Magnetic Microparticles Research Articles

Rapid Production of PDMS Microdevices for Electrodriven Separations and Microfluidics by 3D-Printed Scaffold Removal

In our work, we produced PDMS-based microfluidic devices by mechanical removal of 3D-printed scaffolds inserted in PDMS. Two setups leading to the fabrication of monolithic PDMS-based microdevices and bonded (or stamped) PDMS-based microdevices were designed. In the monolithic devices, the 3D-printed scaffolds were fully inserted in the PDMS and then carefully removed. The bonded devices were produced by forming imprints of the 3D-printed scaffolds in PDMS, followed by bonding the PDMS parts to glass slides. All these microfluidic devices were then successfully employed in three proof-of-concept applications: capture of magnetic microparticles, formation of droplets, and isotachophoresis separation of model organic dyes.

Reconfigurable Magnetic Origami Actuators with On-Board Sensing for Guided Assembly.

Origami utilizes orchestrated transformation of soft 2D structures into complex 3D architectures, mimicking shapes and functions found in nature. In contrast to origami in nature, synthetic origami lacks the ability to monitor the environment and correspondingly adjust its behavior. Here, magnetic origami actuators with capabilities to sense their orientation and displacement as well as detect their own magnetization state and readiness for supervised folding are designed, fabricated, and demonstrated. These origami actuators integrate photothermal heating and magnetic actuation by using composite thin films (≈60µm thick) of shape-memory polymers with embedded magnetic NdFeB microparticles. Mechanically compliant magnetic field sensors, known as magnetosensitive electronic skins, are laminated on the surface of the soft actuators. These ultrathin actuators accomplish sequential folding and recovery, with hinge locations programmed on the fly. Endowing mechanically active smart materials with cognition is an important step toward realizing intelligent, stimuli-responsive structures.

Microfluidic particle accumulation for visual quantitation of copper ions.

Aportable biosensor has been developedbased on microfluidic particle accumulation for visual quantification of copper ions. A copper-dependent DNAzyme is used to connect magnetic microparticles (MMPs) and polystyrene microparticles (PMPs), forming "MMPs-DNAzyme-PMPs." When copper ions are present, the DNAzyme is cleaved, allowing free PMPs to be released from the MMPs-DNAzyme-PMP complex. Using a capillary-flow-based microfluidic device, the MMPs-DNAzyme-PMPs are first separated by a magnetic chamber, allowing the free PMPs to continue flowing until being trapped at a particle dam with a narrowing nozzle. Therefore, as a thermometer-like display, the copper level can be visually quantified by the accumulation length of the free PMPs in the trapping microchannel. The limit of detection (LOD) is 33nM determined by the linear range of 25-100nM, which is 900 times lower than the prevalent standard (~30μM) in Hong Kong. Thesystem shows excellent selectivity (> 1000-folds) against other heavy metal ions and abilities to adapt to multiple water environmental conditions. Tests on tap water samples and three local natural water sources in Hong Kong manifest that thedevice can effectively monitor the quality of freshwater with >70% recovery and 26.16% RSD.

Multiplexed Determination of Fertility‐related Hormones in Saliva Using Amperometric Immunosensing

AbstractThis paper reports a dual immunosensor for the simultaneous determination of two important fertility‐related hormones: 17β‐estradiol, E2, and follicle‐stimulating hormone, FSH. The implemented method involves direct competitive (E2) or sandwich‐type (FSH) immunoassays carried out on magnetic microparticles (MBs) and amperometric detection at screen‐printed dual carbon electrodes (SPdCEs) involving the hydroquinone (HQ)/H2O2 system. The developed immune platform demonstrates LOD values of 6.88 pg mL−1 and 0.11 mIU mL−1 for E2 and FSH standards, respectively and usefulness for the determination in saliva samples collected from different volunteers, giving results in agreement with the conventional ELISA methodologies.

