Rotating Cylinder-Assisted Nanoimprint Lithography for Enhanced Chemisorbable Filtration Complemented by Molecularly Imprinted Polymers.

Rotating cylindrical stamp-based nanoimprint technique has many advantages, including the continuous fabrication of intriguing micro/nanostructures and rapid pattern transfer on a large scale. Despite these advantages, the previous nanoimprint lithography has rarely been used for producing sophisticated nanoscale patterns on a non-planar substrate that has many extended applications. Here, the simple integration of nanoimprinting process with a help of a transparent stamp wrapped on the cylindrical roll and UV optical source in the core to enable high-throughput pattern transfer, particularly on a fabric substrate is demonstrated. Moreover, as a functional resin material, this innovative strategy involves a synergistic approach on the synthesis of molecularly imprinted polymer, which are spatially organized free-standing perforated nanostructures such as nano/microscale lines, posts, and holes patterns on various woven or nonwoven blank substrates. The proposed materials can serve as a self-encoded filtration medium for selective separation of formaldehyde molecules. It is envisioned that the combinatorial fabrication process and attractive material paves the way for designing next-generation separation systems in use to capture industrial or household toxic substances.

Fluorescent Detection of Bovine Serum Albumin Using Surface Imprinted Films Formed on PDMS Microfluidic Channels.

In this article, we describe a facile method to fabricate MIP patterns in specifically designed microfluidic channels. With this design, homogenous and stable MIP films were spatially immobilized inside the patterned PDMS channels. In this system, the fluorescent response was identified by detection of the fluorescence-labeled bovine serum albumin (BSA) template. In comparison, non-imprinted polymer (NIP) was also prepared. From the results of fluorescent response, significant binding behaviors of BSA molecules into the cavities of MIP patterns was observed due to the increased residence time in each ancillary hexagonal channel caused by the turbulent flow. However, the NIP patterns did not show the fluorescent response. Thus, the use of this system provides effective MIP-based microfluidic channels for the application of biosensors.

One-Step Laser Patterned Highly Uniform Reduced Graphene Oxide Thin Films for Circuit-Enabled Tattoo and Flexible Humidity Sensor Application.

The conversion of graphene oxide (GO) into reduced graphene oxide (rGO) is imperative for the electronic device applications of graphene-based materials. Efficient and cost-effective fabrication of highly uniform GO films and the successive reduction into rGO on a large area is still a cumbersome task through conventional protocols. Improved film casting of GO sheets on a polymeric substrate with quick and green reduction processes has a potential that may establish a path to the practical flexible electronics. Herein, we report a facile deposition process of GO on flexible polymer substrates to create highly uniform thin films over a large area by a flow-enabled self-assembly approach. The self-assembly of GO sheets was successfully performed by dragging the trapped solution of GO in confined geometry, which consisted of an upper stationary blade and a lower moving substrate on a motorized translational stage. The prepared GO thin films could be selectively reduced and facilitated from the simple laser direct writing process for programmable circuit printing with the desired configuration and less sample damage due to the non-contact mode operation without the use of photolithography, toxic chemistry, or high-temperature reduction methods. Furthermore, two different modes of the laser operating system for the reduction of GO films turned out to be valuable for the construction of novel graphene-based high-throughput electrical circuit boards compatible with integrating electronic module chips and flexible humidity sensors.

Foldable and wearable supercapacitors for powering healthcare monitoring applications with improved performance based on hierarchically co-assembled CoO/NiCo networks.

