Latest ArticlesThe development of molecular probes or systems with the ability of multiple orthogonal responses is an effective approach to precisely detect biomolecules with similar chemical structures. Herein, we report the synthesis of a water-soluble TPE-based octacationic cage (1) with the compressed TPE-containing bilayer, which endows it with good fluorescence properties and potential conformation chirality. As a result, 1 exhibits molecular recognition for anionic nucleotides within its two “claw”-like cavities to form 1:2 host-guest complexes in water, companying with selective turn-off fluorescence and turn-on CD responses to G/GTP over other nucleotides.
Carbon dots (CDs) have been attracted much attention and widely studied due to their excellent fluorescence (FL) properties, better biocompatibility and outstanding photo/chemical stability. However, the disadvantage of lower quantum yield (QY) still limits its wide application. Herein, we reported a novel and convenient strategy to prepare photo-induced Ag/CDs (p-Ag/CDs) by irradiating the mixed Ag+ and hydrophobic CDs (h-CDs) acetone solution with ultraviolet (UV) light. The obtained p-Ag/CDs exhibit a greatly enhanced FL emission together with a blue shift (460 nm) than h-CDs (520 nm). The QY of p-Ag/CDs is measured to be 51.1%, which is 10.4 times higher than that of h-CDs (4.9%), indicating that photo-induced Ag modulation can effectively improve the optical properties of CDs. The mechanisms for the FL enhancement and blue shift of h-CDs are studied in detail. The results prove that the greatly enhanced FL emission is from the generated Ag nanoparticles (AgNPs) by UV light irradiation based on metal-enhanced fluorescence (MEF), and the increased oxygen-contained groups in this process lead to the blue shift in CDs fluorescence. Interestingly, the p-Ag/CDs exhibit higher sensitivity and selectivity for sulfide ions (S2−) detection than that of h-CDs, which have a lower response to S2−. This work not only offers a novel strategy to improve the FL properties of materials but also endows them with new functions and broadens their application fields.
Drug loading capacity is very important in the construction of targeted drug delivery systems (TDDSs) for the improvement of drug delivery efficiency. However, the drug-loading capacity of most nanomaterials is non-idealistic, and developing the high drug-loading TDDSs is still a critical challenge. In this work, an ultrahigh loading system (denoted as HMPB2) was prepared via J-aggregation of an aza-boron dipyrromethene derivative (Bod) by using hollow MnO2 modified with glucosamine pillar[5]arene as a carrier, which was demonstrated to have typical J-aggregate absorption of Bod, specific cancer cells targeting ability, negligible dark cytotoxicity, and potent phototoxicity. This work provides a successful example to construct an ultrahigh drug-loading system via J-aggregation for targeted delivery.
A dimesitylboryl-ended oligothiophene with tetrazine as core (BTz) was synthesized and its reactivity and spectral changes toward trans-cyclooctene ((4E)-TCO-OH), cis-cyclooctene and bicyclo[6.1.0]non-4-yn-9-ylmethanol were comprehensively studied. The fluorescence intensity of BTz was enhanced up to more than 100 times upon bioorthogonal reaction with (4E)-TCO-OH. In addition, the first crystal structure of isolated product of tetrazine derivative with cyclooctene was determined, which clearly confirmed a dehydrogenation occurred after Diels–Alder reaction under ambient conditions.
Organic long-persistent luminescence (LPL) materials, featuring low preparation cost, eco-friendly synthesis, and easy modification of functional groups, have exhibited extensive applications in information encryption, anti-counterfeiting, and biological imaging. Several design strategies including crystallization-inducement, H-aggregation, and host–guest doping to enhance persistent-room-temperature phosphorescence (RTP) effect by precisely controlling intersystem crossing (ISC) constant and suppressing nonradiative decay rates, those are important strategies to enable LPL performance. Among the strategies, researchers have made several efforts to enhance persistent-RTP effect by host–guest interaction, in which the host matrices provide a rigid environment for phosphor guest molecules. The interaction of the luminescent guest molecules with the host matrix can effectively reduce the vibration and rotation of the luminescent molecules, and suppress the non-radiative inactivation, thereby improving the phosphorescence quantum yield. This review aims to summarize several design strategies of pure organic LPL materials based on persistent-RTP effect through host–guest interaction, and describe some applications of pure organic LPL materials in different fields.
