Latest ArticlesOral squamous cell carcinoma (OSCC) is known as one of the most malignant tumors with high recurrence and fatality rate. The poor tumor-targeting ability of traditional chemotherapeutic drugs has been a grand challenge for anti-OSCC therapy. Beyond that, a large quantity of tumor associated macrophages in OSCC tissues further diminish the anti-tumor effects of these drugs. Therefore, we produced a therapeutic nano drug delivery system (FA-PEG-PLA-JQ1) through encapsulating JQ1 [a small-molecule inhibitor of bromodomain containing protein 4 (BRD4)] into the folic acid (FA)-modified nanoparticle (PEG-PLA), which could prolong the half-life of JQ1 and target the tumor tissues. And then, JQ1 released from this nanoparticle could prevent OSCC growth inducing tumor cell apoptosis, inhibiting tumor angiogenesis and the polarization of M2 type macrophages. In conclusion, our date demonstrated the therapeutic benefits of FA-PEG-PLA-JQ1 against OSCC in vivo or in vitro, which could be a novel treatment strategy for OSCC in coming days.
There are urgent needs of volatile amine gas sensors with high-performance in food quality control, disease monitoring and environmental pollution. Thin-film fluorescent probe is suitable for amine vapour sensing due to its high sensitivity, high selectivity, and no polluting analyte. Herein, a novel fluorescent probe based on indacenodithiophene structure with π conjugated system was designed and synthesized. The experimental results show that the films prepared by this material exhibit rapid and distinct fluorescence quenching after being exposed to saturated vapours of primary amine, secondary amine and tertiary amine represented by n-propylamine, diethylamine and trimethylamine, respectively. The quenching of fluorescence is 84%, 87% and 96%, respectively, within 10 s. The detection mechanism of probe for primary amine is based on specific chemical reaction, while the detection mechanism for secondary amine and tertiary amine is intramolecular charge transfer. Further experiments show that the detection limit of the fluorescent probe for trimethylamine, an important marker of food spoilage, could reach 4.610 ppt. On-site detection based on spoilage of small yellow croaker suggests the material possesses the potential for food freshness detection. This simple fluorogenic probe is an original approach to simplify real-time visual monitoring of volatile amine vapour.
Construction of proton transport channels in metal-organic frameworks (MOFs) with simple synthesis processes, high proton conductivities and good performance stabilities has been of great interest for proton exchange membrane fuel cell (PEMFC). Herein, we mimic the proton transport behavior of amino acid residues in bacteriorhodopsin, select UiO-66-COOH as the host, glycine and aspartic acid as the functional guest molecules, and then functionalize the MOF framework with amino acids to obtain biomimetic proton transport channels. This strategy endows UiO-66-COOH-Asp a high proton conductivity of 1.19 × 10−2 S/cm at 70 ℃ and 98% RH, excellent cycle stability of performances and performance durability, which can be comparable to the reported MOFs-based proton conductors. Moreover, the proton conduction mechanism in UiO-66-COOH-Asp is elaborated in detail due to its visual structure, which is also one of the advantages of adopting MOFs as research platform, making it possible to optimize the structure-activity relationship of advanced materials. Notably, this strategy has clear objectives and simple synthesis, which has made certain contributions to both theoretical research and future industrial production of proton conductors.
Traditional photosensitizers show limited singlet oxygen generation in hypoxic infection lesions, which greatly suppress their performance in antibacterial therapy. Meanwhile, there still is lack of feasible design strategy for developing hypoxia-overcoming photosensitizers agents. Herein, radical generation of π-conjugated small molecules is efficiently manipulated by an individual selenium (Se) substituent. With this strategy, the first proof-of-concept study of a Se-anchored oligo (thienyl ethynylene) (OT-Se) with high-performance superoxide radical (O2•−) and hydroxyl radical (•OH) generation capability is present, and achieves efficient antibacterial activities towards the clinically extracted multidrug-resistant bacteria methicillin-resistant S. aureus (MRSA) and carbapenem-resistant E. coli (CREC) at sub-micromolar concentration under a low white light irradiation (30 mW/cm2). The water-dispersible OT-Se shows a good bacteria-anchoring capability, biocompatibility, and complete elimination of multidrug-resistant bacteria wound infection in vivo. This work offers a strategy to boost type-Ⅰ photodynamic therapy (PDT) performance for efficient antibacterial treatments, advancing the development of antibacterial agents.
Developing fluorescence probes with multiple responses has vital significance but remains challenging. Herein, for the first time, we present a mitochondrial DNA (mtDNA)-triggered pH response signal-amplified fluorescent probe (QCY-DBT) for multiple cell detection. The probe exhibited a large stokes shift (229 nm), excellent DNA selectivity over RNA, and ultrasensitivity of detection limit (DL; 74.0 ng/mL). Thus, QCY-DBT was successfully applied to analyze multiple human peripheral blood cells and visualize mtDNA in healthy and apoptotic cells. In the tumor acidic environment (pH 6.0–7.0), the absorbance of QCY-DBT at 436 nm increased, and the fluorescence signal (665 nm) was amplified by mtDNA, which enabled the direct observation of tumor cells. Our study provides help in designing smart probes with multiple responses for efficient abnormal cell detection.
