Understanding reaction-induced restructuring of well-defined FexOyCz compositions and its effect on CO2 hydrogenation

Andrey S. Skrypnik; Qingxin Yang; Alexander A. Matvienko; Victor Yu Bychkov; Yuriy P. Tulenin; Henrik Lund; Sergey A. Petrov; Ralph Kraehnert; Aleks Arinchtein; Jana Weiss; Angelika Brueckner; Evgenii V. Kondratenko

doi:10.1016/j.apcatb.2021.120121

Understanding reaction-induced restructuring of well-defined Fe_xO_yC_z compositions and its effect on CO₂ hydrogenation

Andrey S. Skrypnik, Qingxin Yang, Alexander A. Matvienko, Victor Yu Bychkov, Yuriy P. Tulenin, Henrik Lund, Sergey A. Petrov, Ralph Kraehnert, Aleks Arinchtein, Jana Weiss, Angelika Brueckner, Evgenii V. Kondratenko

Результат исследования: Научные публикации в периодических изданиях › статья › рецензирование

1 Цитирования (Scopus)

Аннотация

Herein, we provide fundamentals relevant for the development of Fe-based catalysts for CO₂hydrogenation to higher hydrocarbons. It was possible owing to preparation of well-defined Fe_xO_yC_z compositions through controlled decomposition of iron oxalate, determination of their composition under CO₂-FT reaction and catalytic tests in a broad range of CO₂ conversion. Such steady-state composition changes along the catalyst bed. The changes and their strength depend on the initial phase composition. In addition to the reaction-induced catalyst restructuring, reaction pathways leading from CO₂ to CO, CH₄ and higher hydrocarbons were elucidated. A correlation between them and the steady-state composition was established and offers the possibility for tailored catalyst design and preparation. Our best performing promoter-free Fe-based catalyst shows the selectivity to CH₄ below 10 %, while the selectivity to C₂₊-hydrocarbons is about 50 % at CO₂ conversion of about 25 % and 300 °C. The olefin to paraffin ratio among C₂-C₄ hydrocarbons is 5.5.

Язык оригинала	английский
Номер статьи	120121
Журнал	Applied Catalysis B: Environmental
Том	291
DOI	https://doi.org/10.1016/j.apcatb.2021.120121
Состояние	Опубликовано - 15 авг. 2021

Предметные области OECD FOS+WOS

2.04 ХИМИЧЕСКИЕ ТЕХНОЛОГИИ
1.05 НАУКИ О ЗЕМЛЕ И СМЕЖНЫЕ ЭКОЛОГИЧЕСКИЕ НАУКИ

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10.1016/j.apcatb.2021.120121

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Skrypnik, A. S., Yang, Q., Matvienko, A. A., Bychkov, V. Y., Tulenin, Y. P., Lund, H., Petrov, S. A., Kraehnert, R., Arinchtein, A., Weiss, J., Brueckner, A., & Kondratenko, E. V. (2021). Understanding reaction-induced restructuring of well-defined Fe_xO_yC_z compositions and its effect on CO₂ hydrogenation. Applied Catalysis B: Environmental, 291, [120121]. https://doi.org/10.1016/j.apcatb.2021.120121

@article{f250cf93819c4388bd80c8df36136203,

title = "Understanding reaction-induced restructuring of well-defined FexOyCz compositions and its effect on CO2 hydrogenation",

abstract = "Herein, we provide fundamentals relevant for the development of Fe-based catalysts for CO2hydrogenation to higher hydrocarbons. It was possible owing to preparation of well-defined FexOyCz compositions through controlled decomposition of iron oxalate, determination of their composition under CO2-FT reaction and catalytic tests in a broad range of CO2 conversion. Such steady-state composition changes along the catalyst bed. The changes and their strength depend on the initial phase composition. In addition to the reaction-induced catalyst restructuring, reaction pathways leading from CO2 to CO, CH4 and higher hydrocarbons were elucidated. A correlation between them and the steady-state composition was established and offers the possibility for tailored catalyst design and preparation. Our best performing promoter-free Fe-based catalyst shows the selectivity to CH4 below 10 %, while the selectivity to C2+-hydrocarbons is about 50 % at CO2 conversion of about 25 % and 300 °C. The olefin to paraffin ratio among C2-C4 hydrocarbons is 5.5.",

keywords = "CO hydrogenation, Fischer-Tropsch, Iron oxalate decomposition, Iron oxide, Magnetite",

author = "Skrypnik, {Andrey S.} and Qingxin Yang and Matvienko, {Alexander A.} and Bychkov, {Victor Yu} and Tulenin, {Yuriy P.} and Henrik Lund and Petrov, {Sergey A.} and Ralph Kraehnert and Aleks Arinchtein and Jana Weiss and Angelika Brueckner and Kondratenko, {Evgenii V.}",