Microfluidic synthesis of chitosan-coated magnetic alginate microparticles for controlled and sustained drug delivery

The present work aimed to assemble a simple, portable and economical L-junction microfluidic device to realize the adjustment and tunability of homogeneous round-shaped particles synthesis. In this study, we synthesize two kind of microparticles, including magnetic alginate microparticles (MAM) and chitosan-coated magnetic alginate (CMAM) used for controlling the drug release under a mild condition. Comparing to the traditional method, the MAM synthesized via this microfluidic approach has uniform size distribution, adjustable diameter as well as tunable magnetism. By exploring the amoxicillin as model drug, the MAM displays excellent pH-sensitive release, the effect of particle size on the drug release rate was investigated as well. The results show the smaller particles (220 μm) show a faster release rate than the bigger materials (1000 μm) due to their larger specific area, providing more frequency to interact with the reaction solution. The positive polyelectrolyte, chitosan, coated on the magnetic alginate surface endows CMAM time extension in drug release by two times, successfully achieving drug controlled and sustained release via the kinetics analysis. In summary, this microfluidic approach provides a convenient and efficient fluidic design for the well-controlled synthesis of micro-and nanoscale particles, which is a potential choice used for controlled and sustained drug release.

Effect of self-assembly on fluorescence in magnetic multiphase flows and its application on the novel detection for COVID-19.

In the present study, the magnetic field induced self-assembly processes of magnetic microparticles in an aqueous liquid (the pure magnetic fluid) and nonmagnetic microparticles in ferrofluid (the inverse magnetic fluid) are experimentally investigated. The microparticles are formed into chain-like microstructures in both the pure magnetic fluid and the inverse magnetic fluid by applying the external magnetic field. The fluorescence parameters of these self-assembled chain-like microstructures are measured and compared to those without the effect of magnetic field. It is found that the fluorescence in the pure magnetic fluid is weakened, because the scattering and illuminating areas are reduced in the microstructures. On the contrary, the fluorescence in the inverse magnetic fluid is enhanced, because more fluorescent nonmagnetic microparticles are enriched and become detectable under the effect of the magnetic dipole force and the magnetic levitational force, and their unnecessary scattering can be absorbed by the surrounding ferrofluid. The average enhancement of the fluorescence area ratio in the inverse magnetic fluid with 3 μm nonmagnetic microparticles reaches 112.92%. The present work shows that the inverse magnetic fluid has advantages such as low cost, no scattering effect, stable fluorescence intensity, and relatively low magnetic resistance. In the end, a prototype design for the novel detection of coronavirus disease 2019 based on the magnetic field induced self-assembly in the inverse magnetic fluid is proposed, which could support the epidemic prevention and control.

Portable microfluidic device with thermometer-like display for real-time visual quantitation of Cadmium(II) contamination in drinking water

Cadmium (Cd2+) is a toxic metal ion widely existing in water, soil and food. Conventional water quality control heavily relies on expensive, bulky and sophisticated instrument such as spectrometry, which is time-consuming and incompatible with on-site, real-time detection. Here, a portable microfluidic device with thermometer-like visual readouts is developed for real-time quantitation of cadmium (II) contamination in drinking water. We use Cd2+-dependent DNAzyme (Cd16), which is cleaved when Cd2+ is present, creating a single strand DNA which triggers catalytic hairpin assembly (CHA) with two hairpins H1 and H2 as the building blocks. Plenty of H1H2 complex, the product after the Cd2+-mediated CHA, are generated, which can connect magnetic microparticles (MMPs) and polystyrene microparticles (PMPs), forming “MMPs-H1H2-PMPs” sandwich structure. To provide visual readout to quantitate the particle connection, the particle solution is loaded into a portable microfluidic chip. A magnetic separator first removes MMPs and the connected PMPs, while free PMPs can continue flowing until accumulating into a bar at the particle dam. Shown as a thermometer-like display, the accumulating length is inversely proportional to the concentration of Cd2+, enabling quantitative detection of Cd2+ by the naked eye. The proposed device exhibits a limit of detection of 11.3 nM of Cd2+, selectivity >200-fold against other metal ions, high tolerance to the interferents present in drinking water and high recovery rate in tap water. With high analytical performance without any sample preparation step, this portable device is highly promising in real-time monitoring in urban drinking water at sites.

