MnO4--Triggered Immediate-Stable Real-Time Fluorescence Immunosensor with High Response Speed and Low Steady-State Error.

Real-time chemical and biological sensing in vitro is important for application in health and environmental monitoring. Thus, a more rapid and stable detection method is urgently needed. Herein, an immediate-stable real-time fluorescent immunosensor with a high response speed (∼100%, <1 s) and approximately zero steady-state error is constructed. The developed sensor is based on the MnO4--triggered in situ immediate-stable fluorogenic reaction between dopamine and orcinol monohydrate to produce azamonardine (DMTM). The obtained DMTM is identified and characterized by high-resolution mass spectrometry, 1H NMR spectroscopy, 13C NMR spectroscopy, and theoretical calculations. The present sensor achieves a highly sensitive detection of dopamine (DA) with a limit of detection (LOD) of 10 nM as well as alkaline phosphates (ALP) with an LOD of 0.1 mU/mL by using orcinol monohydrate phosphate sodium salt as a substrate. As a proof of concept, ALP-triggered fluorescence ELISA using cardiac troponin I (cTnI) as a model antigen target is further constructed. The developed real-time sensor achieves the detection of cTnI with an LOD of 0.05 ng/mL. Moreover, the sensor proposed by us is successfully applied to assess the cTnI level in clinical serum specimens and yields results consistent with those obtained by the commercial ELISA method. The immediate-stable real-time fluorescence immunosensor provides a promising and powerful platform for the trace detection of biomolecules in clinical diagnosis.

Realizing Ultrahigh Transconductance in Organic Electrochemical Transistor by Co-Doping PEDOT:PSS with Ionic Liquid and Dodecylbenzenesulfonate.

Organic electrochemical transistors (OECTs), especially the ones with high transconductance, are highly promising in sensitive detection of chemical and biological species. However, it is still a great challenge to design and fabricate OECTs with very high transconductance. Herein, an OECT with ultrahigh transconductance is reported by introducing ionic liquid and dodecylbenzenesulfonate (DBSA) simultaneously in poly(3,4-ethylenedioxythiophene): polystyrenesulfonate (PEDOT:PSS) as the semiconductive channel. Compared with the OECT based on pristine PEDOT:PSS, the OECT based on co-doped PEDOT:PSS demonstrates a significant enhancement of transconductance from 1.85 to 22.7 mS, because of the increase in volumetric capacitance and conductivity. The enhanced transconductance is attributed to the DBSA-facilitated phase separation between the ionic liquid and PEDOT:PSS, which helps to form conductive domains of ionic liquid in PEDOT:PSS matrix, and the partial dispersion of ionic liquid in the PEDOT:PSS phase. Furthermore, by using the interdigitated electrodes as the source and drain electrodes, an ultrahigh transconductance of 180 mS is obtained, which is superior to that of the state-of-the-art OECTs. Because of the ultrahigh transconductance, the obtained OECT demonstrates sensitive detection of hydrogen peroxide and glucose, making it promising in clinical diagnosis, health monitoring, and environmental surveillance.

Signal-Enhanced Detection of Multiplexed Cardiac Biomarkers by a Paper-Based Fluorogenic Immunodevice Integrated with Zinc Oxide Nanowires.

Using a single test to comprehensively evaluate multiple cardiac biomarkers for early diagnosis and prevention of acute myocardial infarction (AMI) has faced enormous challenges. Here, we have developed paper-based fluorogenic immunodevices for multiplexed detection of three cardiac biomarkers, namely, human heart-type fatty acid binding protein (FABP), cardiac troponin I (cTnI), and myoglobin, simultaneously. The detection is based on a strategy using zinc oxide nanowires (ZnO NWs) to enhance fluorescence signals (∼5-fold compared to that on pure paper). The immunodevices showed high sensitivity and selectivity for FABP, cTnI, and myoglobin with detection limits of 1.36 ng/mL, 1.00 ng/mL, and 2.38 ng/mL, respectively. Additionally, the paper-based immunoassay was rapid (∼5 min to complete the test) and portable (using a homemade chamber with a smartphone and an ultraviolet lamp). The developed devices integrated with ZnO NWs enable quantitative, sensitive, and simultaneous detection of multiple cardiac biomarkers in point-of-care settings, which provides a useful approach for monitoring AMI diseases and may be extended to other medical diagnostics and environmental assessments.

A transparent paper-based platform for multiplexed bioassays by wavelength-dependent absorbance/transmittance.

