This thesis progresses from a ‘science and technology studies’ (STS) perspective to consider the ways that expert stakeholders perceive and communicate uncertainties and risks attached to carbon dioxide (CO2) capture and storage (CCS) research and development, and how this compares with policy framings and regulatory requirements. The work largely falls within the constructivist tradition in sociology, but also draws on literature from the philosophy of science and policy-­‐oriented literature on risk and uncertainty. CCS describes a greenhouse gas (GHG) mitigation technology system that involves the capture, pressurisation, transportation, geological injection and long-­‐term storage of CO2 as an alternative to atmospheric emissions. Only few and relatively small applications exist at the moment and research efforts are on going in many countries. The case for developing CCS towards large-­‐scale, commercial deployment has largely been presented as follows since the mid-­‐ 1990s: climate change mitigation is the developed world’s historical responsibility and must be addressed urgently; chief amongst GHGs is CO2, which makes up more than three quarters of emissions; the vast majority of CO2 is emitted from the combustion and gasification of hydrocarbons – oil, gas and coal – for energy generation; transitioning away from these high-­‐CO2 primary energy sources will likely take several decades at the least; therefore, CO2 capture systems should be designed for power and industrial emissions in developed countries, as well as emerging economies where energy suppliers will continue to construct relatively cheap and well understood high-­‐CO2 generation plants. The development of large-­‐scale CO2 capture has thus arisen from a concern with engineering a technological system to address a CO2 legacy in the developed world, and a high-­‐CO2 trajectory in developing/emerging countries, rather than on the back of purely scientific curiosity. And the potential for large-­‐scale development has been presented on the back of a variety of scientific and technical evidence, as well as the urgency of the policy objective and related aims. Research activities, often concentrated around technology demonstration projects, are the primary focus of the first part of this thesis. In the second part I consider the extent to which research has shaped policy developments, and how regulations have subsequently informed a more detailed research agenda. I follow a ‘grounded theory’ methodology as developed by Glaser and Strauss (1967) and take additional guidance from Glaser’s (1992) response to Strauss’ later writings as well as Charmaz (2006) and Rennie (2000), and use a mix of qualitative and quantitative analytical methods to assess my data. These include information from 60 semi-­‐structured interviews with geoscientists and policy stakeholders; close readings of scientific publications, newspaper articles, policies and regulatory documents; statistical evidence from a small survey; quantitative analysis of newspaper articles; and social network analysis (SNA) of scientific co-­‐authorship networks. Theory is drawn from STS literature that has been appropriate to address case study materials across each of the 7 substantive chapters. The first section of the thesis considers expert claims, with a focus on geoscience research, and draws on literature from the closely related ‘social shaping of technology’ (SCOT) and ‘sociology of scientific knowledge’ (SSK) programmes, as well as Nancy Cartwright’s philosophy of science. The second half of the thesis draws on the ‘co-­‐production’ framework and Wynne’s (1992) terminology of risk and uncertainty, to assess relations between risk assessment and risk management practices for CCS. I likewise draw on literature from the ‘incrementalist’ tradition in STS to ask whether and how understandings of technology risk, governance and deployment could be improved. Each chapter presents new empirical material analysed with distinct reference to theories covered in the introduction. Chapter 2 provides a general overview of the history, technology, economics and key regulatory issues associated with CCS, which will be useful to assess the theoretically driven arguments in subsequent chapters. Chapter 3 draws on the concept of ‘interpretive flexibility’ (Pinch and Bijker 1984) to assess a range of expert perceptions about uncertainties in science, technology and policy, and I develop a substantive explanation, ‘conditional inevitability’, to account for an epistemic tension between expressions of certitude and the simultaneous acknowledgement of several uncertainties. Chapter 4 continues the enquiry into stakeholder perceptions and draws on Haas’ notion of ‘epistemic communities’ (Haas 1992) to assess geoscientists’ work practices. I complement this framing with a close look at how uncertainty is treated in simulation modelling and how conclusions about storage safety are formulated, by drawing on Nancy Cartwright’s philosophy of science (Cartwright 1999) and Paul Edwards’ account of complex system modelling for climate change (Edwards 2010). The chapter shows how shared understandings of adequate evidence and common analytical tools have been leveraged to present relatively bounded and simple conclusions about storage safety, while geoscientists nevertheless recognise a high degree of uncertainty and contingency in analyses and results. Chapter 5 continues the focus on knowledge production in the geosciences and is supported by SNA data of workflow patterns in the Sleipner demonstration project. The analysis shows how a few actors have had a pivotal role in developing insights related to storage safety particularly on the back of seismic monitoring and other data acquired through industry partnerships. I therefore continue the chapter with a deconstruction of how seismic data has been used to make a case for the safety of CO2 storage, again drawing on Cartwright and others (Glymour 1983) to explain how individual findings are ‘bootstrapped’ when conclusions are formulated. I show how a general case about storage safety has emerged on the back of seismic data from Sleipner as well as a shared understanding among geoscientists of how to account for uncertainties and arrive at probable explanations. Chapter 6 considers to what extent scientific research has given shape to, and in turn been shaped by, CCS policy and regulations in the EU, drawing on Wynne’s (1992) terminology of risk and uncertainty as well as legal scholarship (Heyvaert 2011). I conclude that a ‘rational-­‐instrumental’ interpretation of uncertainty and precaution has furnished a compartmentalised understanding of risk assessment and risk management practices. Chapter 7 continues to look at the ways that risk assessment methodologies influence risk management practices through a case study of the Mongstad CCS demonstration project in Norway. I draw on ‘incrementalist’ literature (Lindblom 1979; Woodhouse and Collingridge 1993) to consider alternative conceptualisations of technology development and risk management when expectations clash with scientific uncertainties and criticism. Chapter 8 draws on insights from across STS (Downs 1972; Collingridge and Reeve 1986; Wynne 1992) to create a novel conceptual model that accounts for recent years’ developments in CCS governance. Here I conclude that setbacks and criticisms should be expected when analyses have largely presented CCS as a technical problem rather than a socially contingent system. Following Stirling (2010) I conclude that scientists and policymakers should instead strive to present complexity in their analyses and to engage with wider publics (Yearley 2006) when technical analysis is inseparable from socially mediated indeterminacies (Wynne 1992), to increase the chance of more successful engagement practices (Wynne 2006). The conclusions at the end of the thesis seek to draw out interpretive and instrumental lessons learned throughout.