Oligonucleotide sensor based on magnetic capture and photoligation of upconverting nanoparticles in solid surfaces

In this work, we present a luminescence platform that can be used as point of care system for determining the presence and concentration of specific oligonucleotide sequences. This sensor exhibited a limit of detection as low as 50 fM by means of: (i) the use of single-stranded DNA (ssDNA) functionalized magnetic microparticles that captured and concentrated ssDNA-upconverting nanoparticles (ssDNA-UCNPs) on a solid support, when the target sequence (miR-21-5p DNA-analogue) was in the sample, and (ii) a photoligation reaction that covalently linked the ssDNA-UCNPs and the ssDNA magnetic microparticles, allowing stringent washes. The presented sensor showed a similar limit of detection when the assays were conducted in samples containing total miRNA extracted from human serum, demonstrating its suitability for detecting small specific oligonucleotide sequences under real-like conditions. The strategy of combining UCNPs, magnetic microparticles, and a photoligation reaction provides new insight into low-cost, rapid, and ultra-sensitive detection of oligonucleotide sequences.

Swimmers Heal on the Move Following Catastrophic Damage.

Herein, we describe the development of 2D self-healing small-scale swimmers capable of autonomous propulsion and "on-the-fly" structural recovery in large containers. Incorporation of magnetic Nd2Fe14B microparticles in specialized printed strips results in rapid reorientation and reattachment of the moving tail to its complementary broken static piece to restore the original swimmer structure and propulsion behavior. The swimmers display functional recovery independent of user input. Measurements of the magnetic hysteresis and fields were used to assess the behavior of the healing mechanism in real swimming situations. Damage position and multiple magnetic strip patterns have been examined and their influence upon the recovery efficiency has been compared. Owing to its versatility, fast response, and simplicity the new self-healing strategy represents an important step toward the development of new "on-the-fly" repairing strategies for small-scale swimmers and robots.

Assessing the viability of recovered phosphorus from eutrophicated aquatic ecosystems as a liquid fertilizer

One of the most important worldwide environmental challenges is the alteration of the biogeochemical cycle of phosphorus (P). P is globally exported from terrestrial to aquatic ecosystems, causing the eutrophication of the receiving waters. In this context, magnetic microparticles (MPs) have been recently proposed for trapping P in natural eutrophicated ecosystems, as well as in treated wastewaters. The main advantage of using MPs is that both P and MPs can be recovered from the treated water. Thus, the working hypothesis of the present study is that P can be desorbed from P-loaded MPs and recovered P can be later used as a fertilizer. To test this hypothesis, the best working conditions for desorbing P from P-loaded MPs were identified; then, an experiment with different plant nutrient solutions (neutralized solutions containing recovered P and an unfertilized control) was carried out with three different plant species: Ocimum basilicum L., Cucumis sativus L. and Cucumis melo L. Finally, germination, height, root and shoot biomass and P concentration in root and shoot were compared among treatments. Our results show that the best conditions for P desorption from P-loaded MPs occurred when using 0.1 M NH4OH and using H3PO4 for neutralizing pH. The greenhouse fertirrigation pot experiment showed that the neutralized solution containing desorbed P from P-loaded MPs can be used as a liquid fertilizer, since its combination with macro and microelements significantly increased plant height, growth rate, shoot and root biomass and shoot and root P concentration. As a result, MPs can be proposed to be used for counteracting the widespread and coupled problems of the exhaustion of the P reserves and the eutrophication of aquatic ecosystems.

Magnetic microparticle concentration and collection using a mechatronic magnetic ratcheting system.

