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The phenomenon of flexoelectricity, wherein mechanical deformation induces alterations in the electron configuration of metal oxides, has emerged as a promising avenue for regulating electron transport. Leveraging this mechanism, stress sensing can be optimized through precise modulation of electron transport. In this study, the electron transport in 2D ultra-smooth In2O3 crystals is modulated via flexoelectricity. By subjecting cubic In2O3 (c-In2O3) crystals to significant strain gradients using an atomic force microscope (AFM) tip, the crystal symmetry is broken, resulting in the separation of positive and negative charge centers. Upon applying nano-scale stress up to 100 nN, the output voltage and power values reach their maximum, e.g. 2.2 mV and 0.2 pW, respectively. The flexoelectric coefficient and flexocoupling coefficient of c-In2O3 are determined as ≈0.49 nC m-1 and 0.4 V, respectively. More importantly, the sensitivity of the nano-stress sensor upon c-In2O3 flexoelectric effect reaches 20 nN, which is four to six orders smaller than that fabricated with other low dimensional materials based on the piezoresistive, capacitive, and piezoelectric effect. Such a deformation-induced polarization modulates the band structure of c-In2O3, significantly reducing the Schottky barrier height (SBH), thereby regulating its electron transport. This finding highlights the potential of flexoelectricity in enabling high-performance nano-stress sensing through precise control of electron transport.
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Non-precious metals have been considered as suitable alternatives for high-performance hydrogen evolution reactions (HER). Although the incorporation of carbon substances is shown to improve the number of active sites, electron transfer pathways, and long-term stability, there have been rare reports on their single-step scalable production. Herein, we realize free-standing two-dimensional (2D) carbon sheets heterostructured with nickel (Ni) nanocatalysts by pyrolyzing ultrathin layers of acetate tetrahydrate (i.e. the single precursor for both Ni and C sources) over water-soluble salt crystals. Such a salt-templated methodology is environmentally friendly and readily scalable without the implementation of sophisticated equipment. The resulting 2D carbon sheets exhibit an average small thickness of â¼ 3 nm and lateral dimensions with tens of micrometers, where a large number of nano-sized Ni particles with an average diameter of 14 nm are uniformly dispersed. Such 2D Ni-C sheets demonstrate a small overpotential of 111 mV at 10 mA/cm2 and a low Tafel slope of 86 mV/dec for HER in 1 M KOH, which is significantly improved over those of reported non-precious metals composited with carbon substances. This work offers new insight into the design and practical production of non-precious metal matrixes for economical HER.
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Organic framework materials, particularly metal-organic frameworks (MOFs), graphene-organic frameworks (GOFs), and covalent organic frameworks (COFs), have led to the revolution across fields including catalysts, sensors, gas capture, and biology mainly owing to their ultra-high surface area-to-volume ratio, on-demand tunable crystal structures, and unique surface properties. While the wet chemistry routes have been the predominant synthesis approach, the crystal phase, morphological parameters, and physicochemical properties of organic framework materials are largely affected by various synthesis parameters and precursors. In this work, we specifically review the influences of synthesis parameters towards crystal structures and chemical compositions of organic framework materials, including selected ligand types and lengths, reaction temperature/solvent/reactant compositions, as well as post-synthesis modification approaches. More importantly, the subsequent impacts on the general electronic, mechanical, surface chemical, and thermal properties as well as the consequent variation in performances towards catalytic, desalination, gas sensing, and gas storage applications are critically discussed. Finally, the current challenges and prospects of organic framework materials are provided.
Assuntos
Estruturas Metalorgânicas , Catálise , Ligantes , Estruturas Metalorgânicas/química , Propriedades de SuperfícieRESUMO
Two-dimensional (2D) metal oxides and chalcogenides (MOs & MCs) have been regarded as a new class of promising electro- and photocatalysts for many important chemical reactions such as hydrogen evolution reaction, CO2 reduction reaction and N2 reduction reaction in virtue of their outstanding physicochemical properties. However, pristine 2D MOs & MCs generally show the relatively poor catalytic performances due to the low electrical conductivity, few active sites and fast charge recombination. Therefore, considerable efforts have been devoted to engineering 2D MOs & MCs by rational structural design and chemical modification to further improve the catalytic activities. Herein, we comprehensively review the recent advances for engineering technologies of 2D MOs & MCs, which are mainly focused on the intercalation, doping, defects creation, facet design and compositing with functional materials. Meanwhile, the relationship between morphological, physicochemical, electronic, and optical properties of 2D MOs & MCs and their electro- and photocatalytic performances is also systematically discussed. Finally, we further give the prospect and challenge of the field and possible future research directions, aiming to inspire more research for achieving high-performance 2D MOs & MCs catalysts in energy storage and conversion fields.
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Two-dimensional (2D) metal oxides (MOs) have attracted a considerable amount of attention for various biological applications due to their unique physicochemcial properties such as high photothermal response, temperature superconductivity, photoluminescence, flexibility, unique catalytic capability, plasmonic tunability and relatively low toxicity. However, the sophisticated physiological environments in biosystems stimulate various explorations of surface functionalization to improve the dispersity, stability and biocompatibility of 2D MOs. Moreover, 2D MOs exhibit remarkably tuneable properties via creating oxygen vacancies or doping, which endow 2D MOs with additional capabilities in biological applications. The large surface to volume ratio inherent in these materials also allows easy functionalization and maximal interaction with the external environment. Much work has been done in tailoring 2D MOs through physical/chemical functionalization for use in a diverse range of biomedical applications such as biosensors, bioimaging, drug/gene delivery carriers or even as therapeutic agents. In this review, current progress on 2D MOs functionalized for various biological applications will be presented. Additional relevant issues concerning the research challenges, technology limitations, and future trends have also been discussed.
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Materiais Biocompatíveis/química , Técnicas Biossensoriais , Metais/química , Imagem Óptica , Óxidos/química , Animais , Materiais Biocompatíveis/farmacologia , Portadores de Fármacos/química , Portadores de Fármacos/farmacologia , Humanos , Metais/farmacologia , Óxidos/farmacologiaRESUMO
A strategy is described for the direct preparation of Au nanoparticles (AuNPs) on a Fe-based support, coated with porous carbon (PC), via pyrolysis of an AuCN functionalised Prussian Blue (PB) metal organic framework (MOF). The composite starting material was prepared with an even distribution of AuCN on the surface via galvanic exchange of PB with a gold salt in solution. The resulting structures after pyrolysis were shown to be active Au-based nanomaterials for model applications including catalysis (4-nitrophenol reduction) and electroanalysis (arsenic (III) detection), suggesting broad application where Au nanoparticles are required at a liquid-solid interface. The Fe based support was seen to consist of Fe, Fe3C and Fe4C phases, and the carbon coating increased the stability and improved the conductivity of the materials. The temperature of pyrolysis was seen to affect the activity of the supported nanoparticles, with an increased Au surface area obtained at the higher pyrolysis temperature (650⯰C) tested. A general strategy is thus confirmed for preparation of noble metal nanoparticles evenly distributed on a magnetic support, allowing easy separation of catalysts from products in heterogeneous applications.