Research output: Contribution to journal › Article › peer-review
Spatially resolved analysis of CO2 hydrogenation to higher hydrocarbons over alkali-metal promoted well-defined FexOyCz. / Skrypnik, Andrey S.; Petrov, Sergey A.; Kondratenko, Vita A. et al.
In: Journal of Catalysis, Vol. 425, 09.2023, p. 286-295.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Spatially resolved analysis of CO2 hydrogenation to higher hydrocarbons over alkali-metal promoted well-defined FexOyCz
AU - Skrypnik, Andrey S.
AU - Petrov, Sergey A.
AU - Kondratenko, Vita A.
AU - Yang, Qingxin
AU - Matvienko, Alexander A.
AU - Kondratenko, Evgenii V.
N1 - Financial support from Deutsche Forschungsgemeinschaft (KO 2261/10-1 and KO 2261/10-2) is gratefully acknowledged. A.S. acknowledges the financial support from DAAD.
PY - 2023/9
Y1 - 2023/9
N2 - A series of catalysts for CO2 hydrogenation to higher (C2+) hydrocarbons were prepared through controlled decomposition of iron (II) oxalate dihydrate impregnated with Li, Na, K, Rb or Cs carbonate. They consist of Fe3O4, Fe5C2, Fe3C and Fe. Their steady-state spatial phase distribution is, however, affected by the presence and the kind of the promoter. These structural characteristics determine catalyst activity and product selectivity. Fe3C seems to favor CH4 formation, while C2+-hydrocarbons are formed over Fe5C2. A positive relationship between the rate of C2+-hydrocarbons formation and the rate constant of dissociation of adsorbed CO2 was established, while an opposite dependence is valid for the rate of CO2 methanation. The rate constant of this reaction increases in the presence of alkali metal and with an increase in its atomic number. Therefore, CH4 is mainly formed over Rb- or Cs-doped catalysts through CO hydrogenation, while CO2 methanation prevails over the remaining catalysts.
AB - A series of catalysts for CO2 hydrogenation to higher (C2+) hydrocarbons were prepared through controlled decomposition of iron (II) oxalate dihydrate impregnated with Li, Na, K, Rb or Cs carbonate. They consist of Fe3O4, Fe5C2, Fe3C and Fe. Their steady-state spatial phase distribution is, however, affected by the presence and the kind of the promoter. These structural characteristics determine catalyst activity and product selectivity. Fe3C seems to favor CH4 formation, while C2+-hydrocarbons are formed over Fe5C2. A positive relationship between the rate of C2+-hydrocarbons formation and the rate constant of dissociation of adsorbed CO2 was established, while an opposite dependence is valid for the rate of CO2 methanation. The rate constant of this reaction increases in the presence of alkali metal and with an increase in its atomic number. Therefore, CH4 is mainly formed over Rb- or Cs-doped catalysts through CO hydrogenation, while CO2 methanation prevails over the remaining catalysts.
KW - Alkali metals
KW - CO2 hydrogenation
KW - Ferrous oxalate
KW - Fischer-Tropsch
KW - Iron oxides
KW - Kinetics
KW - Mechanism
UR - https://www.scopus.com/record/display.uri?eid=2-s2.0-85162899960&origin=inward&txGid=2973a2f2f64bfac05f7a1c7e643801b0
UR - https://www.mendeley.com/catalogue/4246ad99-0561-3a2a-99a3-102a2562e756/
U2 - 10.1016/j.jcat.2023.06.019
DO - 10.1016/j.jcat.2023.06.019
M3 - Article
VL - 425
SP - 286
EP - 295
JO - Journal of Catalysis
JF - Journal of Catalysis
SN - 0021-9517
ER -
ID: 59264919