Search

The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change., Journal of Geophysical Research: Atmospheres, 127 (6), ISSN:0148-0227, ISSN:2169-897X

African mineral dust is transported many thousands of kilometres from its source regions and, because of its ability to nucleate ice, it plays a major role in cloud glaciation around the globe. The ice-nucleating activity of desert dust is influenced by its mineralogy, which varies substantially between source regions and across particle sizes. However, in models it is often assumed that the activity (expressed as active sites per unit surface area as a function of temperature) of atmospheric mineral dust is the same everywhere on the globe. Here, we find that the ice-nucleating activity of African desert dust sampled in the summertime marine boundary layer of Barbados (July and August, 2017) is substantially lower than parameterizations based on soil from specific locations in the Saharan desert or dust sedimented from dust storms. We conclude that the activity of dust in Barbados’ boundary layer is primarily defined by the low K-feldspar content of the dust, which is around 1 %. We propose that the dust we sampled in the Caribbean was from a region in West Africa (in and around the Sahel in Mauritania and Mali), which has a much lower feldspar content than other African sources across the Sahara and Sahel.

The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change.

Copyright © 2019 American Chemical Society. In this study, a computational fluid dynamics approach is implemented to investigate the dynamic behavior of continuous-flow droplet microfluidics. The developed approach predicts both droplet generation and manipulation in a two-step process. First, droplet formation was studied in a flow-focusing junction through an Eulerian-Eulerian approach. Surface tension and wall adhesion were used in the model. The effect of flow rates and geometrical characteristics of the device on droplet size and dispensing rate was investigated. Second, post-generation, droplets were treated as point-like particles, and their deflection across a millimeter, multilaminar flow chamber with five parallel streams was modeled using an Eulerian-Lagrangian approach, thus improving computational efficiency. Flow rates and magnet location were optimized. Our simulated droplet trajectory inside the chamber was contrasted against experimental data, and a good agreement was found between them. This two-step computational model enables the rational optimization of continuous-flow droplet processing, and it can be readily adapted to a broad range of magnetically enabled microfluidic applications.

Clouds containing supercooled water are important for both climate and weather, but our knowledge of which aerosol particle types nucleate ice in these clouds is far from complete. Combustion aerosols have strong anthropogenic sources, and if these aerosol types were to nucleate ice in clouds, they might exert a climate forcing. Here, we quantified the atmospheric ice‐nucleating particle (INP) concentrations during the United Kingdom's annual Bonfire Night celebrations, which are characterized by large amounts of combustion aerosol from bonfires and fireworks. We used three immersion mode techniques covering more than 6 orders of magnitude in INP concentration over the temperature range from −10°C to homogeneous freezing. We found no observable systematic change in the INP concentration on three separate nights, despite more than a factor of 10 increase in aerosol number concentrations, up to a factor of 10 increase in PM10 concentration, and more than a factor of 100 increase in black carbon (BC) mass concentration relative to pre‐event levels. This implies that BC and other combustion aerosol such as ash did not compete with the INPs present in the background air. Furthermore, the upper limit of the ice‐active site surface density, ns(T), of BC generated in these events was shown to be consistent with several other recent laboratory studies, showing a very low ice‐nucleating activity of BC. We conclude that combustion aerosol particles similar to those emitted on Bonfire Night are at most of secondary importance for the INP population relevant for mixed‐phase clouds in typical midlatitude terrestrial locations. © 2020 American Geophysical Union. ISSN:0148-0227 ISSN:2169-897X

The miniaturisation of positron emission tomography (PET) radiotracer production is facilitating a move towards a dose-on-demand strategy that would enable a stratified approach to patient diagnostics, but while the on-chip synthesis steps have been demonstrated, the subsequent quality control (QC) testing steps have received much less attention. As part of the development of an integrated QC platform for PET tracers, we have developed two microfluidic electrochemical detectors for the pulsed amperometric detection (PAD) of carbohydrate-based radiotracers, with a particular view to the QC testing of the most important tracer, [18F]2-fluoro-2-deoxy-d-glucose ([18F]FDG). The first device employed a commercial screen-printed electrode (SPE) to enable a single-use format, while the second device incorporated wire electrodes for use as a more permanent fixture in a QC instrument. A flow-injection analysis (FIA)-style setup was used to inject boluses of d-glucose into the chips in a proxy for intended chromatographic separations prior to PAD. In proof-of-concept testing of the devices, the chips featuring the SPE and the wire electrodes yielded limits of detection of 0.1 ppm and 9 ppm, respectively, each below the required limits for [18F]FDG, and thus making both methodologies viable for the QC testing of PET radiotracers in a dose-on-demand format.

