Nanomaterials-based biomimetic catalysts with multiple functions are necessary to address challenges in artificial enzymes mimicking physiological processes. Here we report a metal-free nanozyme of modified graphitic carbon nitride and demonstrate its bifunctional enzyme-mimicking roles. With oxidase mimicking, hydrogen peroxide is generated from the coupled photocatalysis of glucose oxidation and dioxygen reduction under visible-light irradiation with a near 100% apparent quantum efficiency. Then, the in situ generated hydrogen peroxide serves for the subsequent peroxidase-mimicking reaction that oxidises a chromogenic substrate on the same catalysts in dark to complete the bifunctional oxidase-peroxidase for biomimetic detection of glucose. The bifunctional cascade catalysis is successfully demonstrated in microfluidics for the real-time colorimetric detection of glucose with a low detection limit of 0.8 μM within 30 s. The artificial nanozymes with physiological functions provide the feasible strategies for mimicking the natural enzymes and realizing the biomedical diagnostics with a smart and miniature device.
Herein, we report a novel nanoliter droplet-based microfluidic strategy for continuous and ultrafast synthesis of metal-organic framework (MOF) crystals and MOF heterostructures. Representative MOF structures, such as HKUST-1, MOF-5, IRMOF-3, and UiO-66, were synthesized within a few minutes via solvothermal reactions with substantially faster kinetics in comparison to the conventional batch processes. The approach was successfully extended to the preparation of a demanding Ru3BTC2 structure that requires high-pressure hydrothermal synthesis conditions. Finally, three different types of core-shell MOF composites, i.e., Co3BTC2@Ni3BTC2, MOF-5@diCH3-MOF-5, and Fe3O4@ZIF-8, were synthesized by exploiting a unique two-step integrated microfluidic synthesis scheme in a continuous-flow mode. The synthesized MOF crystals were characterized by X-ray diffraction, scanning electron microscopy, and BET surface area measurements. In comparison with bare MOF-5, MOF-5@diCH3-MOF-5 showed enhanced structural stability in the presence of moisture, and the catalytic performance of Fe3O4@ZIF-8 was examined using Knoevenagel condensation as a probe reaction. The microfluidic strategy allowed continuous fabrication of high-quality MOF crystals and composites exhibiting distinct morphological characteristics in a time-efficient manner and represents a viable alternative to the time-consuming and multistep MOF synthesis processes.
A microfluidic method for the in situ production of monodispersed alginate hydrogels using chaotic mixing is described. Aqueous droplets comprising of alginate and calcium as a cross-linking agent were formed as an immiscible continuous phase, and then the alginate and calcium in the droplet came into contact and were rapidly mixed. Gelation of the hydrogel was achieved in situ by the chaotic mixing of the droplets in the microfluidic device. Important operating parameters included: the capillary number (Ca) and the flow rate of the continuous phase, which mainly influenced the formation of three distinctive flow regimes, such as fluctuation, stable droplets, and laminar flow. Under the stable formation of droplets regime, monodispersed alginate microbeads having a narrow size distribution (below 3% of CV) were produced in the microfluidic device and the size of the microbeads, ranging from 60 to 95 microm, could be easily modulated by varying the flow rate, viscosity, and interfacial tension. In addition, this approach can be applied to the encapsulation of yeast cells in alginate hydrogels with a high monodispersity. This simple microfluidic technique for the production of monodispersed hydrogels and encapsulation of biomolecules shows strong potential for use in biosensors, cell sensors, drug delivery systems, and cell transplantation applications.
Metal doped core–shell Metal‐Organic Frameworks@Covalent Organic Frameworks (MOFs@COFs) are presented as a novel platform for photocatalysis. A palladium (Pd) doped MOFs@COFs in the form of Pd/TiATA@LZU1 shows excellent photocatalytic performance for tandem dehydrogenation and hydrogenation reactions in a continuous‐flow microreactor and a batch system, indicating the great potential of the metal doped MOFs@COFs as a multifunctional platform for photocatalysis. Explanations for the performance enhancement are elucidated. An integrated dual‐chamber microreactor coupled with the metal doped MOFs@COFs is introduced to demonstrate a concept of an intensified green photochemical process, which can be broadly extended to challenging liquid–gas tandem and cascade reactions.
