Hydrodeoxygenation and hydrodenitrogenation of n-hexadecanamide over Pt catalysts : effect of the support

Emma Verkama; Sylvia Albersberger; Aitor Arandia; Kristoffer Meinander; Marja Tiitta; Reetta Karinen; Riikka L. Puurunen

doi:10.1039/d3cy01480k

Hydrodeoxygenation and hydrodenitrogenation of n-hexadecanamide over Pt catalysts : effect of the support

Emma Verkama^*, Sylvia Albersberger, Aitor Arandia, Kristoffer Meinander, Marja Tiitta, Reetta Karinen, Riikka L. Puurunen

^*Tämän työn vastaava kirjoittaja

Neste Corporation

Tutkimustuotos: Lehtiartikkeli › Article › Scientific › vertaisarvioitu

2 Sitaatiot (Scopus)

42 Lataukset (Pure)

Abstrakti

Efficient catalysts for simultaneous hydrodeoxygenation (HDO) and hydrodenitrogenation (HDN) are needed for the production of renewable fuels. In this study, Pt catalysts supported on SiO₂, γ-Al₂O₃, SiO₂-Al₂O₃, ZrO₂, CeO₂-ZrO₂, Nb₂O₅, and TiO₂ were studied for the hydrotreatment of n-hexadecanamide (C16 amide) to n-paraffins at 300 °C and 80 bar H₂. The catalysts favored HDO over HDN, and the initial differences in the nitrogen removal level were smaller than the differences in the oxygen removal level. The Lewis acid properties of the support influenced the initial C16 amide conversion route and HDO activity, which was reflected in the reaction network and condensation reaction selectivity of the catalysts. Pt/Nb₂O₅ and Pt/TiO₂, with intermediate strength Lewis acid sites, initially favored the HDO of C16 amide to nitrogen-containing compounds. In contrast, the other catalysts converted C16 amide to oxygen- and nitrogen-containing compounds with similar selectivity. The HDO of the oxygen-containing compounds proceeded more efficiently on the Pt catalysts supported on oxides with weak Lewis acid sites (Pt/ZrO₂, Pt/CeO₂-ZrO₂) than on the irreducible oxides with strong or no Lewis acid sites (Pt/γ-Al₂O₃, Pt/SiO₂-Al₂O₃, Pt/SiO₂). As the presence of oxygen-containing compounds suppressed HDN activity, the catalysts with the highest HDO activity eventually gave the highest paraffin yield, regardless of which oxygen removal pathway was favored.

Alkuperäiskieli	Englanti
Sivut	431-448
Julkaisu	Catalysis Science and Technology
Vuosikerta	14
Numero	2
Varhainen verkossa julkaisun päivämäärä	15 jouluk. 2023
DOI - pysyväislinkit	https://doi.org/10.1039/d3cy01480k
Tila	Julkaistu - 21 tammik. 2024
OKM-julkaisutyyppi	A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

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10.1039/d3cy01480kLisenssi: CC BY-NC

CHEM_Verkama_et_al_Hydrodeoxygenation_and_hydrodenitrogenation_2024_Catalysis_Science_and_TechnologyFinal published version, 2,29 MBLisenssi: CC BY-NC

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Neste-Aalto HDN Catalyst Development
Puurunen, R. (Vastuullinen tutkija), Arandia Gutierrez, A. (Projektipäällikkö), Chamssine, F. (Projektin jäsen), Karinen, R. (Projektin jäsen), Kattelus, J. (Projektin jäsen), Revitzer, H. (Projektin jäsen) & Verkama, E. (Projektin jäsen)
01/07/2019 → 30/06/2023
Projekti: Other external funding: Other domestic funding

Biotalousinfrastruktuuri
Seppälä, J. (Manager)
Kemian tekniikan korkeakoulu
Laitteistot/tilat: Facility
OtaNano
Rissanen, A. (Manager)
Aalto-yliopisto
Laitteistot/tilat: Facility
OtaNano Nanomikroskopiakeskus
Seitsonen, J. (Manager) & Rissanen, A. (Other)
OtaNano
Laitteistot/tilat: Facility

