J.R. van Ommen
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17 records found
1
Granular flow in stirred bed reactors
Insights through radiation-based imaging techniques
In this dissertation, a deeper understanding of granular flow behavior in these reactors was achieved through detailed experimental measurements using radiation-based imaging. Recognizing the direct link between macro-scale flow behavior and particle-scale phenomena, this research spanned both scales. Although the primary focus of this thesis is on a horizontal stirred bed, experiments were also conducted using two additional lab-scale reactor configurations: a vertical stirred bed and a fluidized bed. High-quality data on flow patterns, phase holdup, and particle dynamics were obtained using X-ray imaging and single-photon emission radioactive particle tracking. A key novelty of this research was the use of industrial-grade powders, such as polypropylene reactor powder, as encountered in horizontal stirred bed reactors. The collected data were thoroughly analyzed to identify the key parameters influencing granular flow behavior, utilizing statistical methods and visualization tools to uncover critical insights.
First, the flow behavior of polypropylene reactor powder in a laboratoryscale horizontal stirred bed reactor (HSBR) was investigated using X-ray imaging. It was observed that agitation significantly dictates overall flow behavior and phase holdup in the HSBR. Gas injection through inlet points at the bottom resulted in spouting behavior, and the gas holdup at fixed agitator positions remained highly consistent across successive revolutions. The presence of liquid was found to deteriorate the flow behavior due to liquid bridging at particle contact points, with particle size and surface morphology influencing the powders’ susceptibility to liquid.
Subsequently, a single-photon emission radioactive particle tracking method was presented, allowing the tracking of individual photon-emitting particles to evaluate the hydrodynamics of multiphase flows. This method directly utilized detected photon hit locations to reconstruct the three-dimensional position of the tracer particle, avoiding assumptions in count rate fluctuations. The tracer particle’s position was determined by finding the intersection point of three two-dimensional planes from the detectors, achieving a spatial accuracy of approximately 1 mm through a subsequent calibration experimentation procedure.
Thereafter, the method was employed to characterize the particle dynamics in the HSBR. It was found that, besides the agitator rotation speed, the flow behavior is significantly influenced by the reactor fill level. At low rotation speeds and fill levels, solids motion was primarily induced by impeller blade passage, resulting in semi-static bed motion and poor solids distribution. Increased fill levels and rotation speeds led to continuous solids motion and uniform distribution. Solids circulation, quantified by a dimensionless cycle number, increased with higher fill levels and rotation speeds. The axial dispersion coefficient ranged from 10-6 to 10-5 m2 s-1, increasing with rotation speed, although no conclusive relationship with fill level was observed.
Thereafter, the fluidization behavior of Geldart B particles in a vertical stirred bed reactor was investigated using X-ray imaging, pressure drop measurements, and numerical simulations via Computational Fluid Dynamics (CFD) coupled with Discrete Element Method (DEM) and Immersed Boundary Method (IBM). The experimentally obtained minimum fluidization curve and time-averaged pressure drop showed good qualitative agreement with simulations. Visual observations indicated that increasing the agitator’s angular velocity reduced bubble size and improved bed homogeneity, as evidenced by reduced pressure fluctuations. Simulations revealed that while the impeller enhances solids agitation, a proper design study is essential, as static immersed bodies like the stirrer shaft can adversely impact solids motion.
Finally, the correlation between the fluidization behavior and flow properties of 10 commercially available cohesive powders was experimentally investigated. The fluidization quality of the powders in a laboratory-scale fluidized bed was assessed using a Fluidization Quality Index (FQI), computed by integrating gas holdup and its temporal variation acquired through X-ray imaging. Flowability was measured in a rotating drum operated at high speeds, which aerated the powder bed, a critical factor in correlating fluidization behavior with flow properties. This study established a positive correlation between cohesive powders’ flowability and fluidization quality, suggesting that fast and user-friendly flowability measurements in a rotating drum instrument can predict fluidization potential, aiding in process optimization and enhancing fluidization studies for cohesive powders.
In summary, the insights acquired from this thesis enhance the understanding of flow behavior and phase holdup in stirred bed reactors and cohesive fluidized beds. These findings can serve as a valuable foundation for designing, optimizing, and intensifying systems for the industrial-scale manufacturing of high-quality PP resins. ...