This communication describes the rational design of a transparent paper-based chemosensing platform for multi-target detection by wavelength-dependent absorbance/transmittance. The platform was successfully applied in the examination of bovine serum albumin (BSA) and cholesterol in serum with a low detection limit of 0.1 µM and 0.1 mM, respectively. With low cost and high sensitivity, the paper-based platform shows great promise for multiplexed bioassays.

Noncontact orientation of objects in three-dimensional space using magnetic levitation.

This paper describes several noncontact methods of orienting objects in 3D space using Magnetic Levitation (MagLev). The methods use two permanent magnets arranged coaxially with like poles facing and a container containing a paramagnetic liquid in which the objects are suspended. Absent external forcing, objects levitating in the device adopt predictable static orientations; the orientation depends on the shape and distribution of mass within the objects. The orientation of objects of uniform density in the MagLev device shows a sharp geometry-dependent transition: an analytical theory rationalizes this transition and predicts the orientation of objects in the MagLev device. Manipulation of the orientation of the levitating objects in space is achieved in two ways: (i) by rotating and/or translating the MagLev device while the objects are suspended in the paramagnetic solution between the magnets; (ii) by moving a small external magnet close to the levitating objects while keeping the device stationary. Unlike mechanical agitation or robotic selection, orienting using MagLev is possible for objects having a range of different physical characteristics (e.g., different shapes, sizes, and mechanical properties from hard polymers to gels and fluids). MagLev thus has the potential to be useful for sorting and positioning components in 3D space, orienting objects for assembly, constructing noncontact devices, and assembling objects composed of soft materials such as hydrogels, elastomers, and jammed granular media.

Tilted Magnetic Levitation Enables Measurement of the Complete Range of Densities of Materials with Low Magnetic Permeability.

Magnetic levitation (MagLev) of diamagnetic or weakly paramagnetic materials suspended in a paramagnetic solution in a magnetic field gradient provides a simple method to measure the density of small samples of solids or liquids. One major limitation of this method, thus far, has been an inability to measure or manipulate materials outside of a narrow range of densities (0.8 g/cm(3) < ρ < 2.3 g/cm(3)) that are close in density to the suspending, aqueous medium. This paper explores a simple method-"tilted MagLev"-to increase the range of densities that can be levitated magnetically. Tilting the MagLev device relative to the gravitational vector enables the magnetic force to be decreased (relative to the magnetic force) along the axis of measurement. This approach enables many practical measurements over the entire range of densities observed in matter at ambient conditions-from air bubbles (ρ ≈ 0) to osmium and iridium (ρ ≈ 23 g/cm(3)). The ability to levitate, simultaneously, objects with a broad range of different densities provides an operationally simple method that may find application to forensic science (e.g., for identifying the composition of miscellaneous objects or powders), industrial manufacturing (e.g., for quality control of parts), or resource-limited settings (e.g., for identifying and separating small particles of metals and alloys).

High-Sensitivity Measurement of Density by Magnetic Levitation.

This paper presents methods that use Magnetic Levitation (MagLev) to measure very small differences in density of solid diamagnetic objects suspended in a paramagnetic medium. Previous work in this field has shown that, while it is a convenient method, standard MagLev (i.e., where the direction of magnetization and gravitational force are parallel) cannot resolve differences in density <10(-4) g/cm(3) for macroscopic objects (>mm) because (i) objects close in density prevent each other from reaching an equilibrium height due to hard contact and excluded volume, and (ii) using weaker magnets or reducing the magnetic susceptibility of the medium destabilizes the magnetic trap. The present work investigates the use of weak magnetic gradients parallel to the faces of the magnets as a means of increasing the sensitivity of MagLev without destabilization. Configuring the MagLev device in a rotated state (i.e., where the direction of magnetization and gravitational force are perpendicular) relative to the standard configuration enables simple measurements along the axes with the highest sensitivity to changes in density. Manipulating the distance of separation between the magnets or the lengths of the magnets (along the axis of measurement) enables the sensitivity to be tuned. These modifications enable an improvement in the resolution up to 100-fold over the standard configuration, and measurements with resolution down to 10(-6) g/cm(3). Three examples of characterizing the small differences in density among samples of materials having ostensibly indistinguishable densities-Nylon spheres, PMMA spheres, and drug spheres-demonstrate the applicability of rotated Maglev to measuring the density of small (0.1-1 mm) objects with high sensitivity. This capability will be useful in materials science, separations, and quality control of manufactured objects.