Small-scale and high-performance energy storage devices have drawn tremendous attention with their portable, lightweight, and multi-functionalized features. Here, we present a foldable supercapacitor with affordable flexibility by adopting a developed design and electrode material system as a way to extend usability. Notably, to resolve the limited energy density of conventional capacitors, we successfully synthesize the CoO/NiCo-layered double hydroxide (LDH) core-shell nanostructure on Ni framework as a cathode material. Further, glucose-based activated carbon (GBAC) is utilized for the anode. The CoO/NiCo-LDH electrodes exhibited a high specific capacitance of âˆ¼284.8 mAh g-1 at 1 A g-1, and GBAC delivers a high specific capacitance of âˆ¼166 F g-1 at 1 A g-1. In the following, the combinatorial integration of these materials enabled the asymmetric supercapacitor (ASC) to increase the energy density by enhancing the capacitance and the voltage window, in which a hydrogel-based electrolyte was facilitated for the foldable and wearable capability. The energy density of the ASC device was âˆ¼24.9 Wh kg-1 at a power density of âˆ¼779.5 W kg-1 with a voltage window of âˆ¼1.6 V. As demonstrated, a self-powered energy source was demonstrated by a serially connected multi-ASC device with a help of a commercial solar cell, which was employed for powering wearable healthcare monitoring devices, including personal alarms for patients and recording the human body's electrical signals. The present work offers a viable approach to preparing potential candidates for high-performance electrodes of supercapacitors with deformable configurations to extend the powering capability of other electronic devices with physical functionalities used in wearable electronics.

3D bioprinting of human mesenchymal stem cells-laden hydrogels incorporating MXene for spontaneous osteodifferentiation.

Contemporary advances in three-dimensional (3D) bioprinting technologies have enabled the fabrication of tailored live 3D tissue mimetics. Furthermore, the development of advanced bioink materials has been highlighted to accurately reproduce the composition of a native extracellular matrix and mimic the intrinsic properties of laden cells. Recent research has shown that MXene is one of promising nanobiomaterials with osteogenic activity for bone grafts and scaffolds due to its unique atomic structure of three titanium layers between two carbon layers. In this study, the MXene-incorporated gelatin methacryloyl (GelMA) and hyaluronic acid methacryloyl (HAMA) (i.e., GelMA/HAMA-MXene) bioinks were prepared to explore if they have the potential to enable the spontaneous osteodifferentiation of human mesenchymal stem cells (hMSCs) when the hMSCs-laden GelMA/HAMA-MXene bioinks were 3D printed. The physicochemical and rheological characteristics of the GelMA/HAMA-MXene hydrogels were proven to be unprecedentedly favorable supportive matrices suited for the growth and survival of hMSCs. Furthermore, hMSCs were shown to spontaneously differentiate into osteoblasts within GelMA-HAMA/MXene composites to provide favorable microenvironments for osteogenesis. Therefore, our results suggest that the remarkable biofunctional advantages of the MXene-incorporated GelMA/HAMA bioink can be utilized in a wide range of strategies for the development of effective scaffolds in bone tissue regeneration.

Mobile Point-of-Care Device Using Molecularly Imprinted Polymer-Based Chemosensors Targeting Interleukin-1ß Biomarker.

Molecularly imprinted polymers (MIPs) have garnered significant attention as a promising material for engineering specific biological receptors with superior chemical complementarity to target molecules. In this study, we present an electrochemical biosensing platform incorporating MIP films for the selective detection of the interleukin-1ß (IL-1ß) biomarker, particularly suitable for mobile point-of-care testing (POCT) applications. The IL-1ß-imprinted biosensors were composed of poly(eriochrome black T (EBT)), including an interlayer of poly(3,4-ethylene dioxythiophene) and a 4-aminothiophenol monolayer, which were electrochemically polymerized simultaneously with template proteins (i.e., IL-1ß) on custom flexible screen-printed carbon electrodes (SPCEs). The architecture of the MIP films was designed to enhance the sensor sensitivity and signal stability. This approach involved a straightforward sequential-electropolymerization process and extraction for leaving behind cavities (i.e., rebinding sites), resulting in the efficient production of MIP-based biosensors capable of molecular recognition for selective IL-1ß detection. The electrochemical behaviors were comprehensively investigated using cyclic voltammograms and electrochemical impedance spectroscopy responses to assess the imprinting effect on the MIP films formed on the SPCEs. In line with the current trend in in vitro diagnostic medical devices, our simple and effective MIP-based analytical system integrated with mobile POCT devices offers a promising route to the rapid detection of biomarkers, with particular potential for periodontitis screening.

Recent Advances of Point-of-Care Devices Integrated with Molecularly Imprinted Polymers-Based Biosensors: From Biomolecule Sensing Design to Intraoral Fluid Testing.

