Latest ArticlesConstructing more stable self-assembled organic nanotubes has been one of the focuses of scientists in recent decades. Hexakis(m-phenylene ethynylene) (m-PE) benzene macrocycles can form stable tubular self-assemblies in nonpolar or weakly polar solvents through the π-π interaction of the main skeleton and the hydrogen bonding of the side chain amide. We covalently linked two macrocyclic units at the para position of the macrocycles using two oligo(β-alanine) linkers through an efficient synthetic route. UV–visible spectroscopy, fluorescence spectroscopy, and circular dichroism spectroscopy were employed to demonstrate that the incorporation of two peptide chains significantly enhances the stability of the self-assemblies. Meanwhile, the average open time of the ion channel formed by the macrocyclic dimer in the lipid bilayer was significantly better than that of the ion channel formed by a single macrocycle. This study shows that this strategy effectively improves the efficiency of self-assembly and the stability of its formed self-assemblies, providing a feasible strategy for constructing organic self-assembled nanotubes in highly polar solvents.
Label-free immunoassay is confronted with a great challenge that its insufficient sensitivity for low concentration analytes, which can be assigned to the low catalytic efficiency of modified materials towards electroactive molecules. Herein, a universal MOF nanozyme-induced catalytic amplification strategy was proposed for constructing highly sensitive label-free electrochemical immunoassay. Specifically, the synthesized CuFe-MOF nanozyme with superior peroxidase (POD)-like activity, regarding as a MOF nanozyme model, can catalyze hydrogen peroxide to produce hydroxyl radicals (•OH), which can efficiently oxidize electroactive probe (such as 1,2-phenylenediamine (o-PD)) accompanying with intense electrochemical signals. Modification of MOF nanozyme on the electrode and capture of antibodies for binding target antigens hinder the catalytic process of MOF nanozyme toward o-PD, resulting in a gradual decrease in electrochemical signal with increasing target antigen concentration, enabling quantitative label-free immunoassay. Thus, a highly sensitive label-free immunosensor using MOF nanozyme-induced catalytic amplification achieved effective detection of Immunoglobulin G (IgG) with a wide linear range of 0.001–50 ng/mL and low detection limit of 0.45 pg/mL. This work proposes a promising nanozyme-induced catalytic amplification strategy for the development of label-free electrochemical immunoassay.
A series of novel crown aldoxime ethers were synthesized, demonstrating notable thermal and hydrolysis stability. The showcased acid-catalyzed and photo-induced cis/trans isomerization, which enables orthogonal control over both guest complexation and the chiroptical effects of these crown aldoxime ethers, manifesting a regulation of complexation through isomerization at binding heteroatoms.
Stimulus-responsive room-temperature phosphorescence (RTP) materials have gained significant attention for their important optoelectronic application prospects. However, the fabrication strategy and underlying mechanism of stimulus-responsive RTP materials remain less explored. Herein, we present a reliable strategy for achieving pH-responsive RTP materials by integrating poly(vinyl alcohol) (PVA) with carboxylic acid or amino group functionalized terpyridine (Tpy) derivatives. The resulting Tpy derivatives-based RTP materials displayed reversible changes in emission color, intensity, and lifetime of both prompt and delayed emission. Notably, the RTP emission undergoes a significant diminish upon exposure to acid due to the protonation of Tpy units. Taking advantage of the decent RTP emission and pH-responsiveness of these RTP films, a spatial-time-resolved anti-counterfeiting application is demonstrated as a proof-of-concept for largely enhancing the security level. This study not only provides new prospects for developing smart RTP materials but also promotes the advancement of optical anti-counterfeiting applications.
Metal-catalyzed alkene arylalkoxylation is a powerful complexity-building strategy for the synthesis of oxygen heterocycles from simple γ-unsaturated alcohols, but only a few examples of catalytic enantioselective methods exist. Herein, an efficient palladium-catalyzed enantioselective arylalkoxylation of γ-hydroxyalkenes with aryl halides is reported. The salient features of this transformation include a remarkable broad substrate scope, mild reaction conditions, and good functional group tolerance, delivering a series of chiral tetrahydrofurans containing a tertiary or quaternary stereocenter in good yields with up to 95% ee. The Xu10 ligand with a suitable side-arm was responsible for the high reactivity and good enantioselectivity of this transformation.
The design and synthesis of organic high-temperature reversible thermochromic materials is one of the difficult issues in the field of organic chromic materials. In this paper, four diacetylene monomers named DBA-PCDA, TBA-PCDA, DBE-PCDA and TBE-PCDA, each containing multiple diacetylene units, were synthesized from 10,12-pentacosadiynoic acid (PCDA) through the amidation or esterification reactions, using 4,4′-diaminobiphenyl, 1,3,5-tris(4-aminophenyl)benzene, 4,4′-dihydroxybiphenyl, and 1,3,5-tris(4-hydroxyphenyl)benzene as bridging units. The effects of functional groups that can form hydrogen bond and π-π interactions on the solid-state polymerization properties of monomers and the thermochromic properties of the corresponding PDAs were investigated. The results show that only DBA-PCDA and TBA-PCDA, which contain functional groups that can form hydrogen bonding interactions, can be polymerized under 254-nm UV irradiation. The corresponding poly(DBA-PCDA) exhibits reversible thermochromic property even heated up to 200 ℃, showing a potential application in the field of high-temperature thermal indicator above 100 ℃. This work provides a new perspective to the development of PDA with high-temperature reversible thermochromic property.
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 facile visible-light-induced 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene (4CzIPN) catalyzed four-component reaction of alkenes, quinoxalin-2(1H)-ones, P4S10 and alcohols has been developed at room temperature. This tandem reaction provides an efficient strategy for the construction of various phosphorodithioate-containing quinoxalin-2(1H)-ones with moderate to good yields by using air (dioxygen) as the green oxidant. Experimental studies revealed a radical process was involved in this photochemical reaction.
Reactive 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.
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.
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