Graphene quantum dots (GQDs) are great promising in various applications owing to the quantum confinement and edge effects in addition to their intrinsic properties of graphene, but the preparation of the GQDs in bulk scale is challenging. We demonstrated in this work that the micrometer sized graphene oxide (GO) sheets could react with Fenton reagent (Fe(2+)/Fe(3+)/H(2)O(2)) efficiently under an UV irradiation, and, as a result, the GQDs with periphery carboxylic groups could be generated with mass scale production. Through a variety of techniques including atomic force microscopy, X-ray photoelectron spectroscopy, gas chromatography, ultraperformance liquid chromatography-mass spectrometry, and total organic carbon measurement, the mechanism of the photo-Fenton reaction of GO was elucidated. The photo-Fenton reaction of GO was initiated at the carbon atoms connected with the oxygen containing groups, and C-C bonds were broken subsequently, therefore, the reaction rate depends strongly on the oxidization extent of the GO. Given the simple and efficient nature of the photo-Fenton reaction of GO, this method should provide a new strategy to prepare GQDs in mass scale. As a proof-of-concept experiment, the novel DNA cleavage system using as-generated GQDs was constructed.
Conventional metal-organic framework (MOF) powders have periodic micro/mesoporous crystalline architectures tuned by their three-dimensional coordination of metal nodes and organic linkers. To add practical macroscopic shapeability and extrinsic hierarchical porosity, fibrous MOF aerogels were produced by synthesizing MOF crystals on the template of TEMPO-cellulose nanofibrils. Cellulose nanofibrils not only offered extrinsic porosities and mechanical flexibility for the resultant MOF aerogels, but also shifted the balance of nucleation and growth for synthesizing smaller MOF crystals, and further decreased their aggregation possibilities. Thanks to their excellent shapeability, hierarchical porosity up to 99%, and low density below 0.1 g/cm, these MOF aerogels could make the most of their pores and accessible surface areas for higher adsorption capacity and rapid adsorption kinetics of different molecules, in sharp contrast to conventional MOF powders. Thus, this scalable and low-cost production pathway is able to convert MOF powders into a shapeable and flexible form and thereby extend their applications in more broad fields, for example, adapting a conventional filtration setup.
Nanometerization of liquid metal in organic systems can facilitate deposition of liquid metals onto substrates and then recover its conductivity through sintering. Although having broader potential applications, producing stable aqueous inks of liquid metals keeps challenging because of rapid oxidation of liquid metal when exposing to water and oxygen. Here, a biocompatible aqueous ink is produced by encapsulating alloy nanodroplets of gallium and indium (EGaIn) into microgels of marine polysaccharides. During sonicating bulk EGaIn in aqueous alginate solution, alginate not only facilitates the downsizing process via coordination of their carboxyl groups with Ga ions but also forms microgel shells around EGaIn droplets. Due to the deceasing oxygen-permeability of microgel shells, aqueous ink of EGaIn nanodroplets can maintain colloidal and chemical stability for a period of >7 d. Crosslinked alginate-gel with tunable thickness can retard the generation and release of toxic cations, thereby affording high biocompatibility. The soft alginate shells also enable to recover electric conductivity of EGaIn layers by "mechanical sintering" for applications in microcircuits, electric-thermal actuators, and wearable sensors, offering huge potential for electronic tattoos, artificial limbs, electric skins, etc.
Electricity harvest from ubiquitous water has been endeavored, using nanogenerators based on carbon nanomaterials, to acquire renewable and clean energy and cope with fossil depletion and pollution as well. Meanwhile, though many biological organisms can harness water for bioelectricity, it is still challenging to produce biological nanogenerators based on biological nanomaterials with billions of tons of annual production in nature. Herein biological nanofibrils, including cellulose, chitin, silk fibroin, and amyloid, are produced either by liquid-exfoliation of biomasses or by supramolecular assembly of bio-macromolecules. With the intrinsic hydrophilicity and charged states, they can capture moisture from air and form hydrated nanochannels, in analogue to ionic channels of cytomembranes. When exposing their aerogels to moist air flow, there is a balance of water absorption and evaporation, thus producing a streaming potential and an open-circuit voltage across the aerogel. With flexibility, sustainability, biocompatibility, and biodegradability, these biological nanogenerators can harvest electricity from moist air flow in nature (e.g., wind, respiration and perspiration) and in industry, and serve for environmentally-friendly, low-cost, high-efficiency, wearable, and miniaturized power devices.
Due to the high peroxidase-like activity and small lateral size of graphene quantum dots (GQDs), the covalently assembled GQDs/Au electrode exhibits great performance and stability in H(2)O(2) detection. It is better or comparable to some enzyme-immobilized electrodes, and thus could be useful in sensing H(2)O(2) changes in biological systems.
Silk, one of the strongest natural biopolymers, was hybridized with Kevlar, one of the strongest synthetic polymers, through a biomimetic nanofibrous strategy. Regenerated silk materials have outstanding properties in transparency, biocompatibility, biodegradability and sustainability, and promising applications as diverse as in pharmaceutics, electronics, photonic devices and membranes. To compete with super mechanic properties of their natural counterpart, regenerated silk materials have been hybridized with inorganic fillers such as graphene and carbon nanotubes, but frequently lose essential mechanic flexibility. Inspired by the nanofibrous strategy of natural biomaterials (e.g., silk fibers, hemp and byssal threads of mussels) for fantastic mechanic properties, Kevlar was integrated in regenerated silk materials by combining nanometric fibrillation with proper hydrothermal treatments. The resultant hybrid films showed an ultimate stress and Young's modulus two times as high as those of pure regenerated SF films. This is not only because of the reinforcing effect of Kevlar nanofibrils, but also because of the increasing content of silk β-sheets. When introducing Kevlar nanofibrils into the membranes of silk nanofibrils assembled by regenerated silk fibroin, the improved mechanic properties further enabled potential applications as pressure-driven nanofiltration membranes and flexible substrates of electronic devices.
2D nanomaterials have various size/morphology-dependent properties applicable in electronics, optics, sensing, and actuating. However, intensively studied inorganic 2D nanomaterials are frequently hindered to apply in some particular and industrial fields, owing to harsh synthesis, high-cost, cytotoxicity, and nondegradability. Endeavor has been made to search for biobased 2D nanomaterials with biocompatibility, sustainability, and biodegradability. A method of hydrophobization-induced interfacial-assembly is reported to produce an unprecedented type of nanosheets from marine chitin. During this process, two layers of chitin aggregations assemble into nanosheets with high aspect ratio. With super stability and amphiphilicity, these nanosheets have super ability in creating highly stable Pickering emulsions with internal phase up to 83.4% and droplet size up to 140 μm, in analogue to graphene oxide. Combining emulsifying and carbonization can further convert these 2D precursors to carbon nanosheets with thickness as low as ≈3.8 nm. Having biologic origin, conductivity, and dispersibility in various solvents, resultant carbon nanosheets start a new scenario of exploiting marine resources for fully biobased electric devices with sustainability and biodegradability, e.g., supercapacitor, flexible circuits, and electronic sensors. Hybrid films of chitin and carbon nanosheets also offer low-cost and environment-friendly alternative of conductive components desirable in green electronics, wearable electronics, biodegradable circuits, and biologic devices.
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