Structured microreactor with gold and palladium on titania: Active, regenerable and durable catalyst coatings for the gas-phase partial oxidation of 1-butanol

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@article{e0e5e9e3574a4ff0978afe4871f585fb,
title = "Structured microreactor with gold and palladium on titania: Active, regenerable and durable catalyst coatings for the gas-phase partial oxidation of 1-butanol",
abstract = "Structured microreactors coated with catalytically active porous layers have emerged as a promising replacement for conventional reactors because they are inherently safe to operate in nearly isothermal conditions within the kinetic regime. Bio-based 1-butanol is commonly produced by acetone-butanol-ethanol (ABE) fermentation and is considered an important platform chemical that will benefit in the share of value-added chemicals through the development of new catalytic processes. In this study, monometallic gold (Au) and palladium (Pd), as well as bimetallic Au-Pd nanoparticles, supported on titania (TiO2) were prepared by a sol-immobilization method, characterized, coated on structured microreactor plates and tested for their catalytic activity in the gas-phase partial oxidation of 1-butanol to n-butyraldehyde. A customized structured catalyst testing microreactor was used. The average noble metal particle size for the catalyst coatings was determined to be approximately 3.6 nm for Au and Au-Pd catalysts, and the noble metal nanoparticles were evenly distributed. The catalyst coating was 17 ± 7 μm in thickness. The studied coated catalysts (TiO2, Au/TiO2, Pd/TiO2, and Au-Pd/TiO2) were all active for the partial oxidation of 1-butanol. The Au/TiO2 (0.6 wt{\%}) catalyst showed the highest yield (20{\%}) of n-butyraldehyde at 300 °C. The introduction of Pd onto Au/TiO2 or TiO2 shifted the product distribution at 250 °C towards retro-hydroformylation and oxidation products (propene, carbon monoxide and carbon dioxide). All of the coated catalysts that were tested were mechanically stable. The nano Au/TiO2 could be regenerated in situ and showed reproducible activities and yields in over 50 test runs. Structured microreactors coated with gold nanoparticles supported on titania show promise as a reusable and mechanically stable device for the process development of n-butyraldehyde production in ABE fermentation plants.",
keywords = "Bio 1-butanol, Coated microreactors, Heterogeneous catalyst, n-Butyraldehyde, Nanogold, Partial oxidation, Titania",
author = "Yaseen Khan and Minna Marin and Tiia Viinikainen and Juha Lehtonen and Puurunen, {Riikka L.} and Reetta Karinen",
year = "2018",
month = "7",
day = "25",
doi = "10.1016/j.apcata.2018.06.010",
language = "English",
volume = "562",
pages = "173--183",
journal = "APPLIED CATALYSIS A-GENERAL",
issn = "0926-860X",
publisher = "Elsevier Science B.V.",

}

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TY - JOUR

T1 - Structured microreactor with gold and palladium on titania

T2 - Active, regenerable and durable catalyst coatings for the gas-phase partial oxidation of 1-butanol

AU - Khan, Yaseen

AU - Marin, Minna

AU - Viinikainen, Tiia

AU - Lehtonen, Juha

AU - Puurunen, Riikka L.

AU - Karinen, Reetta

PY - 2018/7/25

Y1 - 2018/7/25

N2 - Structured microreactors coated with catalytically active porous layers have emerged as a promising replacement for conventional reactors because they are inherently safe to operate in nearly isothermal conditions within the kinetic regime. Bio-based 1-butanol is commonly produced by acetone-butanol-ethanol (ABE) fermentation and is considered an important platform chemical that will benefit in the share of value-added chemicals through the development of new catalytic processes. In this study, monometallic gold (Au) and palladium (Pd), as well as bimetallic Au-Pd nanoparticles, supported on titania (TiO2) were prepared by a sol-immobilization method, characterized, coated on structured microreactor plates and tested for their catalytic activity in the gas-phase partial oxidation of 1-butanol to n-butyraldehyde. A customized structured catalyst testing microreactor was used. The average noble metal particle size for the catalyst coatings was determined to be approximately 3.6 nm for Au and Au-Pd catalysts, and the noble metal nanoparticles were evenly distributed. The catalyst coating was 17 ± 7 μm in thickness. The studied coated catalysts (TiO2, Au/TiO2, Pd/TiO2, and Au-Pd/TiO2) were all active for the partial oxidation of 1-butanol. The Au/TiO2 (0.6 wt%) catalyst showed the highest yield (20%) of n-butyraldehyde at 300 °C. The introduction of Pd onto Au/TiO2 or TiO2 shifted the product distribution at 250 °C towards retro-hydroformylation and oxidation products (propene, carbon monoxide and carbon dioxide). All of the coated catalysts that were tested were mechanically stable. The nano Au/TiO2 could be regenerated in situ and showed reproducible activities and yields in over 50 test runs. Structured microreactors coated with gold nanoparticles supported on titania show promise as a reusable and mechanically stable device for the process development of n-butyraldehyde production in ABE fermentation plants.

AB - Structured microreactors coated with catalytically active porous layers have emerged as a promising replacement for conventional reactors because they are inherently safe to operate in nearly isothermal conditions within the kinetic regime. Bio-based 1-butanol is commonly produced by acetone-butanol-ethanol (ABE) fermentation and is considered an important platform chemical that will benefit in the share of value-added chemicals through the development of new catalytic processes. In this study, monometallic gold (Au) and palladium (Pd), as well as bimetallic Au-Pd nanoparticles, supported on titania (TiO2) were prepared by a sol-immobilization method, characterized, coated on structured microreactor plates and tested for their catalytic activity in the gas-phase partial oxidation of 1-butanol to n-butyraldehyde. A customized structured catalyst testing microreactor was used. The average noble metal particle size for the catalyst coatings was determined to be approximately 3.6 nm for Au and Au-Pd catalysts, and the noble metal nanoparticles were evenly distributed. The catalyst coating was 17 ± 7 μm in thickness. The studied coated catalysts (TiO2, Au/TiO2, Pd/TiO2, and Au-Pd/TiO2) were all active for the partial oxidation of 1-butanol. The Au/TiO2 (0.6 wt%) catalyst showed the highest yield (20%) of n-butyraldehyde at 300 °C. The introduction of Pd onto Au/TiO2 or TiO2 shifted the product distribution at 250 °C towards retro-hydroformylation and oxidation products (propene, carbon monoxide and carbon dioxide). All of the coated catalysts that were tested were mechanically stable. The nano Au/TiO2 could be regenerated in situ and showed reproducible activities and yields in over 50 test runs. Structured microreactors coated with gold nanoparticles supported on titania show promise as a reusable and mechanically stable device for the process development of n-butyraldehyde production in ABE fermentation plants.

KW - Bio 1-butanol

KW - Coated microreactors

KW - Heterogeneous catalyst

KW - n-Butyraldehyde

KW - Nanogold

KW - Partial oxidation

KW - Titania

UR - http://www.scopus.com/inward/record.url?scp=85048251277&partnerID=8YFLogxK

U2 - 10.1016/j.apcata.2018.06.010

DO - 10.1016/j.apcata.2018.06.010

M3 - Article

VL - 562

SP - 173

EP - 183

JO - APPLIED CATALYSIS A-GENERAL

JF - APPLIED CATALYSIS A-GENERAL

SN - 0926-860X

ER -

ID: 26025838