by reducing CO2 and CH4 selectivity. DFT calculations suggest that the promotion of manganese is associated with improved oxygen removal from the catalytically active surface, leading to reduced selectivity towards CO2 and increased liquid fuel yield.
The addition of manganese to cobalt-based Fischer-Tropsch catalysts increases activity and significantly improves liquid fuel yield by decreasing CO2 and CH4 selectivity. These effects are particularly noticeable at high CO conversions where the catalyst is exposed to high H2O, and low CO and H2, partial pressures. Under these conditions, manganese-promotion causes a shift in the maximum liquid fuel yield from 61 C% to 79 C-% (at CO-conversion levels of 78% and 91%, respectively), thus enabling once-through operation. Our CO-TPD and DFT studies show that manganese promotion cannot to be linked to enhanced CO adsorption nor promotion of the C-O bond cleavage (both typically postulated mechanisms). Rather, our DFT-calculations indicate that manganese promotion modelled as a manganese oxide cluster on Co (1 1 1) is associated with improved oxygen removal from the catalytically active surface, explaining the reduced selectivity towards CO2 at high conversion and, thus, reduced methane selectivity and improved liquid fuel yield.(c) 2022 The Authors. Published by Elsevier Inc. This is an open access article under the CC BY license (http:// creativecommons.org/licenses/by/4.0/).
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