Preparation and Characterisation of Ionic Liquids and Investigations into their Potential use in the Absorption and Sequestration of Carbon Dioxide

The first area of the research presented in this thesis pertains to the synthesis and characterisation of novel ionic liquids. Three distinct categories of ionic liquids were synthesised, two of which are imidazolium based, with the latter category based on the phosphonium cations. The first category consist of cations which contain two N-heterocyclic rings and these are combined with a range of conventional anions such as bis(triflimide) and dicyanamide. The second category utilise the same cations but have amino acids as the anion in their carboxylate form, introducing NH2 functionality into the ionic liquids and as such can be used in CO2 absorption investigations. The last category of ionic liquids, are those which contain a phosphonium cation (trioctyl) quaternised with a number of groups containing different functionalities for different potential applications. In particular a pyrrole functionalised quaternary phosphonium salt was successfully polymerised. The novel ionic liquids were employed in two main areas of investigation. Imidazolium ionic liquids containing conventional anions were immobilised onto a polymeric support, after which gases which are found in flue gas systems such as CO2 and N2, are passed through the membrane. The gases pass through at different rates due to the differing affinity of the liquids for the individual gases and as such separation of the gases is possible. These preliminary comparative permeability studies were confined to the first category of ionic liquids due to their lower viscosity and previous literature precedent of these anion types being used for these systems. Both single and binary ionic liquid systems were examined throughout the course of the investigation with the binary systems exhibiting some benefits in CO2/N2 selectivity. Amino acid ionic liquids were immobilised onto a mesoporous silica (MCM-41) and their CO2 absorption capability was investigated. These contained NH2 functionality and as such are capable of CO2 absorption through the formation of a carbamate species. The low volatility of the ionic liquids compared to amines, such as monoethanolamine (MEA), which are currently used in CO2 gas capture technologies, make them an attractive area of research. A preliminary operational evaluation was conducted to examine anionic and cationic effects, as well as temperature and ionic liquid content of the impregnated MCM-41 silica

Preparation and Characterisation of Ionic Liquids and Investigations into their Potential use in the Absorption and Sequestration of Carbon Dioxide

The first area of the research presented in this thesis pertains to the synthesis and characterisation of novel ionic liquids. Three distinct categories of ionic liquids were synthesised, two of which are imidazolium based, with the latter category based on the phosphonium cations. The first category consist of cations which contain two N-heterocyclic rings and these are combined with a range of conventional anions such as bis(triflimide) and dicyanamide. The second category utilise the same cations but have amino acids as the anion in their carboxylate form, introducing NH2 functionality into the ionic liquids and as such can be used in CO2 absorption investigations. The last category of ionic liquids, are those which contain a phosphonium cation (trioctyl) quaternised with a number of groups containing different functionalities for different potential applications. In particular a pyrrole functionalised quaternary phosphonium salt was successfully polymerised. The novel ionic liquids were employed in two main areas of investigation. Imidazolium ionic liquids containing conventional anions were immobilised onto a polymeric support, after which gases which are found in flue gas systems such as CO2 and N2, are passed through the membrane. The gases pass through at different rates due to the differing affinity of the liquids for the individual gases and as such separation of the gases is possible. These preliminary comparative permeability studies were confined to the first category of ionic liquids due to their lower viscosity and previous literature precedent of these anion types being used for these systems. Both single and binary ionic liquid systems were examined throughout the course of the investigation with the binary systems exhibiting some benefits in CO2/N2 selectivity. Amino acid ionic liquids were immobilised onto a mesoporous silica (MCM-41) and their CO2 absorption capability was investigated. These contained NH2 functionality and as such are capable of CO2 absorption through the formation of a carbamate species. The low volatility of the ionic liquids compared to amines, such as monoethanolamine (MEA), which are currently used in CO2 gas capture technologies, make them an attractive area of research. A preliminary operational evaluation was conducted to examine anionic and cationic effects, as well as temperature and ionic liquid content of the impregnated MCM-41 silica

Preparation and Characterisation of Ionic Liquids and Investigations into their Potential use in the Absorption and Sequestration of Carbon Dioxide

