TY - JOUR
T1 - Understanding the Chemical and Electronic Properties of Sub-Monolayer TiO₂ on High Surface Area Silica for Jet Fuel Synthesis Applications
AU - Isaacs, Mark A.
AU - Drivas, Charalampos
AU - Graf, Arthur
AU - Kroon, Sasha
AU - Kumar, Santosh
AU - Liu, Junxi
AU - Torres‐Lopez, Antonio
AU - Price, Cameron
AU - Garland, Edward
AU - Lezcano‐Gonzalez, Ines
AU - Parlett, Christopher M. A.
AU - dos Santos‐Durndell, Vannia C.
AU - Durndell, Lee J.
PY - 2025/7/16
Y1 - 2025/7/16
N2 - 2.5% of global carbon emissions result from air travel, underscoring the need for sustainable aviation fuels (SAF) derived from second-generation lignocellulosic biomass to enhance the green credentials of the aviation sector. This study demonstrates the first solvent-free photocatalytic conversion of furfural (FAL) and cyclopentanone (CPO) to produce 2,5-bis(2-furylmethylidene)cyclopentanone (F2Cp), a jet fuel precursor, using Ti-SBA-15 catalysts, synthesized via alkoxide grafting and controlled titanium surface coverage. Sub-monolayer titania films on SBA-15 supports are achieved with tuneable Ti content, confirmed by XPS (X-ray photoelectron spectroscopy), UPS (ultraviolet photoelectron spectroscopy), REELS (reflectance electron energy loss spectroscopy), ISS (ion scattering spectroscopy), and Raman analysis. XPS analyses reveal coverage-dependent Ti speciation, transitioning from isolated Ti atoms to interconnected Ti-O-Ti networks, with corresponding shifts in Auger parameters, indicating increased surface polarizability and Lewis acidity. Optimized Ti-SBA-15 catalysts exhibit a fourfold activity enhancement in photocatalytic activity over bulk TiO₂, attributed to improved mass transport, active site accessibility, and surface stability. This work highlights the potential of rationally designed hierarchical catalysts for scalable, energy-efficient biomass valorization into SAF precursors, offering a scalable, energy-efficient pathway for sustainable jet fuel production. By elucidating the structure-function relationships in sub-monolayer Ti-SBA-15 materials, this study provides critical insights for advancing photocatalytic technologies in renewable energy applications.
AB - 2.5% of global carbon emissions result from air travel, underscoring the need for sustainable aviation fuels (SAF) derived from second-generation lignocellulosic biomass to enhance the green credentials of the aviation sector. This study demonstrates the first solvent-free photocatalytic conversion of furfural (FAL) and cyclopentanone (CPO) to produce 2,5-bis(2-furylmethylidene)cyclopentanone (F2Cp), a jet fuel precursor, using Ti-SBA-15 catalysts, synthesized via alkoxide grafting and controlled titanium surface coverage. Sub-monolayer titania films on SBA-15 supports are achieved with tuneable Ti content, confirmed by XPS (X-ray photoelectron spectroscopy), UPS (ultraviolet photoelectron spectroscopy), REELS (reflectance electron energy loss spectroscopy), ISS (ion scattering spectroscopy), and Raman analysis. XPS analyses reveal coverage-dependent Ti speciation, transitioning from isolated Ti atoms to interconnected Ti-O-Ti networks, with corresponding shifts in Auger parameters, indicating increased surface polarizability and Lewis acidity. Optimized Ti-SBA-15 catalysts exhibit a fourfold activity enhancement in photocatalytic activity over bulk TiO₂, attributed to improved mass transport, active site accessibility, and surface stability. This work highlights the potential of rationally designed hierarchical catalysts for scalable, energy-efficient biomass valorization into SAF precursors, offering a scalable, energy-efficient pathway for sustainable jet fuel production. By elucidating the structure-function relationships in sub-monolayer Ti-SBA-15 materials, this study provides critical insights for advancing photocatalytic technologies in renewable energy applications.
KW - hierarchical titania
KW - photocatalysis
KW - sustainable aviation fuels
UR - http://dx.doi.org/10.1002/adfm.202502818
UR - https://pearl.plymouth.ac.uk/gees-research/1477/
U2 - 10.1002/adfm.202502818
DO - 10.1002/adfm.202502818
M3 - Article
SN - 1616-301X
JO - Advanced Functional Materials
JF - Advanced Functional Materials
M1 - e02818
ER -