Latest ArticlesThe design and synthesis of photoactive macrocyclic molecules continue to attract attention because such species play important roles in supramolecular chemistry as well as photoelectronic applications. Donor-acceptor (D-A) conjugated macrocycles are an emerging class of photoactive molecules due to their D-A conjugated structural characteristics and tunable optical properties. In addition, the well-defined cavities in such D-A macrocycles endow them with versatile host-guest properties. In this review, we provide a comprehensive summary of D-A conjugated macrocycle chemistry, detailing recent progress in the area of synthetic methods, optical properties, host-guest chemistry and applications of the underlying chemistry to chemical sensors, bioimaging and photoelectronic devices. Our objective is to provide not only a review of the fundamental findings, but also to outline future research directions where D-A conjugated macrocycles and their constructs may have a role to play.
Electrochemical oxidation of aqueous tris(1,3-dichloro-2-propyl) phosphate (TDCPP) by using Ti/SnO2-Sb/La-PbO2 as anode was investigated for the first time, and the degradation mechanisms and toxicity changes of the degradation intermediates were further determined. Results suggested that electrochemical degradation of TDCPP followed pseudo-first-order kinetics, and the reaction rate constant (k) was 0.0332 min−1 at the applied current density of 10 mA/cm2 and Na2SO4 concentration of 10 mmol/L. There was better TDCPP degradation performance at higher current density. Free hydroxy radical (·OH) was proved to play dominant role in TDCPP oxidation via quenching experiment, with a relative contribution rate of 60.1%. A total of five intermediates (M1, C6H11Cl4O4P; M2, C3H7Cl2O4P; M3, C9H16Cl5O5P; M4, C9H14Cl5O6P; M5, C6H10Cl3O6P) were identified, and the intermediates were further degraded prolonging with the reaction time. Flow cytometer results suggested that the toxicity of TDCPP and degradation intermediates significantly reduced, and the detoxification efficiency was achieved at 78.1% at 180 min. ECOSAR predictive model was used to assess the relative toxicity of TDCPP and the degradation intermediates. The EC50 to green algae was 3.59 mg/L for TDCPP, and the values raised to 84, 574, 54.6, 391, and 8920 mg/L for M1, M2, M3, M4, and M5, respectively, indicating that the degradation intermediates are less toxic or not toxic. Electrochemical advanced oxidation process is a valid technology to degrade TDCPP and pose a good detoxification effect.
Derivatives of piperazine, which is one of the most important heterocycles, are often used as linkers to connect active substructures that show promising bioactivities, especially in the field of agrochemicals. From 2000 to 2022, many piperazine-containing compounds were found to exhibit excellent activities against fungi, bacteria, insects, plant viruses, and weeds and have also been used as plant growth regulators. Currently, the development of novel pesticides to prevent the invasion of crop pathogens and ensure the quality and yields of crops is still needed. We herein investigated and summarized the role that piperazine plays in the discovery of pesticides to provide a comprehensive summary of the broad activities of piperazine derivatives in agricultural applications and offer a potential reference for novel pesticide design using piperazine-containing compounds. Moreover, structure–activity relationships (SARs) analyses of bioactive piperazine-containing compounds are also discussed for a deeper understanding.
Metal-based catalysts with different site sizes (e.g., metal nanoparticles (NPs) and single atom catalysts (SACs)) demonstrated outstanding catalytic activities in versatile Fenton-like reactions. However, the surface/structural instability is a critical issue, which will result in rapid passivation in Fenton-like reaction and fail in long-term operation. The catalytic stability of the catalysts with different metal sizes considering versatile peroxides (H2O2, peroxymonosulfate (PMS), and peroxodisulfate (PDS)) should be analyzed. In addition, strategies for catalyst regeneration and recyclability improvement are also important to realize the metal-based catalysts for practical applications. In this review, catalytic stability of catalysts with different metal sizes in the backgrounds of versatile peroxides and water matrixes in Fenton-like reactions were first evaluated. Regeneration of metal catalytic sites with different methods were also reviewed. Finally, major challenges and development of methods concerning the stability and regeneration of metal catalytic sites with different sizes were discussed to understand the future researches of metal catalytic sites in Fenton-like reactions.