In this dissertation, a deeper understanding of granular flow behavior in these reactors was achieved through detailed experimental measurements using radiation-based imaging. Recognizing the direct link between macro-scale flow behavior and particle-scale phenomena, this research spanned both scales. Although the primary focus of this thesis is on a horizontal stirred bed, experiments were also conducted using two additional lab-scale reactor configurations: a vertical stirred bed and a fluidized bed. High-quality data on flow patterns, phase holdup, and particle dynamics were obtained using X-ray imaging and single-photon emission radioactive particle tracking. A key novelty of this research was the use of industrial-grade powders, such as polypropylene reactor powder, as encountered in horizontal stirred bed reactors. The collected data were thoroughly analyzed to identify the key parameters influencing granular flow behavior, utilizing statistical methods and visualization tools to uncover critical insights.
First, the flow behavior of polypropylene reactor powder in a laboratoryscale horizontal stirred bed reactor (HSBR) was investigated using X-ray imaging. It was observed that agitation significantly dictates overall flow behavior and phase holdup in the HSBR. Gas injection through inlet points at the bottom resulted in spouting behavior, and the gas holdup at fixed agitator positions remained highly consistent across successive revolutions. The presence of liquid was found to deteriorate the flow behavior due to liquid bridging at particle contact points, with particle size and surface morphology influencing the powders’ susceptibility to liquid.
Subsequently, a single-photon emission radioactive particle tracking method was presented, allowing the tracking of individual photon-emitting particles to evaluate the hydrodynamics of multiphase flows. This method directly utilized detected photon hit locations to reconstruct the three-dimensional position of the tracer particle, avoiding assumptions in count rate fluctuations. The tracer particle’s position was determined by finding the intersection point of three two-dimensional planes from the detectors, achieving a spatial accuracy of approximately 1 mm through a subsequent calibration experimentation procedure.
Thereafter, the method was employed to characterize the particle dynamics in the HSBR. It was found that, besides the agitator rotation speed, the flow behavior is significantly influenced by the reactor fill level. At low rotation speeds and fill levels, solids motion was primarily induced by impeller blade passage, resulting in semi-static bed motion and poor solids distribution. Increased fill levels and rotation speeds led to continuous solids motion and uniform distribution. Solids circulation, quantified by a dimensionless cycle number, increased with higher fill levels and rotation speeds. The axial dispersion coefficient ranged from 10-6 to 10-5 m2 s-1, increasing with rotation speed, although no conclusive relationship with fill level was observed.
Thereafter, the fluidization behavior of Geldart B particles in a vertical stirred bed reactor was investigated using X-ray imaging, pressure drop measurements, and numerical simulations via Computational Fluid Dynamics (CFD) coupled with Discrete Element Method (DEM) and Immersed Boundary Method (IBM). The experimentally obtained minimum fluidization curve and time-averaged pressure drop showed good qualitative agreement with simulations. Visual observations indicated that increasing the agitator’s angular velocity reduced bubble size and improved bed homogeneity, as evidenced by reduced pressure fluctuations. Simulations revealed that while the impeller enhances solids agitation, a proper design study is essential, as static immersed bodies like the stirrer shaft can adversely impact solids motion.
Finally, the correlation between the fluidization behavior and flow properties of 10 commercially available cohesive powders was experimentally investigated. The fluidization quality of the powders in a laboratory-scale fluidized bed was assessed using a Fluidization Quality Index (FQI), computed by integrating gas holdup and its temporal variation acquired through X-ray imaging. Flowability was measured in a rotating drum operated at high speeds, which aerated the powder bed, a critical factor in correlating fluidization behavior with flow properties. This study established a positive correlation between cohesive powders’ flowability and fluidization quality, suggesting that fast and user-friendly flowability measurements in a rotating drum instrument can predict fluidization potential, aiding in process optimization and enhancing fluidization studies for cohesive powders.
In summary, the insights acquired from this thesis enhance the understanding of flow behavior and phase holdup in stirred bed reactors and cohesive fluidized beds. These findings can serve as a valuable foundation for designing, optimizing, and intensifying systems for the industrial-scale manufacturing of high-quality PP resins.
This thesis focusses on the role that gas bubbles have on the performance of electrolysers: the formation of gas bubbles is inevitable in most electrolysers, since the common electrolysis products (e.g. H2, O2 or CO) have a poor solubility in water. Controlling the behaviour of gas bubbles offers a pathway to lower the cell voltage or improve the mass transport, which allows operation at higher operating current densities. This could help with decreasing the costs of electrolysers, bringing them closer to competing with fossil fuel-based processes... ...