Amphiphilic microgels of different composition based on the hydrophilic, pH-responsive acrylic acid (AA) and the hydrophobic, non-ionic n-butyl acrylate (BuA) were synthesised using a lab-on-a-chip device. Hydrophobic droplets were generated via a microfluidic platform that contained a protected form of AA, BuA, the hydrophobic crosslinker, ethylene glycol dimethacrylate (EGDMA), and a free radical initiator in an organic solvent. These hydrophobic droplets were photopolymerised within the microfluidic channels and subsequently hydrolysed, enabling an integrated platform for the rapid, automated, and in situ production of anionic amphiphilic microgels. The amphiphilic microgels did not feature the conventional core–shell structure but were instead based on random amphiphilic copolymers of AA and BuA and hydrophobic crosslinks. Due to their amphiphilic nature they were able to encapsulate and deliver both hydrophobic and hydrophilic moieties. The model drug delivery and the swelling ability of the microgels were influenced by the pH of the surrounding aqueous solution and the hydrophobic content of the microgels.

The freezing of supercooled water to ice and the materials which catalyse this process are of fundamental interest to a wide range of fields. At present, our ability to control, predict or monitor ice formation processes is poor. The isolation and characterisation of frozen droplets from supercooled liquid droplets would provide a means of improving our understanding and control of these processes. Here, we have developed a microfluidic platform for the continuous flow separation of frozen from unfrozen picolitre droplets based on differences in their density, thus allowing the sorting of ice crystals and supercooled water droplets into different outlet channels with 94 ± 2% efficiency. This will, in future, facilitate downstream or off-chip processing of the frozen and unfrozen populations, which could include the analysis and characterisation of ice-active materials or the selection of droplets with a particular ice-nucleating activity.

A minute fraction of atmospheric particles exert a disproportionate effect on the phase of mixed-phase clouds by acting as ice-nucleating particles (INPs). To understand the effects of these particles on weather and climate, both now and into the future, we must first develop a quantitative understanding of the major INP sources worldwide. Previous work has demonstrated that aerosols such as desert dusts are globally important INPs, but the role of biogenic INPs is unclear, with conflicting evidence for their importance. Here, we show that at a temperate site all INPs active above −18 °C at concentrations >0.1 L−1 are destroyed on heating, consistent with these INPs being of biological origin. Furthermore, we show that a global model of desert dust INPs dramatically underestimates the measured INP concentrations, but is consistent with the thermally-stable component. Notably, the heat sensitive INPs are active at temperatures where shallow cloud layers in Northern Europe are frequently observed to glaciate. Hence, we suggest that biogenic material is important for primary ice production in this region. The prevalence of heat sensitive, most likely biogenic, INPs in this region highlights that, as a community, we need to quantify the sources and transport of these particles as well as determine their atmospheric abundance across the globe and at cloud altitudes.