note = "Funding Information: Financial support from Deutsche Forschungsgemeinschaft ( KO 2261/10-1 ) and Leibniz-Gemeinschaft e.V. ( SAW-2017-LIKAT-1 ) is gratefully acknowledged. A.S. acknowledges the financial support from DAAD. Publisher Copyright: {\textcopyright} 2021 Elsevier B.V. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.",

year = "2021",

month = aug,

day = "15",

doi = "10.1016/j.apcatb.2021.120121",

language = "English",

volume = "291",

journal = "Applied Catalysis B: Environmental",

issn = "0926-3373",

publisher = "Elsevier",

}

Skrypnik, AS, Yang, Q, Matvienko, AA, Bychkov, VY, Tulenin, YP, Lund, H, Petrov, SA, Kraehnert, R, Arinchtein, A, Weiss, J, Brueckner, A & Kondratenko, EV 2021, 'Understanding reaction-induced restructuring of well-defined Fe_xO_yC_z compositions and its effect on CO₂ hydrogenation', Applied Catalysis B: Environmental, том. 291, 120121. https://doi.org/10.1016/j.apcatb.2021.120121

Understanding reaction-induced restructuring of well-defined Fe_xO_yC_z compositions and its effect on CO₂ hydrogenation. / Skrypnik, Andrey S.; Yang, Qingxin; Matvienko, Alexander A. и др.

В: Applied Catalysis B: Environmental, Том 291, 120121, 15.08.2021.

Результат исследования: Научные публикации в периодических изданиях › статья › рецензирование

TY - JOUR

T1 - Understanding reaction-induced restructuring of well-defined FexOyCz compositions and its effect on CO2 hydrogenation

AU - Skrypnik, Andrey S.

AU - Yang, Qingxin

AU - Matvienko, Alexander A.

AU - Bychkov, Victor Yu

AU - Tulenin, Yuriy P.

AU - Lund, Henrik

AU - Petrov, Sergey A.

AU - Kraehnert, Ralph

AU - Arinchtein, Aleks

AU - Weiss, Jana

AU - Brueckner, Angelika

AU - Kondratenko, Evgenii V.

N1 - Funding Information: Financial support from Deutsche Forschungsgemeinschaft ( KO 2261/10-1 ) and Leibniz-Gemeinschaft e.V. ( SAW-2017-LIKAT-1 ) is gratefully acknowledged. A.S. acknowledges the financial support from DAAD. Publisher Copyright: © 2021 Elsevier B.V. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

PY - 2021/8/15

Y1 - 2021/8/15

N2 - Herein, we provide fundamentals relevant for the development of Fe-based catalysts for CO2hydrogenation to higher hydrocarbons. It was possible owing to preparation of well-defined FexOyCz compositions through controlled decomposition of iron oxalate, determination of their composition under CO2-FT reaction and catalytic tests in a broad range of CO2 conversion. Such steady-state composition changes along the catalyst bed. The changes and their strength depend on the initial phase composition. In addition to the reaction-induced catalyst restructuring, reaction pathways leading from CO2 to CO, CH4 and higher hydrocarbons were elucidated. A correlation between them and the steady-state composition was established and offers the possibility for tailored catalyst design and preparation. Our best performing promoter-free Fe-based catalyst shows the selectivity to CH4 below 10 %, while the selectivity to C2+-hydrocarbons is about 50 % at CO2 conversion of about 25 % and 300 °C. The olefin to paraffin ratio among C2-C4 hydrocarbons is 5.5.

AB - Herein, we provide fundamentals relevant for the development of Fe-based catalysts for CO2hydrogenation to higher hydrocarbons. It was possible owing to preparation of well-defined FexOyCz compositions through controlled decomposition of iron oxalate, determination of their composition under CO2-FT reaction and catalytic tests in a broad range of CO2 conversion. Such steady-state composition changes along the catalyst bed. The changes and their strength depend on the initial phase composition. In addition to the reaction-induced catalyst restructuring, reaction pathways leading from CO2 to CO, CH4 and higher hydrocarbons were elucidated. A correlation between them and the steady-state composition was established and offers the possibility for tailored catalyst design and preparation. Our best performing promoter-free Fe-based catalyst shows the selectivity to CH4 below 10 %, while the selectivity to C2+-hydrocarbons is about 50 % at CO2 conversion of about 25 % and 300 °C. The olefin to paraffin ratio among C2-C4 hydrocarbons is 5.5.

KW - CO hydrogenation

KW - Fischer-Tropsch

KW - Iron oxalate decomposition

KW - Iron oxide

KW - Magnetite

UR - http://www.scopus.com/inward/record.url?scp=85102551730&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2021.120121

DO - 10.1016/j.apcatb.2021.120121

M3 - Article

AN - SCOPUS:85102551730

VL - 291

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

SN - 0926-3373

M1 - 120121

ER -