Magnetic ratcheting cytometry is a promising approach to separate magnetically-labeled cells and magnetic particles based on the quantity of magnetic material. We have previously reported on the ability of this technique to separate magnetically-labeled cells. Here, with a new chip design, containing high aspect ratio permalloy micropillar arrays, we demonstrate the ability of this technique to rapidly concentrate and collect superparamagnetic iron oxide particles. The platform consists of a mechatronic wheel used to generate and control a cycling external magnetic field that impinges on a “ratcheting chip.” The ratcheting chip is created by electroplating a 2D array of high aspect ratio permalloy micropillars onto a glass slide, which is embedded in a thin polymer layer to create a planar surface above the micropillars. By varying magnetic field frequency and direction through wheel rotation rate and angle, we direct particle movement on chip. We explore the operating conditions for this system, identifying the effects of varying ratcheting frequency, along with time, on the dynamics and resulting concentration of these magnetic particles. We also demonstrate the ability of the system to rapidly direct the movement of superparamagnetic iron oxide particles of varying sizes. Using this technique, 2.8 μm, 500 nm, and 100 nm diameter superparamagnetic iron oxide particles, suspended within an aqueous fluid, were concentrated. We further define the ability of the system to concentrate 2.8 μm superparamagnetic iron oxide particles, present in a liquid suspension, into a small chip surface area footprint, achieving a 100-fold surface area concentration, and achieving a concentration factor greater than 200%. The achieved concentration factor of greater than 200% could be greatly increased by reducing the amount of liquid extracted at the chip outlet, which would increase the ability of achieving highly sensitive downstream analytical techniques. Magnetic ratcheting-based enrichment may be useful in isolating and concentrating subsets of magnetically-labeled cells for diagnostic automation.

Magnetic microparticle-based multimer detection system for the electrochemical detection of prion oligomers in sheep using a recyclable BDD electrode

There is a strong need of sensitive and accurate diagnostic tests of infectious prion proteins (PrPSc) in pre-symptomatic individuals and animals. This work associates, for the first time, the magnetic microparticle multimer detection system (MDS) with a recyclable boron doped diamond (BDD) electrode for the electrochemical detection of PrPSc in plasma samples from scrapie-infected sheep with clinical signs. The electrochemical results are in agreement with the chemiluminescence results. The main advantages of the electrochemical fluidic system are its recyclability and the use of low quantity of functional magnetic beads.

Fundamentals of Chemical Reactor Engineering: A Multi-Scale Approach.

There is a strong need of sensitive and accurate diagnostic tests of infectious prion proteins (PrPSc) in pre-symptomatic individuals and animals. This work associates, for the first time, the magnetic microparticle multimer detection system (MDS) with a recyclable boron doped diamond (BDD) electrode for the electrochemical detection of PrPSc in plasma samples from scrapie-infected sheep with clinical signs. The electrochemical results are in agreement with the chemiluminescence results. The main advantages of the electrochemical fluidic system are its recyclability and the use of low quantity of functional magnetic beads.

EFFECT OF DEGREE OF SULFONATION IN NANOCELLULOSE/CHITOSAN COMPOSITE ON ADSORPTION OF CATIONIC DYE AS OPIOID SIMULANT

In this study, the effect of nanocellulose sulfonate group content on adsorption of an opioid simulant was tested. The opioid simulant used was Victoria blue R, an amine dye. Nanocellulose filters were fabricated by crosslinking cellulose nanocrystals (CNCs) with chitosan to improve the mechanical stability of freeze-dried CNCs. Thermogravimetric analysis confirmed the filter’s thermal stability and operating temperatures. Conductometric titration, Fourier transform infrared spectroscopy, and scanning electron microscopy techniques were used to characterize the degree of nanocellulose functionalization. Lastly, the adsorption performance of the sulfonated nanocellulose filter was tested and fitted to kinetic models and adsorption isotherms. The adsorption of the dye by the sulfonated nanocellulose followed pseudo-second order kinetics and the Langmuir isotherm. The maximum adsorption of Victoria blue R dye by sulfonated nanocellulose (68.56 mg/g) is significantly higher than those of other adsorbents, like activated carbon (0.59-2.97 mg/g) and magnetic microparticles (40.98 mg/g). Thus, sulfonated cellulose nanocrystals are a promising material for the sequestration of opioids from water.

