Research output: Contribution to journal › Article › peer-review
Activity and selectivity descriptors for iron carbides in CO2 hydrogenation. / Yang, Qingxin; Fedorova, Elizaveta A.; Petrov, Sergey A. et al.
In: Applied Catalysis B: Environmental, Vol. 327, 122450, 15.06.2023.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Activity and selectivity descriptors for iron carbides in CO2 hydrogenation
AU - Yang, Qingxin
AU - Fedorova, Elizaveta A.
AU - Petrov, Sergey A.
AU - Weiss, Jana
AU - Lund, Henrik
AU - Skrypnik, Andrey S.
AU - Kreyenschulte, Carsten Robert
AU - Bychkov, Victor Yu
AU - Matvienko, Alexander A.
AU - Brueckner, Angelika
AU - Kondratenko, Evgenii V.
N1 - Acknowledgement: This work was funded by the Deutsche Forschungsgemeinschaft within the priority program SPP 2080 “Catalysts and reactors under dynamic conditions for energy storage and conversion” (KO 2261/10-1, KO 2261/10-2). Financial support from the Leibniz-Gemeinschaft e.V. (SAW-2017-LIKAT-1) is also acknowledged. Q.Y. thanks Dr. Martin Fait (LIKAT), Dr. Uwe Rodemerck (LIKAT), and Dr. David Linke (LIKAT) for their help in reaction tests. The authors thank Reinhard Eckelt (LIKAT) and Dr. Stephan Bartling (LIKAT) for N2 adsorption-desorption experiments and X-ray photoelectron spectroscopy measurements, respectively. We acknowledge beamline P65 at PETRA III of DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, and CAT-ACT beamline of KIT synchrotron facility, ANKA, for providing the experimental facilities. We would like to thank Dr. Dmitry E. Doronkin (KIT), Dr. Erisa Saraçi (KIT), Dr. Morgane Desmau (DESY), and Dr. Edmund Welter (DESY) for their assistance in using beamline P65 and CAT-ACT.
PY - 2023/6/15
Y1 - 2023/6/15
N2 - CO2 conversion into value-added products provides an attractive way to close carbon cycles and to minimize the dependence on oil-based feedstock. To understand how product distribution in CO2 hydrogenation can be controlled, as required for purposeful catalyst design, we prepared single-phase α-Fe2O3 materials differing in their reducibility due to the different size of crystallites and the presence of planar defects in the iron sublattice. Their structural evolution during reduction and under CO2 hydrogenation conditions as well as their catalytic and adsorptive properties towards CO, CO2, and H2 were elucidated through combining kinetic (spatially resolved), physicochemical and chemisorption analyses. The obtained results suggest that the reducibility of α-Fe2O3 is a key factor affecting in situ transformation of this oxide into Fe5C2 with planar defects, which seem to determine the generation of surface intermediates from CO, CO2, and H2, and accordingly CO2 hydrogenation to CO exclusively or also CO hydrogenation to hydrocarbons.
AB - CO2 conversion into value-added products provides an attractive way to close carbon cycles and to minimize the dependence on oil-based feedstock. To understand how product distribution in CO2 hydrogenation can be controlled, as required for purposeful catalyst design, we prepared single-phase α-Fe2O3 materials differing in their reducibility due to the different size of crystallites and the presence of planar defects in the iron sublattice. Their structural evolution during reduction and under CO2 hydrogenation conditions as well as their catalytic and adsorptive properties towards CO, CO2, and H2 were elucidated through combining kinetic (spatially resolved), physicochemical and chemisorption analyses. The obtained results suggest that the reducibility of α-Fe2O3 is a key factor affecting in situ transformation of this oxide into Fe5C2 with planar defects, which seem to determine the generation of surface intermediates from CO, CO2, and H2, and accordingly CO2 hydrogenation to CO exclusively or also CO hydrogenation to hydrocarbons.
KW - CO2 hydrogenation
KW - Fe-based catalyst
KW - Iron carbides
KW - Product selectivity
KW - Reducibility
UR - https://www.scopus.com/inward/record.url?eid=2-s2.0-85147952401&partnerID=40&md5=c96b396107d344d339a6003901112967
UR - https://www.mendeley.com/catalogue/1fc39275-b0c6-3bd8-80db-d3fef8a18ee1/
U2 - 10.1016/j.apcatb.2023.122450
DO - 10.1016/j.apcatb.2023.122450
M3 - Article
VL - 327
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
SN - 0926-3373
M1 - 122450
ER -
ID: 48884886