Latest ArticlesNear infrared-II (NIR-II) dyes have unique advantages in biomedical applications owing to the powerful ability in penetrating biological tissues. Herein, NIR-II aza-BODIPY dye, QLD-BDP, was developed with julolidine at 1,7-sites and p-dimethylaminophenyl group at 3,5-sites. According to X-ray analysis, QLD-BDP exhibits significant distortion, and this molecule appears a bowl shaped structure. The photothermal conversion efficiency of the self-assembled QLD-BDP nanoparticles (QLD-BDP-NPs) can reach 50.5%, with maximum emission at 998 nm by the aggregate. QLD-BDP-NPs can cause the complete destruction of 4T1 multicellular spheroids (MCSs), indicating a photothermal therapy (PTT) effect.
Control of subsurface interstitial atoms in transition metals is an effective approach to modulate selectivity in hydrogenation reactions. In this study, nickel was alloyed with gallium to form Ni3Ga, thereby regulating the octahedral interstitial sites. Subsequently, carbon atoms were introduced into the Ni3Ga (forming Ni3GaC0.5) via thermal treatment in an acetylene atmosphere, leading to a significant enhancement in selectivity for acetylene hydrogenation reaction. The X-ray diffraction and transmission electron microscopy results demonstrate an increase in the lattice parameter due to the incorporation of carbon atoms and the uniform distribution of carbon in Ni3GaC0.5 nanoparticles. The obtained Ni3GaC0.5/oCNT catalyst exhibits significantly improved selectivity in acetylene hydrogenation reaction, with approximately 82% ethylene selectivity at 98% conversion. Furthermore, it maintains good selectivity at various hydrogen-to-alkyne ratios and displays good stability during long-term operation. The introduction of carbon suppresses the formation of the subsurface hydrogen structure under reaction conditions. Additionally, the charge transfer between carbon and nickel results in the electron deficiency of nickel, effectively inhibiting the over-hydrogenation pathway and enhancing the selectivity. These results provide insights for the design of non-precious metal catalysts in selective hydrogenation reactions.
Multi-stimuli responsive materials controlled and coupled by two or more channels have a broad range of applications in the field of switches, memories, and molecular machines. The exploration of the material is currently focused on the pure organic system, which limits the development of such materials greatly. In this work, we present a new chiral organic-inorganic hybrid salt, (R-3-hydroxypyrrolidinium)2[Fe(CN)5(NO)] (1), which exhibits rare multi-stimuli responsive behaviors in thermal, mechanical and optical channels. In detail, 1 undergoes a C2-P21221 phase transition deriving from the thermal motion of organic cations with the increase of temperature, but the reverse transition can only be induced by mechanical pressure. Moreover, polycrystalline hybrid salt showed photo-responsive performance, i.e., the ground-state N-bound nitrosyl ligand adopts two configurations in excited states caused by light in 532 nm irradiation, accompanying with a photo-induced structural transformation of the anionic framework. Namely, the thermal motion characteristics of organic cations, the photoresponse characteristics of anionic inorganic skeleton and the pressure characteristics from hydrogen bonds are simultaneously integrated in 1. This unprecedented coupling mechanism of multi-stimuli responses makes 1 a potential candidate for future multichannel data storage applications.
The insufficient F(III)/Fe(II) cycling rate resulted from high combination of photogenerated carriers severely hinders the photo-Fenton activity. In this work, 0 dimensional α-Fe2O3 nanoclusters decorated TiO2 heterojunction (FT-x) was prepared via in-situ phase transformation strategy. FT-200 exhibited the optimal photo-Fenton activity for 2,4-dichlorophenol degradation with the kinetic rate constant reaching 1.0806 min−1 under low H2O2 dosage (1 mmol/L), which was 126.1 and 202.8 times higher than that of TiO2 and α-Fe2O3. Radical quenching experiments and electron spin resonance spectra proved that ·OH was the leading reactive specie. The enhanced photo-Fenton activity was attributed to the accelerated F(III)/Fe(II) cycling rate induced by the direct Z-Scheme charge transfer mechanism. Benefiting from the abundant ·OH production, the dechlorinate ratios and mineralization ratios of multiple chlorophenol pollutants (2,4-dichlorophenol, 4-chlorophenol, 2,4,6-trichlorophenol) all exceeded 98%. The biotoxicity of chlorophenol wastewater was greatly reduced after the treatment by Light/H2O2/FT-200 system. Overall, this work constructed a low-cost and highly efficient photo-Fenton system for refractory organic wastewater treatment.
The design of pnictide nonlinear optical crystals is quite different from chalcogenide and oxide those, in which a new paradigm need be developed to regulate the band gap, one of key optical parameters. In this work, two non-centrosymmetric halidepnictides, [Cd2P]2[CdBr4] (CPB) and [Cd2As]2[CdBr4] (CAB) were reported. The complete octet binding electrons of pnictogens were constructed by four Cd-P polar covalent bonds under the anchoring effect of halogens, creating an extremely flat valence band maximum with band dispersion of only 0.17 eV. As expected, the balance of the covalency and ionicity in CPB and CAB was successfully realized, leading to a wide band gap of 2.58 eV and 1.88 eV. Remarkably, CPB not only has a widest band gap among Cd-containing pnictides, but also exhibits a SHG effect of 1.2 × AgGaS2, moderate birefringence (0.088@visible light and calcd. 0.043@2050 nm) and a wide IR transmission range. This is the first time that the octet binding electrons construction strategy was utilized to design non-diamond like NLO pnictides with excellent performances.
