Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel

Zuzana Vajglova; Paivi Maki-Arvela; Olha Yevdokimova; Mark Martinez-Klimov; Irina Simakova; Kari Eranen; Teija Tirri; Jessi E. S. van Hoeven; Anssi Peuronen; Matej Hus; Blaz Likozar; Mika Lastusaari; Johan Linden; Dmitry E. Doronkin; Dmitry Yu. Murzin

doi:10.1016/j.apcata.2025.120307

Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel

Zuzana Vajglova
, Paivi Maki-Arvela
, Olha Yevdokimova
, Mark Martinez-Klimov
, Irina Simakova
, Kari Eranen
, Teija Tirri
, Jessi E. S. van Hoeven
, Anssi Peuronen
, Matej Hus
, Blaz Likozar
, Mika Lastusaari
, Johan Linden
, Dmitry E. Doronkin
, Dmitry Yu. Murzin

Forskningsoutput: Tidskriftsbidrag › Artikel › Vetenskaplig › Peer review

3 Citeringar (Scopus)

10 Nedladdningar (Pure)

Sammanfattning

Solventless hydrodeoxygenation of dihydroeugenol was investigated in a continuous reactor at 300 °C under 30 bar over different nickel-iron catalysts, prepared using a two-step impregnation method. The following catalysts were studied: mesoporous FeNi/Al ₂O ₃, FeNi/SiO ₂ and FeNi/H-MCM-48 as well as microporous FeNi/H-Beta-300, FeNi/H-Beta-38, FeNi/H-Y-5.1, FeNi/H-MCM-48 and FeNi/USY-30. The catalysts were characterized by SEM coupled with energy dispersive X-ray analysis, Mössbauer and X-ray absorption spectroscopy, hydrogen TPR, X-ray diffraction, TEM, nitrogen physisorption and FTIR pyridine adsorption. DFT calculations were performed to elucidate the role of Fe and Ni. The results revealed that FeNi/Al ₂O ₃ was the most active and stable in dihydroeugenol hydrodeoxygenation. Complete conversion of dihydroeugenol was obtained and the yield of the main product propylcyclohexane was varying in the range 84–88 %. FeNi/Al ₂O ₃ catalyst exhibited 3.4 nm metal particles and contained FeNi alloy particles with the fcc metallic structure. No deactivation was observed for FeNi/ Al ₂O ₃ during 5 hours time-on-stream due to the presence of Ni-rich particles with iron-enriched outer surface confirmed by EXAFS. Fe was shown to be responsible for deoxygenation, while Ni promotes hydrogenation. Catalyst deactivation was observed for all other catalysts except for FeNi/Al ₂O ₃ with increasing time-on-stream under the same reaction conditions due to their higher Brønsted to Lewis acid site ratio and larger average metal particle size in comparison to FeNi/Al ₂O ₃.

Originalspråk	Engelska
Artikelnummer	120307
Antal sidor	20
Tidskrift	Applied Catalysis A: General
Volym	701
DOI	https://doi.org/10.1016/j.apcata.2025.120307
Status	Publicerad - 5 juli 2025
MoE-publikationstyp	A1 Tidskriftsartikel-refererad

Finansiering

The authors acknowledge Business Finland for funding through the project: Catalytic Slurry Hydrotreatment . Electron microscopy samples were processed and analyzed at the Electron Microscopy Laboratory, Institute of Biomedicine, University of Turku , which received financial support from Biocenter Finland. We acknowledge DESY (Hamburg, Germany ), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at the light source PETRA III at DESY, a member of the Helmholtz Association (HGF ). We would like to thank Dr. Edmund Welter for his assistance in using the beamline P65, which was allocated for proposal I-20220246. Computational resources were provided by the Institute of Information Science, Maribor, Slovenia through the HPC RIVR consortium and EuroHPC JU. Financial support from the Slovenian Research and Innovation Agency (ARIS) through core funding P2–0152, project funding N2–0316, J1–3020 and infrastructure funding I0–0039 is greatly appreciated.