We investigate the potential of using microcapsules, generated through layer-by-layer assembly, as reaction compartments for bioassays. A streptavidin–biotin and an esterase-fluorescein diacetate (FDA) assay were employed for proof-of-concept. Streptavidin was incorporated into the microcapsules via two methods: (i) physical adsorption onto MnCO3 microcrystal templates or (ii) co-precipitation with CaCO3 to form mixed microcrystals. The streptavidin-loaded template microparticles were then coated with five bi-layers of polyelectrolytes (polyallylamine hydrochloride/polystyrene sulfonate) (PAH/PSS)5 and the templated cores were dissolved using EDTA to form polyelectrolyte microcapsules loaded with streptavidin. Streptavidin loading of around 77 mg streptavidin per mol of CaCO3 was achieved using the co-precipitation method, compared to 5.1 mg streptavidin per mol of MnCO3 using physical adsorption onto the manganese carbonate crystal surface. The microencapsulated streptavidin was allowed to bind to an analyte which was able to freely diffuse through the polyelectrolyte shell from the aqueous media. Biotin-4-fluorescein was added to the streptavidin-loaded microcapsules, with streptavidin-free capsules serving as the control sample. It was found that both types of microcapsules exhibited a similar fluorescence signal intensity, likely due to non-specific binding of biotin-4-fluorescein to charged groups on the polyelectrolyte shell. Therefore, an alternative esterase-FDA assay was investigated as fluorescence is only produced when FDA penetrates the capsule shell and reacts with the esterase enzyme inside which leads to its hydrolysis. Esterase was loaded into the LbL capsules templated on CaCO3via co-precipitation. FDA was added to both the esterase-loaded capsules and esterase-free capsules. It was found that the capsules containing esterase fluoresced, while the esterase-free capsules did not. This indicates that the hydrolysis reaction of FDA with esterase occurred inside the LbL microcapsules. These experiments demonstrate the potential of compartmentalised assays to be carried out inside microcapsules which could be applied in complex matrices or in multiplexing experiments, wherein different barcoded microcapsules contain different reagents to provide independent readouts without interference from larger biomolecules present in the surrounding media.

Cationic, amphiphilic microgels of differing compositions based on hydrophilic, pH, and thermoresponsive 2-(dimethylamino)ethyl methacrylate (DMAEMA) and hydrophobic, nonionic n-butyl acrylate (BuA) are synthesized using a lab-on-a-chip device. Hydrophobic oil-in-water (o/w) droplets are generated via a microfluidic platform, with the dispersed (droplet) phase containing the DMAEMA and BuA, alongside the hydrophobic cross-linker, ethylene glycol dimethacrylate, and a free radical initiator in an organic solvent. Finally, the hydrophobic droplets are photopolymerized via a UV light source as they traverse the microfluidic channel to produce the cationic amphiphilic microgels. This platform enables the rapid, automated, and in situ production of amphiphilic microgels, which do not match the core-shell structure of conventionally prepared microgels but are instead based on random amphiphilic copolymers of DMAEMA and BuA between the hydrophobic cross-links. The microgels are characterized in terms of their swelling and encapsulation abilities, which are found to be influenced by both the pH response and the hydrophobic content of the microgels. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018, 56, 59–66.

© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim We present a simple microfluidic system for rapid screening of Escherichia coli (E. coli) O157:H7 employing the specificity of immunomagnetic separation (IMS) via immiscible filtration assisted by sur face tension (IFAST), and the sensitivity of the subsequent adenosine triphosphate (ATP) assay by the bioluminescence luciferin/luciferase reaction. The developed device was capable of detecting E. coli O157:H7 from just 6 colony forming units (CFU) in 1 mL spiked buffer within 20 min. When tested with wastewater discharged effluent samples, without pre-concentration, the device demonstrated the ability to detect 10 4 CFU per mL seeded; suggesting great potential for point-of-need microbiological water quality monitoring.

High-speed video of freezing water proves ice formation starts at specific and very rare sites where there are surface defects., Understanding how surfaces direct nucleation is a complex problem that limits our ability to predict and control crystal formation. We here address this challenge using high-speed imaging to identify and quantify the sites at which ice nucleates in water droplets on the two natural cleavage faces of macroscopic feldspar substrates. Our data show that ice nucleation only occurs at a few locations, all of which are associated with micron-size surface pits. Similar behavior is observed on α-quartz substrates that lack cleavage planes. These results demonstrate that substrate heterogeneities are the salient factor in promoting nucleation and therefore prove the existence of active sites. We also provide strong evidence that the activity of these sites derives from a combination of surface chemistry and nanoscale topography. Our results have implications for the nucleation of many materials and suggest new strategies for promoting or inhibiting nucleation across a wide range of applications.