As a representative of chronic wounds, the long-term high levels of oxidative stress and blood sugar in chronic diabetic wounds lead to serious complications, making them the biggest challenge in the research on wound healing. Many edible natural biomaterials rich in terpenes, phenols, and flavonoids can act as efficient antioxidants. In this study, okra extract was selected as the main component of a wound dressing. The okra extracts obtained via different methods comprehensively maintained the bioactivity of multiple molecules. The robust antioxidant properties of okra significantly reduced intracellular reactive oxygen species production, thereby accelerating the wound healing process. The results showed that okra extracts and their hydrogel dressings increased cell migration, angiogenesis, and re-epithelization of the chronic wound area, considerably promoting wound remodeling in diabetic rats. Therefore, okra-based hydrogels are promising candidates for skin regeneration and wider tissue engineering applications.
Thiophenol (PhSH) is an important raw material for organic synthesis, while its high toxicity to organisms makes it an environmental pollutant. Therefore, it is crucial to accurately detect PhSH and explore its metabolic process in the living system. Herein, a near-infrared (NIR) fluorescent probe TEM-FB was developed for sensing PhSH with a turn-on fluorescent signal at 719 nm and a large Stokes shift (198 nm) based on generating the intramolecular charge transfer (ICT) process. TEM-FB shows high specificity and significant sensitivity towards PhSH (detection limit: 10 nmol/L) via the aromatic nucleophilic substitution mechanism. Furthermore, it was successfully applied to image PhSH in multiple cell lines and in zebrafish. Notably, we revealed the oxidative stress process caused by PhSH and demonstrated that the hydrogen peroxide (H2O2) in cells would alleviate the poisonousness from exogenous PhSH for the first time. This work provides a promising bioimaging tool for monitoring PhSH in living systems and visualizing the process of oxidative stress induced by PhSH.
The organic carbon source coating LiFexMn1-xPO4 suffers from the problem of non-uniform carbon cladding. Too thick carbon cladding layer instead hinders the de-embedding of lithium ions. In this paper, we choose cornstalk as the carbon source, then LiFe0.5Mn0.5PO4@cornstalk-C (LFMP@C-C) with 3D anchoring structure is prepared by the solvothermal method. The results show that the LFMP with cornstalk as the carbon source has better performance compared to the sucrose-coated LFMP material (LFMP@C). The discharge capacity of LFMP@C-C is 116 mAh/g for the first cycle at 1 C and the capacity retention rate is 94.0% after 500 cycles, and the discharge capacity of LFMP@C-C is more than 17.17% higher than that of LFMP@C.
Spatial configuration has a significant effect on chemical self-assembly. However, the importance of spatial configuration in supramolecular adhesive materials has been frequently ignored. In this study, the effects of the spatial configuration on cohesion and adhesion were investigated. Owing to the diversities of the chemical structures and assembly patterns, 1,2-disubstituted cyclohexane derivatives were used in this combined experimental and theoretical investigation. The self-sorting assembly of enantiopure isomers improved cohesion but had a negative effect on adhesion. In contrast, racemic mixtures displayed stronger adhesion effects. Moreover, it was proven that the cis-configuration was more favorable for supramolecular adhesion than the trans-counterpart. In addition, the influence of the spatial configuration of 1,2-disubstituted cyclohexane derivatives could be effectively mitigated by hydrogen bond donors or acceptors. The addition of natural acids yielded three-dimensional polymeric networks, in which the spatial configuration was not the decisive factor for supramolecular adhesion.
Exosomes offer ideal biomarkers for liquid biopsies. However, high-efficient capture of exosomes has been proven to be extreme challenging. Here, we report a soluble pH-responsive host-guest-based nanosystem (pH-HGN) for homogeneous isolation of exosomes around physiological pH. The pH-HGN consists of two specifically functionalized modules. First, a pH-responsive module, poly-dimethylaminoethyl methacrylate, provides homogeneous capture circumstances and sharp pH-triggered self-assembly separation in aqueous solution to improve capture efficiency and reduce nonspecific adsorption. Second, a host-guest module, poly-acrylamide azobenzene and β-cyclodextrin linked with exosomes-specific antibody, could act as the "cleavable bridge" to specific capture and subsequent rapid release of captured exosomes through host-guest interaction between β-cyclodextrin and AAAB moieties. The pH-HGN offered high capture efficiencies for exosomes from two different cell lines, which were 90.2% ± 0.28% and 87.0% ± 4.6% for H1299 and MCF-7 cell-derived exosomes, respectively. The purity of isolated exosomes was (1.49 ± 0.71) × 1011 particles/μg, which was 4.1 times higher compared with the gold standard ultracentrifugation (UC) method. Furthermore, the isolated exosomes via the pH-HGN can preserve well integrity and biological activity. The developed pH-HGN was further successfully applied to differentiate lung cancer patients from healthy persons. These findings indicated that pH-HGN is a promising strategy in exosomes-based research and downstream applications.
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