This thesis focusses on the role that gas bubbles have on the performance of electrolysers: the formation of gas bubbles is inevitable in most electrolysers, since the common electrolysis products (e.g. H2, O2 or CO) have a poor solubility in water. Controlling the behaviour of gas bubbles offers a pathway to lower the cell voltage or improve the mass transport, which allows operation at higher operating current densities. This could help with decreasing the costs of electrolysers, bringing them closer to competing with fossil fuel-based processes...
Insights from operating under gas-liquid Taylor flow and techno-economic optimisation
Reactor design and economics of CO2 electrolysers
In Chapter 2, we propose a tubular electrolyser design operating under gas-liquid Taylor flow to overcome mass transfer limitations. By developing a numerical model, we investigate the relationship between process conditions, mass transfer, and reactor performance. Insights gained from this model allow us to derive an easy-to-use analytical relation to evaluate the impact of changes in inlet flow rates on Faradaic efficiency and current density. We find that long gaseous CO2 bubbles and low velocities enhance the current density towards CO, outperforming traditional H-cells. However, achieving performance comparable to flow-through electrolysers operated with a gas diffusion electrode (GDE) requires means to increase CO2 solubility in the liquid electrolyte, by for example increasing pressure.
Chapter 3 focuses on experimentally testing how Taylor flow influences the electrolyser performance within the established zero-gap water electrolyser concept adapted for CO2 reduction, by employing a silver gauze as the cathode. Our experimental findings reveal that Taylor flow enhances the Faradaic efficiency towards CO compared to single-phase flow, with minimal influence from gas holdup within the studied velocity range. Contrary to the tubular design, high velocities are desirable to increase the Faradaic efficiency towards CO in the rectangular flow channel. We find that further optimisation of
cathode design and fabrication is needed to fully exploit the potential of this electrolyser concept.
In Chapter 4, techno-economic aspects of electrochemical CO2 conversion are addressed, aiming to optimise operational parameters for industrial applications. A multiscale model capturing mass transfer effects over the channel length of a GDE electrolyser is integrated into an economic framework to analyse the interdependencies of key performance variables on the economic outlook. The analysis indicates that optimal current densities may differ significantly from previously reported benchmarks, emphasising the importance of multi–scale modelling for evaluating electrolyser designs under economic considerations. ...
In Chapter 2, we propose a tubular electrolyser design operating under gas-liquid Taylor flow to overcome mass transfer limitations. By developing a numerical model, we investigate the relationship between process conditions, mass transfer, and reactor performance. Insights gained from this model allow us to derive an easy-to-use analytical relation to evaluate the impact of changes in inlet flow rates on Faradaic efficiency and current density. We find that long gaseous CO2 bubbles and low velocities enhance the current density towards CO, outperforming traditional H-cells. However, achieving performance comparable to flow-through electrolysers operated with a gas diffusion electrode (GDE) requires means to increase CO2 solubility in the liquid electrolyte, by for example increasing pressure.
Chapter 3 focuses on experimentally testing how Taylor flow influences the electrolyser performance within the established zero-gap water electrolyser concept adapted for CO2 reduction, by employing a silver gauze as the cathode. Our experimental findings reveal that Taylor flow enhances the Faradaic efficiency towards CO compared to single-phase flow, with minimal influence from gas holdup within the studied velocity range. Contrary to the tubular design, high velocities are desirable to increase the Faradaic efficiency towards CO in the rectangular flow channel. We find that further optimisation of
cathode design and fabrication is needed to fully exploit the potential of this electrolyser concept.
In Chapter 4, techno-economic aspects of electrochemical CO2 conversion are addressed, aiming to optimise operational parameters for industrial applications. A multiscale model capturing mass transfer effects over the channel length of a GDE electrolyser is integrated into an economic framework to analyse the interdependencies of key performance variables on the economic outlook. The analysis indicates that optimal current densities may differ significantly from previously reported benchmarks, emphasising the importance of multi–scale modelling for evaluating electrolyser designs under economic considerations.
This project focuses on identifying the sources of hydrogen emissions from an electrolysis unit. The goal is to comprehend the depth of this potential issue and investigate possible solutions. This project is carried out in collaboration with Worley, a market leader in the design, construction, and delivery of green H2 facilities. The leakage estimates for the green hydrogen alkaline electrolysis plant are based on Worley’s in-house data. Venting during startup and shutdowns when power is unavailable, as well as hydrogen crossover in the electrolyzer, have been identified as two major contributors to hydrogen emissions. Solutions such as flaring systems to combust the vented hydrogen and battery energy systems to reduce frequent shutdowns and startups are investigated. To reduce emissions from hydrogen crossover, a reactor is modeled to explore the catalytic recombination of hydrogen and oxygen. These solutions are subjected to a techno-economic analysis to determine their viability.
