Unravelling mass transport in hierarchically porous catalysts

Mark A. Isaacs; Neil Robinson; Brunella Barbero; Lee J. Durndell; Jinesh C. Manayil; Christopher M.A. Parlett; Carmine D'Agostino; Karen Wilson; Adam F. Lee

doi:10.1039/c9ta01867k

Unravelling mass transport in hierarchically porous catalysts

Mark A. Isaacs
, Neil Robinson
, Brunella Barbero
, Lee J. Durndell
, Jinesh C. Manayil
, Christopher M.A. Parlett
, Carmine D'Agostino^*
, Karen Wilson
, Adam F. Lee

^*Corresponding author for this work

University of Cambridge
University of Manchester

Research output: Contribution to journal › Article › peer-review

102 Citations (SciVal)

77 Downloads (Pure)

Abstract

Bio-derived platform chemicals and fuels are important for the development of sustainable manufacturing. However, their efficient production from biomass necessitates new catalysts and processes optimised for the selective transformation of large molecules. Mesoporous and hierarchically porous functional materials are promising catalyst candidates for biomass valorisation, but quantitative relationships between pore dimensions/connectivity, mass transport, and corresponding catalytic performance are poorly defined. A family of hierarchical macroporous-mesoporous SBA-15 sulfonic acids were prepared with tunable macropore diameters for carboxylic acid esterification. Turnover frequencies for long-chain (palmitic and erucic) acids were proportional to macropore diameter (≤370 nm), whereas propanoic acid esterification was independent of macropore size. Pulsed field gradient NMR diffusion experiments reveal that larger macropores enhance esterification of bulky carboxylic acids by conferring superior pore interconnectivity and associated mass transport.

Original language	English
Pages (from-to)	11814-11825
Number of pages	12
Journal	Journal of Materials Chemistry A
Volume	7
Issue number	19
DOIs	https://doi.org/10.1039/c9ta01867k
Publication status	Published - 24 Apr 2019

Bibliographical note

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.

Funding

We would like to acknowledge the EPSRC for funding this work (grants EP/G007594/4 and EP/F063423/2). N. R. acknowledges the Catalysis@Cambridge initiative, University of Cambridge, for the award of a PhD studentship. C. D. A. would like to acknowledge Wolfson College, Cambridge, for supporting his research activities. The authors also thank Prof Lynn F. Gladden, University of Cambridge, for access to the NMR equipment.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy
SDG 9 Industry, Innovation, and Infrastructure

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10.1039/c9ta01867kLicence: CC BY 3.0

Unravelling mass transport in hierarchically porous catalysts
This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Final published version, 1.23 MBLicence: CC BY 3.0

Cite this

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title = "Unravelling mass transport in hierarchically porous catalysts",

abstract = "Bio-derived platform chemicals and fuels are important for the development of sustainable manufacturing. However, their efficient production from biomass necessitates new catalysts and processes optimised for the selective transformation of large molecules. Mesoporous and hierarchically porous functional materials are promising catalyst candidates for biomass valorisation, but quantitative relationships between pore dimensions/connectivity, mass transport, and corresponding catalytic performance are poorly defined. A family of hierarchical macroporous-mesoporous SBA-15 sulfonic acids were prepared with tunable macropore diameters for carboxylic acid esterification. Turnover frequencies for long-chain (palmitic and erucic) acids were proportional to macropore diameter (≤370 nm), whereas propanoic acid esterification was independent of macropore size. Pulsed field gradient NMR diffusion experiments reveal that larger macropores enhance esterification of bulky carboxylic acids by conferring superior pore interconnectivity and associated mass transport.",

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AU - Parlett, Christopher M.A.

AU - D'Agostino, Carmine

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N2 - Bio-derived platform chemicals and fuels are important for the development of sustainable manufacturing. However, their efficient production from biomass necessitates new catalysts and processes optimised for the selective transformation of large molecules. Mesoporous and hierarchically porous functional materials are promising catalyst candidates for biomass valorisation, but quantitative relationships between pore dimensions/connectivity, mass transport, and corresponding catalytic performance are poorly defined. A family of hierarchical macroporous-mesoporous SBA-15 sulfonic acids were prepared with tunable macropore diameters for carboxylic acid esterification. Turnover frequencies for long-chain (palmitic and erucic) acids were proportional to macropore diameter (≤370 nm), whereas propanoic acid esterification was independent of macropore size. Pulsed field gradient NMR diffusion experiments reveal that larger macropores enhance esterification of bulky carboxylic acids by conferring superior pore interconnectivity and associated mass transport.

AB - Bio-derived platform chemicals and fuels are important for the development of sustainable manufacturing. However, their efficient production from biomass necessitates new catalysts and processes optimised for the selective transformation of large molecules. Mesoporous and hierarchically porous functional materials are promising catalyst candidates for biomass valorisation, but quantitative relationships between pore dimensions/connectivity, mass transport, and corresponding catalytic performance are poorly defined. A family of hierarchical macroporous-mesoporous SBA-15 sulfonic acids were prepared with tunable macropore diameters for carboxylic acid esterification. Turnover frequencies for long-chain (palmitic and erucic) acids were proportional to macropore diameter (≤370 nm), whereas propanoic acid esterification was independent of macropore size. Pulsed field gradient NMR diffusion experiments reveal that larger macropores enhance esterification of bulky carboxylic acids by conferring superior pore interconnectivity and associated mass transport.

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Unravelling mass transport in hierarchically porous catalysts

Abstract

Bibliographical note

Funding

UN SDGs

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