A miniaturized radio-HPLC detector has been developed comprising a microfluidic device fabricated from plastic scintillator in combination with a silicon photomultiplier light sensor, and tested with samples containing a positron-emitting radionuclide, [18 F]fluoride. This cost-effective, small footprint analytical tool is ideal for incorporation into integrated quality control systems for the testing of positron emission tomography (PET) radiopharmaceuticals to good manufacturing practice (GMP) standards.

Here, we report a single-point detection method for the determination of dynamic surface conditions inside microfluidic channels. The proposed method is based on monitoring fluorescence amplitude as a function of the convolution of a laser beam with segmented flow consisting of two immiscible liquids, one containing fluorescent dye. The fluorescence amplitude is determined by the flow rate and the droplet shape, which is affected by the channel surface properties. We modeled the interaction of a droplet and a laser beam via computer-aided design software, using the laser beam location in relation to the droplet shape as a parameter. The method was applied to fused silica capillaries with both unmodified and modified surfaces, with segmented flow exhibiting water contact angles of ≈ 30° and ≈ 100°, respectively. The method allows discrimination between hydrophillic and hydrophobic surfaces, as well as the quality of the treatment. The results were verified using fluorescence imaging of the droplets via a stroboscopic technique. We also applied this method to the analysis of microfabricated channels with non-circular cross sections. We demonstrated that the technique enables the determination of the hydrophobicity of channel surfaces, a crucial property required for the generation of segmented flow or emulsions for applications such as digital PCR.

Polyelectrolyte (PE) microcapsules for drug delivery are typically fabricated via layer-by-layer (LbL) deposition of PE layers of alternating charge on sacrificial template microparticles, which usually requires multiple incubation and washing steps that render the process repetitive and time-consuming. Here, ferrofluid droplets were explored for this purpose as an elegant alternative of templates that can be easily manipulated via an external magnetic field, and require only a simple microfluidic chip design and setup. Glass microfluidic devices featuring T-junctions or flow focusing junctions for the generation of oil-based ferrofluid droplets in an aqueous continuous phase were investigated. Droplet size was controlled by the microfluidic channel dimensions as well as the flow rates of the ferrofluid and aqueous phases. The generated droplets were stabilised by a surface active polymer, polyvinylpyrrolidone (PVP), and then guided into a chamber featuring alternating, co-laminar PE solutions and wash streams, and deflected across them by means of an external permanent magnet. The extent of droplet deflection was tailored by the flow rates, the concentration of magnetic nanoparticles in the droplets, and the magnetic field strength. PVP-coated ferrofluid droplets were deflected through solutions of polyelectrolyte and washing streams using several iterations of multilaminar flow designs. This culminated in an innovative "Snakes-and-Ladders" inspired microfluidic chip design that overcame various issues of the previous iterations for the deposition of layers of anionic poly(sodium-4-styrene sulfonate) (PSS) and cationic poly(fluorescein isothiocyanate allylamine hydrochloride) (PAH-FITC) onto the droplets. The presented method demonstrates a simple and rapid process for PE layer deposition in

Amphiphilic microgels based on the hydrophilic acrylic acid (AA) and hydrophobic crosslinks of different compositions were synthesised using a lab-on-a-chip device. The microgels were formed by polymerising hydrophobic droplets. The droplets were generated via a microfluidic platform and contained a protected form of AA, a hydrophobic crosslinker (ethylene glycol dimethacrylate, EGDMA) and a free radical initiator in an organic solvent. Following photopolymerisation and subsequent hydrolysis, AA based microgels of amphiphilic nature were produced and it was demonstrated that they can successfully deliver both hydrophilic as well as hydrophobic moieties. The model drug delivery and the swelling ability of the microgels were influenced by the pH of the aqueous solution as well as the crosslinking density and hydrophobic content of the microgels.

We demonstrate diamagnetic repulsion forces for performing continuous multilaminar flow assays on particles based on their intrinsic properties and with a simple setup. The platform could be applied to sandwich assays on polystyrene particles, and to cell-based assays via their suspension in biologically benign magnetic media.

