Two-dimensional (2D) ultrathin SiC has received intense attention due to its broad band gap and resistance to large mechanical deformation and external chemical corrosion. However, the synthesis and application of ultrasmall 2D SiC quantum dots (QDs) has not been explored. Herein, we synthesize a type of monolayered 2D SiC QDs with advanced photoluminescence (PL) properties via a facile hydrothermal route. Their average size and thickness can be easily adjusted by altering the reaction time. The ultrasmall 2D SiC QDs exhibit a long fluorescence lifetime of 2.59 μs due to efficient quantum confinement. The applications of SiC QDs are demonstrated through labeling A549, HeLa, and NHDF cells and delivering agents for intracellular low-abundant microRNA (miRNA) detection. This advance in preparing photoluminescent SiC QDs is of great significance for broadening their potential in biomedical and optical applications.
Photoluminescence (PL) of transition metal dichalcogenides (TMDs) can be engineered by controlling the density of defects, which provide active sites for electron-hole recombination, either radiatively or non-radiatively. However, the implantation of defects by external stimulation, such as uniaxial tension and irradiation, tends to introduce local damages or structural non-homogeneity, which greatly degrades their luminescence properties and impede their applicability in constructing optoelectronic devices. In this paper, we present a strategy to introduce a controllable level of defects into the MoS2 monolayers by adding a hydrogen flow during the chemical vapor deposition, without sacrificing their luminescence characteristics. The density of the defect is controlled directly by the concentration of hydrogen. For an appropriate hydrogen flux, the monolayer MoS2 sheets have three times stronger PL emission at the excitonic transitions, compared with those samples with nearly perfect crystalline structure. The defect-bounded exciton transitions at lower energies arising in the defective samples and are maximized when the total PL is the strongest. However, the B exciton, exhibits a monotonic decline as the defect density increases. The Raman spectra of the defective MoS2 reveal a redshift (blueshift) of the in-plane (out-of-plane) vibration modes as the hydrogen flux increases. All the evidence indicates that the generated defects are in the form of sulfur vacancies. This study renders the high-throughput synthesis of defective MoS2 possible for catalysis or light emitting applications.
Atomic composition tuning and defect engineering are effective strategies toenhance the catalytic performance of multicomponent catalysts by improvingthe synergetic effect; however, it remains challenging to dramatically tune the active sites on multicomponent materials through simultaneous defect engineeringat the atomic scale because of the similarities of the local environment. Herein,using the oxygen evolution reaction (OER) as a probe reaction, we deliberatelyintroduced base-soluble Zn(II) or Al(III) sites into NiFe layered double hydroxides(LDHs), which are one of the best OER catalysts. Then, the Zn(II) or Al(III) siteswere selectively etched to create atomic M(II)/M(III) defects, which dramaticallyenhanced the OER activity. At a current density of 20 mA·cm?2, only 200 mV overpotential was required to generate M(II) defect-rich NiFe LDHs, which is the best NiFe-based OER catalyst reported to date. Density functional theory(DFT) calculations revealed that the creation of dangling Ni–Fe sites (i.e., unsaturated coordinated Ni–Fe sites) by defect engineering of a Ni–O–Fe site at the atomic scale efficiently lowers the Gibbs free energy of the oxygen evolutionprocess. This defect engineering strategy provides new insights into catalysts atthe atomic scale and should be beneficial for the design of a variety of catalysts.
Although gas-filled microbubbles with high echogenicity are widely applied inclinical ultrasonography, the micron scale particle size impedes their use in the treatment of solid tumors,which are accessible to objects less than several hundred nanometers. We herein propose an unusual approach involving apH-induced core–shell micelle-to-vesicle transition to prepare ultrasound-sensitive polymeric nanospheres (polymersomes in structure) possessing multiple features, including nanosize, monodispersity, and incorporation of a phase-transitional imaging agent into the aqueous lumen. These features are not achievable via the conventional double-emulsion method for polymersome preparation. The nanospheres were constructed based on a novel triblock copolymer with dual pH sensitivity. The liquid-to-gas phase transition of the imaging agent induced by external low-frequency ultrasound may destroy the nanospheres for a rapid drug release, with simultaneous tissue-penetrating drug delivery inside a tumor. These effects may provide new opportunities for the development of an effective cancer therapy with few adverse effects.
