Latest ArticlesInnovative 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.
Dion–Jacobson (DJ) phase hybrid perovskites have been proven to improve the photovoltaic performance of the devices due to its unique structure. At present, some DJ hybrid perovskites have been reported and used for photodetection filed, but most of them are based on lead-bromide systems, which is not conducive to construct broadband photodetection devices due to the limitation of intrinsic absorption. Herein, we constructed a bilayered DJ hybrid perovskite (3AMPY)(EA)Pb2I7 (3AMPY2+ is 3-(aminomethyl)pyridinium, EA+ is ethylammonium) using an aromatic spacer, which exhibit large current on/off ratios of ~104 under 520 and 637 nm illumination. In particular, the single crystal device based on (3AMPY)(EA)Pb2I7 shows a distinguished detectivity of 7.4 × 1012 Jones and a high responsivity of 0.89 A/W under 637 nm illumination. Such finding not only enriches the quantities of DJ hybrid perovskites, but also provides useful assistance for constructing high-performance optoelectronic device in the future.
Nor-seco-cucurbit[10]uril (ns-CB[10]) is a kinetic product with unique structure. The single bridged methylene in its structure makes the molecular cavity of ns-CB[10] more deformable when compared to ordinary cucurbit[n]uril, reducing its structural stability. Repeated experiments showed that ns-CB[10] gradually cracks in an acidic solution and changes the specificity of cucurbit[5]uril (CB[5]) and cucurbit[8]uril (CB[8]) under more robust acidic solutions and when heated. A series of experiments were designed to study the transformation behavior of ns-CB[10]. It was found that the concentration of ns-CB[10] was correlated with the content distribution of CB[5] and CB[8]. This study explores the influencing factors and mechanisms of the transformation of ns-CB[10] to CB[5] and CB[8]. The results are of great significance for the application of ns-CB[10], understanding the formation mechanism of cucurbit[n]urils. Furthermore, it provides a new pathway for synthesizing new cucurbit[n]urils.
Cholelithiasis affects approximately 10%-20% of the adult population globally. And cholesterol accumulation and nucleation of cholesterol crystals are commonly recognized as the primary process in the initiation and progression of gallstones. Hydroxypropyl-β-cyclodextrin (HPCD) is a supramolecular host compound that can solubilize cholesterol, potentially serving as a preventative or therapeutic agent for cholelithiasis. However, we found that the administration of HPCD treatment did not impede the formation of gallstones in mice, mainly attributed to the pre-complexation of its cavity during the transition process. Here we synthesized a prodrug of HPCD and prepared a HPCD nanoparticle (HPCD-NP), which can be transported efficiently to the gallbladder through the hepatobiliary system following an intravenous injection. In the bile, the HPCD-NP degraded into free HPCD, bound to cholesterol crystals and gallstones within the gallbladder and effectively increased cholesterol solubilization, leading to gallstones regression. Given the established safety of both HPCD and cyclodextrin-based nanoparticles in numerous animal and human studies, HPCD-NP shows considerable promise for the prevention and treatment of human cholelithiasis.
Na3V2(PO4)3 (NVP) is regarded as alternative cathode material for sodium-ion batteries (SIBs) due to its potential high-rate performance and pronounced long-term cycle stability. However, electronic conductivity and tap density are difficult to be balanced. Herein, we report that high-temperature shock (HTS) can prepare "single crystalline like" NVP which combines high-rate capability with high tap density together into one with the assistance of carbon framework and large particle. Thus, high reversible capacity of 110 mAh/g at 0.1 C with 89.9% capacity retention after 1600 cycles at 1 C and specific capacity of 83.5 mAh/g at 50 C rate has been exhibited. This study provides a novel strategy to guide the production of high tap density, and rate performance polyanionic cathode materials.
