Latest ArticlesReactive oxygen species (ROS) are essential in various pathological and physiological processes. Developing nanosystems that generate ROS in a controlled manner is of great interest for nanomedicine. DNA nanotechnology offers a promising approach to constructing programmable ROS-generating platforms. By incorporating photosensitizers or metal ions, DNA nanostructures can be designed to produce ROS in a spatially and temporally desired fashion. DNA-based ROS-generating nanosystems hold great potential in intracellular homeostasis regulation, drug release, and cancer therapy. This review summarizes recent advances in developing DNA-based ROS-generating nanosystems, highlights their emerging biomedical applications, and discusses the opportunities and challenges for further applications. DNA nanotechnology provides a versatile toolkit to construct biocompatible ROS-generating platforms for next-generation nanomedicines.
Microbial fabrication of metal nanoparticles (MNPs) has received significant attention due to the advantages of low toxicity, energy efficiency and ecological safety. Diverse groups of MNPs can be synthesized intracellularly or extracellularly by various wild-type microorganisms, including bacteria, fungi, algae and viruses. Synthetic biology approaches, represented by genetic engineering, have been applied to overcome the shortcomings in productivity, stability, and controllability of biosynthetic MNPs. Scanning electron microscope (SEM), transmission electron microscope (TEM) and other characterization techniques assist in deciphering their unique properties. In addition, biosynthetic MNPs have been widely explored for the utilization in environmental remediation and contaminant detection. And machine learning contains a great potential for designing targeted MNPs and predicting their toxicity. This review provides a comprehensive overview of the research progress in the microbial synthesis of MNPs. An outlook on the current challenges and future prospects in the biologically controllable synthesis and engineering environmental applications of MNPs is also provided in this review.
A photocatalyst-free visible-light-promoted three-component reaction of thianthrenium salts, isothiocyanates, and amines is presented, which affords a rapid and efficient approach to S-arylisothioureas under mild conditions. This developed method exhibits the advantages of readily available raw materials, broad substrate scope, good functional tolerance, and operational simplicity. It is worth mentioning that the byproduct thianthrene can be recycled in quantity, ultimately maximizing the atomic economy of the reaction and avoiding chemical waste. Mechanism investigations support the strategy involving a photoinduced EDA complex.
A new 1,4-amidocyanation of 1,3-enynes with N-amidopyridin-1-ium salts and TMSCN using a copper and photoredox synergetic catalysis for producing α-amido allenyl nitriles is developed. Employing N-amidopyridin-1-ium salts as the amidyl radical precursors, the reaction enables the formation of two new bonds, one C(sp3)-N bond and one C(sp2)-C(sp) bond, in a single reaction step. This reaction represents a mild, general route to the construction of the α-amido allenyl nitrile architectures, which characterizes a broad scope, a good functional group compatibility and an excellent selectivity.
Efficient activation of molecular oxygen (O2) is considered a promising technique for the removal of antibiotics. However, how to effectively regulate electrons distribution to promote O2 activation remains a challenge at present. In this study, phosphorus and sodium co-doped carbon nitride (PNaCN) were designed to rearrange the electrons distribution to activate O2 for the degradation of tetracycline. The generation of •O2−was innovatively observed via in-situ O2 fitting Fourier transform infrared (FTIR) spectroscopy, demonstrating the outstanding O2 activation ability of PNa5. Density functional theory (DFT) further confirmed that the rational co-doping led to the rearrangement of local electrons, resulting in electron-rich Na sites and electron-deficient P sites. These sites exhibited greater susceptibility to O2 adsorption and charge transfer. Besides, the degradation rate of tetracycline was increased by 2.44 times using co-doped CN. This study provides a new inspiration for enhancing O2 activation by inducing electrons rearrangement.
Water-soluble inorganic ions (WSIIs) play a pivotal role in atmospheric chemical reactions, particularly influencing the formation of secondary particulate matter. A comprehensive grasp of the vertical distribution of atmospheric pollutants holds immense significance in understanding the diffusion and transportation of these pollutants. This study investigates the WSIIs of PM2.5 and size-segregated particles at the top (~2060 m a.s.l.) and foot of Mt. Hua during the winter of 2020. All the measured ions present significant higher concentrations (1.9~6.9 times) at the foot than the top. Cl− and K+ at the foot are more than 4 times of those at the top, whereas Ca2+ and Mg2+ are only 1.3–1.9 times higher. The particle size distribution of NO3−, SO42−, K+ and Cl− demonstrate a single peak distribution (0.7–1.1 µm) at the foot, but with a bimodal distribution (0.7–1.1 µm and 4.7–5.8 µm) at the top. These differences suggest that the aerosol at the alpine region is mainly transported via long-distance from Northwest/North China, but limited influenced by vertical transport through valley breeze. The changes of concentration and size distribution of WSIIs in dust event and non-dust period indicate that the effects of dust event on aerosols at ground surface were weaker than that of the free troposphere of Guanzhong Plain. Notably, our study underscores the dominant influence of NO3− in shaping the gas-particle distribution of ammonia within the winter free troposphere. Our results highlight the significant role of long-range transport on aerosols in the free troposphere in Guanzhong Plain, Northwest China.
