Aqueous-phase reforming of Fischer-Tropsch alcohols over nickel-based catalysts to produce hydrogen: Product distribution and reaction pathways

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Aqueous-phase reforming of Fischer-Tropsch alcohols over nickel-based catalysts to produce hydrogen : Product distribution and reaction pathways. / Coronado, Irene; Pitínová, Martina; Karinen, Reetta; Reinikainen, Matti; Puurunen, Riikka L.; Lehtonen, Juha.

In: Applied Catalysis A: General, Vol. 567, 25.10.2018, p. 112-121.

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@article{68d6ddf1318a4fd3ae39cf126abae43b,
title = "Aqueous-phase reforming of Fischer-Tropsch alcohols over nickel-based catalysts to produce hydrogen: Product distribution and reaction pathways",
abstract = "Catalytic aqueous-phase reforming (APR) can be applied to process the organic compounds in the water fractions derived from the Fischer-Tropsch (FT) synthesis. This work aimed at finding an active nickel-based catalyst to convert organic compounds typically found in FT-derived waters, such as alcohols, into hydrogen. In addition, this work aimed at proposing potential reaction pathways that explain the product distribution resulting from the APR of C1–C3 alcohols. Solutions with 5{\%} mass fraction of either methanol, ethanol, propan-1-ol or propan-2-ol in water were processed in APR at 230 °C and 3.2 MPa over different nickel-based catalysts in a continuous packed-bed reactor. Methanol was successfully reformed into hydrogen and carbon monoxide with conversions up to 60{\%}. The conversion of C2–C3 alcohols achieved values in the range of 12{\%} to 55{\%}. The results obtained in the APR of C2–C3 alcohols suggest that in addition to reforming to hydrogen and carbon monoxide, the alcohols underwent dehydrogenation and decarbonylation. The most stable catalyst, nickel-copper supported on ceria-zirconia, reached feedstock conversions between 20{\%} and 60{\%} and high hydrogen selectivity. Monometallic nickel supported on ceria-zirconia catalysts reached higher H2 yields; however, the yield of side products, such as alkanes, was also higher over the monometallic catalysts. Accordingly, ceria-zirconia nickel-based supported catalysts constitute suitable candidates to process the alcohols in the water fractions derived from the FT synthesis.",
keywords = "Alcohols, Aqueous-phase reforming, Fischer-Tropsch water fraction, Hydrogen, Nickel-based catalysts",
author = "Irene Coronado and Martina Pit{\'i}nov{\'a} and Reetta Karinen and Matti Reinikainen and Puurunen, {Riikka L.} and Juha Lehtonen",
year = "2018",
month = "10",
day = "25",
doi = "10.1016/j.apcata.2018.09.013",
language = "English",
volume = "567",
pages = "112--121",
journal = "APPLIED CATALYSIS A-GENERAL",
issn = "0926-860X",
publisher = "Elsevier Science B.V.",

}

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TY - JOUR

T1 - Aqueous-phase reforming of Fischer-Tropsch alcohols over nickel-based catalysts to produce hydrogen

T2 - Product distribution and reaction pathways

AU - Coronado, Irene

AU - Pitínová, Martina

AU - Karinen, Reetta

AU - Reinikainen, Matti

AU - Puurunen, Riikka L.

AU - Lehtonen, Juha

PY - 2018/10/25

Y1 - 2018/10/25

N2 - Catalytic aqueous-phase reforming (APR) can be applied to process the organic compounds in the water fractions derived from the Fischer-Tropsch (FT) synthesis. This work aimed at finding an active nickel-based catalyst to convert organic compounds typically found in FT-derived waters, such as alcohols, into hydrogen. In addition, this work aimed at proposing potential reaction pathways that explain the product distribution resulting from the APR of C1–C3 alcohols. Solutions with 5% mass fraction of either methanol, ethanol, propan-1-ol or propan-2-ol in water were processed in APR at 230 °C and 3.2 MPa over different nickel-based catalysts in a continuous packed-bed reactor. Methanol was successfully reformed into hydrogen and carbon monoxide with conversions up to 60%. The conversion of C2–C3 alcohols achieved values in the range of 12% to 55%. The results obtained in the APR of C2–C3 alcohols suggest that in addition to reforming to hydrogen and carbon monoxide, the alcohols underwent dehydrogenation and decarbonylation. The most stable catalyst, nickel-copper supported on ceria-zirconia, reached feedstock conversions between 20% and 60% and high hydrogen selectivity. Monometallic nickel supported on ceria-zirconia catalysts reached higher H2 yields; however, the yield of side products, such as alkanes, was also higher over the monometallic catalysts. Accordingly, ceria-zirconia nickel-based supported catalysts constitute suitable candidates to process the alcohols in the water fractions derived from the FT synthesis.

AB - Catalytic aqueous-phase reforming (APR) can be applied to process the organic compounds in the water fractions derived from the Fischer-Tropsch (FT) synthesis. This work aimed at finding an active nickel-based catalyst to convert organic compounds typically found in FT-derived waters, such as alcohols, into hydrogen. In addition, this work aimed at proposing potential reaction pathways that explain the product distribution resulting from the APR of C1–C3 alcohols. Solutions with 5% mass fraction of either methanol, ethanol, propan-1-ol or propan-2-ol in water were processed in APR at 230 °C and 3.2 MPa over different nickel-based catalysts in a continuous packed-bed reactor. Methanol was successfully reformed into hydrogen and carbon monoxide with conversions up to 60%. The conversion of C2–C3 alcohols achieved values in the range of 12% to 55%. The results obtained in the APR of C2–C3 alcohols suggest that in addition to reforming to hydrogen and carbon monoxide, the alcohols underwent dehydrogenation and decarbonylation. The most stable catalyst, nickel-copper supported on ceria-zirconia, reached feedstock conversions between 20% and 60% and high hydrogen selectivity. Monometallic nickel supported on ceria-zirconia catalysts reached higher H2 yields; however, the yield of side products, such as alkanes, was also higher over the monometallic catalysts. Accordingly, ceria-zirconia nickel-based supported catalysts constitute suitable candidates to process the alcohols in the water fractions derived from the FT synthesis.

KW - Alcohols

KW - Aqueous-phase reforming

KW - Fischer-Tropsch water fraction

KW - Hydrogen

KW - Nickel-based catalysts

UR - http://www.scopus.com/inward/record.url?scp=85053823666&partnerID=8YFLogxK

U2 - 10.1016/j.apcata.2018.09.013

DO - 10.1016/j.apcata.2018.09.013

M3 - Article

VL - 567

SP - 112

EP - 121

JO - APPLIED CATALYSIS A-GENERAL

JF - APPLIED CATALYSIS A-GENERAL

SN - 0926-860X

ER -

ID: 28561031