Latest ArticlesThe homochiral compounds play an important role in human health and pharmaceutical industry. Currently, the chromatographic enantioseparation has become one of the most effective and practical approach to obtain pure enantiomers. Herein, the exploration of advanced materials, using as chromatographic chiral stationary phases for racemic separation, has attracted great attention. Thanks to their high enantioselectivity and controllable synthesis, the emerging chiral metal-organic frameworks (CMOFs) have been widely studied as the stationary phase in chromatographic technology. In this review, we will summarize the principles of synthetic strategies and mechanism of chiral microenvironment. In particular, the recent progress and research hotspot of CMOFs regarding as the chiral stationary phases in gas chromatography (GC), high-performance liquid chromatography (HPLC), and capillary electrochromatography (CEC), are elucidated systematically according to the published work. Last but not the least, we also highlight the challenges and perspectives of rational design of CMOFs, as well as their corresponding racemic separation. We envision that the review will provide a further understanding of CMOFs and facilitate the development of chromatographic enantioselective applications.
Under "green architecture" principles, electrochromic smart windows are employed to adjust optical transmittance and indoor temperature, yet their high costs limit the wide application. Here, an electrochromic window is driven by a redox flow battery (RFB), where TOC and deposition layers are no longer needed. The transmittance of the electrochromic window is modulated by the state of oxidation (SOC) of aqueous posolyte Fe(phen)3Cl2, which is coupled with BTMAP-Vi negolyte in RFB. Under optimized conditions, average CE, VE, and EE reach 93.25%, 92.61%, and 86.35% for RFB with a capacity fading rate of 1.57% per cycle. 88.66% optical modulation and 9.36 cm2/C coloration efficiency are achieved in the electrochromic process, and 72.34% optical modulation is maintained after 12000 s. Essentially, the indoor temperature declines 3 ℃ for posolyte with 100% SOC when compared with the control experiment using circulating water for a model house. This means minimum electricity of 0.0185 kWh is saved when using an air conditioner to cool a 100 m3 house, which corresponds to declined CO2 emission (COE) of 0.0185 kg. This work provides a novel and cost-efficient strategy for modulating indoor comfort via electrochromic windows driven by RFB.
Two lindenane-type sesquiterpene (LDS) trimers with unprecedented carbon skeletons, holotrichones A (1) and B (2), were obtained from the whole plant of Chloranthus holostegius var. trichoneurus by a ultra performance liquid chromatography-photodiode array detector-mass spectrometry (UPLC-PDA-MS)-guided isolation strategy. Compound 1 represents the first LDS trimer incorporating a unique 3/5/6/6-fused framework, in which a lindenane-type monomer and the 2-methylbutyryl substituent of an LDS dimer is bridged by a six-membered ring system. Compound 2 is the first hetero-trimer fused by an LDS dimer with a p-benzoquinone-meroterpenoid, featuring an unusual 3/5/6/6/3/5/6/6/6 nonacyclic system fused by the sesquiterpenoid unit and a 2-geranyl-6-methyl-2,5-cyclohexadien-1,4-dione moiety. In compound 2, the dimeric LDS moiety is equipped with a rare oxaspiro[4.5]decane system. Their structures, including absolute configurations, were established by spectroscopic methods, GIAO NMR calculations and DP4+ probability analyses, electronic circular dichroism (ECD) calculations, and single-crystal X-ray diffraction analysis. The plausible biogenetic pathway speculation indicated that hetero- and homo-Diels-Alder additions may dominate the formation of these highly fused polycyclic frameworks. Both compounds 1 and 2 induced the human acute myeloid leukemia MV-4–11 cell death via apoptosis induction, which deserves further investigation on this new chemical class of LDS oligomers for their anti-leukemic potential.