Growing concerns about climate change and the inevitable depletion of fossil fuel resources have led to an increased focus on renewable energy technologies and reducing GHG emissions. Limiting the atmospheric level of CO2 is essential to prevent the most damaging effects of climate change. Among renewable energy resources, biomass combustion has the largest potential to contribute to global energy demands, however it is considered to be a carbon neutral solution and so only limits CO2 concentrations rather than reducing them. Through pyrolysis rather than combustion, biomass can lead to carbon negative liquid, gaseous and solid fuels while also offering a route for long term carbon storage in the form of biochar. Biochar is a carbonaceous material which has shown potential for improving soil fertility, reducing GHG emissions and most importantly long term C storage in the environment. However many questions still remain unanswered with regard to biochar, especially the influence that process conditions can have on its performance in soil as well as any potential trade-offs between soil amendment, C sequestration and heat/power generation. This thesis is therefore focused on assessing the influence that process conditions and feedstock selection have on biochar properties related to carbon stabilisation, improving soil fertility (functional properties) as well as the distribution of energy amongst the pyrolysis co-products. To achieve this, a systematic set of biochar samples was produced, using a wide range of pyrolysis parameters (highest treatment temperature (HTT), heating rate, residence time, carrier gas flow rate and feedstock type), and analysed for physicochemical and functional properties. Pyrolysis HTT consistently showed a dominant influence on determining the final yields and properties of biochar, while the effect of other production parameters was varied. In this thesis the candidate first studied the effect that process conditions had on the long term stability of biochar, as an important indicator of its ability to sequester carbon. While increasing the HTT resulted in a decrease in biochar yield, overall the yield of stable-C increased with temperature. This meant that by applying a higher HTT during pyrolysis a higher C sequestration potential for biochar was achieved. Next to be examined was the influence that process conditions had on other functional properties (labile-C yield, biochar pH, extractable nutrients and cation exchange capacity (CEC)) was then examined. The labile-C yield of biochar decreased with increasing HTT due to the release of volatile matter, while the CEC and concentration of extractable nutrients tended to be higher in biochar produced at 450oC rather than greater HTTs. Biochar pH was also highly alkaline at elevated HTT. This indicated that while high HTT favoured C sequestration and biochar pH, lower HTT may be more favourable for other functional properties. Furthermore by assessing the mass and energy distribution amongst the solid, liquid and gaseous fractions, it was possible to determine the energy balance of the process and through this evaluate the trade-off between the C sequestration potential of biochar and the energy output of the liquid and gas fractions. As the severity of pyrolysis was raised, the total energy stored within the liquid and gaseous co-products increased at the expense of the energy content of biochar, therefore increasing the available energy output of the system and reducing the energy lost when using biochar for carbon storage rather than for bioenergy. This also demonstrated that the pyrolysis process could be fine-tuned to increase the amount of stored C while also improving the heat/power generation of the system. The higher energy content of the gas stream at elevated HTT was also seen to contain sufficient energy to sustain the pyrolysis process, which would free up the solid and liquid fractions for higher value applications while reducing the necessity for external fuel sources. Finally, the data set was used to produce statistical models enabling the prediction of biochar stable-C yield as well as the heating value of biochar. The results of this thesis therefore demonstrate that through applying high HTT the potential energy output of the pyrolysis system can be increased while producing a biochar product with high C sequestration potential and positive functional properties for soil amendment. Due to potential trade-offs, the final choice of process conditions and feedstock would then be made based on the specific requirements of a selected site for biochar application. Understanding the influence that production conditions have on the functional properties of biochar as well as the energy balance of the system is critical to developing specifically engineered bespoke biochar, be it for agricultural use, carbon storage, energy generation or combinations of the three.