A new approach for high voltage capillary electrophoresis (CE) is proposed, which replaces the standard high voltage power supply with a Van de Graaff generator, a low current power source. Because the Van de Graaff generator is a current-limited source (10 μA), potentials exceeding 100 kV can be generated for CE when the electrical resistance of the capillary is maximized. This was achieved by decreasing the capillary diameter and reducing the buffer ionic strength. Using 2 mM borate buffer and a 5 μm i.d. capillary, fluorescently labeled amino acids were separated with efficiencies up to 3.5 million plates; a 5.7 fold improvement in separation efficiency compared to a normal power supply (NPS) typically used in CE. This separation efficiency was realized using a simple set-up without significant Joule heating, making the Van de Graaff generator a promising alternative for applying the high potentials required for enhancing resolution in the separation and analysis of highly complex samples, for example mixtures of glycans.

Magnetic particles have become popular in recent years for immunoassays due to their high surface-to-volume ratio and the ease of their manipulation. However, such assays also require multiple reaction and washing steps that are both time-consuming and manually laborious. Here, we describe a setup and methodology for performing rapid immunoassays on magnetic particles in continuous flow via their deflection through multiple laminar flow streams of reagents and washing solutions. In particular, we focus on the use of the microfluidic platform for a C-reactive protein (CRP) sandwich immunoassay in less than 60 s.

Magnetic particles have become popular in recent years for immunoassays due to their high surface-to-volume ratio and the ease of their manipulation. However, such assays also require multiple reaction and washing steps that are both time-consuming and manually laborious. Here, we describe a setup and methodology for performing rapid immunoassays on magnetic particles in continuous flow via their deflection through multiple laminar flow streams of reagents and washing solutions. In particular, we focus on the use of the microfluidic platform for a C-reactive protein (CRP) sandwich immunoassay in less than 60 s.

The processing of particles, cells, and droplets for reactions, analyses, labeling, and coating is an important aspect of many microfluidic workflows. However, performing multi-step processes is typically a laborious and time-consuming endeavor. By exploiting the laminar nature of flow within microchannels, such procedures can benefit in terms of both speed and simplicity. This can be achieved either by manipulating the flow streams around the objects of interest, particularly for the localized perfusion of cells, or by manipulating the objects themselves within the streams via a range of forces. Here, we review the variety of methods that have been employed for performing such "multilaminar flow" procedures on particles, cells, and droplets.

We demonstrate a rapid method of coating a layer of polymer onto magnetically modified yeast cells, so-called “cyborg cells”, in continuous flow within a microfluidic chamber. Laminar flow streams of polyelectrolyte and washing buffers were generated across the chamber, and the magnetic cells were deflected sequentially through the co-flowing streams via an external magnet, allowing polyelectrolyte deposition onto the cells immediately followed by the washing step, all in less than 90 s. This simple deposition technique shows promise for the functionalization of such cyborg cells for applications including bioelectronics, bioanalysis, and toxicity screening, while the addition of more reagent streams would enable the fabrication of multilayered capsules.

Microfluidic devices have shown great potential for the production of positron emission tomography (PET) radiotracers, but most devices have focused only on the synthesis step of the procedure, typically neglecting the other important steps such as [ 18 F]fluoride pre-concentration and radiotracer purification that could equally benefit from miniaturisation. Here, we demonstrate the development of microfluidic modules for the purification of PET radiotracers, particularly 2-[ 18 F]fluoro-2-deoxy- d -glucose ([ 18 F]FDG), via the use of on-chip solid-phase extraction (SPE). In these initial tests, the SPE modules were able to yield [ 18 F]FDG with up to 90% radiochemical purity, and methods are proposed for further increasing this value.

We demonstrate the use of the miniaturised Medipix positron sensor for detection of the clinical PET radiotracer, [(68)Ga]gallium-citrate, on a silica-based monolith, towards microfluidic quality control. The system achieved a far superior signal-to-noise ratio compared to conventional sodium iodide-based radio-HPLC detection and allowed real-time visualisation of positrons in the monolith.

