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Oakley, William (2024) Continuous synthesis and scaled shaping of archetypal metal-organic frameworks for carbon capture applications. PhD thesis, University of Nottingham.

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Abstract

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.

Item Type:	Thesis (University of Nottingham only) (PhD)
Supervisors:	Lester, Edward Grant, David
Keywords:	Metal-organic frameworks; Carbon capture systems
Subjects:	Q Science > QD Chemistry
Faculties/Schools:	UK Campuses > Faculty of Engineering > Department of Chemical and Environmental Engineering
Item ID:	78273
Depositing User:	Oakley, William
Date Deposited:	18 Jul 2024 04:40
Last Modified:	18 Jul 2024 04:40
URI:	https://eprints.nottingham.ac.uk/id/eprint/78273

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