Findings from Aalto University Yields New Data on Chemicals and Chemistry (Hydrodeoxygenation and Hydrodenitrogenation of n -hexadecanamide Over Pt Catalysts: Effect of the Support)
Karinen, R., Puurunen, R. & Verkama, E.
22/01/2024
1 kohde/ Medianäkyvyys
Lehdistö/media: Esiintyminen mediassa

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@article{970c1c8a61c54198b4f795a26a207aab,

title = "Hydrodeoxygenation and hydrodenitrogenation of n-hexadecanamide over Pt catalysts : effect of the support",

abstract = "Efficient catalysts for simultaneous hydrodeoxygenation (HDO) and hydrodenitrogenation (HDN) are needed for the production of renewable fuels. In this study, Pt catalysts supported on SiO2, γ-Al2O3, SiO2-Al2O3, ZrO2, CeO2-ZrO2, Nb2O5, and TiO2 were studied for the hydrotreatment of n-hexadecanamide (C16 amide) to n-paraffins at 300 °C and 80 bar H2. The catalysts favored HDO over HDN, and the initial differences in the nitrogen removal level were smaller than the differences in the oxygen removal level. The Lewis acid properties of the support influenced the initial C16 amide conversion route and HDO activity, which was reflected in the reaction network and condensation reaction selectivity of the catalysts. Pt/Nb2O5 and Pt/TiO2, with intermediate strength Lewis acid sites, initially favored the HDO of C16 amide to nitrogen-containing compounds. In contrast, the other catalysts converted C16 amide to oxygen- and nitrogen-containing compounds with similar selectivity. The HDO of the oxygen-containing compounds proceeded more efficiently on the Pt catalysts supported on oxides with weak Lewis acid sites (Pt/ZrO2, Pt/CeO2-ZrO2) than on the irreducible oxides with strong or no Lewis acid sites (Pt/γ-Al2O3, Pt/SiO2-Al2O3, Pt/SiO2). As the presence of oxygen-containing compounds suppressed HDN activity, the catalysts with the highest HDO activity eventually gave the highest paraffin yield, regardless of which oxygen removal pathway was favored.",

author = "Emma Verkama and Sylvia Albersberger and Aitor Arandia and Kristoffer Meinander and Marja Tiitta and Reetta Karinen and Puurunen, {Riikka L.}",

note = "Funding Information: Dr. Hua Jiang is acknowledged for the STEM images, and Ellen J{\"a}rvinen is acknowledged for assistance with the batch reactor experiments. Dr. Yingnan Zhao and the Research Analytics department of Neste Corporation are acknowledged for the guidance with the acid site characterization and for access to the equipment that was used for the pyridine FTIR measurements. All members of the Neste-Aalto HDN catalyst development project group are gratefully acknowledged for fruitful discussions. This study was funded by Neste Corporation (Neste-Aalto HDN catalyst development project). The Bioeconomy and Raw materials research infrastructures at Aalto University and the OtaNano Nanomicroscopy Center were used for the study. Publisher Copyright: {\textcopyright} 2024 The Royal Society of Chemistry.",

year = "2024",

month = jan,

day = "21",

doi = "10.1039/d3cy01480k",

language = "English",

volume = "14",

pages = "431--448",

journal = "Catalysis Science and Technology ",

issn = "2044-4753",

publisher = "Royal Society of Chemistry",

number = "2",

}

TY - JOUR

T1 - Hydrodeoxygenation and hydrodenitrogenation of n-hexadecanamide over Pt catalysts : effect of the support

AU - Verkama, Emma

AU - Albersberger, Sylvia

AU - Arandia, Aitor

AU - Meinander, Kristoffer

AU - Tiitta, Marja

AU - Karinen, Reetta

AU - Puurunen, Riikka L.

N1 - Funding Information: Dr. Hua Jiang is acknowledged for the STEM images, and Ellen Järvinen is acknowledged for assistance with the batch reactor experiments. Dr. Yingnan Zhao and the Research Analytics department of Neste Corporation are acknowledged for the guidance with the acid site characterization and for access to the equipment that was used for the pyridine FTIR measurements. All members of the Neste-Aalto HDN catalyst development project group are gratefully acknowledged for fruitful discussions. This study was funded by Neste Corporation (Neste-Aalto HDN catalyst development project). The Bioeconomy and Raw materials research infrastructures at Aalto University and the OtaNano Nanomicroscopy Center were used for the study. Publisher Copyright: © 2024 The Royal Society of Chemistry.

