Latest ArticlesMetal complexes hold significant promise in tumor diagnosis and treatment. However, their potential applications in photodynamic therapy (PDT) are hindered by issues such as poor photostability, low yield of reactive oxygen species (ROS), and aggregation-induced ROS quenching. To address these challenges, we present a molecular self-assembly strategy utilizing aggregation-induced emission (AIE) conjugates for metal complexes. As a proof of concept, we synthesized a mitochondrial-targeting cyclometalated Ir(III) photosensitizer Ir-TPE. This approach significantly enhances the photodynamic effect while mitigating the dark toxicity associated with AIE groups. Ir-TPE readily self-assembles into nanoaggregates in aqueous solution, leading to a significant production of ROS upon light irradiation. Photoirradiated Ir-TPE triggers multiple modes of death by excessively accumulating ROS in the mitochondria, resulting in mitochondrial DNA damage. This damage can lead to ferroptosis and autophagy, two forms of cell death that are highly cytotoxic to cancer cells. The aggregation-enhanced photodynamic effect of Ir-TPE significantly enhances the production of ROS, leading to a more pronounced cytotoxic effect. In vitro and in vivo experiments demonstrate this aggregation-enhanced PDT approach achieves effective in situ tumor eradication. This study not only addresses the limitations of metal complexes in terms of low ROS production due to aggregation but also highlights the potential of this strategy for enhancing ROS production in PDT.
In our work, polymorphism strategy has been successfully applied to tune up chromism and luminescence properties of viologen-based materials. Two polymorphs of viologen-based complexes of α-CdBr2(PHSQ)2(H2O)2 (1) and β-CdBr2(PHSQ)2(H2O)2 (2) (PHSQ = N-(4-sulfophenyl)-4,4′-bipyridinium) were synthesized by changing the solvent. They can both respond to UV light and electricity in the manner of chromism visible to the naked eye and the coloration states have good reversibility, through which an inkless erasable printing model has been established. But the coloration contrast of 1 is higher compared to 2. Meanwhile, they both exhibit photoluminescence properties and the intensity of 1 is twice that of 2, which is accompanied by photoquenching upon continuous UV light irradiation. The only divergence of disordered/ordered O atoms in the two crystalline compounds leads to significantly different chromic and luminescent properties. Further explorations simultaneously demonstrate that the different chromic performance between 1 and 2 should attribute to the alteration of stimulus-induced (light/ electricity) electron transfer channels caused by the ordered/disordered O atoms in the complexes, which is achieved through CH···O and OH···O interactions to change crystal arrangement and structural rigidity, thus affect luminescent properties.
Organic pollutants are harmful and toxic chemical substances that adversely threaten human health and the living environment all over the world. More and more studies have been investigating the relationship between low level of human exposure of organic compounds and various internal diseases. For the sake of assessing disease risk due to organic compounds contact in a particular location, it is imperative for relevant government departments to make a human health risk assessment in view of the organic pollutants’ bioavailability and their dosage-response correlations. It is inevitable to make use of an efficient method to detect organic pollutants, which is significant for public health and safety. Fluorescent assays based on carbon dots thus would provide a very plausible candidate method. After consulting a large number of literatures, we offer a comprehensive review of the sensing applications of carbon dots for organic pollutants.
Chloroform is a common and excellent solvent for preparing high-efficient organic solar cells (OSCs), however, it is toxic and poisonable chemical. In comparisons, deuterated chloroform (DC) is less toxic and costly, and particularly, it is non-poisonable chemical. In this paper, we use DC to replace ultra-dry chloroform (UC) as the processing solvent for preparation of active layers of organic solar cells. First, we selected PM6:BTP-eC9 as the basic binary and counted 100 solar cells' data, from which comparable device performance were obtained with use of DC and UC. Interestingly, DC showed better reproducibility, superior storage under a nitrogen atmosphere and a little better performance than UC. Both DC and UC gave rise of comparable hole and electron mobilities and similar charge recombination losses. Second, we based PM6:Y6 and D18-Cl: Y6 as the binaries and similar effects were obtained from both UC and DC when counting 30 devices for each binary. Third, the universality of the use of DC for preparing high-efficient OSCs were again checked with several binary and ternary systems. In all, this study demonstrate that DC can replace UC for use in the field of OSCs.