Skins expose to kinds of risk factors for damage, such as the hormone drugs, skin care products and ultraviolet radiation, which is accompanied by the production of excessive reactive oxygen species (ROS) and eventually leads to hypertrichosis. This skin disease is not aesthetically pleasing and even causes psychological and spiritual problems such as inferiority, anxiety and irritability. Current therapies are limited and often unsatisfactory, such as pharmacological and physical therapies, which have adverse effects and cause the irreversible destruction of hair follicles. Gold nanoclusters have good biocompatibility and their biosynthesis in vivo is responsive to oxidative stress microenvironment (OSM), which could be a safe and effective drug for ROS-induced skin injury. In our study, we demonstrated that zero valence fluorescent gold nanoclusters (FGNCs) were in situ biosynthesized in the plucking-induced damaged skin but not in the normal skin after the administration of gold precursors (+3), while FGNCs inhibited hair follicle regeneration by negatively regulating nuclear transcription factor kappa B (NFκB)-mediated inflammatory response signaling pathway (NFκB/tumor necrosis factor-α (TNF-α) axis). This OSM-responsive in situ biosynthesis method is facile and safe and holds great promise for curing hypertrichosis associated with skin dermatitis and injury.
Acute lung injury (ALI) was characterized by excessive reactive oxygen species (ROS) levels and inflammatory response in the lung. Scavenging ROS could inhibit the excessive inflammatory response, further treating ALI. Herein, we designed a novel nanozyme (P@Co) comprised of polydopamine (PDA) nanoparticles (NPs) loading with ultra-small Co, combining with near infrared (NIR) irradiation, which could efficiently scavenge intracellular ROS and suppress inflammatory responses against ALI. For lipopolysaccharide (LPS) induced macrophages, P@Co + NIR presented excellent antioxidant and anti-inflammatory capacities through lowering intracellular ROS levels, decreasing the expression levels of interleukin-6 (IL-6) and tumor necrosis factor-α (TNF-α) as well as inducing macrophage M2 directional polarization. Significantly, it displayed the outstanding activities of lowering acute lung inflammation, relieving diffuse alveolar damage, and up-regulating heat shock protein 70 (HSP70) expression, resulting in synergistic enhanced ALI therapy effect. It offers a novel strategy for the clinical treatment of ROS related diseases.
Preparing free-base porphyrinoid radicals that can function as coordination ligands is a challenging task. Here we report the synthesis of a stable, free-base benzocorrole (BC) radical containing only two inner NH protons via a retro-Diels-Alder conversion. The radical character of BC was fully supported by crystallographic analysis, spectroscopic evidence, and theoretical calculations. This neutral radical ligand allowed easy insertion of Zn(Ⅱ), Ga(Ⅲ), and Pd(Ⅱ) ions to produce radical complexes. All these radicals exhibited luminescence-on responses under weak reducing atmosphere, corresponding to the conversion to their aromatic anions. The red fluorescence was observed for BC and its Zn(Ⅱ) and Ga(Ⅲ) complexes, and the near-infrared phosphorescence (> 900 nm) was detected for Pd(Ⅱ) complex at room temperature. Furthermore, Ga(Ⅲ) corrole exhibited a variation in fluorescence in response to axial coordination. Our findings provide a promising radical platform for coordination and developing novel functional materials with switchable spin and emission.
The development of innovative and sustainable catalytic strategies for organic synthesis is a pivotal aspect of advancing material science and chemical engineering. This research presents a new catalytic method for the aminoacylation of N-sulfonyl ketimines by utilizing a potassium-doped graphite-like carbon nitride (g-C3N4) framework. This method not only enhances the catalytic efficiency and broadens the light absorption spectrum of g-C3N4 but also significantly reduces the recombination rate of electron-hole pairs, thereby increasing the reaction yield and selectivity. Importantly, our approach facilitates the synthesis of aminoacylated N-heterocycles, expanding the applicability of potassium-modified g-C3N4 in photocatalytic organic synthesis. A notable accomplishment of this study is the unprecedented generation of carbamoyl radicals via heterogeneous photocatalysis, which can be easily recycled after reaction. This advancement highlights the capability of potassium-doped g-C3N4 (namely K-CN) as an advanced heterogeneous photocatalyst for the formation of complex organic compounds.
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