The intimate host-anion interactions will regulate thermodynamics and kinetics in the self-assembly of cationic cages mimicking biological counterparts. Herein, we report construction and transformation of three Pd(Ⅱ)-based metal-organic cages (MOCs) depending on different anions. Stoichiometric conversions of the lantern-shaped MOC-34 into either octahedral MOC-35 or tricapped trigonal prism MOC-36 are induced by BF4‒ or NO3‒, respectively. MOC-36 is kinetically favored and can undergo quantitative conversion to the thermodynamically preferred MOC-35 upon heating, accelerated by excess BF4‒ to motivate dissociative dynamics of Pd-vertices and lower activation barrier of cage transformation. The guest encapsulation behaviors of MOC-35 and MOC-36 have also been tested. These results manifest a significance of host-anion dynamics beyond complementary anion template, shedding light on the understanding of intricate anion recognition in nature.
The lithium (Li) metal batteries (LMBs) are considered one of the most promising next-generation batteries due to its extremely high theoretical specific capacity. However, there are a couple of issues, e.g., the serious side reactions that occurred at the solid-liquid interface between the electrolyte and Li metal anode, hindering the broad commercialization of LMBs. Thus, a comprehensive understanding of the mechanisms underlying the decomposition of electrolytes is crucial to the design of LMBs. Herein, we utilize density functional theory simulations to explore the decomposition mechanism of electrolytes. The most commonly used ether electrolyte solvents, i.e., 1,2-dimethoxyethane (DME) and 1,3-dioxalane (DOL), based on suitable lithium salts, namely bis(trifluoromethanesulfonyl)imide (LiTFSI), are chosen to model the actual situations. We explicitly demonstrate that an electron-rich environment near the interface accelerates the decomposition of electrolytes. For ether electrolytes, we show that the LiTFSI degradation path is depending on the ratio of DOL to DME. In addition, the solvation structures of lithium-ion undergo a series of transformations upon electrolyte degradation, becoming thermodynamically more favorable and having a higher reduction potential in an electron-rich environment. Our finding provides new insights into the decomposition mechanisms of electrolytes and paves the way for the rational design of high-performance LMBs.
Thermocatalytic nonoxidative ethane dehydrogenation (EDH) is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability; exploring technology that permits efficient EDH by solar energy remains a giant challenge. Herein, we present that an oxygen vacancy (Ov)-rich LaVO4 (LaVO4-Ov) catalyst is highly active and stable for photocatalytic EDH, through a dynamic lattice oxygen (Olatt.) and Ov co-mediated mechanism. Irradiated by simulated sunlight at mild conditions, LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a conversion of 2.3%. By loading a small amount of Pt cocatalyst, the evolution and selectivity of C2H4 are enhanced to 275 µmol h−1 g−1 and 96.8%. Of note, LaVO4-Ov appears nearly no carbon deposition after the reaction. The isotope tracked reactions reveal that the consumed Olatt. recuperates by exposing the used catalyst with O2, thus establishing a dynamic cycle of Olatt. and achieving a facile catalyst regeneration to preserve its intrinsic activity. The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305. The Ov promotes photo absorption, boosts ethane adsorption/activation, and accelerates charge separation/transfer, thus improving the photocatalytic efficiency. The possible photocatalytic EDH mechanism is proposed, considering the key intermediates predicted by density functional theory (DFT) and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS).
Aluminosilicate small pore zeolites belonging to ABC-6 family play crucially important roles in the high methanol conversion with the high selectivity of light olefins, gas separation and storage, and selective catalytic reduction of NOx. In this work, we report a general method, called the epitaxial growth approach, for designing ABC-6 family small pore zeolites. It is mainly realized through the epitaxial growth on the nonporous SOD-type zeolite in the presence of inorganic cations (Na+ and K+) combined with a variety of organic structure directing agents (OSDAs). In this case, a series of ABC-6 family small pore zeolites such as ERI-, SWY-, LEV-, AFX-, and PTT-type zeolites have been successfully synthesized within a few hours. More importantly, the advanced focused ion beam (FIB) and the low-dose high-resolution transmission electron microscopy (HRTEM) imaging technique have been utilized for unraveling the zeolite heterojunction at the atomic level during the epitaxial growth process. It turns out (222) crystallographic planes of the SOD-type zeolite substrate provide unique pre-building units, which facilitate the growth of targeted ABC-6 family small pore zeolites along its c-axis. Moreover, the morphologies of ERI-type zeolite can also be tuned through the epitaxial growth approach, achieving a longer lifetime in the methanol conversion.
Monitoring α-glucosidase (α-Glu) activity is of great significance for the early diagnosis of type II diabetes. Here the blue fluorescent carbon dots (CDs) were integrated with two different recognizing molecules, β-cyclodextrin and phenylboronic acid, for assembling a multifunctional CDs (mCDs) nanoplatform for sensitively analyzing α-Glu and its inhibitors. The hydrolyzed product of 4-nitrophenyl-α-d-glucopyranoside (α-Glu substrate), p-nitrophenol, could efficiently quench the fluorescence of mCDs due to its cooperative molecular recognition with β-cyclodextrin and phenylboronic acid. The mCDs could be utilized for the detection of α-Glu activity with the limit of detection of 0.030 U/L. Moreover, the present α-Glu detection platform revealed a high selectivity, and other natural enzymes showed scarcely any effect on the present mCDs system. The proposed method could be facilely used to screen α-Glu inhibitors with satisfying performance. The rational mCDs is expected to supplement more comprehensive biosensing platforms for highly sensitive and specific recognition of disease-relevant biomarkers with clinical importance.
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