Latest ArticlesA decomposable and sono-enzyme co-triggered nanoparticle (pTCP-CR NP) with “AND gate” logic was synthesized, combining a meso‑carboxyl-porphyrin-based sonosensitizer (5,10,15,20-tetrakis(carboxyl)porphyrin, TCP) and a thiophenyl-croconium (2,5-bis[(2-(2-(2-hydroxyethoxy)ethoxy)ethyl-4-carboxylate-piperidylamino)thiophenyl]-croconium, CR) via ester groups. TCP releases carbon monoxide (CO) under ultrasound (US) irradiation, offering both sonodynamic and gas therapy. CR decomposes into stronger reactive oxygen species (ROS) compared to oxygen-based radicals. The Förster resonance energy transfer (FRET) effect between TCP and CR inhibits ROS and CO generation until triggered by tumor cell overexpressed carboxylesterase (CEs). pTCP-CR NPs “AND gate” logic ensures activation only in the presence of both CEs and US, targeting tumor cells while safety in normal tissues. The ROS and CO generation abilities, as well as the releasing of SO4•− have been systemically examined. pTCP-CR can be thoroughly decomposed into low-toxic molecules post the treatment, showing the safety with negligible phototoxic reactions. In vivo anti-cancer therapy has been evaluated using mice bearing hepatocellular carcinoma.
Developing BiVO4 photoanode with efficient carrier transfer and fast water oxidation kinetics is the permanent pursuit to achieve the state-of-art solar-driven photoelectrochemical (PEC) water splitting. The capacity to increase the PEC activity of BiVO4 by loading oxygen evolution co-catalysts (OECs) has been proven, however it suffers from sluggish charge carriers dynamics brought on by the complicated interface between BiVO4 and OECs as well as poor long-term durability. Herein, we connected OECs (NiFeOx) and photoanode with a Al-O bridge for bettering the PEC performance of BiVO4. The Al-O bridge served as a channel to extract hole from BiVO4 to NiFeOx, thus boosting charge carriers′ separation and preventing BiVO4 from photo-corrosion. The Al-O bridging photoanode (NiFeOx/Al2O3/BiVO4) demonstrated a high photocurrent density of 5.87 mA/cm2 at 1.23 V vs. RHE and long-term photostability in comparison to NiFeOx/BiVO4 photoanode. This study proposes a unique technique to boost charge carriers′ separation between BiVO4 and OECs for high-efficiency solar-driven PEC water splitting.
Glioma is the most common malignant tumor of the brain. The postoperative recurrence rate was high, and the 2-year survival rate only increased by 20%–25%. The reason is the blood-brain barrier (BBB). BBB is a physical barrier that stabilizes the physiological environment of brain tissue and protects the central nervous system from the invasion of harmful substances. Drug delivery based on nanotechnology and nanocarriers has attracted much attention due to its biological safety, continuous drug release time, increasing solubility, biological drug activity, and enhanced BBB permeability. By modifying different substances on the surface of nanocarriers, the BBB is bypassed by receptor-mediated and cell endocytosis and exocytosis. In addition, the purpose of bypassing BBB-targeted drug delivery can also be achieved by intranasal administration and local administration. This paper reviews different target transport mechanisms, mainly in invasive and non-invasive strategies, the nanocarriers that have made progress and the nanocarrier strategy of bypassing BBB are listed.
Degrading volatile organic compounds at low temperatures and active sites aggregation are still challenging. In this study, a novel mesoporous zeolite silicalite-1 (S-1-meso) enveloped Pt–Ni bimetallic catalysts (noted as Pt1Ni1@S-1-meso) were synthesized via a facile in situ mesoporous template-free method. The Pt–Ni bimetallic nanoparticles were uniformly distributed and displayed a large specific surface area and enriched mesopores to facilitate the deep oxidation of toluene. The presence of the Pt–NiO interface both increased the dispersion of the catalyst and improved its catalytic performance, thereby reducing the consumption of Pt. The Mars-van Krevelen mechanism and density function theory (DFT) calculations revealed that the Pt–NiO interface effect changed the electronic structure of Pt and Ni species, reduced the activation potential for oxygen, formed reactive oxygen species, and facilitated the adsorption and activation of reactants in the direction favorable to the toluene oxidation. This study provides a guideline for minimizing the proportion of precious metals used in practical applications and a promising method for toluene elimination at low temperatures.
Photoheranostics have emerged as a promising tool for cancer theranostics owing to their real-time feedback on treatment and their precise diagnosis. Among them, how to improve the photothermal conversion efficiency (PCE) of phototheranostic agents (PTAs) is the key factor for phototheranostic systems. Herein, we provided an efficient method to improve PCE and constructed a biocompatible nano-material ICR-Qu@NH2-Fe3O4@PEG (QNFP) by combing near-infrared second region (NIR-Ⅱ) molecular dye ICR-Qu and amino-modified magnetic nanoparticles and then encapsulated by DSPE-mPEG2000. QNFP exhibited excellent performance for photothermal therapy with a high PCE of 95.6%. Both in vitro and in vivo experiments indicated that QNFP could inhibit the growth of tumors under laser irradiation with low toxicity and realized real-time NIR-Ⅱ fluorescent imaging of tumors. In general, we realized a simple but efficient method to improve the PCE of NIR-Ⅱ molecular dye without reduce its quantum yield, which is an ideal choice for cancer diagnosis and treatment.