This thesis has addressed several gaps in the knowledge with regards to the calcium looping cycle for carbon dioxide capture, including identification of engineering challenges associated with the scale-up of the technology to pilot scale and beyond; assessment of changes in sorbent morphology during the pilot scale capture process; and partitioning of elemental impurities in the limestone between the solid and gaseous phase during the carbon dioxide capture process. Hydrodynamic investigations identified the optimum superficial velocities required for the reactor in order to optimise solids entrainment and flux, and to minimise gas bypassing. Estimations made in determining how particle attrition would affect minimum fluidisation velocity confirmed a decrease of approximately 0.09m/s for every 5 % reduction in particle size. Amendments made to the exhaust diameter and position, and the loop seals, improved the pressure balance of the system thus enhancing solids transfer. Reactor and process modifications, including modification of carbonator temperature, and maintenance of temperature above 420°C in standpipes resulted in improved carbon dioxide capture %. Increasing bed inventory had a positive effect of carbon dioxide capture % due to an increased Ca looping ratio. Steam addition also benefitted the carbonation process, due to improved sorbent morphology and therefore carbon dioxide diffusion into the sorbent. Sulfur dioxide was considered to have a detrimental effect on carbon dioxide capture due to pore pluggage, although burner- derived steam had a positive effect in maintaining capture %. Gaseous elemental emissions from the process were low for all elements, but concentrations of elements in the solid sorbent phase were influenced by bed inventory, implying that filtering systems may be required in industry for the large masses of sorbent required. Concentrations of elements in the sorbent were identified to be below levels typical of cement, with the exception of Ni, implying that there is potential for spent sorbent to be used in the cement industry with adequate mitigation measures in place.

published_or_final_version / abstract / Physics / Doctoral / Doctor of Philosophy

New phosphonium and ammonium ionic liquids were prepared for use in two green applications. Ionic liquids are generating considerable current interest as media for electrochemical processes such as electrodeposition, which can be used to create thin films of a variety of compounds. For the first time, silicon deposition has been achieved in the phosphonium ionic liquid triethyl(2-methoxyethyl)phosphonium bis(trifluoromethylsulfonyl)amide (P201-TFSI). Subsequently, silicon has been deposited from a wide variety of precursors in order to optimize the thickness and morphology of the deposited films. The silicon films electrodeposited in the phosphonium ionic liquid show marked differences from those deposited in organic solvents, imidizolium and pyrrolidinium based ionic liquids. Phosphonium and ammonium ionic liquids were also investigated for use in carbon dioxide capture. Task-specific ionic liquids have shown great promise as agents for the physisorption and chemisorption of CO2 from combustion gas streams. Efforts to synthesize new task specific ionic liquids with multiple amine functionalities for CO2 capture are reported. Four different reaction pathways were explored for the synthesis of these materials. While this goal was not achieved in this work, task-specific phosphonium and ammonium ionic liquids offer the promise of opening up new areas in ionic liquid research. / text

Two Inattentional Blindness type experiments involving 446 participants were performed in order to examine how unexpected objects are noticed. Perception of these unexpected objects was measured using explicit and implicit measurements. Despite initial difficulty in determining implicit perception, results showed a dissociation between implicit measurements and explicit measurements, providing strong evidence for unconscious processing. Research into attention capture often emphasizes the role of either expectations or stimulus properties in attention capture; the current research examines both. Critical objects presented were either of a colour that participants were familiar with, or of a new colour. The different patterns of results for these two categories of objects provide evidence for two separate mechanisms of attention capture: a parallel process driven by the features of objects, and a serial process, driven by the intentions of the observer. Predications of the recent theoretical work produced by Most, Scholl, Clifford & Simons, (2005) are examined, and support is obtained for their theoretical formulation.

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The purpose of this investigation was to study the radiations of the 169/Tm nucleus as it de-excites after the electron capture decay of the 169/Yb. Numerous unreported gammas were present in the sample. The origins of these gamma rays were found.