Recent developments of point-of-care testing (POCT) and in vitro diagnostic medical devices have provided analytical capabilities and reliable diagnostic results for rapid access at or near the patient's location. Nevertheless, the challenges of reliable diagnosis still remain an important factor in actual clinical trials before on-site medical treatment and making clinical decisions. New classes of POCT devices depict precise diagnostic technologies that can detect biomarkers in biofluids such as sweat, tears, saliva or urine. The introduction of a novel molecularly imprinted polymer (MIP) system as an artificial bioreceptor for the POCT devices could be one of the emerging candidates to improve the analytical performance along with physicochemical stability when used in harsh environments. Here, we review the potential availability of MIP-based biorecognition systems as custom artificial receptors with high selectivity and chemical affinity for specific molecules. Further developments to the progress of advanced MIP technology for biomolecule recognition are introduced. Finally, to improve the POCT-based diagnostic system, we summarized the perspectives for high expandability to MIP-based periodontal diagnosis and the future directions of MIP-based biosensors as a wearable format.

Ternary MXene-loaded PLCL/collagen nanofibrous scaffolds that promote spontaneous osteogenic differentiation.

Conventional bioinert bone grafts often have led to failure in osseointegration due to low bioactivity, thus much effort has been made up to date to find alternatives. Recently, MXene nanoparticles (NPs) have shown prominent results as a rising material by possessing an osteogenic potential to facilitate the bioactivity of bone grafts or scaffolds, which can be attributed to the unique repeating atomic structure of two carbon layers existing between three titanium layers. In this study, we produced MXene NPs-integrated the ternary nanofibrous matrices of poly(L-lactide-co-ε-caprolactone, PLCL) and collagen (Col) decorated with MXene NPs (i.e., PLCL/Col/MXene), as novel scaffolds for bone tissue engineering, via electrospinning to explore the potential benefits for the spontaneous osteogenic differentiation of MC3T3-E1 preosteoblasts. The cultured cells on the physicochemical properties of the nanofibrous PLCL/Col/MXene-based materials revealed favorable interactions with the supportive matrices, highly suitable for the growth and survival of preosteoblasts. Furthermore, the combinatorial ternary material system of the PLCL/Col/MXene nanofibers obviously promoted spontaneous osteodifferentiation with positive cellular responses by providing effective microenvironments for osteogenesis. Therefore, our results suggest that the unprecedented biofunctional advantages of the MXene-integrated PLCL/Col nanofibrous matrices can be expanded to a wide range of strategies for the development of effective scaffolds in bone tissue regeneration.

Strain-tunable optical microlens arrays with deformable wrinkles for spatially coordinated image projection on a security substrate.

As a new concept in materials design, a variety of strategies have been developed to fabricate optical microlens arrays (MLAs) that enable the miniaturization of optical systems on the micro/nanoscale to improve their characteristic performance with unique optical functionality. In this paper, we introduce a cost-effective and facile fabrication process on a large scale up to ~15 inches via sequential lithographic methods to produce thin and deformable hexagonally arranged MLAs consisting of polydimethylsiloxane (PDMS). Simple employment of oxygen plasma treatment on the prestrained MLAs effectively harnessed the spontaneous formation of highly uniform nanowrinkled structures all over the surface of the elastomeric microlenses. With strain-controlled tunability, unexpected optical diffraction patterns were characterized by the interference combination effect of the microlens and deformable nanowrinkles. Consequently, the hierarchically structured MLAs presented here have the potential to produce desirable spatial arrangements, which may provide easily accessible opportunities to realize microlens-based technology by tunable focal lengths for more advanced micro-optical devices and imaging projection elements on unconventional security substrates.

Combinatorial wound healing therapy using adhesive nanofibrous membrane equipped with wearable LED patches for photobiomodulation.

