Latest ArticlesEthylene carbonate (EC) is the conventional and promising solvent to achieve high energy lithium metal battery. However, the innate low energy level of lowest unoccupied molecular orbital (LUMO) in EC makes it incompatible with lithium metal, causing uncontrolled lithium growth and low Coulombic efficiency (CE). Herein, we introduced bis(2,2,2-trifluoroethyl) carbonate (TFEC), a carbonate with a strong electron-withdrawing effect (-CF3), which enhances the stability of EC at electrode interface by reducing ion-dipole interactions between Li+ and EC. As the interaction between Li and EC weakens, TFEC and more PF6− anions coordinate with Li+, promoting the formation of contact ion pairs (CIPs) and aggregates (AGGs), thereby increasing the inorganic composition within the solid electrolyte interphase. Additionally, the distinct solvated sheath structure favors the decomposition of fluorinated solvents and PF6− anions, forming inorganic-rich electrode-electrolyte interfaces (SEI and CEI), thereby ensuring high stability for both the Li anode and high-voltage cathode. Hence, when applied in the full-cell LiLiMn0.8Fe0.2PO4, it displays consistent cycling performance, exhibiting minimal capacity decay with a retention rate of 62.5% after 800 cycles, substantially surpassing that of cells using base electrolytes (29.8%).
Zirconium-based metal-organic cages (Zr-MOCs) typically exhibit high stability, but their structural and application reports are scarce due to stringent crystallization conditions. We have successfully fluorinated the classical Zr-MOCs (ZrT-3) for the first time, obtaining the fluorinated MOCs (ZrT-3-F). Notably, ZrT-3-F not only inherits the high stability of its parent structure, but also acts as a catalyst for the effective oxidation of benzyl thioether for the first time. The reaction can reach a conversion rate of 99% in 6 h, and the selectivity reaches 95%, which far exceeds the non-fluorinated ZrT-3. This work proves that the specific functionalization of the classical Zr-MOCs can further expand their application potential, such as catalysis.
Radiotherapy (RT) is a widely used cancer treatment, and the use of metal-based nano-radiotherapy sensitizers has shown promise in enhancing its efficacy. However, efficient accumulation and deep penetration of these sensitizers within tumors remain challenging. In this study, we present the development of bismuth/manganese biomineralized nanoparticles (BiMn/BSA) with multiple radiosensitizing mechanisms, including high atomic number element-mediated radiation capture, catalase-mimic oxygenation, and activation of the stimulator of interferon genes (STING) pathway. Significantly, we demonstrate that low-dose RT induces the recruitment of macrophages and subsequent upregulation of Matrix metalloproteinases (MMP)-2 and MMP-9 that degrade the extracellular matrix (ECM). This dynamic process facilitates the targeted delivery and deep penetration of BiMn/BSA nanoparticles within tumors, thereby enhancing the effectiveness of RT. By combining low-dose RT with BiMn/BSA nanoparticles, we achieved complete suppression of tumor growth in mice with excellent biocompatibility. This study provides a novel and clinically relevant strategy for targeted nanoparticle delivery to tumors, and establishes a safe and effective sequential radiotherapy approach for cancer treatment. These findings hold great promise for improving the outcomes of RT and advancing the field of nanomedicine in cancer therapy.
The anti-oxidative characteristic and immunosuppressive microenvironment contribute to a high resistance of tumor to many treatments. In this work, a glutathione (GSH)-responsive metal-coordinated oxidative stress amplifier (designated as CuPA) is fabricated to suppress tumor growth through elevating the cellular level of reactive oxygen species (ROS) and eliminating M2 macrophages. Among which, cooper ion (Cu2+) is capable of coordinating with thioredoxin (Trx) inhibitor of PX-12 and signal transducer and activator of transcription 6 (STAT6) inhibitor of AS1517499 with the assistance of distearoyl phosphoethanolamine-PEG2000 (DSPE-PEG2000), which can extensively increase the stability to enhance drug delivery in vitro and in vivo. Furthermore, CuPA can upregulate intracellular ROS to cause tumor cell death through restraining Trx and degrading GSH. Also, CuPA-mediated STAT6 inhibition results in the elimination of M2 macrophage to reverse the immunosuppressive tumor microenvironment. Finally, the elevated oxidative stress and increased immune activation amplify the synergistic antitumor effect without causing obvious side effect. This work provides a new sight for synergistic tumor suppression through chemo-immunotherapy in consideration of the complex resistant tumor microenvironment.
The usage of flexible ligands in constructing MOF materials (FL-MOFs) has been widely studied due to its numerous advantages, including the structural diversity, polynuclear MOFs, transmitting magnetic exchanges, enantioselective separation, asymmetric catalysis, etc. However, the field still faces challenges in deeply understanding the effect of ligand configuration on the properties of these materials. Here, we employ a flexible aggregation-induced emission ligand (4,4′-((1E, 1′E)-anthracene-9,10-diylbis(ethene-2,1-diyl))dibenzoic acid) with great mechanical stability to construct FL-MOFs to lock the ligand configuration to explore the pressure-induced evolution of the ligand with coordination restriction, involving changes in fluorescence and intermolecular interaction. In-situ high-pressure fluorescence, Raman, and FT-IR experiments have revealed that the intermolecular interaction of AIE-Mn-MOF with configuration restriction increased more rapidly than that of free AIE-L. This discovery offers valuable insights for synthesizing MOF materials with exceptional mechanical stability and significantly advances our understanding of the impact of coordination restriction in FL-MOFs on their response to external stimuli.