Small peptides have attracted increasing attention for their unique features and diverse biological functions. Achieving rapid separation and accurate quantification, however, remains a challenge because of their low abundance and the co-existence of numerous structural isomers. In this study, we developed a novel approach using isotope chemical labeling for ultrasensitive determination of di/tripeptides in biological samples. We successfully synthesized a novel derivatization reagent, 4-(2-(ethoxymethylene)-3-oxobutanamido)-N,N,N-trimethylbenzenaminium iodide (EOTMBA) as well as its deuterium-labeled isotope reagent (d3-EOTMBA). A total of 97 small peptides, including 89 dipeptides and 8 tripeptides, could be completely derivatized in methanol within 1.5 h at 60 ℃. After EOTMBA labeling, analysis of these di/tripeptides were achieved within 22 min by LC-MS/MS analysis. The method demonstrated 86.3%–113% accuracy and the limit of quantification ranged from 0.25 fmol/L to 5 nmol/L. Using this method, we achieved ultrasensitive and accurate quantification of di/tripeptides in 147 plasma, 49 urine and 46 bile samples obtained from healthy individuals and patients with biliary tract diseases. The identified differential di/tripeptide biomarker panels showed promising diagnostic performance for patients with biliary tract cancer with area under the receiver operating curve values from 0.870 to 0.996. Furthermore, this method was successfully applied to quantify di/tripeptides in the extract of an animal-derived traditional Chinese medicine, Eupolyphaga sinensis Walker. These findings highlight the possible application of the analytical method in clinics and for the purposes of quality control of traditional Chinese medicines.
Roxarsone (ROX) is a commonly used antibacterial and growth-promoting additive to animal feed. The development of an effective method for detecting ROX and its conversion products is of importance because of their potential harm to human health and ecosystem. Herein, we report the designed synthesis of a novel one-dimensional covalent organic framework (1D COF), named EP-COF, and its application as a fluorescent probe for ROX sensing. EP-COF is constructed based on imine linkages, exhibiting high crystallinity, strong fluorescence emission, and good dispersibility in water. It displays a remarkable capability to efficiently detect ROX, with an impressive detection limit of 4.5 nmol/L. Moreover, EP-COF also offers advantages of excellent selectivity, and high structural stability. This work not only presents a promising approach for the detection of harmful substances like ROX, but also serves as a valuable reference for exploring application of 1D COFs in chemical sensing.
Magnesium rechargeable batteries (MRBs) present opportunities for grid-scale energy storage applications as a complement to Li-ion batteries (LIBS). The major challenges are the low reversible capacity, inferior cycling stability and unsatisfactory energy densities. Na3VCr0.5Fe0.5(PO4)3 with a well-defined NASION-type structure is used as cathode in Mg cell. Two-electrons reaction (~116 mAh/g), 1.5 V average voltage and 65% of capacity retention over 100 cycles are accomplished. Mg is inserted by a biphasic reaction with the participation of V3+/V4+/V5+ redox couples in the electrochemical reaction while the non-active redox couples such as Cr3+/Cr4+ and Fe2+/Fe3+ served as stabilizer to buffer the volume variation. A thermal stability up to ~412 ℃ is also exhibited. Therefore, incorporating a mixture of three transition metal (V/Cr/Fe) in this type of structures will broaden new perspectives for realizing high performance cathodes for MRBs.
Hidden natural products are representative of defensive strategies produced in vivo in diseased plants, a process that is induced by the plant immune system. The first transcriptome library of uninfected and pathogen infected Hibiscus tiliaceus stems was constructed by transcriptome sequencing technology, genes related to cadinene-type sesquiterpenoid biosynthesis were screened and combined with ultra-performance liquid chromatography-quadrupole-time of flight mass spectrometry (UPLC-QTOF-MS) analysis data, which indicated pathological tissue had potential to produce novel carbon skeletons of cadinane sesquiterpenoid dimers. Successfully, two cadinane-derived sesquiterpenoid dimers with unprecedented carbon skeletons, hibisceusanols A (1) and B (2) were isolated for the first time from the stems of H. tiliaceus induced by plant-microbial interactions. Their structures and absolute configurations were unambiguously established by spectroscopy, advanced chemistry development (ACD) and electronic circular dichroism (ECD) methods. Compounds 1 and 2 exhibited significant antitumor activity in vitro with half maximal inhibitory concentration (IC50) values of 2.3–7.2 µmol/L. The anticancer effect was generated via the induction of HepG2 cell apoptosis by inhibiting the phosphatidylinositol 3-kinase (PI3K) pathway.
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