Latest ArticlesIn this study, we proposed a novel and efficient way to strengthen polyvinyl alcohol (PVA) fiber using graphene quantum dots (GQDs). PVA molecular chains were grafted onto the surface of GQDs through Friedel-Crafts alkylation reaction to obtain functionalized GQDs (f-GQDs), and PVA/f-GQDs composite fiber was successfully prepared by wet spinning and post-treatment. The tensile strength and Young’s modulus of the composite fiber reached up to 1229.24 MPa and 35.36 GPa which were approximately twice and 4 times those of the pure PVA fiber, respectively. Moreover, the composite fiber was demonstrated excellent resistance to solvents. In addition, the PVA/f-GQDs composite fiber showed intense and uniform cyan fluorescence, meanwhile, it could maintain stable solid-state fluorescence in acid and alkali solutions and particularly after long-term immersion in water (1 month). This study proposes a promising route for obtaining high-performance conventional fibers with some new functions.
Accurate determination of lung cancer margins at the molecular level is of great significance to determine the optimal extent of resection during surgical operation and reduce the risk of postoperative recurrence. In this study, internal extractive electrospray ionization mass spectrometry (iEESI-MS) was used to trace potential molecular tumor margins in lung cancer tissue. Molecular differential model for the determination of lung cancer tumor margin was established via partial least-squares discriminant analysis (PLS-DA) of iEESI-MS data collected from lung tissue pieces within cancer tumor area and iEESI-MS data collected from lung tissue pieces outside cancer tumor area. Proof-of-concept data demonstrate that the developed molecular differential model yields ca. 1–2 mm wider potential molecular tumor margin of a lung cancer compared to the conventional histological analysis, showing promising potential of iEESI-MS to increase the accuracy of tumor margins determination and lower risk of lung cancer postoperative recurrence. Furthermore, our results revealed that creatine and taurine showed positive correlations with lung cancer.
Birefringent crystals play an irreplaceable role in optical systems by adjusting the polarization state of light in optical devices. This work successfully synthesized a new thiophosphate phase of β-Pb3P2S8 through the high-temperature solid-state spontaneous crystallization method. Different from the cubic α-Pb3P2S8, the β-Pb3P2S8 crystallizes in the orthorhombic Pbcn space group. Notably, β-Pb3P2S8 shows a large band gap of 2.37 eV in lead-based chalcogenides, wide infrared transparent window (2.5−15 µm), and excellent thermal stability. Importantly, the experimental birefringence shows the largest value of 0.26@550 nm in chalcogenides, even larger than the commercialized oxide materials. The Barder charge analysis result indicates that the exceptional birefringence effect is mainly from the Pb2+ and S2− in the [PbSn] polyhedrons. Meanwhile, the parallelly arranged polyhedral layers could improve the structural anisotropic. Therefore, this work supports a new method for designing chalcogenides with exceptional birefringence effect in the infrared region.
Carbon dots (CDs), due to their low cost, high stability, and high luminous efficiency, have emerged as an excellent material for the emissive layer in next-generation electroluminescent light-emitting diodes (ELEDs). However, improving the efficiency of fluorescent CDs-based ELEDs remains challenging, primarily because it is difficult to utilize triplet excitons in the electroluminescence process. Therefore, enhancing the exciton utilization efficiency of CDs during electroluminescence is crucial. Based on this, we exploited the characteristic large exciton binding energy commonly found in CDs to develop exciton-emitting CDs. These CDs facilitate the radiative recombination of excitons during electroluminescence, thereby improving the electroluminescent efficiency. By rationally selecting precursors, we developed high quantum efficiency CDs and subsequently constructed CDs-based ELEDs. The blue-light device exhibited an external quantum efficiency of over 4%. This study introduces a novel design concept for CDs, providing a new strategy for developing high-performance blue ELEDs based on CDs.
Semi-heterogeneous photocatalysis has emerged as a powerful and productive platform in organic chemistry, which provides mild and eco-friendly conditions for a diverse range of bond-forming reactions. The synergy of homogeneous catalysts and heterogeneous catalysts inherits their main advantages, such as higher activities, easy separation and superior recyclability. In this review, we summarize the recent advances in recyclable semi-heterogenous protocols for the light promoted bond-forming reactions and identify directions for future research according to the different photocatalysts/metal/redox catalysts involved. Notably, this review is not a comprehensive description of reported literature but aim to highlight and illustrate key concepts, strategies, reaction model, reaction conditions and mechanisms.