PY - 2024/1/21

Y1 - 2024/1/21

N2 - Efficient catalysts for simultaneous hydrodeoxygenation (HDO) and hydrodenitrogenation (HDN) are needed for the production of renewable fuels. In this study, Pt catalysts supported on SiO2, γ-Al2O3, SiO2-Al2O3, ZrO2, CeO2-ZrO2, Nb2O5, and TiO2 were studied for the hydrotreatment of n-hexadecanamide (C16 amide) to n-paraffins at 300 °C and 80 bar H2. The catalysts favored HDO over HDN, and the initial differences in the nitrogen removal level were smaller than the differences in the oxygen removal level. The Lewis acid properties of the support influenced the initial C16 amide conversion route and HDO activity, which was reflected in the reaction network and condensation reaction selectivity of the catalysts. Pt/Nb2O5 and Pt/TiO2, with intermediate strength Lewis acid sites, initially favored the HDO of C16 amide to nitrogen-containing compounds. In contrast, the other catalysts converted C16 amide to oxygen- and nitrogen-containing compounds with similar selectivity. The HDO of the oxygen-containing compounds proceeded more efficiently on the Pt catalysts supported on oxides with weak Lewis acid sites (Pt/ZrO2, Pt/CeO2-ZrO2) than on the irreducible oxides with strong or no Lewis acid sites (Pt/γ-Al2O3, Pt/SiO2-Al2O3, Pt/SiO2). As the presence of oxygen-containing compounds suppressed HDN activity, the catalysts with the highest HDO activity eventually gave the highest paraffin yield, regardless of which oxygen removal pathway was favored.

AB - Efficient catalysts for simultaneous hydrodeoxygenation (HDO) and hydrodenitrogenation (HDN) are needed for the production of renewable fuels. In this study, Pt catalysts supported on SiO2, γ-Al2O3, SiO2-Al2O3, ZrO2, CeO2-ZrO2, Nb2O5, and TiO2 were studied for the hydrotreatment of n-hexadecanamide (C16 amide) to n-paraffins at 300 °C and 80 bar H2. The catalysts favored HDO over HDN, and the initial differences in the nitrogen removal level were smaller than the differences in the oxygen removal level. The Lewis acid properties of the support influenced the initial C16 amide conversion route and HDO activity, which was reflected in the reaction network and condensation reaction selectivity of the catalysts. Pt/Nb2O5 and Pt/TiO2, with intermediate strength Lewis acid sites, initially favored the HDO of C16 amide to nitrogen-containing compounds. In contrast, the other catalysts converted C16 amide to oxygen- and nitrogen-containing compounds with similar selectivity. The HDO of the oxygen-containing compounds proceeded more efficiently on the Pt catalysts supported on oxides with weak Lewis acid sites (Pt/ZrO2, Pt/CeO2-ZrO2) than on the irreducible oxides with strong or no Lewis acid sites (Pt/γ-Al2O3, Pt/SiO2-Al2O3, Pt/SiO2). As the presence of oxygen-containing compounds suppressed HDN activity, the catalysts with the highest HDO activity eventually gave the highest paraffin yield, regardless of which oxygen removal pathway was favored.

UR - http://www.scopus.com/inward/record.url?scp=85180968916&partnerID=8YFLogxK

U2 - 10.1039/d3cy01480k

DO - 10.1039/d3cy01480k

M3 - Article

AN - SCOPUS:85180968916

SN - 2044-4753

VL - 14

SP - 431

EP - 448

JO - Catalysis Science and Technology

JF - Catalysis Science and Technology

IS - 2

ER -

Hydrodeoxygenation and hydrodenitrogenation of n-hexadecanamide over Pt catalysts : effect of the support

Abstrakti

YK:n kestävän kehityksen tavoitteet

Pääsy asiakirjaan

Muut tiedostot ja linkit

Sormenjälki

Projektit

Neste-Aalto HDN Catalyst Development

Laitteet

Biotalousinfrastruktuuri

OtaNano

OtaNano Nanomikroskopiakeskus

Lehtileikkeet

Findings from Aalto University Yields New Data on Chemicals and Chemistry (Hydrodeoxygenation and Hydrodenitrogenation of n -hexadecanamide Over Pt Catalysts: Effect of the Support)

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