| Title: | Kinetic modelling of catalytic 5-hydroxymethylfurfural hydrogenation to value-added chemicals : doctoral dissertation |
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| Authors: | ID Pomeroy, Brett (Author)
ID Likozar, Blaž (Mentor) More about this mentor...  |
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| Files: |  DOK_Pomeroy_Brett_2024.pdf (12,16 MB)
MD5: D721BC84C2E13845F7DF0CF4D94910C4
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| Language: | English |
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| Work type: | Doctoral dissertation |
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| Typology: | 2.08 - Doctoral Dissertation |
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| Organization: | FKKT - Faculty of Chemistry and Chemical Engineering
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| Abstract: | Lignocellulosic biomass has been widely recognized as a renewable feedstock that has enormous potential for the production of bio-based fuels and platform chemicals. Obtained from the dehydration of sugars, 5-hydroxymethylfurfural (HMF) in particular has received extensive consideration due to its diverse functionality and versatility. However, despite its potential, major technical and economic challenges still need to be addressed before HMF valorization technologies can be competitive with current processes that rely on fossil fuels.
This doctoral study specifically focuses on the catalytic hydrogenation of HMF into various platform chemicals while utilizing nickel-based catalysts. The overall goal of this dissertation is to advance these technologies through innovative catalyst design and catalyst characterization techniques that allowed for a systematic investigation into the major catalyst surface properties that influence activity and product selectivity. Various characterization techniques were applied to acquire relevant catalyst surface and structural properties including temperature-programmed reduction, temperature-programmed desorption, X-ray powder diffraction, and transition electron microscopy, N2 physisorption, and diffuse reflectance infrared Fourier transform spectroscopy. A detailed kinetic model was also established that takes into account the number of metallic active sites that provides comparative kinetic parameters to better understand catalyst activity.
The main discoveries obtained during this doctoral thesis include the determination of the critical influence that the support material has on catalyst activity and tuning the reaction network. Particularly, it was found that carbon as a relatively neutral support was effective for hydrodeoxygenation, however, an alumina support was necessary to activate the furan ring and facilitate ring saturation and ring opening reactions. The solvent system was also found to be impactful where incorporating water as a co-solvent completely eliminated all dehydration side reactions. Structural-activity correlations indicate that both acid and basic active sites could play a pivotal role in dictating between the two competing reactions of ring saturation and ring opening. The results presented in this doctoral dissertation provide crucial details for more optimal catalyst design and operating conditions for the effective conversion of 5-hydroxymethylfurfural via hydrogenation for the purpose of advancing sustainable bio-based chemical production. |
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| Keywords: | biomass, catalysis, kinetics, hydrogenation, 5-hydroxymethylfurfural |
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| Place of publishing: | Maribor |
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| Place of performance: | Maribor |
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| Publisher: | [B. Pomeroy] |
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| Year of publishing: | 2024 |
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| Number of pages: | XV, 139 str. |
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| PID: | 20.500.12556/DKUM-86593 |
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| UDC: | 544.4:66.094.25(043.3) |
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| COBISS.SI-ID: | 208207107 |
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| Publication date in DKUM: | 19.09.2024 |
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| Views: | 182 |
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| Downloads: | 35 |
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| Metadata: |    |
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| Categories: | KTFMB - FKKT
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