Flare systems and battery energy systems are both deemed feasible. In the long
run, however, installing a battery energy system would be preferable to combusting the hydrogen product. In comparison to other battery technologies such as Li-ion and lead-acid batteries, vanadium redox flow battery systems have been found to provide the maximum incentives and highest optimal capacities at the lowest overall costs. To avoid emissions from hydrogen crossover in a low-pressure alkaline electrolysis unit, the most cost-effective design involves a single-stage compression followed by a scrubber, heater, and reactor. However, this design is still costly because the annualized costs are four times greater than the costs offset by emissions reductions per year. Governments can encourage the adoption of such solutions by providing financial incentives to businesses. ...
This project focuses on identifying the sources of hydrogen emissions from an electrolysis unit. The goal is to comprehend the depth of this potential issue and investigate possible solutions. This project is carried out in collaboration with Worley, a market leader in the design, construction, and delivery of green H2 facilities. The leakage estimates for the green hydrogen alkaline electrolysis plant are based on Worley’s in-house data. Venting during startup and shutdowns when power is unavailable, as well as hydrogen crossover in the electrolyzer, have been identified as two major contributors to hydrogen emissions. Solutions such as flaring systems to combust the vented hydrogen and battery energy systems to reduce frequent shutdowns and startups are investigated. To reduce emissions from hydrogen crossover, a reactor is modeled to explore the catalytic recombination of hydrogen and oxygen. These solutions are subjected to a techno-economic analysis to determine their viability.
Flare systems and battery energy systems are both deemed feasible. In the long
run, however, installing a battery energy system would be preferable to combusting the hydrogen product. In comparison to other battery technologies such as Li-ion and lead-acid batteries, vanadium redox flow battery systems have been found to provide the maximum incentives and highest optimal capacities at the lowest overall costs. To avoid emissions from hydrogen crossover in a low-pressure alkaline electrolysis unit, the most cost-effective design involves a single-stage compression followed by a scrubber, heater, and reactor. However, this design is still costly because the annualized costs are four times greater than the costs offset by emissions reductions per year. Governments can encourage the adoption of such solutions by providing financial incentives to businesses.
Large scale utilisation of CO2 in the chemical industry is currently limited to a few applications (e.g. synthesis of urea, carboxylic acids, food industry) and generally requires high purity feedstock. Integrated processes that combine CO2 capture from diluted sources (e.g. industrial flue gases, air) and its conversion to value-added chemicals represent a solution to enhance the utilisation of CO2 and mitigate its emissions. CH4 is an abundant hydrocarbon with diversified sources ranging from fossil-based (natural gas, shale gas) to renewable ones (biomass, biogas), which can potentially substitute oil for the synthesis of valuable chemicals and fuels, including higher hydrocarbons. At the moment, however, CH4 utilisation is circumscribed to combustion for heat and energy production or energy-intensive production of H2 and syngas (H2 + CO) via steam reforming, resulting in a high carbon footprint.
In general, the thermodynamic stability of CO2 and CH4 molecules imposes severe limitations to their exploitation as chemical feedstocks, in terms of low conversion efficiencies and control on the selectivity of products. Their efficient conversion requires harsh reaction conditions (high temperatures and pressures, highly chemically reactive substances) at which the stability of the desired products is threatened, resulting in low selectivity. In this scenario, catalysis is essential to identify functional materials and develop new catalytic processes able to maximise the selective conversion of CO2 and CH4 feedstocks to value-added products.
Unsteady-state operation in catalysis is an option to overcome the thermodynamic constraints imposed by the conventional steady-state operation. Integrated CO2 capture and conversion, sorption-enhanced reactions, chemical looping combustion are examples of intrinsically unsteady-state catalytic processes that demonstrated enhanced performances compared to their steady state analogues. Moreover, the analysis of the transient catalytic behaviour developed in unsteady-state conditions leads to a deeper understanding of the catalytic processes in terms of identification of specific reactant-catalyst interactions, the steps involved in products formation and the mechanism of catalyst deactivation.
This dissertation deals with the catalytic activation of CO2 and CH4 molecules targeting at their valorisation to important chemical commodities as CO (syngas) and light hydrocarbons. Unsteady-state catalysis is explored as a means to overcome thermodynamic constraints associated to the conventional CO2 and CH4 conversion routes.... ...