Downregulation of chloroplast RPS1 negatively modulates nuclear heat-responsive expression of HsfA2 and its target genes in Arabidopsis.

Heat stress commonly leads to inhibition of photosynthesis in higher plants. The transcriptional induction of heat stress-responsive genes represents the first line of inducible defense against imbalances in cellular homeostasis. Although heat stress transcription factor HsfA2 and its downstream target genes are well studied, the regulatory mechanisms by which HsfA2 is activated in response to heat stress remain elusive. Here, we show that chloroplast ribosomal protein S1 (RPS1) is a heat-responsive protein and functions in protein biosynthesis in chloroplast. Knockdown of RPS1 expression in the rps1 mutant nearly eliminates the heat stress-activated expression of HsfA2 and its target genes, leading to a considerable loss of heat tolerance. We further confirm the relationship existed between the downregulation of RPS1 expression and the loss of heat tolerance by generating RNA interference-transgenic lines of RPS1. Consistent with the notion that the inhibited activation of HsfA2 in response to heat stress in the rps1 mutant causes heat-susceptibility, we further demonstrate that overexpression of HsfA2 with a viral promoter leads to constitutive expressions of its target genes in the rps1 mutant, which is sufficient to reestablish lost heat tolerance and recovers heat-susceptible thylakoid stability to wild-type levels. Our findings reveal a heat-responsive retrograde pathway in which chloroplast translation capacity is a critical factor in heat-responsive activation of HsfA2 and its target genes required for cellular homeostasis under heat stress. Thus, RPS1 is an essential yet previously unknown determinant involved in retrograde activation of heat stress responses in higher plants.

Folding analytical devices for electrochemical ELISA in hydrophobic R(H) paper.

This work describes a device for electrochemical enzyme-linked immunosorbent assay (ELISA) designed for low-resource settings and diagnostics at the point of care. The device is fabricated entirely in hydrophobic paper, produced by silanization of paper with decyl trichlorosilane, and comprises two zones separated by a central crease: an embossed microwell, on the surface of which the antigen or antibody immobilization and recognition events occur, and a detection zone where the electrodes are printed. The two zones are brought in contact by folding the device along this central crease; the analytical signal is recorded from the folded configuration. Two proof-of-concept applications, an electrochemical direct ELISA for the detection of rabbit IgG as a model antigen in buffer and an electrochemical sandwich ELISA for the detection of malarial histidine-rich protein from Plasmodium falciparum (Pf HRP2) in spiked human serum, show the versatility of this device. The limit of detection of the electrochemical sandwich ELISA for the quantification of Pf HRP2 in spiked human serum was 4 ng mL(-1) (10(2) pmol L(-1)), a value within the range of clinically relevant concentrations.

Chemical routes to top-down nanofabrication.

In fabricating materials at the nanometer scale, nanotechnologists typically employ two general strategies: bottom-up and top-down. While the bottom-up approach constructs nanomaterials from basic building blocks like atoms or molecules, the top-down approach produces nanostructures by deconstructing larger materials with the use of lithographic tools (i.e., physical top-down) or through chemical-based processes (i.e., chemical top-down). This tutorial review summarizes the various top-down nanofabrication methods, with great emphasis on the chemical routes that can generate nanoporous materials and ordered arrays of nanostructures with three-dimensional features. The chemical top-down routes that are discussed in detail include (1) templated etching, (2) selective dealloying, (3) anisotropic dissolution, and (4) thermal decomposition. These emerging nanofabrication tools open up new avenues in the creation of functional nanostructures with a wide array of promising applications.

Charge Dispersion Strategy for High-Performance and Rain-Proof Triboelectric Nanogenerator.

Triboelectric nanogenerator (TENG) is becoming a sustainable and renewable way of energy harvesting and self-powered sensing because of low cost, simple structure, and high efficiency. However, the output current of existing TENGs is still low. It is proposed that the output current of TENGs can be dramatically improved if the triboelectric charges can distribute inside the triboelectric layers. Herein, a novel single-electrode conductive network-based TENG (CN-TENG) is developed by introducing a conductive network of multiwalled carbon nanotubes in dielectric triboelectric layer of thermoplastic polyurethane (TPU). In this CN-TENG, the contact electrification-induced charges distribute on both the surface and interior of the dielectric TPU layer. Thus, the short-circuit current of CN-TENG improves for 100-fold, compared with that of traditional dielectric TENG. In addition, this CN-TENG, even without packing, can work stably in high-humidity environments and even in the rain, which is another main challenge for conventional TENGs due to charge leakage. Further, this CN-TENG is applied for the first time, to successfully distinguish conductive and dielectric materials. This work provides a new and effective strategy to fabricate TENGs with high output current and humidity-resistivity, greatly expanding their practical applications in energy harvesting, movement sensing, human-machine interaction, and so on.