Multimodal bioorthogonal small molecule probes play a pivotal role in drug-focused biomedical research. However, existing drug tracking and imaging techniques face obstacles in living organisms, hindering precise drug localization and target protein capture. Herein, we introduced a multimodal probe named 1-(azidomethyl)pyrene-4,5–dione (AMPD). The probe incorporates adjacent dione structures at the pyrene core. AMPD selectively interacts with oxygen-rich alkene-labeled drug molecules under ice-blue LED light exposure, producing specific fluorescence emission and enabling in vivo tracking and flow cytometry sorting. A methyl azide group was also introduced at the pyrene core to help efficiently enrich target proteins via click chemistry with alkyne-functionalized beads. AMPD demonstrates exceptional biocompatibility, rendering it highly suitable for visual photo-triggered tracking studies. Combined with metabolic labeling using an oxygen-rich alkene-tagged drug molecule probe, AMPD is effective for live animal, tissue, cellular, and in-gel imaging, as well as target protein identification through magnetic capture. With its versatile capabilities, AMPD enhances our comprehension of drug-target interactions at the in vivo level and expedites the process of drug discovery.
Most photodynamic therapies (PDT) rely on reactive oxygen species (ROS) produced by type Ⅱ mechanisms. However, since the production of type Ⅰ ROS is not limited by oxygen content, making it more favorable for antimicrobial phototherapy in complex microenvironments. Herein, we report a substituent cationization design strategy that not only improves the hydrophilicity of the prepared phthalocyanine molecule, but also promotes the electron transfer process in the photosensitizer, resulting in the strong type Ⅰ photodynamic effect of the phthalocyanine self-assembled photosensitizer to efficiently generate O2•- under both normal and hypoxic conditions. This in combination with its excellent bacteria recognition capability derived from the cationic part on its surface and intrinsic photothermal therapy effect of the phthalocyanine macrocycle endows the phthalocyanine self-assembled photosensitizer with excellent phototherapeutic antimicrobial properties in preclinical models, effectively promoting the wound healing process. This work provides a promising strategy for designing efficient multi-mode photosensitizers.
Radiotherapy (RT) is a widely used cancer treatment, and the use of metal-based nano-radiotherapy sensitizers has shown promise in enhancing its efficacy. However, efficient accumulation and deep penetration of these sensitizers within tumors remain challenging. In this study, we present the development of bismuth/manganese biomineralized nanoparticles (BiMn/BSA) with multiple radiosensitizing mechanisms, including high atomic number element-mediated radiation capture, catalase-mimic oxygenation, and activation of the stimulator of interferon genes (STING) pathway. Significantly, we demonstrate that low-dose RT induces the recruitment of macrophages and subsequent upregulation of Matrix metalloproteinases (MMP)-2 and MMP-9 that degrade the extracellular matrix (ECM). This dynamic process facilitates the targeted delivery and deep penetration of BiMn/BSA nanoparticles within tumors, thereby enhancing the effectiveness of RT. By combining low-dose RT with BiMn/BSA nanoparticles, we achieved complete suppression of tumor growth in mice with excellent biocompatibility. This study provides a novel and clinically relevant strategy for targeted nanoparticle delivery to tumors, and establishes a safe and effective sequential radiotherapy approach for cancer treatment. These findings hold great promise for improving the outcomes of RT and advancing the field of nanomedicine in cancer therapy.
The prodrug strategy provides an opportunity for improving the therapeutic index of drugs and avoiding their side effects. The main challenge lies in the fast and effective release of the parent drugs at the desired site under specific stimuli. Herein, a cooperative prodrug activation approach with exogenous native enzyme and endogenous tumor small molecule biomarkers was developed. Chemically, precursors of methylene blue (MB) and resorufin (RSF) react with horseradish peroxidase (HRP)/hydrogen peroxide (H2O2) to quickly and quantitatively release parent dyes and drugs containing amines or carboxylic acids. The application of this approach in mammalian cells was demonstrated with cooperative-activated photodynamic therapy based on a precursor of MB. Compared with free MB, much higher selectivity toward cancer cells was achieved with this approach as evaluated by the selectivity index (SI). This study provides a new method for fast and effective targeted prodrug activation with no need for antibody modification compared with traditional enzyme/prodrug therapy.
The increasing demand for energy density pushes LiCoO2 (LCO) to work at higher voltage (≥4.5 V), which brings a series of problems including detrimental phase transition and structural instability. Various elemental doping has been proven an effective strategy to improve its structure stability. However, the understanding of elemental doping homogeneity effect is not enough, whether in terms of the controllability of doping homogeneity or its complex consequences. In this work, LCO powders with different Al doping homogeneity were synthesized and tested under high voltage (≥4.5 V) in both half and full cell at room and high temperature, respectively. The results show that the Al homogeneously doped LCO showed better cycling stability and rate performance compared to the inhomogeneous LCO sample. Particularly, the discharge capacity of Al homogeneously doped LCO after 500 cycles under 4.5 V in full cells could reach 160.1 mAh/g at 1.0 C with 94.1% capacity retention. Postmortem characterization demonstrates that a better doping homogeneity favors the stability of both the bulk and interface as well as the kinetic conditions. This study provided new insights about LCO performance fading, which sheds new light on the development of high-voltage LCO products
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