Self-motile Janus colloids are important for enabling a wide variety of microtechnology applications as well as for improving our understanding of the mechanisms of motion of artificial micro- and nanoswimmers. We present here micro/nanomotors which possess a reversed Janus structure of an internal catalytic “chemical engine”. The catalytic material (here platinum (Pt)) is embedded within the interior of the mesoporous silica (mSiO2)-based hollow particles and triggers the decomposition of H2O2 when suspended in an aqueous peroxide (H2O2) solution. The pores/gaps at the noncatalytic (Pt) hemisphere allow the exchange of chemical species in solution between the exterior and the interior of the particle. By varying the diameter of the particles, we observed size-dependent motile behavior in the form of enhanced diffusion for 500 nm particles, and self-phoretic motion, toward the nonmetallic part, for 1.5 and 3 μm ones. The direction of motion was rationalized by a theoretical model based on self-phoresis. For the 3 μm particles, a change in the morphology of the porous part is observed, which is accompanied by a change in the mechanism of propulsion via bubble nucleation and ejection as well as a change in the direction of motion.
We report a newly synthesized inorganic polymer photoresist with a high ceramic yield by the functionalization of polyvinylsilazane (KiON VL20) with 2‐isocyanatoethyl methacrylate via linkage or insertion reaction routes. The chemistry of the synthesis and the pyrolytic conversion as well as the mechanical evaluation were investigated by using various analytical instruments. We show for the first time that this photosensitive resin is a novel precursor for the fabrication of complex 3D SiCN ceramic microstructures with a 210 nm resolution via a two‐photon absorbed crosslinking process and subsequent pyrolysis at 600 °C under a nitrogen atmosphere. Moreover, the dimensional deformation during pyrolysis was significantly reduced by adding silica nanoparticles as a filler. In particular, the ceramic microstructures containing 40 wt % silica nanoparticles exhibited a relatively isotropic shrinkage owing to its sliding free from the substrate during pyrolysis.
In this study, we report a neo-conceptive three-dimensionally (3D) crossing manifold micromixer (CMM) embedded in microchannel. Fabricated by sequential processes of photolithography and two photon absorption stereolithography, this leads to a microfluidic system with a built-in micromixer in a site controlled manner. The effectiveness of CMM is investigated numerically and experimentally. Through the numerical simulation, it is estimated that a high mixing ratio of 90% can be obtained even in a channel length shorter than five times the channel width. This compares well with the conventional passive type of micromixers that have a gradual increase in mixing efficiency with the length of the channel. Furthermore, the mixing performance of the realized CMM built-in microchannel is observed by confocal microscopy.
This study presents a simple synthetic approach for the in situ preparation of monodisperse hybrid Janus microspheres (HJM) having organic and inorganic parts in a PDMS‐based microfluidic device. Based on the mechanism of shear‐force‐driven break‐off, merged droplets of two photocurable oligomer solutions having distinctive properties are generated into an immiscible continuous phase. Functionalized perfluoropolyether (PFPE) as the organic phase and hydrolytic allylhydridopolycarbosilane (AHPCS) as the inorganic phase are used for the generation in aqueous medium of HJM with well‐defined morphology and high monodispersity (average diameter of 162 µm and a 3.5% coefficient of variation). The size and shape of the HJM is controlled by varying the flow rate of the disperse and continuous phases. The HJM have two distinctive regions: a hydrophobic hemisphere (PFPE) having a smooth surface and a relatively hydrophilic region (AHPCS) with a rough, porous surface. In addition, pyrolysis and subsequent oxidation of these HJM convert them into SiC‐based ceramic hemispheres through the removal of the organic portion and etching off the silica shell. The selective incorporation of magnetic nanoparticles into the inorganic part shows the feasibility of the forced assembly of HJM in an applied magnetic field.
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