The ability to detect radiation in microfluidic devices is important for the on-chip analysis of radiopharmaceuticals, but previously reported systems have largely suffered from various limitations including cost, complexity of fabrication, and insufficient sensitivity and/or speed. Here, we present the use of sensitive, low cost, small-sized, commercially available silicon photomultipliers (SiPMs) for the detection of radioactivity inside microfluidic channels fabricated from a range of conventional microfluidic chip substrates. We demonstrate the effects of chip material and thickness on the detection of the positron-emitting isotope, [(18)F]fluoride, and find that, while the SiPMs are light sensors, they are able to detect radiation even through opaque chip materials via direct positron and gamma (γ) ray interaction. Finally, we employed the SiPM platform for analysis of the PET (positron emission tomography) radiotracers 2-[(18)F]fluoro-2-deoxy-d-glucose ([(18)F]FDG) and [(68)Ga]gallium-citrate, and highlight the ability to detect the γ ray emitting SPECT (single photon emission computed tomography) radiotracer, [(99m)Tc]pertechnetate.

Superconducting magnets enable the study of high magnetic fields on materials and objects, for example in material synthesis, self-assembly or levitation experiments. The setups employed often lack in precise spatial control of the object of interest within the bore of the magnet. Microfluidic technology enables accurate manipulation of fluidic surroundings and we have investigated the integration of microfluidic devices into superconducting magnets to enable controlled studies of objects in high magnetic fields. Polymeric microparticles similar in size to biological cells were manipulated via diamagnetic repulsion. The particles were suspended in an aqueous paramagnetic medium of manganese (II) chloride and pumped into a microfluidic chip, where they were repelled in continuous flow by the high magnetic field. The extent of deflection was studied as a function of increasing (1) particle size, (2) paramagnetic salt concentration, and (3) magnetic field strength. Optimizing these parameters allowed for the spatial separation of two particle populations via on-chip free-flow diamagnetophoresis. Finally, preliminary findings on the repulsion of air bubbles are shown.

The ability to engage and inspire younger generations in novel areas of science is important for bringing new researchers into a burgeoning field, such as lab-on-a-chip. We recently held a lab-on-a-chip workshop for secondary school students, for which we developed a number of hands-on activities that explained various aspects of microfluidic technology, including fabrication (milling and moulding of microfluidic devices, and wax printing of microfluidic paper-based analytical devices, so-called μPADs), flow regimes (gradient formation via diffusive mixing), and applications (tissue analysis and μPADs). Questionnaires completed by the students indicated that they found the workshop both interesting and informative, with all activities proving successful, while providing feedback that could be incorporated into later iterations of the event.

The continuous flow focussing and manipulation of particles and cells are important factors in microfluidic applications for performing accurate and reproducible procedures downstream. Many particle focussing methods require complex setups or channel designs that can limit the process and its applications. Here, we present diamagnetic repulsion as a simple means of focussing objects in continuous flow, based only on their intrinsic properties without the requirement of any label. Diamagnetic polystyrene particles were suspended in a paramagnetic medium and pumped through a capillary between a pair of permanent magnets, whereupon the particles were repelled by each magnet into the central axis of the capillary, thus achieving focussing. By investigating this effect, we found that the focussing was greatly enhanced with (i) increased magnetic susceptibility of the medium, (ii) reduced flow rate of the suspension, (iii) increased particle size, and (iv) increased residence time in the magnetic field. Furthermore, we applied diamagnetic repulsion to the flow focussing of living, label-free HaCaT cells.

We have developed an integrated microfluidic platform for producing 2-[(18)F]-fluoro-2-deoxy-D-glucose ((18)F-FDG) in continuous flow from a single bolus of radioactive isotope solution, with constant product yields achieved throughout the operation that were comparable to those reported for commercially available vessel-based synthesisers (40-80%). The system would allow researchers to obtain radiopharmaceuticals in a dose-on-demand setting within a few minutes. The flexible architecture of the platform, based on a modular design, can potentially be applied to the synthesis of other radiotracers that require a two-step synthetic approach, and may be adaptable to more complex synthetic routes by implementing additional modules. It can therefore be employed for standard synthesis protocols as well as for research and development of new radiopharmaceuticals.

