A country-level assessment of the deployment potential of greenhouse gas removal technologies.

The deployment of greenhouse gas removal (GGR) technologies has been identified as an indispensable option in limiting global warming to 1.5 °C by the end of the century. Despite this, many countries are yet to include and promote this option in their long-term plans owing to factors such as uncertainty in technical potential, deployment feasibility and economic impact. This work presents a country-level assessment of the deployment potential of five GGR technologies, including forestation, enhanced weathering (EW), direct air carbon capture and storage (DACCS), bioenergy with carbon capture and storage (BECCS) and biochar. Using a multi criteria decision analysis (MCDA) approach consisting of bio-geophysical and techno-economic factors, priority regions for the deployment of these GGR technologies were identified. The extent of carbon dioxide removable by 2100 via these technologies was also estimated for each of the 182 countries considered. While the obtained results indicate the need for regional cooperation among countries, it also provides useful evidence on the need for countries to include and prioritise GGR technologies in their revised nationally determined contributions (NDCs).

Assessment of optimal conditions for the performance of greenhouse gas removal methods.

In this study, a comparative literature-based assessment of the impact of operational factors such as climatic condition, vegetation type, availability of land, water, energy and biomass, management practices, cost and soil characteristics was carried out on six greenhouse gas removal (GGR) methods. These methods which include forestation, enhanced weathering (EW), soil carbon sequestration (SCS), biochar, direct air capture with carbon storage (DACCS) and bioenergy with carbon capture and storage (BECCS) were accessed with the aim of identifying the conditions and requirements necessary for their optimum performance. The extent of influence of these factors on the performance of the various GGR methods was discussed and quantified on a scale of 0-5. The key conditions necessary for optimum performance were identified with forestation, EW, SCS and biochar found to be best deployed within the tropical and temperate climatic zones. The CCS technologies (BECCS and DACCS) which have been largely projected as major contributors to the attainment of the emission mitigation targets were found to have a larger locational flexibility. However, the need for cost optimal siting of the CCS plant is necessary and dependent on the presence of appropriate storage facilities, preferably geological. The need for global and regional cooperation as well as some current efforts at accelerating the development and deployment of these GGR methods were also highlighted.

Synthesis of Size-Tunable CO2-Philic Imprinted Polymeric Particles (MIPs) for Low-Pressure CO2 Capture Using Oil-in-Oil Suspension Polymerization.

Highly selective molecularly imprinted poly[acrylamide-co-(ethylene glycol dimethacrylate)] polymer particles (MIPs) for CO2 capture were synthesized by suspension polymerization via oil-in-oil emulsion. Creation of CO2-philic, amide-decorated cavities in the polymer matrix led to a high affinity to CO2. At 0.15 bar CO2 partial pressure, the CO2/N2 selectivity was 49 (corresponding to 91% purity of the gas stream after regeneration), and reached 97 at ultralow CO2 partial pressures. The imprinted polymers showed considerably higher CO2 uptakes compared to their nonimprinted counterparts, and the maximum equilibrium CO2 capture capacity of 1.1 mmol g-1 was achieved at 273 K. The heat of adsorption was below 32 kJ mol-1 and the temperature of onset of intense thermal degradation was 351-376 °C. An increase in monomer-to-cross-linker molar ratio in the dispersed phase up to 1:2.5 led to a higher affinity toward CO2 due to higher density of selective amide groups in the polymer network. MIPs are a promising option for industrial packed and fluidized bed CO2 capture systems due to large particles with a diameter up to 1200 µm and irregular oblong shapes formed due to arrested coalescence during polymerization, occurring as a result of internal elasticity of the partially polymerized semisolid drops.

Prediction and control of drop formation modes in microfluidic generation of double emulsions by single-step emulsification.

HYPOTHESIS: Predicting formation mode of double emulsion drops in microfluidic emulsification is crucial for controlling the drop size and morphology. EXPERIMENTS AND MODELLING: A three-phase Volume of Fluid-Continuum Surface Force (VOF-CSF) model was developed, validated with analytical solutions, and used to investigate drop formation in different regimes. Experimental investigations were done using a glue-free demountable glass capillary device with a true axisymmetric geometry, capable of readjusting the distance between the two inner capillaries during operation. FINDINGS: A non-dimensional parameter (ζ) for prediction of double emulsion formation mode as a function of the capillary numbers of all fluids and device geometry was developed and its critical values were determined using simulation and experimental data. At logζ>5.7, drops were formed in dripping mode; the widening jetting occurred at 5

Semipermeable Elastic Microcapsules for Gas Capture and Sensing.

