Latest ArticlesNanomaterials provide an ideal platform for biomolecular display due to their dimensions approach the molecular scale, facilitating binding behavior akin to that observed in solution-based processes. DNA nanoprobes hold great promise as miniature detectives capable of detecting miRNAs within cells. However, current nanoprobes face a challenge in achieving the required precision for accurate miRNA detection, particularly within the intricate confines of the cellular microenvironment, due to interference with biological autofluorescence, off-target effects, and a lack of spatiotemporal control. Here, we have designed a dual-stimuli responsive DNA tracker, synergistically utilizing specific intracellular cues and external triggers, which enables spatiotemporal-controlled and precise detection and imaging of miRNAs "on demand". The tracker, which combines zeolitic imidazolate framework-67 (ZIF-67) and unique hairpin DNA structures, effectively anchored onto the ZIF-67 through electrostatic interactions, remains in a dormant state until activated by abundant cellular ATP, resulting in the release of the hairpin structures that include a PC linker incorporated into the loop region. Subsequent irradiation triggers specific recognition of the target miRNA. The newly developed HP-PC-BT@ZIF-67 tracker demonstrates precise spatiotemporal miRNA detection and exhibits excellent biocompatibility, enabling specific miRNA recognition "on demand" within cancer cells. This research presents a reliable miRNA imaging platform in the intricate cellular environment, opening up the possibilities for precise biomedical analysis and disease diagnosis.
Exploring transition metal sulfide electrocatalysts with high-efficiency for hydrogen evolution reaction (HER) is essential to produce H2 fuel through water splitting. Herein, novel nickel tungsten sulfide heterojunction (NiS-WS2) with a nanowoven ball-like structure were directed synthetized by a facile hydrothermal method. The hierarchical NiS-WS2 exhibited excellent HER activity with a relatively small overpotential of 142 and 137 mV at 10 mA/cm2 in 0.5 mol/L H2SO4 and 1 mol/L KOH, which is much better than that of single NiS and WS2. The impressive performance of NiS-WS2 heterojunction is owed to the collective synergy of special morphological and more exposed active sites between the crystal interfacial of NiS and WS2. In addition, the hierarchical NiS-WS2 can facilitate the transport of charge/mass by optimized electronic structure, which further improves the HER activity of electrocatalysts. These outcomes provide a simple method to prospect towards the design and application of heterostructures as efficient electrocatalysts, shedding some light on the development of functional materials in energy chemistry.
Multiple switchable physical channels within one material or device, encompassing optical, electrical, thermal, and mechanical pathways, can enable multifunctionality in mechanical-thermal-opto-electronic applications. Achieving integrated encryption and enhanced performance in storage and sensing presents a formidable challenge in the synthesis and functionality of new materials. In an effort to overcome the complexities associated with these multiple physical functions, this study investigates the large-size crystal of DPACdCl4 (DPA = diisopropylammonium), revealing significant features in rare multi-channel switches. This compound demonstrates the ability to switch between "OFF/0" and "ON/1" states in the mechanical-thermal-opto-electronic channels. Consequently, DPACdCl4 possesses four switchable physical channels, characterized by a higher phase transition temperature of 440.7 K and a competitive piezoelectric coefficient of 46 pC/N. Furthermore, solid-state NMR analysis indicates that thermally activated molecular vibrations significantly contribute to its multifunctional switching capabilities.
Designing highly active electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution and reduction reactions (OER and ORR) is pivotal to renewable energy technology. Herein, based on density functional theory (DFT) calculations, we systematically investigate the catalytic activity of iron-nitrogen-carbon based covalent organic frameworks (COF) monolayers with axially coordinated ligands (denotes as FeN4-X@COF, X refers to axial ligand, X = -SCN, -I, -H, -SH, -NO2, -Br, -ClO, -Cl, -HCO3, -NO, -ClO2, -OH, -CN and -F). The calculated results demonstrate that all the catalysts possess good thermodynamic and electrochemical stabilities. The different ligands axially ligated to the Fe active center could induce changes in the charge of the Fe center, which further regulates the interaction strength between intermediates and catalysts that governs the catalytic activity. Importantly, FeN4-SH@COF and FeN4OH@COF are efficient bifunctional catalysts for HER and OER, FeN4OH@COF and FeN4-I@COF are promising bifunctional catalysts for OER and ORR. These findings not only reveal promising bifunctional HER/OER and OER/ORR catalysts but also provide theoretical guidance for designing optimum iron-nitrogen-carbon based catalysts.
Phosphorus-based anode is a promising anode for sodium-ion batteries (SIBs) due to its high specific capacity, however, suffers from poor electronic conductivity and unfavorable electrochemical reversibility. Incorporating metals such as copper (Cu) into phosphorus has been demonstrated to not only improve the electronic conductivity but also accommodate the volume change during cycling, yet the underline sodiation mechanism is not clear. Herein, take a copper phosphide and reduced graphene oxide (CuP2/C) composite as an example, which delivers a high reversible capacity of > 900 mAh/g. Interestingly, it is revealed that the native oxidation PO components of the CuP2/C composite show higher electrochemical reversibility than the bulk CuP2, based on a quantitative analysis of high-resolution solid-state 31P NMR, ex-situ XPS and synchrotron X-ray diffraction characterization techniques. The sodiation products Na3PO4 and Na4P2O7 derived from PO could react with Na-P alloys and regenerate to PO during charge process, which probably accounts for the high reversible capacity of the CuP2/C anode. The findings also illustrate that the phosphorus transforms into nanocrystalline Na3P and NaP alloys, which laterally shows crystallization-amorphization evolution process during cycling.