We demonstrate the application of a multilaminar flow platform, in which functionalized magnetic particles are deflected through alternating laminar flow streams of reagents and washing solutions via an external magnet, for the rapid detection of the inflammatory biomarker, C-reactive protein (CRP). The two-step sandwich immunoassay was accomplished in less than 60 s, a vast improvement on the 80-300 min time frame required for enzyme-linked immunosorbent assays (ELISA) and the 50 min necessary for off-chip magnetic particle-based assays. The combination of continuous flow and a stationary magnet enables a degree of autonomy in the system, while a detection limit of 0.87 μg mL(-1) makes it suitable for the determination of CRP concentrations in clinical diagnostics. Its applicability was further proven by assaying real human serum samples and comparing those results to values obtained using standard ELISA tests.

We report the rapid on‐chip generation and subsequent manipulation of magnetic droplets in continuous flow. Magnetic droplets were formed using aqueous‐based ferrofluid as the dispersed phase and fluorocarbon oil as the continuous phase. Droplet manipulation was demonstrated with simple permanent magnets using two microfluidic platforms: (i) flow focusing droplet generation followed by their splitting into daughter droplets containing different amounts of magnetic nanoparticles, and (ii) droplet generation at a T‐junction and their downstream deflection across a chamber for sorting based on the applied magnetic field and magnetite loading of the droplet. Both systems show great potential for performing a wide range of high throughput continuous flow processes including sample dilution, cell sorting and screening, and microparticle fabrication.

We explore the potential of a microfluidic continuous flow particle separation system based on the repulsion of diamagnetic materials from a high magnetic field. Diamagnetic polystyrene particles in paramagnetic manganese (II) chloride solution were pumped into a microfluidic chamber and their deflection behaviour in a high magnetic field applied by a superconducting magnet was investigated. Two particle sizes (5 and 10 μm) were examined in two concentrations of MnCl2 (6 and 10%). The larger particles were repelled to a greater extent than the smaller ones, and the effect was greatly enhanced when the particles were suspended in a higher concentration of MnCl2. These findings indicate that the system could be viable for the separation of materials of differing size and/or diamagnetic susceptibility, and as such could be suitable for the separation and sorting of small biological species for subsequent studies.

Free-flow magnetophoresis is becoming a popular technique for the separation and manipulation of magnetic particles and materials in microsystems. A wide variety of magnetic particles are commercially available that differ greatly in size and in magnetic properties. To investigate the suitability of different particle types for magnetophoretic operations in microfluidic devices, we compared a range of particles from three manufacturers by pumping them through a microfluidic separation chamber and deflecting them from the direction of laminar flow by applying an external magnetic field. The on-chip deflection of particles was compared to data provided by the manufacturers and magnetisation data obtained from vibrating sample magnetometer (VSM) measurements. Additionally, the extent of deflection was examined over a range of temperatures. Deflection distances were found to increase significantly with increasing temperature. Further to this, a separation of 2.8 and 1.0 μm magnetic particles was performed at different temperatures. Separation resolution was found to improve at higher temperatures. Hence, temperature manipulation provides a simple and effective means for improving a magnetic separation or for controlling the angle at which a particle is deflected from its hydrodynamic flow path.

We explore the potential of a microfluidic continuous flow particle separation system based on the repulsion of diamagnetic materials from a high magnetic field. Diamagnetic polystyrene particles in paramagnetic manganese (II) chloride solution were pumped into a microfluidic chamber and their deflection behaviour in a high magnetic field applied by a superconducting magnet was investigated. Two particle sizes (5 and 10 μm) were examined in two concentrations of MnCl2 (6 and 10%). The larger particles were repelled to a greater extent than the smaller ones, and the effect was greatly enhanced when the particles were suspended in a higher concentration of MnCl2. These findings indicate that the system could be viable for the separation of materials of differing size and/or diamagnetic susceptibility, and as such could be suitable for the separation and sorting of small biological species for subsequent studies.

We demonstrate the application of magnetic forces for the simultaneous trapping of two types of particles, magnetic and diamagnetic, via a single set of magnets. Furthermore, we show how this simple setup can be employed for performing assays with a negative control, or for achieving multiple simultaneous analyses.