Photocatalytic hydrogen peroxide (H2O2) production has been considered as a promising strategy for H2O2 synthesis due to its environmentally friendly. Among various photocatalysts, carbon nitride-based materials are excellent candidates for H2O2 production because of their excellent visible-light response, low cost and high stability. In this review, we summarize in detail the research progress on the photocatalytic production of H2O2 by carbon nitride. First, we summarize the basic principles of photocatalysis and photocatalytic H2O2 production. Second, the classification and modification methods of carbon-nitride-based materials are discussed, including morphology modulation, noble metal loading, defect control, heterojunction regulation, molecular structure engineering and elemental doping. Finally, the different in-situ applications of H2O2 via photosynthesis were discussed, including disinfection and antibiotic resistant genes degradation, organic pollutants degradation, medical applications and fine chemical synthesis. This review brings great promise for in-situ H2O2 photosynthesis, which is expected to serve as a key component in future applications.
Atomically precise metal nanoclusters (NCs) have been deemed as a new generation of metal nanomaterials in the field of solar energy conversion due to their unique atomic stacking manner, quantum confinement effects, light-harvesting capability and multitude of active sites. Nonetheless, wide-spread application of monometallic NCs is blocked by the ultrashort carrier lifespan, uncontrollable charge transport pathway, and light-induced poor stability, impeding the construction of robust and stable metal NC-based photosystems. Herein, we report the fabrication of stable alloy (Au1-xPtx) NCs photosystem, for which tailor-made negatively charged l-glutathione (GSH)-capped Au1-xPtx NCs as the building blocks are controllably deposited on the BiVO4 (BVO) by a self-assembly approach for steering enhanced light absorption and interfacial charge transfer over alloy NCs-based photoanodes (Au1-xPtx/BVO). The self-assembled Au1-xPtx/BVO composite photoanode exhibits the significantly enhanced photoelectrochemical water oxidation performances compared with pristine BVO and Aux/BVO photoanodes, which is caused by the Pt atom doping into the Aux NCs for elevating photosensitivity and boosting the stability. The synergy of Au and Pt atoms in alloy NCs protects the gold core from rapid oxidation, improving the photostability and accelerating the surface charge transfer kinetics. Our work would significantly inspire ongoing interest in unlocking the charge transport characteristics of atomically precise alloy NCs for solar energy conversion.
In-situ enhanced bioreduction by functional materials is a cost-effective technology to remove chlorinated hydrocarbons in groundwater. Herein, a novel polydopamine (PDA)-modified biochar (BC)-based composite containing nanoscale zero-valent iron (nZVI) and poly-l-lactic acid (PLLA) (PB-PDA-Fe) was synthesized to enhance the removal of 1,1,1-trichloroethane (1,1,1-TCA) in simulated groundwater with actual site sediments. Its impact on functional microbial community structure in system was also investigated. The typical characterizations revealed uniform dispersion of PLA and nZVI particles on the BC surface, being smoother after PDA coating. The composite exhibited a significantly higher performance on 1,1,1-TCA removal (82.38%, initial concentration 100 mg/L) than Fe-PDA and PB-PDA treatments. The diversity and richness of the microbial community in the composite treatment consistently decreased during incubation due to a synergistic effect between PLLA-BC and nZVI. Desulfitobaterium, Pedobacter, Sphaerochaeta, Shewanella, and Clostridium were identified as enriched genera by the composite through DNA-stable isotope probing (DNA-SIP), playing a crucial role in the bioreductive dechlorination process. All the above results demonstrate that this novel composite selectively enhances the activity of microorganisms with extracellular respiration functions to efficiently dechlorinate 1,1,1-TCA. These findings could contribute to understanding the responsive microbial community by carbon-iron composites and expedite the application of in-situ enhanced bioreduction for effective remediation of chlorinated hydrocarbon-contaminated groundwater.
