Latest ArticlesCovalent organic frameworks (COFs) are crystalline porous polymeric materials composed of organic monomers connected by strong covalent bonds and offer high stability, good crystallinity, a large specific surface area, and controllable structures. COFs are widely used in the fields of adsorption and separation, catalysis, photovoltaics, and drug-delivery. The structural regulation and performance optimization of COFs can be realized through the modification of ligands and the selection of linkage methods. In which, the types of linkage are closely related to the stability and performance of COFs. In this review, nitrogen-containing linkage-bonds (NCLBs) in COFs are divided into N-containing double bonds, N-containing conjugated rings and N-containing unconjugated rings. The association between structure and performance of COFs is elaborated and the synthesis methods of COFs are systematically summarized. Moreover, the structural design, theoretical prediction and machinable application of COFs are prospected
Electrochemical nitrate reduction (NO3RR) offers a promising avenue for treating nitrate-contaminated water and recovering ammonia (NH3), yet the complexities of direct electron transfer (DET) and hydrogen atom transfer (HAT) mechanisms crucial for efficiency remain elusive. This study bridges the gap with a combined experimental and theoretical approach, elucidating the impact of catalyst structure on NO3RR pathways. We discover that catalysts favoring strong NO3− adsorption and efficient water dissociation were more inclined towards DET, enhancing denitrification. The Fe@Fe3O4/FF cathode, leveraging the synergistic interplay between metallic Fe and Fe3O4, excelled in NO3RR via DET, achieving an NH3 yield of 0.28 mmol h−1 cm−2 and a Faradaic efficiency of 95.7% for NH3 at -1.6 V (vs. SCE), with minimal nitrite accumulation at 100 mmol/L nitrate. Conversely, the Fe/FF and Fe3O4/CC cathodes showed reduced NH3 production and increased nitrite levels, attributed to the lack of Fe3O4 and metallic Fe, respectively, resulting in a dominant HAT mechanism. Moreover, Fe@Fe3O4/FF facilitated complete denitrification in real wastewater treatment by harnessing Cl− for electrochemically mediated breakpoint chlorination. This research not only deepens our understanding of NO3RR mechanisms but also paves the way for designing superior nitrate reduction catalysts.
Studies widely acknowledge the enhancement of permanganate (Mn(Ⅶ)) oxidation of organic contaminants by coexisting matrices in water. This study investigated the positive influence of Mn(Ⅱ), a common soluble metal ion, on the removal of trace organic pollutants by Mn(Ⅶ). Results showed that introducing 20 µmol/L Mn(Ⅱ) at pH 5.0 accelerated trace organic pollutant removal by promoting colloidal MnO2 formation. UV−vis spectrum, quenching, and probe experiments confirmed role of MnO2 in sulfamethoxazole (SMX) oxidation, with Mn(Ⅲ) playing a predominant role. Meanwhile, in situ-generated MnO2 facilitated Mn(Ⅶ)* formation, enhancing oxidation performance, as indicated by Raman spectroscopy and electrochemical analysis. Eleven transformation products (TPs) of SMX in the Mn(Ⅶ)/Mn(Ⅱ) process were detected by UPLC-QTOF-MS/MS. Subsequently, the reaction pathways of SMX were elucidated through Fukui index analysis and the identification of TPs. Additionally, toxicity simulations with Toxicity Estimation Software Tool (T.E.S.T.) software revealed significantly lower cytotoxicity of TPs of SMX compared to the parent compound. This study unveils an effective strategy to enhance Mn(Ⅶ)-mediated degradation of organic pollutants in water, elucidating Mn(Ⅱ)-induced Mn(Ⅶ) activation mechanisms.
Venetoclax (Vene), a BCL-2 inhibitor, is widely used as a chemotherapeutic drug in acute myeloid leukemia (AML). However, its treatment specificity for leukemia cells is limited, often leading to side effects and treatment resistance. In this study, we utilized l-phenylalanine as an efficient nanocarrier to enhance the delivery of Vene, forming the complex Vene@8P6. This complex was then applied to AML mouse models and human AML cell lines. The in vitro analysis showed that THP-1 and HL60 cells rapidly absorbed the Vene@8P6 nanoparticles. This absorption resulted in severe DNA damage, increased reactive oxygen species (ROS) production, elevated apoptosis rates, and decreased cell proliferation compared to the administration of Vene alone. In vivo studies demonstrated that Vene@8P6 more efficiently targeted leukemia cells than normal hematopoietic cells within the bone marrow and other major organs in AML mice, as evidenced by bioluminescence imaging and flow cytometry analysis. Furthermore, Vene@8P6 treatment resulted in reduced drug side effects and improved therapeutic efficacy in AML mice. Overall, Vene@8P6 represents a novel and efficient therapeutic agent for AML, offering enhanced leukemia target specificity, reduced side effects, and improved treatment outcomes.
As PEGylated liposomes have witnessed remarkable advancements in drug delivery, their immunogenicity has emerged as a notable challenge. In this study, we discovered that a simple pre-injection of folic acid (FA) effectively mitigated the immunogenicity of PEGylated liposomes and enhanced their in vivo performance by tolerating splenic marginal zone B cells. FA specifically inhibited the internalization of PEGylated liposomes by splenic marginal zone B cells, thereby reducing splenic lymphocyte proliferation and specific IgM secretion. This modulation alleviated IgM-mediated accelerated blood clearance and adverse accumulation of the PEGylated liposomes in the skin. These findings provide new insights into the immunomodulatory effects of FA and promising avenues to enhance the efficacy and safety of PEGylated liposomal nanomedicines.
