Research output: Contribution to journal › Article › peer-review
Identifying Performance Descriptors in CO2 Hydrogenation over Iron-Based Catalysts Promoted with Alkali Metals. / Yang, Qingxin; Kondratenko, Vita A.; Petrov, Sergey A. et al.
In: Angewandte Chemie - International Edition, Vol. 61, No. 22, e202116517, 23.05.2022.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Identifying Performance Descriptors in CO2 Hydrogenation over Iron-Based Catalysts Promoted with Alkali Metals
AU - Yang, Qingxin
AU - Kondratenko, Vita A.
AU - Petrov, Sergey A.
AU - Doronkin, Dmitry E.
AU - Saraçi, Erisa
AU - Lund, Henrik
AU - Arinchtein, Aleks
AU - Kraehnert, Ralph
AU - Skrypnik, Andrey S.
AU - Matvienko, Alexander A.
AU - Kondratenko, Evgenii V.
N1 - Funding Information: This work was funded by the Deutsche Forschungsgemeinschaft (DFG) under the priority program SPP 2080 (grants no. KO 2261/10‐1, KO 2261/10‐2). Financial support from the Leibniz‐Gemeinschaft e. V. is also acknowledged (SAW‐2017‐LIKAT‐1). The authors thank Dr. Stephan Bartling for X‐ray photoelectron spectroscopic analyses. The authors acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for providing the experimental facilities. Parts of this research were carried out at PETRA III and we would like to thank Dr. Morgane Desmau and Dr. Edmund Welter for their assistance in using beamline P65. The authors gratefully acknowledge the efforts of Frau Laura Kraußer for translating the English original manuscript into German. Open Access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
PY - 2022/5/23
Y1 - 2022/5/23
N2 - Alkali metal promoters have been widely employed for preparation of heterogeneous catalysts used in many industrially important reactions. However, the fundamentals of their effects are usually difficult to access. Herein, we unravel mechanistic and kinetic aspects of the role of alkali metals in CO2 hydrogenation over Fe-based catalysts through state-of-the-art characterization techniques, spatially resolved steady-state and transient kinetic analyses. The promoters affect electronic properties of iron in iron carbides. These carbide characteristics determine catalyst ability to activate H2, CO and CO2. The Allen scale electronegativity of alkali metal promoter was successfully correlated with the rates of CO2 hydrogenation to higher hydrocarbons and CH4 as well as with the rate constants of individual steps of CO or CO2 activation. The derived knowledge can be valuable for designing and preparing catalysts applied in other reactions where such promoters are also used.
AB - Alkali metal promoters have been widely employed for preparation of heterogeneous catalysts used in many industrially important reactions. However, the fundamentals of their effects are usually difficult to access. Herein, we unravel mechanistic and kinetic aspects of the role of alkali metals in CO2 hydrogenation over Fe-based catalysts through state-of-the-art characterization techniques, spatially resolved steady-state and transient kinetic analyses. The promoters affect electronic properties of iron in iron carbides. These carbide characteristics determine catalyst ability to activate H2, CO and CO2. The Allen scale electronegativity of alkali metal promoter was successfully correlated with the rates of CO2 hydrogenation to higher hydrocarbons and CH4 as well as with the rate constants of individual steps of CO or CO2 activation. The derived knowledge can be valuable for designing and preparing catalysts applied in other reactions where such promoters are also used.
KW - CO Utilization
KW - Heterogeneous Catalysis
KW - Hydrogenation
KW - Iron
KW - Kinetics
UR - http://www.scopus.com/inward/record.url?scp=85127435385&partnerID=8YFLogxK
U2 - 10.1002/anie.202116517
DO - 10.1002/anie.202116517
M3 - Article
C2 - 35244964
AN - SCOPUS:85127435385
VL - 61
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
IS - 22
M1 - e202116517
ER -
ID: 35841210