Spinel LiMn2O4 is a widely utilized cathode material for Li-ion batteries. However, its applications are limited by its poor energy density and power density. Herein, a novel hierarchical porous onion-like LiMn2O4(LMO) was prepared to shorten the Li+ diffusion pathway with the presence of uniform pores and nanosized primary particles. The growth mechanism of the porous onion-like LiMn2O4 was analyzed to control the morphology and the crystal structure so that it forms a polyhedral crystal structure with reduced Mn dissolution. In addition, graphene was added to the cathode (LiMn2O4/graphene) to enhance the electronic conductivity. The synthesized LiMn2O4/graphene exhibited an ultrahigh-rate performance of 110.4 mAh·g–1 at 50 C and an outstanding energy density at a high power density, maintaining 379.4 Wh·kg–1 at 25,293 W·kg–1. Besides, it shows durable stability, with only 0.02% decrease in the capacity per cycle at 10 C. Furthermore, the (LiMn2O4/graphene)/graphite full-cell exhibited a high discharge capacity. This work provides a promising method for the preparation of outstanding, integrated cathodes for potential applications in lithium ion batteries.
Ribonucleic acids (RNAs) possess great therapeutic potential and can be used to treat a variety of diseases. The unique biophysical properties of RNAs, such as high molecular weight, negative charge, hydrophilicity, low stability, and potential immunogenicity, require chemical modification and development of carriers to enable intracellular delivery of RNAs for clinical use. A variety of nanomaterials have been developed for the effective in vivo delivery of short/ small RNAs, messenger RNAs, and RNAs required for gene editing technologies including clustered regularly interspaced palindromic repeat (CRISPR)/Cas. This review outlines the challenges of delivering RNA therapeutics, explores the chemical synthesis of RNA modifications and carriers, and describes the efforts to design nanomaterials that can be used for a variety of clinical indications. 相似文献
As an attractive alternative to plasmid DNA, messenger RNA (mRNA) has recently emerged as a promising class of nucleic acid therapeutics for biomedical applications. Advances in addressing the inherent shortcomings of mRNA and in the development of nanoparticle-based delivery systems have prompted the development and clinical translation of mRNA-based medicines. In this review, we discuss the chemical modification strategies of mRNA to improve its stability, minimize immune responses, and enhance translational efficacy. We also highlight recent progress in nanoparticle-based mRNA delivery. Considerable attention is given to the increasingly widespread applications of mRNA nanomedicine in the biomedical fields of vaccination, protein-replacement therapy, gene editing, and cellular reprogramming and engineering. 相似文献
The development of photocatalysts that can effectively harvest visible light is essential for advances in high-efficiency solar-driven hydrogen generation. Herein, we synthesized water soluble CuInS2 (CIS) and Cu-In-Zn-S (CIZS) quantum dots (QDs) by using one-pot aqueous method. The CIZS QDs are well passivated by glutathione ligands and are highly stable in aqueous conditions. We subsequently applied these QDs as a light harvesting material for photocatalytic hydrogen generation. Unlike most small band gap materials that show extremely low efficiency, these new QDs display remarkable energy conversion efficiency in the visible and near-infrared regions. The external quantum efficiency at 650 nm is ～1.5%, which, to the best of our knowledge, is the highest value achieved until now in the near-infrared region.
We explore the impact of edge states in three types of transition metal dichalcogenides (TMDs), namely metallic Td-phase WTe2 and semiconducting 2H-phase MoTe2 and MoS2, by patterning thin flakes into ribbons with varying channel widths. No obvious charge depletion at the edges is observed for any of these three materials, in contrast to observations made for graphene nanoribbon devices. The semiconducting ribbons are characterized in a three-terminal field-effect transistor (FET) geometry. In addition, two ribbon array designs have been carefully investigated and found to exhibit current levels higher than those observed for conventional one-channel devices. Our results suggest that device structures incorporating a high number of edges can improve the performance of TMD FETs. This improvement is attributed to a higher local electric field, resulting from the edges, increasing the effective number of charge carriers, and the absence of any detrimental edge-related scattering.
The luminescence of semiconductor quantum dots (QDs) can be adjusted using the piezotronic effect. An external mechanical force applied on the QD generates a piezoelectric potential, which alters the luminescence of the QD. A small mechanical force may induce a significant change on the emission spectrum. In the case of InN QDs, it is demonstrated that the unforced emission wavelength is more than doubled by a force of 1 μN. The strategy of using the piezotronic effect to tune the color of the emission leads to promising noncontact forcemeasurement applications in biological and medical sensors and force-sensitive displays. Several piezoelectric semiconductor materials have been investigated in terms of the tunability of the emission wavelength in the presence of an external applied force. It is found that CdS and CdSe demonstrate much higher tunability δλ/δF, which makes them suitable for micro/nano-newton force measurement applications.