The potential of metal nanoclusters in biomedical applications is limited due to aggregation-caused quenching (ACQ). In this study, an in situ self-assembled pitaya structure was proposed to obtain stable fluorescence emission through protein coronas-controlled distance between gold nanoclusters (Au NCs). Interestingly, the gold ion complexes coated with proteins of low isoelectric point (pI) nucleate at the secondary structure of proteins with high pI through ionic exchange within cells, generating fluorescent Au NCs. It is worth noting that due to the steric hindrance formed by the protein coronas on the surface of Au NCs, the distance between Au NCs can be controlled, avoiding electron transfer caused by close proximity of Au NCs and inhibiting fluorescence ACQ. This strategy can achieve fluorescence imaging of clinical tissue samples without observable side effects. Therefore, this study proposes a distance-controllable self-assembled pitaya structure to provide a new approach for Au NCs with stable fluorescence.
Breath analysis can be used to diagnose diseases non-invasively. Accurate measurement of volatolomics is critical for breath analysis to be a gold standard. Tedlar bags (TB) are often used to collect breath samples, but they emit contaminants that affect accuracy. This issue was overlooked in previous studies. We found contamination issues with TB (e.g., siloxanes and aromatic impurities) that affect the identification of volatile organic compounds (VOCs) due to impurities. Then, home-designed equipment (HD) made with poly-tetrafluoride (PTFE) and quartz glass for breath collection was developed and employed in clinical trials. 15 healthy individuals and 32 non-small cell lung cancer (NSCLC) patients at IA stage participated in this study. 610 VOCs can be collected through TB, which is less than HD (1109 VOCs), demonstrating that the inner wall of the TB easily adsorbs VOCs, leading to decreased detection concentrations. Otherwise, utilizing orthogonal partial least squares discriminant analysis (OPLS-DA), we identified chemical markers with significant discriminatory power (VIP > 1.5, P < 0.05). The HD method identified 12 target VOCs, surpassing the 3 target VOCs discerned by the TB method. A model combined with a machine learning algorithm for distinguishing early-stage lung cancer patients was established based on biomarkers, which were selected based on OPLS-DA. The results showed strong predictive capabilities for the HD-based model. It indicated that 12 biomarkers derived from the HD model were more effective in distinguishing NSCLC patients, with an AUC value of 0.92, compared to the AUC value of 0.5 from 3 markers obtained from the TB model. The sensitivity and specificity in the confusion matrix reached 100% and 80% for the HD test, but TB test reached only 40% and 60%. This work demonstrated that optimizing and standardizing VOCs collection methodology from breath of lung cancer patients is essential to identify actual volatiles, which could promote disease volatolomics worldwide.
H2O2 is an environmentally friendly oxidizing agent with minimal secondary pollution; however, its application has always been constrained by factors such as storage and transportation. In this study, we propose an innovative method for storing and releasing H2O2 using hydrogels. Commercial hydrogels (sodium polyacrylate) can undergo swelling and absorb H2O2 in aqueous solutions, and the swollen hydrogel can continuously release H2O2 under osmotic pressure. And the characteristics of osmotic pressure drive ensure the recyclability of hydrogel for H2O2 storage. Experimental results demonstrate that H2O2 can stably exist within the hydrogel for an extended period, and this strategy helps to avoid explosion the risk and potential environmental hazards during the transportation of H2O2. Finally, experiments confirm that the hydrogel controlled sustained release of H2O2 is effective in both Fenton reactions and the process of bacterial inactivation. This work introduces new ideas for the storage of H2O2, and the sustained release of H2O2 may have significant implications in the fields of healthcare, environmental science, catalysis, and beyond.
Programmed cell death protein 1/programmed cell death 1 ligand 1(PD-1/PD-L1) protein-protein interaction represents an appealing target for cancer therapy. Several antibody drugs have been developed to target this interaction, but they are less effective in the treatment of melanoma. To overcome the limitations, the first proteolysis-targeting chimeric (PROTAC) small molecules simultaneously targeting PD-L1 and Src homology phosphotyrosyl phosphatase 2 (SHP2) were designed. By employment of PD-1/PD-L1 inhibitors BMS01 or BMS-37, SHP2 inhibitor SHP099 and E3 ligase ligands, a series of potent PD-L1 and SHP2 dual PROTACs were synthesized. The most promising compounds BS-7C-V2 and BS327V2 efficiently induced PD-L1 and SHP2 degradation and demonstrated significantly improved immune potency in B16-F10 and A375 cell lines. More importantly, the efficacy of BS-7C-V2 and BS327V2 in a B16-F10 transplanted mouse model was further evaluated based on their degradation ability in vivo. Taken together, our work qualifies the new dual PROTACs as a potent degrader of PD-L1 and SHP2. The biological and mechanism investigations with BS-7C-V2 and BS327V2 prove that dual PROTACs can play an anti-tumor role in vivo and in vitro, and can provide a new therapeutic strategy for melanoma.
Proteolysis-targeting chimera (PROTAC) has emerged as an efficient strategy to accurately control intracellular protein levels. However, conventional PROTACs are generally limited by nonspecific protein degradation and off-tissue side effects. Particularly, there is a lack of effective chemical tools for visualizing protein degradation. Herein, a near-infrared fluorescent and theranostic PROTAC (PRO-S-DCM) was designed for imaging the degradation of bromodomain-containing protein 4 (BRD4). PRO-S-DCM could be tumor-specifically activated and exhibited favorable imaging effects both in vitro and in vivo. PRO-S-DCM was proven to be a theranostic probe, which potently inhibited growth, invasion and migration of HeLa cells and induced cell apoptosis.
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