Green Flexible Electronics: Natural Materials, Fabrication, and Applications.

The emergence of plastic electronics satisfies the increasing demand for flexible electronics. However, it has caused severe ecological problems. Flexible electronics based on natural materials are increasing to hopefully realize the "green" and eco-friendly concept. Herein, recent advances in the design and fabrication of green flexible electronics are reviewed. First, this review comprehensively introduces various natural materials and derivatives, focusing particularly on fibroin and silk, wood and paper, plants, and biomass. Second, fabrication techniques for modifying natural materials, including physical and chemical methods, are presented, after which their merits and demerits are thoroughly discussed. Green flexible electronics based on natural materials, comprising electrical wires/electrodes, antennas, thermal management devices, transistors, memristors, sensors, energy-harvesting devices, energy-storage devices, displays, actuators, electromagnetic shielding, and integration systems, are described in detail. Finally, perspectives on the existing challenges and opportunities to employ natural materials in green flexible electronics are presented.

Density-of-States Matching-Induced Ultrahigh Current Density and High-Humidity Resistance in a Simply Structured Triboelectric Nanogenerator.

Triboelectric nanogenerators (TENGs) can covert mechanical energy into electricity in a clean and sustainable manner. However, traditional TENGs are mainly limited by the low output current, and thus their practical applications are still limited. Herein, a new type of TENG is developed by using conductive materials as the triboelectric layers and electrodes simultaneously. Because of the matched density of states between the two triboelectric layers, this simply structured device reaches an open-circuit voltage of 1400 V and an ultrahigh current density of 1333 mA m-2 when poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) film and copper (Cu) or aluminum (Al) foil are used as the triboelectric pair. The current density increases by nearly three orders of magnitude compared with traditional TENGs. More importantly, this device can work stably in high-humidity environments, which is always a big challenge for traditional TENGs. Surprisingly, this TENG can even perform well in the presence of water droplets. This work provides a new and effective strategy for constructing high-performance TENGs, which can be used in many practical applications in the near future.

High-Performance Organic Electrochemical Transistor Based on Photo-annealed Plasmonic Gold Nanoparticle-Doped PEDOT:PSS.

Organic electrochemical transistors (OECTs), particularly the ones based on PEDOT:PSS, are excellent candidates for chemical and biological sensing because of their unique advantages. Improving the sensitivity and stability of OECTs is crucially important for practical applications. Herein, the transconductance of OECT is improved by 8-fold to 14.9 mS by doping the PEDOT:PSS channel with plasmonic gold nanoparticles (AuNPs) using a solution-based process followed by photo annealing. In addition, the OECT also possesses high flexibility and cyclic stability. It is revealed that the doping of AuNPs increases the conductivity of PEDOT:PSS and the photo annealing improves the crystallinity of the PEDOT:PSS channel and the interaction between AuNPs and PEDOT:PSS. These changes lead to the increase in transconductance and cyclic stability. The prepared OECTs are also demonstrated to be effective in sensitive detection of glucose within a wide concentration range of 10 nM-1 mM. Our OECTs based on photo-annealed plasmonic AuNP-doped PEDOT:PSS may find great applications in chemical and biological sensing, and this strategy may be extended to prepare many other high-performance OECT-based devices.

Hydrogel-Based Flexible Electronics.

Flexible electronics is an emerging field of research involving multiple disciplines, which include but not limited to physics, chemistry, materials science, electronic engineering, and biology. However, the broad applications of flexible electronics are still restricted due to several limitations, including high Young's modulus, poor biocompatibility, and poor responsiveness. Innovative materials aiming for overcoming these drawbacks and boost its practical application is highly desirable. Hydrogel is a class of 3D crosslinked hydrated polymer networks, and its exceptional material properties render it as a promising candidate for the next generation of flexible electronics. Here, the latest methods of synthesizing advanced functional hydrogels and the state-of-art applications of hydrogel-based flexible electronics in various fields are reviewed. More importantly, the correlation between properties of the hydrogel and device performance is discussed here, to have better understanding of the development of flexible electronics by using environmentally responsive hydrogels. Last, perspectives on the current challenges and future directions in the development of hydrogel-based multifunctional flexible electronics are provided.

Metal corrosion for nanofabrication.