The first area of the research presented in this thesis pertains to the synthesis and characterisation of novel ionic liquids. Three distinct categories of ionic liquids were synthesised, two of which are imidazolium based, with the latter category based on the phosphonium cations. The first category consist of cations which contain two N-heterocyclic rings and these are combined with a range of conventional anions such as bis(triflimide) and dicyanamide. The second category utilise the same cations but have amino acids as the anion in their carboxylate form, introducing NH2 functionality into the ionic liquids and as such can be used in CO2 absorption investigations. The last category of ionic liquids, are those which contain a phosphonium cation (trioctyl) quaternised with a number of groups containing different functionalities for different potential applications. In particular a pyrrole functionalised quaternary phosphonium salt was successfully polymerised. The novel ionic liquids were employed in two main areas of investigation. Imidazolium ionic liquids containing conventional anions were immobilised onto a polymeric support, after which gases which are found in flue gas systems such as CO2 and N2, are passed through the membrane. The gases pass through at different rates due to the differing affinity of the liquids for the individual gases and as such separation of the gases is possible. These preliminary comparative permeability studies were confined to the first category of ionic liquids due to their lower viscosity and previous literature precedent of these anion types being used for these systems. Both single and binary ionic liquid systems were examined throughout the course of the investigation with the binary systems exhibiting some benefits in CO2/N2 selectivity. Amino acid ionic liquids were immobilised onto a mesoporous silica (MCM-41) and their CO2 absorption capability was investigated. These contained NH2 functionality and as such are capable of CO2 absorption through the formation of a carbamate species. The low volatility of the ionic liquids compared to amines, such as monoethanolamine (MEA), which are currently used in CO2 gas capture technologies, make them an attractive area of research. A preliminary operational evaluation was conducted to examine anionic and cationic effects, as well as temperature and ionic liquid content of the impregnated MCM-41 silica

Preparation and Characterisation of Ionic Liquids and Investigations into their Potential use in the Absorption and Sequestration of Carbon Dioxide

The first area of the research presented in this thesis pertains to the synthesis and characterisation of novel ionic liquids. Three distinct categories of ionic liquids were synthesised, two of which are imidazolium based, with the latter category based on the phosphonium cations. The first category consist of cations which contain two N-heterocyclic rings and these are combined with a range of conventional anions such as bis(triflimide) and dicyanamide. The second category utilise the same cations but have amino acids as the anion in their carboxylate form, introducing NH2 functionality into the ionic liquids and as such can be used in CO2 absorption investigations. The last category of ionic liquids, are those which contain a phosphonium cation (trioctyl) quaternised with a number of groups containing different functionalities for different potential applications. In particular a pyrrole functionalised quaternary phosphonium salt was successfully polymerised. The novel ionic liquids were employed in two main areas of investigation. Imidazolium ionic liquids containing conventional anions were immobilised onto a polymeric support, after which gases which are found in flue gas systems such as CO2 and N2, are passed through the membrane. The gases pass through at different rates due to the differing affinity of the liquids for the individual gases and as such separation of the gases is possible. These preliminary comparative permeability studies were confined to the first category of ionic liquids due to their lower viscosity and previous literature precedent of these anion types being used for these systems. Both single and binary ionic liquid systems were examined throughout the course of the investigation with the binary systems exhibiting some benefits in CO2/N2 selectivity. Amino acid ionic liquids were immobilised onto a mesoporous silica (MCM-41) and their CO2 absorption capability was investigated. These contained NH2 functionality and as such are capable of CO2 absorption through the formation of a carbamate species. The low volatility of the ionic liquids compared to amines, such as monoethanolamine (MEA), which are currently used in CO2 gas capture technologies, make them an attractive area of research. A preliminary operational evaluation was conducted to examine anionic and cationic effects, as well as temperature and ionic liquid content of the impregnated MCM-41 silica

Highly-parallelized simulation of a pixelated LArTPC on a GPU

The rapid development of general-purpose computing on graphics processing units (GPGPU) is allowing the implementation of highly-parallelized Monte Carlo simulation chains for particle physics experiments. This technique is particularly suitable for the simulation of a pixelated charge readout for time projection chambers, given the large number of channels that this technology employs. Here we present the first implementation of a full microphysical simulator of a liquid argon time projection chamber (LArTPC) equipped with light readout and pixelated charge readout, developed for the DUNE Near Detector. The software is implemented with an end-to-end set of GPU-optimized algorithms. The algorithms have been written in Python and translated into CUDA kernels using Numba, a just-in-time compiler for a subset of Python and NumPy instructions. The GPU implementation achieves a speed up of four orders of magnitude compared with the equivalent CPU version. The simulation of the current induced on $10^3$ pixels takes around 1 ms on the GPU, compared with approximately 10 s on the CPU. The results of the simulation are compared against data from a pixel-readout LArTPC prototype

