Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications
The research presented in this thesis focuses on the holistic advancement of archetypal metal-organic frameworks (MOFs) towards post-combustion carbon capture applications. Advancements are made to develop continuous synthesis routes for previously batch produced carbon capture frameworks and to pro...
| Main Author: | |
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| Format: | Thesis (University of Nottingham only) |
| Language: | English |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://eprints.nottingham.ac.uk/78273/ |
| _version_ | 1848801064375025664 |
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| author | Oakley, William |
| author_facet | Oakley, William |
| author_sort | Oakley, William |
| building | Nottingham Research Data Repository |
| collection | Online Access |
| description | The research presented in this thesis focuses on the holistic advancement of archetypal metal-organic frameworks (MOFs) towards post-combustion carbon capture applications. Advancements are made to develop continuous synthesis routes for previously batch produced carbon capture frameworks and to produce practical MOF macroscopic structures ready for industrial application. Importantly, where possible these novel methodologies were demonstrated at industrially relevant scales, with examples ranging from multi-gram to multi-kilogram scales achieved. This has enabled the direct utilisation of the materials produced within bespoke carbon capture systems, ranging from bench scale to an industrial pilot unit evaluated in field trials at Drax Power Station.
Chapter 1 starts by discussing the theoretical background behind the impact of CO2 emissions,
followed by detailing the common processes utilised for engineered carbon capture. In line with this
thesis, a literature review covering the current state-of-the-art research from; MOF synthesis and MOF
shaping fields alongside the known challenges to MOF scale up, is presented.
Chapter 2 details the
experimental methodology used for all research described throughout this thesis, in addition to a
background summary on the analytical techniques employed.
Chapter 3 details the use of continuous hydrothermal synthesis of amino functionalised mixed linker
MIL-53(Al), involving a design of experiments assessment of H2BDC-NH2 incorporation into the linker
solution and synthesis temperature upon CO2 adsorption capacity, surface area and space time yield.
Additionally, in-situ FTIR spectroscopy was demonstrated for inline monitoring.
Chapter 4 contains the development of an automated pelletization procedure for the air stable
aluminium fumarate MOF, an isostructural relative of MIL-53(Al). Both binderless and binder
containing approaches were investigated and evaluated, prior to a multi-kilogram scaled demonstration of the binderless pelleting method.
Chapter 5 covers the investigation into the shaping of air sensitive HKUST-1 via air drying of binder
loaded methanolic slurries, to generate cubic monolith structures. This involved the screening and
selection of additive components, a binder and surfactant, followed by loading optimization.
Additionally, assessments into the impact of feedstock variability and geometric mould scaling were
undertaken.
Chapter 6 extends the use of polyvinylpyrrolidone (PVP) loaded methanolic HKUST-1 slurries towards
the generation of macroscopic coatings upon metallic substrates. These coated components could
then be utilised fortemperature-swing adsorption post-combustion carbon capture. Optimum coating
conditions were applied to varying scales of custom-built finned heat exchangers. Additionally, both
shaping procedures developed in Chapters 5/6 were utilised in a pilot scale (20.5 kg HKUST-1_PVP
adsorbent) twin column temperature (vacuum) swing adsorption post-combustion carbon capture
unit, in collaboration with Promethean Particles and Drax. Preliminary CO2 adsorption tests were
conducted on industrial flue gas at Drax Power Station.
Chapter 7 provides a summary of the work conducted in each chapter followed by a discussion on
potential future work. |
| first_indexed | 2025-11-14T21:01:31Z |
| format | Thesis (University of Nottingham only) |
| id | nottingham-78273 |
| institution | University of Nottingham Malaysia Campus |
| institution_category | Local University |
| language | English |
| last_indexed | 2025-11-14T21:01:31Z |
| publishDate | 2024 |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | nottingham-782732025-02-28T15:21:02Z https://eprints.nottingham.ac.uk/78273/ Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications Oakley, William The research presented in this thesis focuses on the holistic advancement of archetypal metal-organic frameworks (MOFs) towards post-combustion carbon capture applications. Advancements are made to develop continuous synthesis routes for previously batch produced carbon capture frameworks and to produce practical MOF macroscopic structures ready for industrial application. Importantly, where possible these novel methodologies were demonstrated at industrially relevant scales, with examples ranging from multi-gram to multi-kilogram scales achieved. This has enabled the direct utilisation of the materials produced within bespoke carbon capture systems, ranging from bench scale to an industrial pilot unit evaluated in field trials at Drax Power Station. Chapter 1 starts by discussing the theoretical background behind the impact of CO2 emissions, followed by detailing the common processes utilised for engineered carbon capture. In line with this thesis, a literature review covering the current state-of-the-art research from; MOF synthesis and MOF shaping fields alongside the known challenges to MOF scale up, is presented. Chapter 2 details the experimental methodology used for all research described throughout this thesis, in addition to a background summary on the analytical techniques employed. Chapter 3 details the use of continuous hydrothermal synthesis of amino functionalised mixed linker MIL-53(Al), involving a design of experiments assessment of H2BDC-NH2 incorporation into the linker solution and synthesis temperature upon CO2 adsorption capacity, surface area and space time yield. Additionally, in-situ FTIR spectroscopy was demonstrated for inline monitoring. Chapter 4 contains the development of an automated pelletization procedure for the air stable aluminium fumarate MOF, an isostructural relative of MIL-53(Al). Both binderless and binder containing approaches were investigated and evaluated, prior to a multi-kilogram scaled demonstration of the binderless pelleting method. Chapter 5 covers the investigation into the shaping of air sensitive HKUST-1 via air drying of binder loaded methanolic slurries, to generate cubic monolith structures. This involved the screening and selection of additive components, a binder and surfactant, followed by loading optimization. Additionally, assessments into the impact of feedstock variability and geometric mould scaling were undertaken. Chapter 6 extends the use of polyvinylpyrrolidone (PVP) loaded methanolic HKUST-1 slurries towards the generation of macroscopic coatings upon metallic substrates. These coated components could then be utilised fortemperature-swing adsorption post-combustion carbon capture. Optimum coating conditions were applied to varying scales of custom-built finned heat exchangers. Additionally, both shaping procedures developed in Chapters 5/6 were utilised in a pilot scale (20.5 kg HKUST-1_PVP adsorbent) twin column temperature (vacuum) swing adsorption post-combustion carbon capture unit, in collaboration with Promethean Particles and Drax. Preliminary CO2 adsorption tests were conducted on industrial flue gas at Drax Power Station. Chapter 7 provides a summary of the work conducted in each chapter followed by a discussion on potential future work. 2024-07-18 Thesis (University of Nottingham only) NonPeerReviewed application/pdf en cc_by https://eprints.nottingham.ac.uk/78273/1/Continuous%20Synthesis%20and%20Scaled%20Shaping%20of%20Archetypal%20Metal-Organic%20Frameworks%20for%20Carbon%20Capture%20Applications_William%20Oakley_Corrected%20Final_For%20Submission.pdf Oakley, William (2024) Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications. PhD thesis, University of Nottingham. Metal-organic frameworks; Carbon capture systems |
| spellingShingle | Metal-organic frameworks; Carbon capture systems Oakley, William Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| title | Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| title_full | Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| title_fullStr | Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| title_full_unstemmed | Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| title_short | Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| title_sort | continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications |
| topic | Metal-organic frameworks; Carbon capture systems |
| url | https://eprints.nottingham.ac.uk/78273/ |