Dopamine, a pivotal excitatory neurotransmitter, plays a crucial role in metabolic, cardiovascular, renal, central nervous, and endocrine systems. Abnormal dopamine within the human body can cause various diseases. Therefore, the precise quantification of dopamine levels, both in vivo and in vitro, holds paramount significance for clinical applications and physiological investigations. Carbon dots (CDs) exhibit a plethora of remarkable properties, including a substantial specific surface area, robust electrical conductivity, commendable biocompatibility, minimal toxicity, and high photostability. Considering these unique characteristics, CDs demonstrate substantial potential for fluorescent sensors, colorimetric sensors, and electrochemical sensors for dopamine detection. This review systematically examined the challenges and prospects for the utilization of CDs-based fluorescent sensors, electrochemical biosensors, and colorimetric sensors for monitoring dopamine levels in recent years. These findings unveil promising avenues for further advancements in the field of dopamine detection.
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.
Patients with oral squamous cell carcinoma (OSCC) encounter challenges in achieving efficient antitumor immunity, primarily due to the inherent pathophysiological characteristics of solid tumors affecting drug accumulation and penetration. Insufficient T-cells and immune escape induced by tumor-associated macrophages (TAMs) further exacerbate these issues. This study utilized M1 macrophage membrane-modified spatial dimension conversion drug delivery systems (SDDDSs) and introduced photosensitizers chlorophyll Pyro and the immune agonist R848. This innovative approach enhanced tumor targeting and accumulation by transforming stimulus-responsive size-reductive SDDDSs into smaller-sized iRGD-Pyro and R848 within the extracellular tumor microenvironment (TME). This facilitated effective drug penetration into deep tumor regions and cellular uptake. The synergistic treatment strategy for OSCC, combining photodynamic therapy (PDT) and tumor immunotherapy, induced tumor cell apoptosis, triggered immunogenic cell death (ICD), polarized TAMs towards the M1 phenotype, promoted sufficient T-cell infiltration, and resulted in significant therapeutic outcomes. This approach offers a promising avenue for future OSCC therapeutic interventions.
Photodynamic therapy has been widely employed as an alternative strategy against bacterial infection. Molecular structure has a profound effect on the antibacterial ability of photosensitizers (PSs). Herein, we designed and synthesized a series of boron dipyrromethene (BODIPY)-based photosensitizers with different alkyl chain lengths, and then their antibacterial activities were compared. Among these BODIPYs, the BODIPY with octyl (BDP-8) exhibits the best antibacterial effect, while the antibacterial performance of BODIPY with dodecyl (BDP-12) is the worst. This work provides instructive information for further development of effective photodynamic antimicrobial agents.
Bacterial endotoxin (a type of lipopolysaccharide, LPS) that acts as the strongest immune stimulant exhibits high toxicity to human health. The golden standard detection methods rely heavily on the use of a large amount of tachypleus amebocyte lysate (TAL) reagents, extracted from the unique blue blood of legally protected horseshoe crabs. Herein, a cost-effective distance-based lateral flow (D-LAF) sensor is demonstrated for the first time based on the coagulation cascade process of TAL induced by endotoxin, which causes the generation of gel-state TAL. The gelation process can increase the amount of trapped water molecules and shorten the lateral flow distance of the remaining free water on the pH paper. The water flow distance is directly correlated to the concentration of endotoxin. Noteworthy, the D-LAF sensor allows the detection of endotoxin with the reduced dosage of TAL reagents than the golden standard detection methods. The detection limit of endotoxin is calculated to be 0.0742 EU/mL. This method can be applied to the detection of endotoxin in real samples such as household water and clinical injection solution with excellent performance comparable to the commercial ELISA kit.
Pyrroles are important structural units of natural products, drug molecules, biomolecules and functional material molecules. Efficient synthesis of α-functionalized pyrroles with different substituents from easily accessible starting materials is still challenging. Herein, a facile and regioselective coarctate reaction of enynals involving a free carbene intermediate has been developed, which allows the divergent and practical de novo synthesis of various α-furanyl pyrroles and α-cyclopropenyl pyrroles derivatives with good to excellent yields and high efficiency under mild conditions. This approach features readily accessible starting materials, high functional group compatibility, step economy and scalability, which would complement previous methods and support expansion of the toolbox for the synthesis of valuable, but previously inaccessible, highly substituted and electron-rich α-functionalized pyrroles.
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