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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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä

Date

2018-07-25

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en

Pages

11
173-183

Series

Applied Catalysis A: General, Volume 562

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.

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Keywords

Bio 1-butanol, Coated microreactors, Heterogeneous catalyst, n-Butyraldehyde, Nanogold, Partial oxidation, Titania

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Citation

Khan, Y, Marin, M, Viinikainen, T, Lehtonen, J, Puurunen, R L & Karinen, R 2018, ' Structured microreactor with gold and palladium on titania : Active, regenerable and durable catalyst coatings for the gas-phase partial oxidation of 1-butanol ', Applied Catalysis A: General, vol. 562, pp. 173-183 . https://doi.org/10.1016/j.apcata.2018.06.010