Using MALDI-TOF mass spectrometry in peripheral blood for the follow up of newly diagnosed multiple myeloma patients treated with daratumumab-based combination therapy

BackgroundDaratumumab-based combination therapies have shown high rates of complete response (CR) and minimal residual disease negativity in patients with multiple myeloma. However, daratumumab, an IgGκ monoclonal antibody, interferes with electrophoretic techniques making it difficult to reliably define residual disease versus CR, especially in patients with IgGκ multiple myeloma. MethodsEnrichment with polyclonal sheep antibody-coated magnetic microparticles combined with MALDI-TOF mass spectrometry (MALDI-TOF MS) analysis was used to detect M−proteins in serial samples from newly diagnosed multiple myeloma patients treated with daratumumab-based therapy. The performance of the MALDI-TOF MS assay was compared to that of a routine test panel (serum protein electrophoresis (SPEP), immunofixation (IFE) and serum free light chain (FLC)). ResultsComparison of MALDI-TOF MS to SPEP/IFE/FLC showed a concordance of 84.9% (p < 0.001). When MALDI-TOF MS and FLC results were combined, the M−protein detection rate was the same or better than the routine test panel. For the 9 patients who obtained CR during follow-up, MALDI-TOF MS detected an M−protein in 46% of subsequent samples. Daratumumab could be distinguished from the M−protein in 215/222 samples. ConclusionMALDI-TOF MS is useful in assessing CR in patients treated with monoclonal antibody-based therapies.

Functionally graded adhesive joints using magnetic microparticles with a polyurethane adhesive

The present work focuses on using a recently proposed method to create functionally graded adhesive joints using a polyurethane adhesive and iron microparticles. Functionally graded joints were created with the application of a suitable magnetic field in the centre of the overlap region. This field is able to move the iron microparticles and create a tailored particle distribution. The main goal of this work was to create a particle concentration gradient that changes from particle rich in the middle of the overlap to poor in the ends. Consequentially, the stiffness of the resulting composite is made to vary along the bondline. A numerical simulation was performed to determine the optimal distance between the magnet and the adhesive layer as well as the application time of the external magnetic field. In order to assess the influence of the iron particles on the adhesive, different particle amounts were experimentally considered and two particles distributions were evaluated (uniform and graded distributions). The predicted particles trajectories were validated through a study of the single lap joint (SLJ) fracture surfaces, showing that the magnetic particles follow the magnetic field lines towards the middle of the overlap. Also, by observing the same fracture surfaces, the recently proposed method was validated, a non-uniform particle distribution. Finally, SLJs containing 1% of iron microparticles with a graded distribution were found to exhibit the best mechanical performance. Thus, this method has been demonstrated to be a viable technique to enhance the mechanical properties of bonded joints, leading to a more uniform stress distribution along the bondline.

Liquid Crystal Elastomer-Based Magnetic Composite Films for Reconfigurable Shape-Morphing Soft Miniature Machines.

Stimuli-responsive and active materials promise radical advances for many applications. In particular, soft magnetic materials offer precise, fast, and wireless actuation together with versatile functionality, while liquid crystal elastomers (LCEs) are capable of large reversible and programmable shapemorphing with high work densities in response to various environmental stimuli, e.g., temperature, light, and chemical solutions. Integrating the orthogonal stimuli-responsiveness of these two kinds of active materials could potentially enable new functionalities and future applications. Here, magnetic microparticles (MMPs) are embedded into an LCE film to take the respective advantages of both materials without compromising their independent stimuli-responsiveness. This composite material enables reconfigurable magnetic soft miniature machines that can self-adapt to a changing environment. In particular, a miniature soft robot that can autonomously alter its locomotion mode when it moves from air to hot liquid, a vine-like filament that can sense and twine around a support, and a light-switchable magnetic spring are demonstrated. The integration of LCEs and MMPs into monolithic structures introduces a new dimension in the design of soft machines and thus greatly enhances their use in applications in complex environments, especially for miniature soft robots, which are self-adaptable to environmental changes while being remotely controllable.