Rational design of heterogeneous catalysts with high activity and stability is crucial in peroxymonosulfate (PMS)-based oxidation treatment of wastewater. Herein, the graphite oxide-cobalt ferrite (GO-CoFe2O4) composite was constructed, and its morphological, component and structural characteristics were thoroughly examined, respectively. GO-CoFe2O4 obviously boosted PMS catalytic performance on di-n–butyl phthalate removal (DBP, RDBP = 90%, RTOC = 37%), which indicated by the first-order kinetic constant (kDBP = 0.060 min−1) being roughly 4 times than pure CoFe2O4 (kDBP = 0.015 min−1). The fabrication of GO-CoFe2O4 brought the favorable stability and repeatability up to six cycles. Moreover, the method of batch dosing catalyst was creatively proposed to improve the PMS utilization efficiency. The coupling of GO enhanced the dispersion of CoFe2O4 particles to obtain sufficient active sites, additionally, the plentiful C=O groups and free-flowing electrons on GO promoted GO-CoFe2O4 to coordinate a redox process during PMS activation. With the aid of theoretical calculations, GO-CoFe2O4 was revealed to exhibit a strong affinity toward PMS adsorption, where PMS spontaneously dissociated into sulfate radical (SO4•−), hydroxyl radical (•OH) and singlet oxygen (1O2), acting as the reactive oxygen species (ROSs). Electrons cycling between Co, Fe and O species ensured continuous ROSs generation and excellent catalytic performance.
Herein, we review the significant of ordered macroporous (OM) TiO2-based catalysts for boosting photocatalytic CO2 reduction. Based on the need to improve the three key factors of photogenerated charge separation efficiency, solar energy utilization and CO2 adsorption rate during the conversion of CO2 to H2O, we summarized five modification measures: including doping ions into OM TiO2, introducing second semiconductor coupling and noble metal nanoparticles for fabricating multiple Z-scheme heterojunctions, constructing hierarchical pore and carbon-loaded OM TiO2 materials, which effectively enhance the absorption rate of visible light, the separation rate of electrons-hole pairs and the selection of multiple active sites. The OM structured TiO2-based photocatalysts solve the single or multiple key factors for enhancing photocatalytic performances during CO2 conversion. The catalytic mechanism and pathways of OM structured TiO2-based photocatalysts for CO2 reduction are discussed and summarized. It provides new insights on the development of high-efficient catalyst for photocatalytic CO2 conversion to solar fuels.
Phenylspirodrimanes are a kind of meroterpenoids with structural diversity and complexity, exhibiting a wide of biological properties, especially for the lactam derivatives consisting a γ-lactam moiety and N-linked side chains. These compounds were derived from multi-step combination of enzymatic and non-enzymatic conversions of intermediates in their biosynthetic pathways. Stachbotrydial (2) with an o-phthalaldehyde unit was supposed as the high-reactivity intermediate of phenylspirodrimane lactams via nonenzymatic reaction with amines. In the present work, an effective and non-enzymatic diversification strategy was developed for the structural diversification of phenylspirodrimane lactams including monomers and dimers from 2 by feeding structurally various mono- and diamines in the fungus Stachybotrys chartarum cultures. In total, 24 phenylspirodrimane lactams (1, 3–25) including 18 new compounds were synthesized. Among them, stachybocin A (1), a bioactive phenylspirodrimane lactam dimer, was produced with the yield of 18.7 mg/g of cell dry weight. The structures of these compounds were elucidated by extensive spectroscopic data, single-crystal X-ray diffraction (Cu Kα), and calculated electronic circular dichroism (ECD) analyses. Bioassay revealed that compounds 1, 17, and 24 displayed significant inhibitory effect on the inactivated state of hNaV 1.2 channels with IC50 values of 0.22, 2.08, and 0.53 µmol/L, respectively. In addition, 1 showed potent protein tyrosine phosphatase 1B (PTP1B) inhibitory, N-methyl-D-aspartate (NMDA) receptor antagonistic, and anti-inflammatory activities.
Three-dimensional (3D) histology has exhibited tremendous potential in fundamental research and clinical disease grading, but compatible labeling techniques are still lacking. Recently in Science Advances, Pac et al. report a new histological technique termed 3DNFC, which realizes 3D fluorescence imaging of thick tissues via citrate-based in situ fluorophore formation.
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