Customized design of well-defined cathode structures with abundant adsorption sites and rapid diffusion dynamics, holds great promise in filling capacity gap of carbonaceous cathodes towards high-performance Zn-ion hybrid supercapacitors (ZHC). Herein, we fabricate a series of dynamics-oriented hierarchical porous carbons derived from the unique organic-inorganic interpenetrating polymer networks. The interpenetrating polymer networks are obtained through physically knitting polyferric chloride (PFC) network into the highly crosslinked resorcinol-formaldehyde (RF) network. Instead of covalent bonding, physical interpenetrating force in such RF-PFC networks efficiently relieves the RF skeleton shrinkage upon pyrolysis. Meanwhile, the in-situ PFC network sacrifices as a structure-directing agent to suppress the macrophase separation, and correspondingly 3D hierarchical porous structure with plentiful ion-diffusion channels (pore volume of 1.35 cm3/g) is generated in the representative HPC4 via nanospace occupation and swelling effect. Further removal of Fe fillers leaves behind a large accessible specific surface area of 1550 m2/g for enhanced Zn-ion adsorption. When used as the cathode for ZHC, HPC4 demonstrates a remarkable electrochemical performance with a specific capacity of 215.1 mAh/g at 0.5 A/g and a high Zn2+ ion diffusion coefficient of 11.1 × 10−18 cm2/s. The ZHC device yields 117.0 Wh/kg energy output at a power density of 272.1 W/kg, coupled with good cycle lifespan (100,000 cycles@10 A/g). This work inspires innovative insights to accelerate Zn diffusion dynamics by structure elaboration towards high-capacity cathode materials.
As the global population ages, osteoporotic bone fractures leading to bone defects are increasingly becoming a significant challenge in the field of public health. Treating this disease faces many challenges, especially in the context of an imbalance between osteoblast and osteoclast activities. Therefore, the development of new biomaterials has become the key. This article reviews various design strategies and their advantages and disadvantages for biomaterials aimed at osteoporotic bone defects. Overall, current research progress indicates that innovative design, functionalization, and targeting of materials can significantly enhance bone regeneration under osteoporotic conditions. By comprehensively considering biocompatibility, mechanical properties, and bioactivity, these biomaterials can be further optimized, offering a range of choices and strategies for the repair of osteoporotic bone defects.
Vascular disrupting agents (VDAs) can destroy tumor vasculature and lead to tumor ischemia and hypoxia, resulting in tumor necrosis. However, VDAs are easy to induce the upregulation of genes that are associated with cancer cell drug resistance and angiogenesis in tumor cells. Hypoxia-activated chemotherapy will be an ideal supplement to VDAs therapy since it can help to fully utilize the ischemia and hypoxia induced by VDAs to realize a synergistic antitumor therapeutic outcome. Here, we design a liposome whose surface is modified with a tumor-homing peptide Cys-Arg-Glu-Lys-Ala (CREKA, which can specifically target tumor vessels and stroma) and whose aqueous cavity and lipid bilayer are loaded by a hypoxia-activatable drug banoxantrone dihydrochloride (AQ4N) and a VDA combretastatin A4 (CA4), respectively. CA4 can selectively target vascular endothelial cells and destroy the tumor blood vessels, which will cause the rapid inhibition of blood flow in tumor and enhance the hypoxia in the tumor region. As a consequence, AQ4N can exert its boosted cytotoxicity under the enhanced hypoxic environment. The as-prepared liposome with a uniform particle size exhibits good stability and high cancer cell killing efficacy in vitro. In addition, in vivo experiments confirm the excellent tumor-targeting/accumulation, tumor vasculature-damaging, and tumor inhibition effects of the liposome. This work develops a liposomal which can achieve safe and effective tumor suppression without external stimulus excitation by only single injection, and is expected to benefit the future development of effective antitumor liposomal drugs.
High-efficient rubber antioxidants for enhanced heat resistance without compromising mechanical properties remain an enormous and long-term challenge for the rubber industry. Herein, we employed the in-situ growth of Ce-doped Co-metal-organic framework (CeCo-MOF) in dendritic mesoporous organosilica nanoparticles (DMONs@CeCo-MOF, denoted as DCCM) to prepare a novel antioxidant that exhibit outstanding thermal stability. Dendritic mesoporous organosilica nanoparticles (DMONs) effectively alleviated the incompatibility of CeCo-MOF in the polymer matrix, and the effective scavenging of free radicals was attributed to the various oxidation states of metal ions in CeCo-MOF. Surprising, by adding only 0.5 phr (parts per hundred of rubber) of DMONs@CeCo-MOF to silicone rubber, (SR), the retention rate of tensile strength increased from 37.3% to 61.6% after aging 72 h at 250 ℃, and the retention rate of elongation at break of DCCM/SR1 composites reached 68%, which was 5.43 times of SR. The strategy of anchoring MOFs on the surface of silica also provides a viable method for preparing effective compound functionalized rubber antioxidant.
All-solid-state Li batteries (ASSLBs) using solid electrolytes (SEs) have gained significant attention in recent years considering the safety issue and their high energy density. Despite these advantages, the commercialization of ASSLBs still faces challenges regarding the electrolyte/electrodes interfaces and growth of Li dendrites. Elemental doping is an effective and direct method to enhance the performance of SEs. Here, we report an Al-F co-doping strategy to improve the overall properties including ion conductivity, high voltage stability, and cathode and anode compatibility. Particularly, the Al-F co-doping enables the formation of a thin Li-Al alloy layer and fluoride interphases, thereby constructing a relatively stable interface and promoting uniform Li deposition. The similar merits of Al-F co-doping are also revealed in the Li-argyrodite series. ASSLBs assembled with these optimized electrolytes gain good electrochemical performance, demonstrating the universality of Al-F co-doping towards advanced SEs.
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