A visual bio-barcode immunoassay for sensitive detection of triazophos based on biochip silver staining signal amplification

Herein, a novel visual method for detecting triazophos based on competitive bio-barcode immunoassay was described. The competitive immunoassay was established by gold nanoparticles (AuNPs), magnetic microparticle (MMPs) and triazophos, combined with biochip hybridization system to detect the residual of triazophos in water and apple. Because AuNPs carried many bio-barcodes, which hybridized with labeled DNA on the biochip, catalyzed signal amplification using silver staining was detected by grayscale values as well as the naked eye. Notably, the grayscale values decreases with increasing the concentrations of triazophos, and the color change weakened gradually. The detection range was in between 0.05 and 10 ng/mL and the minimum detection limit was set at 0.04 ng/mL. Percent recovery calculated from spiked water and apple samples ranged between 55.4 and 107.8% with relative standard deviations (RSDs) of 12.4–24.9%. It has therefore been shown that this protocol provides a new insight for rapid detection of small molecule pesticides in various matrices.

Preparation, properties, and applications of magnetic hematite microparticles.

Hematite microparticles are becoming increasingly important components in the soft matter field. The remarkable combination of magnetic and photocatalytic properties that characterize them, coupled with the variety of uniform and monodisperse shapes that they can be synthesized in, makes them a one of a kind colloidal model system. Thanks to these properties, hematite microparticles have been recently applied in several important soft matter applications, spanning from novel colloidal building blocks for self-assembly to necessary tools to investigate and understand fundamental problems. In this review article we provide a detailed overview of the traditional methods available for the preparation of hematite microparticles of different shapes, devoting special attention on some of the most common hiccups that could hider a successful synthesis. We furthermore review the particles' most important physico-chemical properties and their most relevant applications in the soft matter field.

Radioprotective effect of nanoceria and magnetic flower-like iron oxide microparticles on gamma radiation-induced damage in BSA protein

<abstract><sec> <title>Purpose</title> Gamma radiation at therapeutic doses can cause conformation changes in proteins and consequently damage cells/tissues associated with the initiation of several pathological disorders. In this study, serum albumin, the most abundant protein in plasma, was chosen as the protein sample. </sec><sec> <title>Methods and Materials</title> Bovine serum albumin (BSA) was exposed to gamma radiation at a therapeutic dose (3 Gy) in the absence and presence of Ceria nanoparticles (CNPs) and flower-like Fe₃O₄ microparticles (FIOMPs). The conformational changes in BSA including primary, secondary, tertiary structures were then studied by UV-Vis, circular dichroism (CD), and fluorescence spectroscopy, respectively. </sec><sec> <title>Results</title> The primary structure of gamma-irradiated BSA (IR-BSA) was conserved, whereas the secondary and tertiary structures were considerably changed. IR-BSA showed α-helix to β-sheet and random coil structure transition along with reduced fluorescence emission intensity compared to non-irradiated native BSA. Both CNPs and FIOMPs could inhibit the secondary and tertiary structural changes in IR-BSA by scavenging the reactive oxygen species produced during the radiolysis of water. </sec><sec> <title>Conclusions</title> The radioprotective property of CNPs arises from enzyme mimetic activities (catalase, superoxide dismutase, and peroxidase) and their antioxidant capability against hydroxyl radicals. In case of FIOMPs, the radioprotective property is attributed to catalase mimetic activity (CAT), and a porous structure leading to increased ROS recombination with each other in the same radiolytic track, and subsequently decreased encounters with BSA. The latter mechanism of restricting ROS migration seems to be more dominant for FIOMPs. Both CNPs/FIOMPs themselves at low concentrations do not show a significant effect on the native protein conformation. These findings indicate that the proposed NPs/MPs can be good candidates for developing strong nano-radioprotectors. </sec></abstract>