Large scale utilisation of CO2 in the chemical industry is currently limited to a few applications (e.g. synthesis of urea, carboxylic acids, food industry) and generally requires high purity feedstock. Integrated processes that combine CO2 capture from diluted sources (e.g. industrial flue gases, air) and its conversion to value-added chemicals represent a solution to enhance the utilisation of CO2 and mitigate its emissions. CH4 is an abundant hydrocarbon with diversified sources ranging from fossil-based (natural gas, shale gas) to renewable ones (biomass, biogas), which can potentially substitute oil for the synthesis of valuable chemicals and fuels, including higher hydrocarbons. At the moment, however, CH4 utilisation is circumscribed to combustion for heat and energy production or energy-intensive production of H2 and syngas (H2 + CO) via steam reforming, resulting in a high carbon footprint.
In general, the thermodynamic stability of CO2 and CH4 molecules imposes severe limitations to their exploitation as chemical feedstocks, in terms of low conversion efficiencies and control on the selectivity of products. Their efficient conversion requires harsh reaction conditions (high temperatures and pressures, highly chemically reactive substances) at which the stability of the desired products is threatened, resulting in low selectivity. In this scenario, catalysis is essential to identify functional materials and develop new catalytic processes able to maximise the selective conversion of CO2 and CH4 feedstocks to value-added products.
Unsteady-state operation in catalysis is an option to overcome the thermodynamic constraints imposed by the conventional steady-state operation. Integrated CO2 capture and conversion, sorption-enhanced reactions, chemical looping combustion are examples of intrinsically unsteady-state catalytic processes that demonstrated enhanced performances compared to their steady state analogues. Moreover, the analysis of the transient catalytic behaviour developed in unsteady-state conditions leads to a deeper understanding of the catalytic processes in terms of identification of specific reactant-catalyst interactions, the steps involved in products formation and the mechanism of catalyst deactivation.
This dissertation deals with the catalytic activation of CO2 and CH4 molecules targeting at their valorisation to important chemical commodities as CO (syngas) and light hydrocarbons. Unsteady-state catalysis is explored as a means to overcome thermodynamic constraints associated to the conventional CO2 and CH4 conversion routes....
A robust material for the production of microfluidic liquid-liquid extraction chips
Evaluation of a robust ALD coating to reduce irradiation-induced surface modifications on polymers and quartz for the usage of microfluidic liquid-liquid extraction chips
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Urban Facades
Photocatalytic Building Envelope for Passive Remediation of Air Pollution
TiO2 coating has been used in building materials for its self-cleaning property. However, its capability to break down NOx compounds has broadened its scope for pollution abatement. Though it can be applied as a coating, the performance of the photocatalyst in urban scenarios is affected by contact wind speeds and incident UV irradiation. Also, increased surface area provides more area of photo catalytically active sites. These factors are governed by the geometrical form of the panel. Hence, the main objective of this research is to design a façade panel with enlarged surface area and surface roughness to manipulate the environmental factors to favor photocatalysis. Also, its air purification effect is quantified to understand the effectiveness of this passive strategy and the design.
The façade concept has been designed following a series of strategies to respond to wind and irradiation. The concept with optimum surface enlargement and irradiation is developed into modular panels which are materialized by choosing the material with least environmental impact. The final part of this graduation project is about applying these panels in the street canyons, a controlled urban environment and evaluating the pollution abatement. The results indicate a pollution abatement of 3.5% - 8.9% in winter and 18% - 37.5% in percentage in summer for London. ...
TiO2 coating has been used in building materials for its self-cleaning property. However, its capability to break down NOx compounds has broadened its scope for pollution abatement. Though it can be applied as a coating, the performance of the photocatalyst in urban scenarios is affected by contact wind speeds and incident UV irradiation. Also, increased surface area provides more area of photo catalytically active sites. These factors are governed by the geometrical form of the panel. Hence, the main objective of this research is to design a façade panel with enlarged surface area and surface roughness to manipulate the environmental factors to favor photocatalysis. Also, its air purification effect is quantified to understand the effectiveness of this passive strategy and the design.
The façade concept has been designed following a series of strategies to respond to wind and irradiation. The concept with optimum surface enlargement and irradiation is developed into modular panels which are materialized by choosing the material with least environmental impact. The final part of this graduation project is about applying these panels in the street canyons, a controlled urban environment and evaluating the pollution abatement. The results indicate a pollution abatement of 3.5% - 8.9% in winter and 18% - 37.5% in percentage in summer for London.
Fluidized Nanoparticle Agglomerates
Formation, Characterization, and Dynamics