The DUNE Far Detector Vertical Drift Technology, Technical Design Report

International audienceDUNE is an international experiment dedicated to addressing some of the questions at the forefront of particle physics and astrophysics, including the mystifying preponderance of matter over antimatter in the early universe. The dual-site experiment will employ an intense neutrino beam focused on a near and a far detector as it aims to determine the neutrino mass hierarchy and to make high-precision measurements of the PMNS matrix parameters, including the CP-violating phase. It will also stand ready to observe supernova neutrino bursts, and seeks to observe nucleon decay as a signature of a grand unified theory underlying the standard model. The DUNE far detector implements liquid argon time-projection chamber (LArTPC) technology, and combines the many tens-of-kiloton fiducial mass necessary for rare event searches with the sub-centimeter spatial resolution required to image those events with high precision. The addition of a photon detection system enhances physics capabilities for all DUNE physics drivers and opens prospects for further physics explorations. Given its size, the far detector will be implemented as a set of modules, with LArTPC designs that differ from one another as newer technologies arise. In the vertical drift LArTPC design, a horizontal cathode bisects the detector, creating two stacked drift volumes in which ionization charges drift towards anodes at either the top or bottom. The anodes are composed of perforated PCB layers with conductive strips, enabling reconstruction in 3D. Light-trap-style photon detection modules are placed both on the cryostat's side walls and on the central cathode where they are optically powered. This Technical Design Report describes in detail the technical implementations of each subsystem of this LArTPC that, together with the other far detector modules and the near detector, will enable DUNE to achieve its physics goals

The DUNE Far Detector Vertical Drift Technology, Technical Design Report

International audienceDUNE is an international experiment dedicated to addressing some of the questions at the forefront of particle physics and astrophysics, including the mystifying preponderance of matter over antimatter in the early universe. The dual-site experiment will employ an intense neutrino beam focused on a near and a far detector as it aims to determine the neutrino mass hierarchy and to make high-precision measurements of the PMNS matrix parameters, including the CP-violating phase. It will also stand ready to observe supernova neutrino bursts, and seeks to observe nucleon decay as a signature of a grand unified theory underlying the standard model. The DUNE far detector implements liquid argon time-projection chamber (LArTPC) technology, and combines the many tens-of-kiloton fiducial mass necessary for rare event searches with the sub-centimeter spatial resolution required to image those events with high precision. The addition of a photon detection system enhances physics capabilities for all DUNE physics drivers and opens prospects for further physics explorations. Given its size, the far detector will be implemented as a set of modules, with LArTPC designs that differ from one another as newer technologies arise. In the vertical drift LArTPC design, a horizontal cathode bisects the detector, creating two stacked drift volumes in which ionization charges drift towards anodes at either the top or bottom. The anodes are composed of perforated PCB layers with conductive strips, enabling reconstruction in 3D. Light-trap-style photon detection modules are placed both on the cryostat's side walls and on the central cathode where they are optically powered. This Technical Design Report describes in detail the technical implementations of each subsystem of this LArTPC that, together with the other far detector modules and the near detector, will enable DUNE to achieve its physics goals

Highly-parallelized simulation of a pixelated LArTPC on a GPU

The rapid development of general-purpose computing on graphics processing units (GPGPU) is allowing the implementation of highly-parallelized Monte Carlo simulation chains for particle physics experiments. This technique is particularly suitable for the simulation of a pixelated charge readout for time projection chambers, given the large number of channels that this technology employs. Here we present the first implementation of a full microphysical simulator of a liquid argon time projection chamber (LArTPC) equipped with light readout and pixelated charge readout, developed for the DUNE Near Detector. The software is implemented with an end-to-end set of GPU-optimized algorithms. The algorithms have been written in Python and translated into CUDA kernels using Numba, a just-in-time compiler for a subset of Python and NumPy instructions. The GPU implementation achieves a speed up of four orders of magnitude compared with the equivalent CPU version. The simulation of the current induced on $10^3$ pixels takes around 1 ms on the GPU, compared with approximately 10 s on the CPU. The results of the simulation are compared against data from a pixel-readout LArTPC prototype

The DUNE Far Detector Vertical Drift Technology, Technical Design Report

DUNE is an international experiment dedicated to addressing some of the questions at the forefront of particle physics and astrophysics, including the mystifying preponderance of matter over antimatter in the early universe. The dual-site experiment will employ an intense neutrino beam focused on a near and a far detector as it aims to determine the neutrino mass hierarchy and to make high-precision measurements of the PMNS matrix parameters, including the CP-violating phase. It will also stand ready to observe supernova neutrino bursts, and seeks to observe nucleon decay as a signature of a grand unified theory underlying the standard model. The DUNE far detector implements liquid argon time-projection chamber (LArTPC) technology, and combines the many tens-of-kiloton fiducial mass necessary for rare event searches with the sub-centimeter spatial resolution required to image those events with high precision. The addition of a photon detection system enhances physics capabilities for all DUNE physics drivers and opens prospects for further physics explorations. Given its size, the far detector will be implemented as a set of modules, with LArTPC designs that differ from one another as newer technologies arise. In the vertical drift LArTPC design, a horizontal cathode bisects the detector, creating two stacked drift volumes in which ionization charges drift towards anodes at either the top or bottom. The anodes are composed of perforated PCB layers with conductive strips, enabling reconstruction in 3D. Light-trap-style photon detection modules are placed both on the cryostat's side walls and on the central cathode where they are optically powered. This Technical Design Report describes in detail the technical implementations of each subsystem of this LArTPC that, together with the other far detector modules and the near detector, will enable DUNE to achieve its physics goals