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

Yaseen Khan (Corresponding Author), Minna Marin, Tiia Viinikainen, Juha Lehtonen, Riikka L. Puurunen, Reetta Karinen

Research output: Contribution to journalArticleScientificpeer-review

1 Citation (Scopus)

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.

Original languageEnglish
Pages (from-to)173-183
Number of pages11
JournalApplied Catalysis A: General
Volume562
DOIs
Publication statusPublished - 25 Jul 2018
MoE publication typeA1 Journal article-refereed

Fingerprint

1-Butanol
Palladium
Butenes
Gold
Titanium
Gases
Coatings
Oxidation
Catalysts
Butanols
Precious metals
Acetone
Fermentation
Ethanol
Nanoparticles
Hydroformylation
Metal nanoparticles
Polymethyl Methacrylate
Carbon Monoxide
Sols

Keywords

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

Cite this

@article{287009b9c14d4d98b49b6b6eab13202d,
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.",
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author = "Yaseen Khan and Minna Marin and Tiia Viinikainen and Juha Lehtonen and Puurunen, {Riikka L.} and Reetta Karinen",
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Structured microreactor with gold and palladium on titania : Active, regenerable and durable catalyst coatings for the gas-phase partial oxidation of 1-butanol. / Khan, Yaseen (Corresponding Author); Marin, Minna; Viinikainen, Tiia; Lehtonen, Juha; Puurunen, Riikka L.; Karinen, Reetta.

In: Applied Catalysis A: General, Vol. 562, 25.07.2018, p. 173-183.

Research output: Contribution to journalArticleScientificpeer-review

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

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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.

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KW - Coated microreactors

KW - Heterogeneous catalyst

KW - n-Butyraldehyde

KW - Nanogold

KW - Partial oxidation

KW - Titania

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