Wound healing is the dynamic tissue regeneration process replacing devitalized and missing tissue layers. With the development of photomedicine techniques in wound healing, safe and noninvasive photobiomodulation therapy is receiving attention. Effective wound management in photobiomodulation is challenged, however, by limited control of the geometrical mismatches on the injured skin surface. Here, adhesive hyaluronic acid-based gelatin nanofibrous membranes integrated with multiple light-emitting diode (LED) arrays are developed as a skin-attachable patch. The nanofibrous wound dressing is expected to mimic the three-dimensional structure of the extracellular matrix, and its adhesiveness allows tight coupling between the wound sites and the flexible LED patch. Experimental results demonstrate that our medical device accelerates the initial wound healing process by the synergetic effects of the wound dressing and LED irradiation. Our proposed technology promises progress for wound healing management and other biomedical applications.

Benefits of a Skull-Interfaced Flexible and Implantable Multilight Emitting Diode Array for Photobiomodulation in Ischemic Stroke.

Photobiomodulation (PBM) has received attention due to its potential for improving tissue function and enhancing regeneration in stroke. A lightweight, compact, and simple system of miniaturized electronic devices consisting of packaged light-emitting diodes (LEDs) that incorporates a flexible substrate for in vivo brain PBM in a mouse model is developed. Using this device platform, the preventive and therapeutic effects of PBM affixed to the exposed skull of mice in the photothrombosis and middle cerebral artery occlusion stroke model are evaluated. Among the wavelength range of 630, 850, and 940 nm LED array, the PBM with 630-nm LED array is proved to be the most effective for reducing the infarction volume and neurological impairment after ischemic stroke. Moreover, the PBM with 630 nm LED array remarkably improves the capability of spatial learning and memory in the chronic poststroke phase, attenuates AIM2 inflammasome activation and inflammasome-mediated pyroptosis, and modulates microglial polarization in the hippocampus and cortex 7 days following ischemic stroke. Thus, PBM may prevent tissue and functional damage in acute ischemic injury, thereby attenuating the development of cognitive impairment after stroke.

A Sustainable and Flexible Microbrush-Faced Triboelectric Generator for Portable/Wearable Applications.

Triboelectric nanogenerators (TENGs) are put forward as a state-of-the-art energy-scavenging technology for self-powered electronics, but their severe wear and degradation driven by inevitable friction can pose significant durability and sustainability concerns. Here, an array of microfibers is reported that functions as a robust and sustainable TENG in both in-plane sliding and vertical contact-separation modes, with excellent electrical potential as high as 20 V and a high cyclability of 3000. The design flexibility of this microbrush TENG (MB-TENG) on the counter materials facilitates the further improvement of electrical outputs, benefiting numerous applications of human-interactive triboelectrification. Significantly, these MB-TENGs offer sufficient output power for successfully driving a smartwatch as well as an electromyography module. This technology uses a simple and cost-effective manner to provide a robust and reliable monolithic TENG module, which is expected to serve as a promising energy-harvesting source for self-powered electronics in the near future.

A Simple Route to the Complexation of Lutein with Reduced Graphene Oxide Nanocarriers and Antioxidant Protection Against Blue Light.

BACKGROUND: The excellent physicochemical properties of graphene-based materials, including graphene oxide (GO) and reduced GO (rGO), offer significant technological potential as multifunctional nanomaterials in biomedical fields. Lutein is a type of carotenoid that forms human macular pigments in the retina, where it inhibits harmful blue light and contributes to the strengthening of the antioxidant defense of retinal pigment epithelium cells. METHODS: Synthesis of the Lutein-rGO (Lu-rGO) complex was carried out for the optimized concentration. Then characterization of material was analyzed through ultraviolet-visible spectrophotometer (UV-Vis spectra), Fourier-transform infrared spectroscopy (FT-IR), Raman spectroscopy, x-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM). Antioxidant activity of Lu-rGO complex was measured by 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), 2.2-diphenyl-1-picrylhydrazyl (DPPH), glutathione (GSH) oxidation assay. Then, oxidative stress induction by blue light and analyzed intracellular reactive oxygen species (ROS). RESULTS AND CONCLUSION: Based on the FT-IR measurement, the reduction efficiency defined by area was found to be 87.3%, the ID/IG ratio of 0.98 demonstrated by the Lu-rGO complex in the Raman spectrum was slightly higher than that of the original GO. The exhibited significant decrease in the peak intensities of the oxygen functional groups of the XPS spectra of the Lu-rGO complex was observed compared with the GO. In the TEM image for the Lu-rGO complex, folded and wrinkled nanostructures over the lutein-covered rGO surface were evidenced by tight molecular binding. The Lu-rGO complex provided superior DPPH and ABTS radical scavenging activity than GO and lutein alone, and the oxidation of GSH was suppressed. It was confirmed that the content of intracellular ROS and lysosomes, increased by blue light, was reduced after treatment with the Lu-rGO complex on ARPE-19 cells. In summary, graphene-based nanocarriers could function as preventative antioxidants during photochemical ROS generation based on the mechanism of antioxidant action.