In recent years, sodium-ion batteries (SIBs) have become one of the hot discussions and have gradually moved toward industrialization. However, there are still some shortcomings in their performance that have not been well addressed, including phase transition, structural degradation, and voltage platform. High entropy materials have recently gained significant attention from researchers due to their effects on thermodynamics, dynamics, structure, and performance. Researchers have attempted to use these materials in sodium-ion batteries to overcome their problems, making it a modification method. This paper aims to discuss the research status of high-entropy cathode materials for sodium-ion batteries and summarize their effects on sodium-ion batteries from three perspectives: Layered oxide, polyanion, and Prussian blue. The influence on material structure, the inhibition of phase transition, and the improvement of ion diffusivity are described. Finally, the advantages and disadvantages of high-entropy cathode materials for sodium-ion batteries are summarized, and their future development has prospected.
Idiopathic pulmonary fibrosis (IPF) is a progressive lung disease with high mortality rate but effective therapeutics are still lacking. Phosphodiesterase-4 (PDE4) inhibitors were reported to be promising anti-IPF agents. Herein, series of biflavonoids isolated from Selaginella uncinate were found to be PDE4 inhibitors and the most active amentoflavone gave a half maximal inhibitory concentration (IC50) of 12 nmol/L, which was further validated by isothermal titration calorimetry with Kd of 23 nmol/L. Besides, co-crystal structure of PDE4-amentoflavone was determined and gave a different binding pattern from roflumilast with multiple H-bonds between it and key residues such as Asn321/Thr333/Gln369/Gly371. So far, this was the first reported co-crystal structure of amentoflavone with its potential binding target in despite of the extensive investigations of this common natural biflavonoid. Furthermore, amentoflavone exhibited remarkable anti-IPF effects in vivo and in vitro, suggesting it as a novel anti-fibrotic agent by targeting PDE4.
A highly sensitive zinc ion fluorescent probe NOD-NY with controlled release of nitric oxide was designed, synthesized and used for tracking intracellular zinc ions in living A549 cells. NOD-NY was prepared from naphthalimide as the fluorophore and N,N-bis(2-pyridylmethyl)amine as the zinc ion recognition receptor, the amide N atom of the naphthalimide was connected to n-butylamine. Under the irradiation of ultraviolet light, NOD-NY can quantitatively release nitric oxide and generate a highly sensitive zinc ion probe Zn-HN, accompanied by a red-shift process of maximum ultraviolet absorption from 350 nm to 450 nm. Upon addition of Zn2+ to the solutions of Zn-HN, a remarkable fluorescence enhancement was observed, which could be attributed to the photo-induced electron transfer (PET) mechanism. By replaced the n-butylamine on NOD-NY with diethylene glycolamine or triphenylphosphine structures, NOD-AY with good biocompatibility and NOD-BY that can target mitochondria were obtained respectively. In addition, the nitric oxide released by NOD-NY enriched in lysosome can diffuse into mitochondria. The released nitric oxide can stimulate metallothionein to release zinc ions, and the light-induced in situ generated zinc ion probe Zn-HN can have a highly sensitive fluorescence response to free zinc ions in living A549 cells.
A strategy for copper-catalyzed and biphosphine ligand controlled boracarboxylation of 1,3-dienes and CO2 with 3,4-selectivity was developed. The CuCl coupled with DPPF (1,1′-bis(diphenylphosphino)ferrocene) was assigned to be the best catalyst, with 84% yield and exclusive 3,4-selectivity. The ligand effect on both catalytic activity and regioselectivity of boracarboxylation was disclosed, which is rarely reported in any copper catalyzed boracarboxylation. The borocupration process is revealed to be a vital step for the biphosphine participated boracarboxylation of 1,3-dienes with CO2. The minimal substrate distortion occurring in 3,4-borocupration favors the 3,4-regioselectivity of boracarboxylation. The “pocket” confinement and suitable βn (92°–106°) of bisphosphine ligands are demonstrated to be in favour of the interaction between LCu-Bpin complex (the catalytic precursor) and 1,3-diene substrate to decrease their interaction energy ∆Eint(ζ) in 3,4-borocupration, thus promoting the 3,4-boracarboxylation.
Tuning the nanozyme′s activity and specificity is very crucial for developing highly sensitive sensors for various applications. Herein, selenium-doped porous N-doped carbon skeletons (Se/NC) nanozymes with highly specific peroxidase-like activity were synthesized by a MOF-pyrolysis-doping protocol. Se doping adjusted the electronic structure of NC by introducing more vacancies, defective carbon and graphitic N, and endowed the resultant Se/NC enhanced charge transfer and substrate affinity. The Se/NC exhibited specific peroxidase-mimicking activity and could catalyze 3,3′,5,5′-tetramethylbenzidine oxidation by H2O2. Density functional theory (DFT) calculations and experimental trials indicated that both Se=O and C–Se–C species were the main active sites of Se/NC. The C–Se–C bond is the main catalytic active site endowing Se/NC with the property of nanozyme, while the Se=O bond effectively enhances its affinity to H2O2 and accelerate H2O2 dissociation. The Se/NC showed an approximately 185-fold increase in peroxidase-like activity compared to NC. Based on the inhibition of the peroxidase-like activity of Se/NC by methimazole, a colorimetric sensor was developed to achieve its sensitive detection with 2 nmol/L of limit of detection. It was successfully used for detecting methimazole in real samples. Current Se doping strategy simplifies the fabrication process of high performance specific nanozyme and promises great potential for environmental analysis.
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