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
N1 - Funding Information:
The Academy of Finland MICATOX project is acknowledged for funding this work. Giovanni Marin is thanked for the XRF-analysis, Hannu Revitzer for the ICP-OES-analysis, Eveliina Mäkelä for the physisorption measurements, Suvi Nummipuro for assistance in catalyst preparation, Janne-Joonas Tiitinen for assistance in running experiments, Hua Jing for TEM images and Eero Haimi for SEM images at Aalto University. Professor Tapio Salmi and his team are thanked for their valuable discussions on 1-butanol oxidation reactions. The Bioeconomy Infrastructure and Nanomicroscopy Center (Aalto-NMC) at Aalto University were used to complete the work.
Publisher Copyright:
© 2018 Elsevier B.V.
Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.
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
AN - SCOPUS:85048251277
SN - 0926-860X
VL - 562
SP - 173
EP - 183
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
ER -