Latest ArticlesBenzo[4,5]imidazo[1,2-a]pyrimidine-based derivatives play crucial roles in medicines, pesticides, tracers and photoelectric materials. However, their synthesis approach still needs to be optimized, and their fluorescent properties in intracellular microenvironment are unclear. Here, a Cu(Ⅱ)-catalyzed cascade coupling cyclization reaction was successfully developed to synthesize benzo[4,5]imidazo[1,2-a]pyrimidine scaffold with mild reaction conditions, broad substrate scopes and high yields. After a system study, we found that compound 4aa displayed an optimal viscosity-specific response with remarkable fluorescence enhancement (102-fold) for glycerol at 490 nm. Particularly, 4aa possessed excellent structure-inherent targeting (SIT) capability for lysosome (P = 0.95) with high pH stability and large Stokes shift. Importantly, 4aa was validated for its effectiveness in diagnosing lysosomal storage disorders (LSD) in living cells. The 4aa also showed its potential to map the micro-viscosity and its metabolism process in zebrafish. This work not only affords an efficient protocol to fabricate benzo[4,5]imidazo[1,2-a]pyrimidine derivatives, reveals this skeleton has excellent SIT features for lysosome, but also manifests that 4aa can serve as a practical tool to monitor lysosomal viscosity and diagnose LSD.
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.
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.
Highly active transition metal nitrides are desirable for electrocatalytic reactions, but their long-term stability is still unsatisfactory and thus limiting commercial applications. Herein, for the first time, we report a unique and universal room-temperature urea plasma method for controllable synthesis of N-doped carbon coated metal (Fe, Co, Ni, etc.) nitrides arrays electrocatalysts. The preformed metal oxides arrays can be successfully converted into metal nitrides arrays with preserved nanostructures and a thin layer of N-doped carbon (N-C) via one-step urea plasma. Typically, as a representative case, N-C@CoN nanowire arrays are illustrated and corresponding formation mechanism by plasma is proposed. Notably, the designed N-C@CoN catalysts deliver excellent electrocatalytic activity and long-term stability both in oxygen evolution reaction (OER) and urea oxidation reaction (UOR). For OER, a low overpotential (264 mV at 10 mA/cm2) and high stability (>50 h at 20 mA/cm2) are acquired. For UOR, a current density of 100 mA/cm2 is achieved at only 1.39 V and maintain over 100 h. Theoretical calculations reveal that the synergetic coupling effect of CoN and N-C can significantly facilitate the charge-transfer process, optimize adsorbed intermediates binding strength and further greatly decrease the energy barrier. This strategy provides a novel method for fabrication of N-C@ metal nitrides as highly active and stable catalysts.
The supramolecular Förster resonance energy transfer (FRET) is seen as a promising approach for organic photocatalysis using dyes as catalysts, because it combines the high efficiency of energy transfer with the dynamic responsiveness based on non-covalent interactions. Here we propose a supramolecular FRET photocatalysis strategy for α-oxyamination reaction based on supramolecular confinement effect. The well-designed benzothiadiazole-based cationic monomer as energy donor and the dyes of Nile Red as acceptor are doped into the amphiphilic surfactants of sodium dodecyl sulfate (SDS). Benefitting from the supramolecular confinement space provided by SDS in aqueous environment, the FRET process between the monomer and Nile Red is effectively achieved (exciton migration rate: 3.99 × 1014 L mol‒1 s‒1). On this basis, the supramolecular FRET system is used as an efficient energy source to catalyze α-oxyamination reactions between a series of 1,3-dicarbonyl compounds and 2,2,6,6-tetramethylpiperidine-1-oxyl under white LED light, showing a yield as high as 94% and a turnover frequency value of 3.92 h‒1. This photocatalytic result shows a great enhancement compared to that of Nile Red alone.
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.
Nanographenes (NGs) with twisted backbones are emerging as new candidates for chiroptical materials. In this work, we describe a new strategy for synthesizing a [10]twistacene-embedded NG which exhibits a rare flag-hinge-like geometry. By neatly creating steric crowding on the [6]helicene breaches of the NG skeleton, the synthesis only provided homochiral isomers without generating the "meso‑" isomer. The formed NGs showed high luminescence with quantum yield up to 52%, and promising circularly polarized luminescence (CPL) performance with |glum| up to 5.0 × 10−3. Besides, these NGs also showed outstanding CPL brightness (BCPL) up to 305 L mol−1 cm−1 among chiral NGs.
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.
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