Enhanced third harmonic generation in ultrathin free-standing ß-Ga2O3 nanomembranes: study on surface and bulk contribution.

Third harmonic generation (THG) has proven its value in surface and interface characterization, high-contrast bio-imaging, and sub-wavelength light manipulation. Although THG is observed widely in general solid and liquid substances, when laser pulses are focused at nanometer-level ultra-thin films, the bulk THG has been reported to play the dominant role. However, there are still third harmonics (TH) generated at the surface of the thin-films, not inside the bulk solid - so-called surface TH, whose relative contribution has not been quantitatively revealed to date. In this study, we quantitatively characterized the surface and bulk contributions of THG at ultra-thin ß-Ga2O3 nanomembranes with control of both the laser and thin-nanomembranes parameters, including the laser peak power, polarization state, number of layers, and nanomembranes thicknesses. Their contributions were studied in detail by analyzing the TH from freestanding ß-Ga2O3 nanomembranes compared with TH from ß-Ga2O3 nanomembranes on glass substrates. The contribution of the TH field from the ß-Ga2O3-air interface was found to be 5.12 times more efficient than that from the ß-Ga2O3-glass interface, and also 1.09 times stronger than the TH excited at bulk 1-µm-thick ß-Ga2O3. Besides, TH from the ß-Ga2O3-air interface was found to be 20% more sensitive to the crystalline structure than that from the ß-Ga2O3-glass interface. This research work deepens our understanding of surface and bulk THG from crystalline materials and provides new possibilities towards designing highly efficient nonlinear optical materials for bio-imaging, energy-harvesting, and ultrafast laser development.

Spontaneously promoted osteogenic differentiation of MC3T3-E1 preosteoblasts on ultrathin layers of black phosphorus.

Recently, black phosphorus (BP) has garnered great attention as one of newly emerging two-dimensional nanomaterials. Especially, the degraded platelets of BP in the physiological environment were shown to be nontoxic phosphate anions, which are a component of bone tissue and can be used for mineralization. Here, our study presents the potential of BP as biofunctional and biocompatible nanomaterials for the application to bone tissue engineering and regeneration. An ultrathin layer of BP nanodots (BPNDs) was created on a glass substrate by using a flow-enabled self-assembly process, which yielded a highly uniform deposition of BPNDs in a unique confined geometry. The BPND-coated substrates represented unprecedented favorable topographical microenvironments and supportive matrices suitable for the growth and survival of MC3T3-E1 preosteoblasts. The prepared substrates promoted the spontaneous osteodifferentiation of preosteoblasts, which had been confirmed by determining alkaline phosphatase activity and extracellular calcium deposition as early- and late-stage markers of osteogenic differentiation, respectively. Furthermore, the BPND-coated substrates upregulated the expression of some specific genes (i.e., RUNX2, OCN, OPN, and Vinculin) and proteins, which are closely related to osteogenesis. Conclusively, our BPND-coating strategy suggests that a biologically inert surface can be readily activated as a cell-favorable nanoplatform enabled with excellent biocompatibility and osteogenic ability.

Highly Aligned Polymeric Nanowire Etch-Mask Lithography Enabling the Integration of Graphene Nanoribbon Transistors.