The prodrug strategy provides an opportunity for improving the therapeutic index of drugs and avoiding their side effects. The main challenge lies in the fast and effective release of the parent drugs at the desired site under specific stimuli. Herein, a cooperative prodrug activation approach with exogenous native enzyme and endogenous tumor small molecule biomarkers was developed. Chemically, precursors of methylene blue (MB) and resorufin (RSF) react with horseradish peroxidase (HRP)/hydrogen peroxide (H2O2) to quickly and quantitatively release parent dyes and drugs containing amines or carboxylic acids. The application of this approach in mammalian cells was demonstrated with cooperative-activated photodynamic therapy based on a precursor of MB. Compared with free MB, much higher selectivity toward cancer cells was achieved with this approach as evaluated by the selectivity index (SI). This study provides a new method for fast and effective targeted prodrug activation with no need for antibody modification compared with traditional enzyme/prodrug therapy.
In view of widespread existence and toxicity, removal and detection of bisphenols is imperative to assess environmental risks and reduce harm to human health. Although many techniques have been reported, constructing fast and sensitive method remains a challenge. Herein, porous poly(divinylbenzene) polymer was synthesized in-situ on the Fe3O4 particles by means of distillation-precipitation polymerization and functioned as sorbents to extract bisphenols. Employing Fe3O4@poly(divinylbenzene) as sorbent, a magnetic solid-phase extraction coupling with liquid chromatography was developed to detect trace bisphenols in water. This method presented low detection limits (0.01–0.03 ng/mL), high enrichment ability (enrichment factor, 327–343), and good reproducibility. Moreover, the method showed satisfactory recoveries in the detection of lake water (80.60%-116.2%) and egg sample (75.17%-120.0%). Impressively, Fe3O4@PDVB has excellent adsorption capacity, which can realize rapid kinetic adsorption of bisphenols with equilibrium time all less than 10 s. The maximum adsorption capacities reached 1074.8, 1049.7, 1299.1 and 1329.5 mg/g for bisphenol F, bisphenol A, bisphenol B and bisphenol AF with Langmuir isotherm model. The adsorption mechanism of Fe3O4@PDVB to bisphenols was investigated and demonstrated that hydrophobic interactions played a key role, together with assistance of stacking interactions and hydrogen interactions. Overall, this work provides a promising sorbent material with ultra-fast and large adsorption capacities for extraction of bisphenols from water.
Graphene-like materials and metal-organic framework (MOF) materials hold significant promise for advanced energy systems. However, the accumulation of two-dimensional (2D) material and the low conductivity of MOF have seriously affected their practical application. The universal method for synthesizing homogeneous nitrogen-doped graphene-like carbon/metal-organic framework (N-GLC/MOF) composites, including N-GLC/MOF-74, N-GLC/ZIF-8, N-GLC/Cu-BTC, and N-GLC/FeCo-PBA was presented. Thanks to the synergistic effect of the two components, the N-GLC/MOF-74 composite exhibits a specific capacitance of 470.18 F/g at 1 A/g and maintains a coulombic efficiency of 95.04% at 5 A/g over 5500 cycles. Our work lays a solid foundation for the design and synthesis of N-GLC-based composites. We anticipate that this research will furnish valuable insights for the advancement of N-GLC/MOF composites, with a primary focus on enhancing supercapacitor performance.
Colorectal cancer is a common cancer worldwide. Traditional chemotherapeutic drugs often face limitations such as poor aqueous solubility and high systemic toxicity, which can lead to adverse side effects and limited therapeutic efficacy. In this study, a library of one kind of biodegradable and biocompatible polymer, leucine based-poly(ester amide)s (Leu-PEAs) was developed and utilized as drug carrier. The structure of Leu-PEAs can be tuned to alter their physicochemical properties, enhancing drug loading capacity and delivery efficiency. Leu-PEAs can self-assemble into nanoparticles by nanoprecipitation and load paclitaxel (PTX) with the diameter of ~108 nm and PTX loading capacity of ~8.5%. PTX-loaded Leu-PEAs nanoparticles (PTX@Leu-PEAs) demonstrated significant inhibition of CT26 cell growth in vitro. In vivo, these nanoparticles exhibited prolonged tumor accumulation and antitumor effects, with no observed toxicity to normal organs. Furthermore, blank Leu-PEAs nanoparticles also showed antitumor effects in vitro and in vivo, which may be attributed to the activation of the mammalian target of rapamycin (mTOR) pathway by leucine. Consequently, this biocompatible Leu-PEAs nano-drug delivery system shows potential as a promising strategy for colorectal cancer treatment, warranting further investigation.
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