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10.1016/j.apcata.2025.120307Licens: CC BY

1-s2.0-S0926860X2500208X-mainSlutlig publicerad version, 11,3 MBLicens: CC BY

https://urn.fi/URN:NBN:fi-fe20251210116746

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Vajglova, Z., Maki-Arvela, P., Yevdokimova, O., Martinez-Klimov, M., Simakova, I., Eranen, K., Tirri, T., van Hoeven, J. E. S., Peuronen, A., Hus, M., Likozar, B., Lastusaari, M., Linden, J., Doronkin, D. E., & Murzin, D. Y. (2025). Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel. Applied Catalysis A: General, 701, Artikel 120307. https://doi.org/10.1016/j.apcata.2025.120307

@article{73a49a968cef4fbebdcf18f12f9f31ca,

title = "Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel",

abstract = "Solventless hydrodeoxygenation of dihydroeugenol was investigated in a continuous reactor at 300 °C under 30 bar over different nickel-iron catalysts, prepared using a two-step impregnation method. The following catalysts were studied: mesoporous FeNi/Al 2O 3, FeNi/SiO 2 and FeNi/H-MCM-48 as well as microporous FeNi/H-Beta-300, FeNi/H-Beta-38, FeNi/H-Y-5.1, FeNi/H-MCM-48 and FeNi/USY-30. The catalysts were characterized by SEM coupled with energy dispersive X-ray analysis, M{\"o}ssbauer and X-ray absorption spectroscopy, hydrogen TPR, X-ray diffraction, TEM, nitrogen physisorption and FTIR pyridine adsorption. DFT calculations were performed to elucidate the role of Fe and Ni. The results revealed that FeNi/Al 2O 3 was the most active and stable in dihydroeugenol hydrodeoxygenation. Complete conversion of dihydroeugenol was obtained and the yield of the main product propylcyclohexane was varying in the range 84–88 \%. FeNi/Al 2O 3 catalyst exhibited 3.4 nm metal particles and contained FeNi alloy particles with the fcc metallic structure. No deactivation was observed for FeNi/ Al 2O 3 during 5 hours time-on-stream due to the presence of Ni-rich particles with iron-enriched outer surface confirmed by EXAFS. Fe was shown to be responsible for deoxygenation, while Ni promotes hydrogenation. Catalyst deactivation was observed for all other catalysts except for FeNi/Al 2O 3 with increasing time-on-stream under the same reaction conditions due to their higher Br{\o}nsted to Lewis acid site ratio and larger average metal particle size in comparison to FeNi/Al 2O 3.",

keywords = "Dihydroeugenol, Fe-Ni catalysts, Hydrodeoxygenation",

author = "Zuzana Vajglova and Paivi Maki-Arvela and Olha Yevdokimova and Mark Martinez-Klimov and Irina Simakova and Kari Eranen and Teija Tirri and \{van Hoeven\}, \{Jessi E. S.\} and Anssi Peuronen and Matej Hus and Blaz Likozar and Mika Lastusaari and Johan Linden and Doronkin, \{Dmitry E.\} and Murzin, \{Dmitry Yu.\}",

year = "2025",

month = jul,

day = "5",

doi = "10.1016/j.apcata.2025.120307",

language = "English",

volume = "701",

journal = "Applied Catalysis A: General",

issn = "0926-860X",

publisher = "Elsevier",

}

Vajglova, Z, Maki-Arvela, P , Yevdokimova, O , Martinez-Klimov, M, Simakova, I, Eranen, K , Tirri, T, van Hoeven, JES, Peuronen, A, Hus, M, Likozar, B, Lastusaari, M, Linden, J, Doronkin, DE & Murzin, DY 2025, 'Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel', Applied Catalysis A: General, vol. 701, 120307. https://doi.org/10.1016/j.apcata.2025.120307

TY - JOUR

T1 - Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel

AU - Vajglova, Zuzana

AU - Maki-Arvela, Paivi

AU - Yevdokimova, Olha

AU - Martinez-Klimov, Mark

AU - Simakova, Irina

AU - Eranen, Kari

AU - Tirri, Teija

AU - van Hoeven, Jessi E. S.

AU - Peuronen, Anssi

AU - Hus, Matej

AU - Likozar, Blaz

AU - Lastusaari, Mika

AU - Linden, Johan

AU - Doronkin, Dmitry E.

