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.
| Original language | English |
|---|---|
| Pages (from-to) | 112-121 |
| Number of pages | 10 |
| Journal | Applied Catalysis A: General |
| Volume | 567 |
| DOIs | |
| Publication status | Published - 25 Oct 2018 |
| MoE publication type | Not Eligible |
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Keywords
- Alcohols
- Aqueous-phase reforming
- Fischer-Tropsch water fraction
- Hydrogen
- Nickel-based catalysts
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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 (Corresponding Author); Pitínová, Martina; Karinen, Reetta; Reinikainen, Matti; Puurunen, Riikka L.; Lehtonen, Juha.
In: Applied Catalysis A: General, Vol. 567, 25.10.2018, p. 112-121.Research output: Contribution to journal › Article › Scientific › peer-review
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
AN - SCOPUS:85053823666
VL - 567
SP - 112
EP - 121
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
SN - 0926-860X
ER -