Energy-dense sustainable aviation fuel-range hydrocarbons from cyclohexanone as a biomass-derived feedstock via sequential catalytic aldol condensation and hydrodeoxygenation

• Biomass-derivable cyclohexanone as a feedstock for high-density aviation fuel. • NbOPO 4 catalyst exhibited excellent activity for aldol condensation and alkylation. • Ni/NbOPO 4 catalyst exhibited superior hydrogenation of adducts than Pd/Al 2 O 3. • Similar results from one-pot and two-pot aldol-condensation followed hydrogenation. • Liquid compositions linked to types of coke/char deposits observed on catalyst. Climate change is the main driver for sustainable aviation fuels production as a means of decarbonising/defossilising the sector. In this work, several catalysts have been screened to produce aviation fuel (C 6 -C 16 ) component hydrocarbons from cyclohexanone, a model compound of lignin-derived bio-oils. Using a two-stage two-pot approach, up to 99 % cyclohexanone conversion was achieved in the presence of hydrogen gas. In the first stage, catalytic activities of NbOPO 4 , Al 2 O 3 , SiO 2 , and ZrO 2 -SiO 2 to promote aldol condensation were tested at 160 °C for 3 h. The NbOPO 4 exhibited the highest selectivity towards C-C coupling adducts with mainly C 12 to C 18 . In the second stage, 30 wt% Ni catalysts on three different supports and 5 wt% Pd/Al 2 O 3 were used to catalyse the hydrogenation of the first-stage adducts at 300 °C for 3 h. The 30 wt%Ni/NbOPO 4 was most effective, promoting the formation of bi-cycloalkanes, alkyl aromatic, and partially hydrogenated polyaromatic hydrocarbons. In comparison, a one-pot two-step approach was tested by sequentially reacting cyclohexanone with hydrogen gas over the two temperatures for 3 h each, using 30 wt%Ni/NbOPO 4 as catalyst. Reacting cyclohexanone with 10 wt% bio-oil samples led to significantly reduced first stage conversion, and enhanced yields of single C-C coupled oxygenates and almost no hydrocarbons in the second stage. Overall, combination of catalysts and hydrogen gas over staged reactions has effectively converted pure cyclohexanone into naphthene-rich liquid hydrocarbons and cyclohexanone/bio-oil mixed feedstocks into their oxygenated precursors. These results support potential targeted production of bio-derived sustainable alternative fuels for the defossilisation of aviation industry

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Publication Details

Journal
Chemical Engineering Journal
Published
2025-03-11
DOI
https://doi.org/10.1016/j.cej.2025.161494
Citations
15
Primary Topic
Catalysis for Biomass Conversion
Type
article
Field-Weighted Citation Impact
10.11
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article

Energy-dense sustainable aviation fuel-range hydrocarbons from cyclohexanone as a biomass-derived feedstock via sequential catalytic aldol condensation and hydrodeoxygenation

Abarasi Hart, Jude A. Onwudili, Eyüp Yıldırır, Seyed Emad Hashemnezhad
15 citations
Chemical Engineering Journal
Catalysis for Biomass Conversion
10.11
article

Energy-dense sustainable aviation fuel-range hydrocarbons from cyclohexanone as a biomass-derived feedstock via sequential catalytic aldol condensation and hydrodeoxygenation

Abarasi Hart, Jude A. Onwudili, Eyüp Yıldırır, Seyed Emad Hashemnezhad
article en
15 citations

Abstract

• Biomass-derivable cyclohexanone as a feedstock for high-density aviation fuel. • NbOPO 4 catalyst exhibited excellent activity for aldol condensation and alkylation. • Ni/NbOPO 4 catalyst exhibited superior hydrogenation of adducts than Pd/Al 2 O 3. • Similar results from one-pot and two-pot aldol-condensation followed hydrogenation. • Liquid compositions linked to types of coke/char deposits observed on catalyst. Climate change is the main driver for sustainable aviation fuels production as a means of decarbonising/defossilising the sector. In this work, several catalysts have been screened to produce aviation fuel (C 6 -C 16 ) component hydrocarbons from cyclohexanone, a model compound of lignin-derived bio-oils. Using a two-stage two-pot approach, up to 99 % cyclohexanone conversion was achieved in the presence of hydrogen gas. In the first stage, catalytic activities of NbOPO 4 , Al 2 O 3 , SiO 2 , and ZrO 2 -SiO 2 to promote aldol condensation were tested at 160 °C for 3 h. The NbOPO 4 exhibited the highest selectivity towards C-C coupling adducts with mainly C 12 to C 18 . In the second stage, 30 wt% Ni catalysts on three different supports and 5 wt% Pd/Al 2 O 3 were used to catalyse the hydrogenation of the first-stage adducts at 300 °C for 3 h. The 30 wt%Ni/NbOPO 4 was most effective, promoting the formation of bi-cycloalkanes, alkyl aromatic, and partially hydrogenated polyaromatic hydrocarbons. In comparison, a one-pot two-step approach was tested by sequentially reacting cyclohexanone with hydrogen gas over the two temperatures for 3 h each, using 30 wt%Ni/NbOPO 4 as catalyst. Reacting cyclohexanone with 10 wt% bio-oil samples led to significantly reduced first stage conversion, and enhanced yields of single C-C coupled oxygenates and almost no hydrocarbons in the second stage. Overall, combination of catalysts and hydrogen gas over staged reactions has effectively converted pure cyclohexanone into naphthene-rich liquid hydrocarbons and cyclohexanone/bio-oil mixed feedstocks into their oxygenated precursors. These results support potential targeted production of bio-derived sustainable alternative fuels for the defossilisation of aviation industry

Chemical Engineering JournalVol. 509
Aston University (GB)
Responsible consumption and production
Openalex Percentile: Top 1%
Catalysis for Biomass Conversion
10.11
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