Flexible energy storage devices have been paid much attention and adapts to apply in various fields. Benefiting from the active sites of boron (B) and phosphorus (P) doping materials, co-doped carbon materials are widely used in energy storage devices for the enhanced electrochemical performance. Herein, B and P co-doped flexible carbon nanofibers with nitrogen-rich (B-P/NC) are investigated with electrospinning for sodium-ion battery. The flexible of binderless B-P/NC with annealing of 600 ℃ (B-P/NC-600) exhibits the remarkable performance for the robust capacity of 200 mAh/g at 0.1 A/g after 500 cycles and a durable reversible capacity of 160 mAh/g even at 1 A/g after 12, 000 cycles, exhibiting the equally commendable stability of flexible B-P/NC-600. In addition, B-P/NC-600 delivers the reversible capacity of 265 mAh/g with the test temperature of 60 ℃. More importantly, the flexible B-P/NC-600 is fabricated as anode for the whole battery, delivering the capacity of 90 mAh/g at 1 A/g after 200 cycles. Meanwhile, theoretical calculation further verified that boron and phosphorus co-doping can improve the adsorption capacity of nitrogen carbon materials. The favorable performance of flexible B-P/NC-600 can be ascribed to the nitrogen-rich carbon nanofibers with three-dimensional network matrix for the more active site of boron and phosphorus co-doping. Our work paves the way for the improvement of flexible anodes and wide-operating temperature of sodium-ion batteries by doping approach of much heteroatom.
Gastric Carcinoma (GC) is a highly fatal malignant tumor with a poor prognosis. Its elevated mortality rates are primarily due to its proclivity for late-stage metastasis. Exploring the metabolic interactions between tumor microenvironment and the systemic bloodstream could help to clearly understand the mechanisms and identify precise biomarkers of tumor growth, proliferation, and metastasis. In this study, an integrative approach that combines plasma metabolomics with mass spectrometry imaging of tumor tissue was developed to investigate the global metabolic landscape of GC tumorigenesis and metastasis. The results showed that the oxidized glutathione to glutathione ratio (GSSH/GSH) became increased in non-distal metastatic GC (M0), which means an accumulation of oxidative stress in tumor tissues. Furthermore, it was found that the peroxidation of polyunsaturated fatty acids, such as 9,10-EpOMe, 9-HOTrE, etc., were accelerated in both plasma and tumor tissues of distal metastatic GC (M1). These changes were further confirmed the potential effect of CYP2E1 and GGT1 in metastatic potential of GC by mass spectrometry imaging (MSI) and immunohistochemistry (IHC). Collectively, our findings reveal the integrated multidimensional metabolomics approach is a clinical useful method to unravel the blood-tumor metabolic crosstalk, illuminate reprogrammed metabolic networks, and provide reliable circulating biomarkers.
Precise tumor targeting and therapy is a major trend in cancer treatment. Herein, we designed a tumor acidic microenvironment activatable drug loaded DNA nanostructure, in which, we made a clever use of the sequences of AS1411 and i-motif, which can partially hybridize, and designed a simple while robust DNA d-strand nanostructure, in which, i-motif sequence was designed to regulate the binding ability of the AS1411 aptamer to target tumor. In the normal physiological environment, i-motif inhibits the targeting ability of AS1411. In the acidic tumor microenvironment, i-motif forms a quadruplex conformation and dissociates from AS1411, restoring the targeting ability of AS1411. Only when acidic condition and tumor cell receptor are present, this nanostructure can be internalized by the tumor cells. Moreover, the structure change of this nanostructure can realize the release of loaded drug. This drug loaded A-I-Duplex DNA structure showed cancer cell and spheroid targeting and inhibition ability, which is promising in the clinical cancer therapy.
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