AU - Murzin, Dmitry Yu.

PY - 2025/7/5

Y1 - 2025/7/5

N2 - Solventless hydrodeoxygenation of dihydroeugenol was investigated in a continuous reactor at 300 °C under 30 bar over different nickel-iron catalysts, prepared using a two-step impregnation method. The following catalysts were studied: mesoporous FeNi/Al 2O 3, FeNi/SiO 2 and FeNi/H-MCM-48 as well as microporous FeNi/H-Beta-300, FeNi/H-Beta-38, FeNi/H-Y-5.1, FeNi/H-MCM-48 and FeNi/USY-30. The catalysts were characterized by SEM coupled with energy dispersive X-ray analysis, Mössbauer and X-ray absorption spectroscopy, hydrogen TPR, X-ray diffraction, TEM, nitrogen physisorption and FTIR pyridine adsorption. DFT calculations were performed to elucidate the role of Fe and Ni. The results revealed that FeNi/Al 2O 3 was the most active and stable in dihydroeugenol hydrodeoxygenation. Complete conversion of dihydroeugenol was obtained and the yield of the main product propylcyclohexane was varying in the range 84–88 %. FeNi/Al 2O 3 catalyst exhibited 3.4 nm metal particles and contained FeNi alloy particles with the fcc metallic structure. No deactivation was observed for FeNi/ Al 2O 3 during 5 hours time-on-stream due to the presence of Ni-rich particles with iron-enriched outer surface confirmed by EXAFS. Fe was shown to be responsible for deoxygenation, while Ni promotes hydrogenation. Catalyst deactivation was observed for all other catalysts except for FeNi/Al 2O 3 with increasing time-on-stream under the same reaction conditions due to their higher Brønsted to Lewis acid site ratio and larger average metal particle size in comparison to FeNi/Al 2O 3.

AB - Solventless hydrodeoxygenation of dihydroeugenol was investigated in a continuous reactor at 300 °C under 30 bar over different nickel-iron catalysts, prepared using a two-step impregnation method. The following catalysts were studied: mesoporous FeNi/Al 2O 3, FeNi/SiO 2 and FeNi/H-MCM-48 as well as microporous FeNi/H-Beta-300, FeNi/H-Beta-38, FeNi/H-Y-5.1, FeNi/H-MCM-48 and FeNi/USY-30. The catalysts were characterized by SEM coupled with energy dispersive X-ray analysis, Mössbauer and X-ray absorption spectroscopy, hydrogen TPR, X-ray diffraction, TEM, nitrogen physisorption and FTIR pyridine adsorption. DFT calculations were performed to elucidate the role of Fe and Ni. The results revealed that FeNi/Al 2O 3 was the most active and stable in dihydroeugenol hydrodeoxygenation. Complete conversion of dihydroeugenol was obtained and the yield of the main product propylcyclohexane was varying in the range 84–88 %. FeNi/Al 2O 3 catalyst exhibited 3.4 nm metal particles and contained FeNi alloy particles with the fcc metallic structure. No deactivation was observed for FeNi/ Al 2O 3 during 5 hours time-on-stream due to the presence of Ni-rich particles with iron-enriched outer surface confirmed by EXAFS. Fe was shown to be responsible for deoxygenation, while Ni promotes hydrogenation. Catalyst deactivation was observed for all other catalysts except for FeNi/Al 2O 3 with increasing time-on-stream under the same reaction conditions due to their higher Brønsted to Lewis acid site ratio and larger average metal particle size in comparison to FeNi/Al 2O 3.

KW - Dihydroeugenol

KW - Fe-Ni catalysts

KW - Hydrodeoxygenation

UR - https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=aboakademi&SrcAuth=WosAPI&KeyUT=WOS:001483593000001&DestLinkType=FullRecord&DestApp=WOS_CPL

U2 - 10.1016/j.apcata.2025.120307

DO - 10.1016/j.apcata.2025.120307

M3 - Article

SN - 0926-860X

VL - 701

JO - Applied Catalysis A: General

JF - Applied Catalysis A: General

M1 - 120307

ER -

Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel

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