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Controlling the production of acid catalyzed products of furfural hydrogenation by Pd/TiO2

Controlling the production of acid catalyzed products of furfural hydrogenation by Pd/TiO2
Controlling the production of acid catalyzed products of furfural hydrogenation by Pd/TiO2

We demonstrate a modified sol-immobilization procedure using (MeOH)x/(H2O)1-x solvent mixtures to prepare Pd/TiO2 catalysts that are able to reduce the formation of acid catalyzed products, e. g. ethers, for the hydrogenation of furfural. Transmission electron microscopy found a significant increase in polyvinyl alcohol (PVA) deposition at the metal-support interface and temperature programmed reduction found a reduced uptake of hydrogen, compared to an established Pd/TiO2 preparation. We propose that the additional PVA hinders hydrogen spillover onto the TiO2 support and limits the formation of Brønsted acid sites, required to produce ethers. Elsewhere, the new preparation route was able to successfully anchor colloidal Pd to the TiO2 surface, without the need for acidification. This work demonstrates the potential for minimizing process steps as well as optimizing catalyst selectivity – both important objectives for sustainable chemistry.

furfural hydrogenation, hydrogen spillover, palladium nanoparticles, sol-immobilization, X-ray absorption spectroscopy
1867-3880
5121-5133
Tierney, George F.
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Alijani, Shahram
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Panchal, Monik
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Decarolis, Donato
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de Gutierrez, Martha Briceno
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Mohammed, Khaled M.H.
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Callison, June
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Gibson, Emma K.
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Thompson, Paul B.J.
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Collier, Paul
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Dimitratos, Nikolaos
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Corbos, E. Crina
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Pelletier, Frederic
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Villa, Alberto
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Wells, Peter P.
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Tierney, George F.
5a1b1e97-5868-4933-a321-9b2cdfb69c5a
Alijani, Shahram
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Panchal, Monik
ed0fef23-7e85-4bbe-b173-31cd7a4ef7ad
Decarolis, Donato
aa002823-ac92-4afe-aa03-83562110dd3c
de Gutierrez, Martha Briceno
37de3174-4b42-4f1e-b37e-8d983b9a58db
Mohammed, Khaled M.H.
1c3c5641-4d0a-4c4d-bb26-fe733b8dbf63
Callison, June
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Gibson, Emma K.
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Thompson, Paul B.J.
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Collier, Paul
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Dimitratos, Nikolaos
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Corbos, E. Crina
c3416249-22f8-4a77-ad36-f665010e9bdd
Pelletier, Frederic
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Villa, Alberto
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Wells, Peter P.
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Tierney, George F., Alijani, Shahram, Panchal, Monik, Decarolis, Donato, de Gutierrez, Martha Briceno, Mohammed, Khaled M.H., Callison, June, Gibson, Emma K., Thompson, Paul B.J., Collier, Paul, Dimitratos, Nikolaos, Corbos, E. Crina, Pelletier, Frederic, Villa, Alberto and Wells, Peter P. (2021) Controlling the production of acid catalyzed products of furfural hydrogenation by Pd/TiO2. ChemCatChem, 13 (24), 5121-5133. (doi:10.1002/cctc.202101036).

Record type: Article

Abstract

We demonstrate a modified sol-immobilization procedure using (MeOH)x/(H2O)1-x solvent mixtures to prepare Pd/TiO2 catalysts that are able to reduce the formation of acid catalyzed products, e. g. ethers, for the hydrogenation of furfural. Transmission electron microscopy found a significant increase in polyvinyl alcohol (PVA) deposition at the metal-support interface and temperature programmed reduction found a reduced uptake of hydrogen, compared to an established Pd/TiO2 preparation. We propose that the additional PVA hinders hydrogen spillover onto the TiO2 support and limits the formation of Brønsted acid sites, required to produce ethers. Elsewhere, the new preparation route was able to successfully anchor colloidal Pd to the TiO2 surface, without the need for acidification. This work demonstrates the potential for minimizing process steps as well as optimizing catalyst selectivity – both important objectives for sustainable chemistry.

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ChemCatChem - 2021 - Tierney - Controlling the Production of Acid Catalyzed Products of Furfural Hydrogenation by Pd TiO2 - Version of Record
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Accepted/In Press date: 10 October 2021
e-pub ahead of print date: 15 December 2021
Additional Information: Funding Information: The authors wish to acknowledge N. Ramanan and V. Celorrio for measuring Pd NP samples as part of the UK Catalysis Hub block access grant (BAG) (SP19850) on the B18 beamline at the Diamond Light Source, U.K. XMaS is a UK national research facility supported by EPSRC. We are grateful to all the beamline team staff for their support (experiment number CH5827). The RCaH core staff are also acknowledged for use of facilities. The electron microscopy department of Johnson Matthey Technology Centre, Sonning Common are acknowledged for their support in acquiring STEM HAADF and EDX images of fresh and used Pd/TiO catalysts. D.D. acknowledges funded received through the UK Catalysis Hub and the UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC grant: EP/K014706/2, EP/K014668/1, EP/K014854/1, EP/K014714/1 or EP/M013219/1. P.P.W and K.M.H.M acknowledge the STFC GCRF START project for funding the position of K.M.H.M: ST/R002754/1. 2 Publisher Copyright: © 2021 The Authors. ChemCatChem published by Wiley-VCH GmbH Copyright: Copyright 2021 Elsevier B.V., All rights reserved.
Keywords: furfural hydrogenation, hydrogen spillover, palladium nanoparticles, sol-immobilization, X-ray absorption spectroscopy
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Identifiers

Local EPrints ID: 453632
URI: http://eprints.soton.ac.uk/id/eprint/453632
DOI: doi:10.1002/cctc.202101036
ISSN: 1867-3880
PURE UUID: d79316ef-0551-4697-9c47-781195173928
ORCID for Khaled M.H. Mohammed: ORCID iD orcid.org/0000-0002-9538-0936
ORCID for Peter P. Wells: ORCID iD orcid.org/0000-0002-0859-9172

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Date deposited: 20 Jan 2022 17:40
Last modified: 18 Mar 2024 03:55

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Contributors

Author: George F. Tierney
Author: Shahram Alijani
Author: Monik Panchal
Author: Donato Decarolis
Author: Martha Briceno de Gutierrez
Author: Khaled M.H. Mohammed ORCID iD
Author: June Callison
Author: Emma K. Gibson
Author: Paul B.J. Thompson
Author: Paul Collier
Author: Nikolaos Dimitratos
Author: E. Crina Corbos
Author: Frederic Pelletier
Author: Alberto Villa
Author: Peter P. Wells ORCID iD

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