Graphene nanoribbons are a greatly intriguing form of nanomaterials owing to their unique properties that overcome the limitations associated with a zero bandgap of two-dimensional graphene at room temperature. Thus, the fabrication of graphene nanoribbons has garnered much attention for building high-performance field-effect transistors. Consequently, various methodologies reported previously have brought significant progress in the development of highly ordered graphene nanoribbons. Nonetheless, easy control in spatial arrangement and alignment of graphene nanoribbons on a large scale is still limited. In this study, we explored a facile, yet effective method for the fabrication of graphene nanoribbons by employing orientationally controlled electrospun polymeric nanowire etch-mask. We started with a thermal chemical vapor deposition process to prepare graphene monolayer, which was conveniently transferred onto a receiving substrate for electrospun polymer nanowires. The polymeric nanowires act as a robust etching barrier underlying graphene sheets to harvest arrays of the graphene nanoribbons. On varying the parametric control in the process, the size, morphology, and width of electrospun polymer nanowires were easily manipulated. Upon O2 plasma etching, highly aligned arrays of graphene nanoribbons were produced, and the sacrificial polymeric nanowires were completely removed. The graphene nanoribbons were used to implement field-effect transistors in a bottom-gated configuration. Such approaches could realistically yield a relatively improved current on-off ratio of ~30 higher than those associated with the usual micro-ribbon strategy, with the clear potential to realize reproducible high-performance devices.

Graphene Templated DNA Arrays and Biotin-Streptavidin Sensitive Bio-Transistors Patterned by Dynamic Self-Assembly of Polymeric Films Confined within a Roll-on-Plate Geometry.

Patterning of surfaces with a simple strategy provides insights into the functional interfaces by suitable modification of the surface by novel techniques. Especially, highly ordered structural topographies and chemical features from the wide range of interfaces have been considered as important characteristics to understand the complex relationship between the surface chemistries and biological systems. Here, we report a simple fabrication method to create patterned surfaces over large areas using evaporative self-assembly that is designed to produce a sacrificial template and lithographic etch masks of polymeric stripe patterns, ranging from micrometer to nanoscale. By facilitating a roll-on-plate geometry, the periodically patterned surface structures formed by repetitive slip-stick motions were thoroughly examined to be used for the deposition of the Au nanoparticles decorated graphene oxide (i.e., AuNPs, ~21 nm) and the formation of conductive graphene channels. The fluorescently labeled thiol-modified DNA was applied on the patterned arrays of graphene oxide (GO)/AuNPs, and biotin-streptavidin sensitive devices built with graphene-based transistors (GFETs, effective mobility of ~320 cm2 V-1 s-1) were demonstrated as examples of the platform for the next-generation biosensors with the high sensing response up to ~1 nM of target analyte (i.e., streptavidin). Our strategy suggests that the stripe patterned arrays of polymer films as sacrificial templates can be a simple route to creating highly sensitive biointerfaces and highlighting the development of new chemically patterned surfaces composed of graphene-based nanomaterials.

Selectively Patterned Regrowth of Bilayer Graphene for Self-Integrated Electronics by Sequential Chemical Vapor Deposition.

There is a critical demand for the highly qualified synthesis of graphene with precisely controlled thickness over a large coverage area. Selective growth can be considered as one method of preparing a vertically stacked graphene, but it usually requires elaborately alloyed substrates for chemical vapor deposition (CVD). Here, we report on a newly developed synthesis strategy for a selectively patterned grown graphene sheet in a spatially defined multithickness scale, exhibiting single- and bilayer graphene produced by a conventional CVD process. In particular, a sequential CVD growth technique on a single Cu substrate was used to produce highly ordered and alternatively patterned single- and bilayer graphene, maintaining its continuous configuration in a simplified and scalable manner. Our regrowth process did not require multiple transfer procedures or an alloying catalytic substrate to satisfy the properties of graphene associated with the needs for various applications. We also investigated the most valid mechanisms for our regrowth CVD process, which suggests that it is useful for the cost-effective synthetic approach into a built-in heterostructured single- and bilayer graphene. Finally, we demonstrated the possible accesses of transparent flexible electrodes and monolithically self-integrated all-graphene-based thin-film transistors to fully utilize regrown graphene.