Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 123, Issue 42, Pages 25657-25667Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.9b06745
Keywords
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Funding
- National Natural Science Foundation of China [21673268]
- Chinese Academy of Science
- Synfuels China Co., Ltd.
- state of Mecklenburg-Vorpommern
- Leibniz Foundation
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Experimentally, surface carbon hydrogenation on metallic iron forms CH4, ethylene/ethane, and propene/propane, while previous density functional theory studies showed that these reactions are highly endothermic. This disagreement can be attributed to the shortcoming of low coverage of surface carbon atoms and the underestimated role of surface hydrogen. On a p(4 x 4) Fe(110) surface with 0.25 ML carbon coverage (4 C atoms) and other free sites filled with H atoms, we studied surface C hydrogenation with spectators and found that the formation of CH4, ethylene/ethane, and propene/propane becomes exothermic. Coupling of CH + CH and CH3C + CH to acetylene and propylene is favored thermodynamically. Next, CHCH and CH3CCH can be hydrogenated into CH2CH and CH3CHCH, and the subsequent hydrogenation of CH2CH and CH3CHCH determines the formation and selectivity of alkenes and alkanes. The most important surface species is carbide HC for chain initiation or CH3C (RC for higher homolog) for chain propagation. This model of high coverage with spectators may help understand the mechanism of heterogeneous catalysis under real conditions.
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