Monodispersed microcapsules for gas capture and sensing were developed consisting of elastic semipermeable polymer shells of tunable size and thickness and pH-sensitive, gas selective liquid cores. The microcapsules were produced using glass capillary microfluidics and continuous on-the-fly photopolymerization. The inner fluid was 5-30 wt % K2CO3 solution with m-cresol purple, the middle fluid was a UV-curable liquid silicon rubber containing 0-2 wt % Dow Corning 749 fluid, and the outer fluid was aqueous solution containing 60-70 wt % glycerol and 0.5-2 wt % stabilizer (poly(vinyl alcohol), Tween 20, or Pluronic F-127). An analytical model was developed and validated for prediction of the morphology of the capsules under osmotic stress based on the shell properties and the osmolarity of the storage and core solutions. The minimum energy density and UV light irradiance needed to achieve complete shell polymerization were 2 J·cm(-2) and 13.8 mW·cm(-2), respectively. After UV exposure, the curing time for capsules containing 0.5 wt % Dow Corning 749 fluid in the middle phase was 30-40 min. The CO2 capture capacity of 30 wt % K2CO3 capsules was 1.6-2 mmol/g depending on the capsule size and shell thickness. A cavitation bubble was observed in the core when the internal water was abruptly removed by capillary suction, whereas a gradual evaporation of internal water led to buckling of the shell. The shell was characterized using TGA, DSC, and FTIR. The shell degradation temperature was 450-460 °C.

Structured Biodegradable Polymeric Microparticles for Drug Delivery Produced Using Flow Focusing Glass Microfluidic Devices.

Biodegradable poly(DL-lactic acid) (PLA) and poly(lactic-co-glycolic acid) (PLGA) microparticles with tunable size, shape, internal structure and surface morphology were produced by counter-current flow focusing in axisymmetric (3D) glass capillary devices. The dispersed phase was composed of 0.5-2 wt % polymer solution in a volatile organic solvent (ethyl acetate or dichloromethane) and the continuous phase was 5 wt % aqueous poly(vinyl alcohol) solution. The droplets with a coefficient of variation in dripping regime below 2.5% were evaporated to form polymeric particles with uniform sizes ranging between 4 and 30 µm. The particle microstructure and surface roughness were modified by adding nanofiller (montmorillonite nanoclay) or porogen (2-methylpentane) in the dispersed phase to form less porous polymer matrix or porous particles with golf-ball-like dimpled surface, respectively. The presence of 2-4 wt % nanoclay in the host polymer significantly reduced the release rate of paracetamol and prevented the early burst release, as a result of reduced polymer porosity and tortuous path for the diffusing drug molecules. Numerical modeling results using the volume of fluid-continuum surface force model agreed well with experimental behavior and revealed trapping of nanoclay particles in the dispersed phase upstream of the orifice at low dispersed phase flow rates and for 4 wt % nanoclay content, due to vortex formation. Janus PLA/PCL (polycaprolactone) particles were produced by solvent evaporation-induced phase separation within organic phase droplets containing 3% (v/v) PLA/PCL (30/70 or 70/30) mixture in dichloromethane. A strong preferential adsorption of Rhodamine 6G dye onto PLA was utilized to identify PLA portions of the Janus particles by confocal laser scanning microscopy (CLSM). Uniform hemispherical PCL particles were produced by dissolution of PLA domes with acetone.

Dynamics of double emulsion break-up in three phase glass capillary microfluidic devices.

Pinch-off of a compound jet in 3D glass capillary microfluidic device, which combines co-flowing and countercurrent flow focusing geometries, was investigated using an incompressible three-phase axisymmetric Volume of Fluid-Continuum Surface Force (VOF-CSF) numerical model. The model showed good agreement with the experimental drop generation and was capable of predicting formation of core/shell droplets in dripping, narrowing jetting and widening jetting regimes. In dripping and widening jetting regimes, the presence of a vortex flow around the upstream end of the necking thread facilitates the jet break-up. No vortex flow was observed in narrowing jetting regime and pinch-off occurred due to higher velocity at the downstream end of the coaxial thread compared to that at the upstream end. In all regimes, the inner jet ruptured before the outer jet, preventing a leakage of the inner drop into the outer fluid. The necking region moves at the maximum speed in the narrowing jetting regime, due to the highest level of shear at the outer surface of the thread. However, in widening jetting regime, the neck travels the longest distance downstream before it breaks.