The annual cost of corrosion has been increasing globally, and it has now reached beyond 3% of the world's gross domestic product. It remains a challenge to reduce or prevent unwanted corrosion effectively after many decades of effort. Nowadays, more efforts are being made to develop anti-corrosion platforms for decreasing the huge cost of corrosion. In parallel, it is also highly expected to be able to use corrosion for producing useful materials with reduced energy consumption. In this review, recent progress in how methods for controlling metal corrosion can be used to produce structure-diversified nanomaterials are summarized along with a presentation of their applications. As a valuable addition to the scientists' toolbox, metal corrosion strategies can be applied to different metals and their alloys for the production of various nanostructured materials; this also provides insights into how metal corrosion can be further prevented and into how corrosion wastage can be reduced.

Introduction to flexible nanomaterials: microscopic mechanisms and macroscopic applications.

Yuan Cheng, Zibiao Li, Junfeng Gao, Hai-Dong Yu and Gang Zhang introduce this themed collection on flexible nanomaterials.

Simple, Skin-Attachable, and Multifunctional Colorimetric Sweat Sensor.

In situ analysis of sweat provides a simple, convenient, cost-effective, and noninvasive approach for the early diagnosis of physical illness in humans and is particularly useful in family care. In this study, a flexible and skin-attachable colorimetric sweat sensor for multiplexed analysis is developed using a simple, cost-effective, and convenient method. The obtained sweat sensor can be used to simultaneously detect glucose, lactate, urea, and pH value in sweat, as well as sweat loss and skin temperature. Only 2.5 µL of sweat is enough for the whole test, and the sweat loss and chemical-sensing results can be read out conveniently by naked eyes or a smartphone. In addition, body temperature can also be detected with an additional electrical circuit. Our sweat sensor provides a new, cost-effective, and convenient approach for in vitro diagnosis of multiple components in sweat, and the easy fabrication and cost-effectiveness make our sensor commercializable in the near future.

Facile Fabrication of Lignin-Cellulose Green Nanogels.

There has been increasing exploration of the development and production of biodegradable polymers in response to issues with petrol-based polymers and their impact on the environment. Here we report a new approach to synthesize a natural nanogel from lignin and nanocellulose. First, lignin nanobeads were synthesized by a solvent-shifting method, which showed a spherical shape with a diameter of 159.7 nm. Then the lignin nanobeads were incorporated into a nanocellulose network to form the lignin/cellulose nanogels. The nanocellulose fibrils (CNF-C) nanogels reveal a higher storage modulus than the nanocellulose crystal (CNC-C) ones due to the denser network with self-entanglement of longer cellulose chains. The presence of lignin nanobeads in the nanogels helped to increase the viscoelasticity of the nanogels. This work highlights that the new kinds of green nanogels could be potentially utilized in a variety of biomedical applications such as drug delivery and wound dressing.

Recent Development of Gas Sensing Platforms Based on 2D Atomic Crystals.

Sensors, capable of detecting trace amounts of gas molecules or volatile organic compounds (VOCs), are in great demand for environmental monitoring, food safety, health diagnostics, and national defense. In the era of the Internet of Things (IoT) and big data, the requirements on gas sensors, in addition to sensitivity and selectivity, have been increasingly placed on sensor simplicity, room temperature operation, ease for integration, and flexibility. The key to meet these requirements is the development of high-performance gas sensing materials. Two-dimensional (2D) atomic crystals, emerged after graphene, have demonstrated a number of attractive properties that are beneficial to gas sensing, such as the versatile and tunable electronic/optoelectronic properties of metal chalcogenides (MCs), the rich surface chemistry and good conductivity of MXenes, and the anisotropic structural and electronic properties of black phosphorus (BP). While most gas sensors based on 2D atomic crystals have been incorporated in the setup of a chemiresistor, field-effect transistor (FET), quartz crystal microbalance (QCM), or optical fiber, their working principles that involve gas adsorption, charge transfer, surface reaction, mass loading, and/or change of the refractive index vary from material to material. Understanding the gas-solid interaction and the subsequent signal transduction pathways is essential not only for improving the performance of existing sensing materials but also for searching new and advanced ones. In this review, we aim to provide an overview of the recent development of gas sensors based on various 2D atomic crystals from both the experimental and theoretical investigations. We will particularly focus on the sensing mechanisms and working principles of the related sensors, as well as approaches to enhance their sensing performances. Finally, we summarize the whole article and provide future perspectives for the development of gas sensors with 2D materials.