Environment-sensitive fluorescent probes are commonly utilized in various fields, including fluorescence sensing and imaging. This paper describes the synthesis and photophysical properties of a novel class of solvatochromic fluorophores that incorporate biisoindolylidene as the core backbone. This study investigates the structure-property relationships of these newly developed fluorophores. The central biisoindolylidene acts as an efficient electron acceptor, and by modifying the aryl ring substituent at the 3,3′ position, the photophysical properties of the fluorophores can be significantly enhanced, particularly in terms of photoluminescence quantum efficiency. Furthermore, when an electron-donor group replaces the aryl ring at the 3,3′ position, intriguing solvatochromic behavior is observed. This leads to a red-shift in the maximum emission wavelength and an increase in the Stokes shift with increasing solvent polarity. In solvent dimethyl sulfoxide (DMSO), the maximum emission wavelength can reach up to 750 nm, with a Stokes shift of approximately 150 nm. Finally, the potential application of the fluorophore in the detection of volatile acids is explored in a preliminary manner.
Innovative anti-cancer therapies that activate the immune system show promise in combating cancers resistant to conventional treatments. Photodynamic therapy (PDT) is one such treatment, which not only directly eliminates tumor cells but also functions as an in situ tumor vaccine by enhancing tumor immunogenicity and triggering anti-tumor immune responses through immunogenic cell death (ICD). However, the effectiveness of PDT in enhancing immune responses is influenced by factors, such as photosensitizers and the tumor microenvironment, particularly hypoxia. Current clinically used PDT heavily relies on oxygen (O2) availability and can be limited by tumor hypoxia. Additionally, the tumor immunosuppressive microenvironment induced by hypoxia affects the anti-tumor immunity of tumor-infiltrating effector T cells. Meanwhile, the immunosuppressive myeloid-lineage cells are recruited to the hypoxic tumor tissue and exhibit higher immunosuppressive capabilities under hypoxia conditions. Consequently, numerous strategies have been developed to modulate tumor hypoxia or to create hypoxia-compatible PDT, aiming to reduce the effects of tumor hypoxia on PDT-driven immunotherapy. This review investigates these strategies, including approaches to alleviate, exploit, and disregard tumor hypoxia within the context of PDT/immunotherapy. It also emphasizes the role of advanced nanomedicine and its benefits in these strategies, while outlining current challenges and future prospects in the field.
In chemical science, the vertical ionization potential (VIP) is a crucial metric for understanding the electronegativity, hardness and softness of chemical material systems as well as the electronic structure and stability of molecules. Ever since the last century, the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights. However, their performance in realm of the vertical electron processes of molecular systems has been rarely explored. In this study, we for the first time benchmarked the model chemistry composite methods (e.g., CBS-QB3, G4 and W1BD) in comparison with the commonly used Koopmans's theorem (KT), electron propagator theory (e.g., OVGF, D2, P3 and P3+) and CCSD(T) methods in calculating the VIP for up to 613 molecular systems with available experimental measurements. The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy, economy and applicability. Notably, the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 eV at all calculation levels, which have strong hints that their VIP experimental values should be re-investigated.
The interface modulation significantly affects the photocatalytic performances of supported metal phthalocyanines (MPc)-based systems. Herein, ZnPc was loaded on nanosized Au-modified TiO2 nanosheets (Au-T) to obtain wide-spectrum ZnPc/Au-T photocatalysts. Compared with large Au NP (8 nm)-mediated ZnPc/Au-T photocatalyst, ultrasmall Au NP (3 nm)-mediated one shows advantageous photoactivity, achieving 3- and 10-fold CO2 conversion rates compared with reference ZnPc/T and pristine TiO2 nanosheets, respectively. Employing monochromatic beam-assisted surface photovoltage and photocurrent action, etc., the introduction of ultrasmall Au NPs more effectively facilitates intrinsic interfacial charge transfer. Moreover, ZnPc molecules are found more dispersed with the existence of small Au NPs hence exposing abundant Zn2+sites as the catalytic center for CO2 reduction. This work provides a feasible design strategy and renewed recognition for supported MPc-based photocatalyst systems.
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