Ice-nucleating particles (INPs) play a significant role in the climate and hydrological cycle by triggering ice formation in supercooled clouds, thereby causing precipitation and affecting cloud lifetimes and their radiative properties. However, despite their importance, INP often comprise only 1 in 103–106 ambient particles, making it difficult to ascertain and predict their type, source, and concentration. The typical techniques for quantifying INP concentrations tend to be highly labour-intensive, suffer from poor time resolution, or are limited in sensitivity to low concentrations. Here, we present the application of microfluidic devices to the study of atmospheric INPs via the simple and rapid production of monodisperse droplets and their subsequent freezing on a cold stage. This device offers the potential for the testing of INP concentrations in aqueous samples with high sensitivity and high counting statistics. Various INPs were tested for validation of the platform, including mineral dust and biological species, with results compared to literature values. We also describe a methodology for sampling atmospheric aerosol in a manner that minimises sampling biases and which is compatible with the microfluidic device. We present results for INP concentrations in air sampled during two field campaigns: (1) from a rural location in the UK and (2) during the UK’s annual Bonfire Night festival. These initial results will provide a route for deployment of the microfluidic platform for the study and quantification of INPs in upcoming field campaigns around the globe, while providing a benchmark for future lab-on-a-chip-based INP studies. Electronic supplementary material The online version of this article (10.1007/s10404-018-2069-x) contains supplementary material, which is available to authorized users.

Despite recent advances in microfluidic-based integrated diagnostic systems, the sample introduction interface, especially with regards to large volume samples, has often been neglected. We present a sample introduction interface that allows direct on-chip processing of crude stool samples for the detection of Helicobacter pylori (H. pylori). The principle of IFAST (immiscible filtration assisted by surface tension) was adapted to include a large volume sample chamber with a septum-based interface for stool sample introduction. Solid chaotropic salt and dry superparamagnetic particles (PMPs) could be stored on-chip and reconstituted upon sample addition, simplifying the process of release of DNA from H. pylori cells and its binding to the PMPs. Finally, the PMPs were pulled via a magnet through a washing chamber containing an immiscible oil solution and into an elution chamber where the DNA was released into aqueous media for subsequent analysis. The entire process required only 7 min while enabling a 40-fold reduction in working volume from crude biological samples. The combination of a real-world interface and rapid DNA extraction offers the potential for the methodology to be used in point-of-care (POC) devices.

Ice-nucleating particles (INPs) are of atmospheric importance because they catalyse the freezing of supercooled cloud droplets, strongly affecting the lifetime and radiative properties of clouds. There is a need to improve our knowledge of the global distribution of INPs, their seasonal cycles and long-term trends, but our capability to make these measurements is limited. Atmospheric INP concentrations are often determined using assays involving arrays of droplets on a cold stage, but such assays are frequently limited by the number of droplets that can be analysed per experiment, often involve manual processing (e.g. pipetting of droplets), and can be susceptible to contamination. Here, we present a microfluidic platform, the LOC-NIPI (Lab-on-a-Chip Nucleation by Immersed Particle Instrument), for the generation of water-in-oil droplets and their freezing in continuous flow as they pass over a cold plate for atmospheric INP analysis. LOC-NIPI allows the user to define the number of droplets analysed by simply running the platform for as long as required. The use of small (∼100 μm diameter) droplets minimises the probability of contamination in any one droplet and therefore allows supercooling all the way down to homogeneous freezing (around −36 °C), while a temperature probe in a proxy channel provides an accurate measure of temperature without the need for temperature modelling. The platform was validated using samples of pollen extract and Snomax®, with hundreds of droplets analysed per temperature step and thousands of droplets being measured per experiment. Homogeneous freezing of purified water was studied using >10 000 droplets with temperature increments of 0.1 °C. The results were reproducible, independent of flow rate in the ranges tested, and the data compared well to conventional instrumentation and literature data. The LOC-NIPI was further benchmarked in a field campaign in the Eastern Mediterranean against other well-characterised instrumentation. The continuous flow nature of the system provides a route, with future development, to the automated monitoring of atmospheric INP at field sites around the globe.