Latest ArticlesA 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.
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.
Photocatalytic activation of peroxymonosulfate (PMS) has garnered a lot of interest in the field of wastewater treatment. Herein, a plasmonic Ag nanoparticles decorated MIL-101(Fe) hybrid was synthesized through a photodeposition process. Upon light irradiation, the Ag/MIL-101(Fe) exhibit reinforced photocatalytic activities for elimination of bisphenol A (BPA) with PMS. The optimized 2.0% Ag/MIL-101(Fe) composite presented the highest photocatalytic activity with kinetic constant k of 0.102 min−1, which was about 10-fold of the pristine MIL-101(Fe). Loading of plasmonic Ag into MIL-101(Fe) boosts photoinduced carrier separation and accelerates PMS activation to generate strong oxidative radicals. Photoelectrochemical tests and multiple spectroscopic studies confirmed the promoted charge carrier separation and transfer capability of Ag/MIL-101(Fe). Combining the results of radical trapping experiments and electron spin resonance (ESR), the formed SO4•−, •OH, •O2− and 1O2 had a significant role in the photocatalytic process. According to intermediate study, the degradation pathway was studied, and the possible mechanism was proposed.
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.
Herein, two antimony sulfates, named RbSb(SO4)2 (1) and CsSb(SO4)2 (2), have been successfully synthesized with the introduction of Sb3+ cation with stereochemically active lone pairs (SCALP) into sulfates by the conventional hydrothermal method. Both two compounds endow short ultraviolet (UV) absorption edges (281 nm and 278 nm, respectively) and large birefringence (0.171@546 nm and 0.174@546 nm, respectively), which means that they are promising short-wave UV optical materials. Interestingly, though both of the two compounds exhibit similar 1D chained structures, and possess the same functional moieties including SbO4 seesaws and SO4 tetrahedral groups, they exhibit significantly opposite macroscopic symmetries, i.e., compound 1 crystallizes in a centrosymmetric (CS) manner (P21/n) and compound 2 in a noncentrosymmetric (NCS) manner (P212121), due to the size of cations [r(Rb+) = 1.56 Å, r(Cs+) = 1.67 Å] affects the orientation of SCALP of the adjacent Sb3+.
DNA circuits are powerful tools in various applications such as logical computation, molecular diagnosis and synthetic biology. Leakage is a major problem in constructing complex DNA circuits. It directly affects the output signal and harms the circuit's performance significantly. In the traditional DNA circuits, the gate complex is a duplex structure. There are insufficient energy barriers to prevent spontaneous detachment of strands, resulting in a leak prone. Herein, we have developed triplex-structure based DNA circuit with ultra-low leakage and high signal-to-noise ratio (SNR). The triplex structure improves the stability in the absence of input. At the same time, the driving force of the strand displacement cascades reduces the influence of the triplex structure on the desired reaction. The SNR of the DNA circuit was increased to 695, while the desired reaction rate remained 90% of the conventional translator circuit. The triplex-structure mediated leakage prevention strategy was further tested at different temperatures and in DNA translator and seesaw circuits. We also constructed modular basic logic gates with a high efficiency and low leakage. On this basis, we further constructed triplex-structure based tertiary DNA logic circuits, and the SNR reached 295, which, to the best of our knowledge, was among the highest of the field. We believe that our scheme provides a novel, valid, and general tool for reducing leakages, and we anticipate that it will be widely adopted in DNA nanotechnology.
Fluorescent silicon quantum dots (Si QDs) were hydrothermally synthesized from a mixture of 3(2-aminoethylamino) propyl (dimethoxymethylsilane) (AEAPDMMS) and poly(vinylpyrrolidine) (PVP). The resulting Si QDs exhibited good water solubility and high stability. Under the optimized conditions, the probe revealed an excellent linear fluorescence quenching effect on Co2+ ranging from 1 µmol/L to 120 µmol/L with a limit of detection of 0.37 µmol/L (based on 3 s/k). The quenching mechanism was studied, showing that static quenching (SQE) causes the main effect. Furthermore, the test paper based on Si QDs was prepared, which is cost-effective, high sensitivity, good selectivity, easy to use and show excellent anti-interference capability. This method was applied to analyze the content of Co2+ in environmental water samples with satisfying results.
Photothermal effect has been widely employed in the H2 evolution process at the advantage of using clean energy sources to produce another one of higher benefits. The solar-to-heat conversion have various forms and heat can facilitate reactions in a variety of dimensions. Hence, summarizing the sources and destinations of heat is important for constructing hydrogen production systems of higher efficiency. This view mainly focuses on the recent state-of-art progress of hydrogen evolution reaction (HER) based on photothermal effect. First, we introduce the main pathways of photothermal conversions applied in H2 evolution. Then, the functions of the photothermal effect are clearly summarized. Furthermore, we go beyond the catalytic reaction and introduce a method to improve the catalytic system by changing the catalytic bulk phase through thermal means. In the end, we sort out the challenges and outlook to offer some noble insights for this promising area.
Alcohol consumption is one of the leading causes of death worldwide. Adolescence is a critical period of structural and functional maturation of the brain. Adolescent alcohol use can alter epigenetic modifications. However, little is known on the long-term effects of alcohol consumption during adolescence on RNA epigenetic modifications in brain. Herein, we systematically explored the long-term effects of alcohol exposure during adolescence on small RNA modifications in adult rat brain tissues by comprehensive liquid chromatography-electrospray ionization-tandem mass spectrometry (LC-ESI-MS/MS) analysis. We totally detected 26 modifications in small RNA of brain tissues. Notably, we observed most of these modifications were decreased in brain tissues. These results suggest that alcohol exposure during adolescence may impose a long-lasting impact on RNA modifications in brain tissues. This is the first report that alcohol use during adolescence can alter RNA modifications in adult brain. Collectively, this study suggests a long-term adverse effects of alcohol consumption on brain from RNA epigenetics angle by comprehensive mass spectrometry analysis.
Molecular doping has become a widely used method to modulate the electric performance of organic semiconductors (OSC). Highly effective charge transfer during molecular doping is desired to achieve ideal electrical conductivity. Two types of charge transfer mechanisms are widely accepted in molecular doping process: integer charge transfer (ICT) and charge transfer complex (CTC). In this review, fundamental principles of two mechanisms are revisited and the characterization methods are depicted. The key points for the formation of two mechanisms are highlighted from aspects of molecular structure and process engineering. Then, the strategies to improve the proportion of ICT are discussed. Finally, the challenges and perspectives for future developments in the molecular doping of polymer semiconductors are provided.