Latest ArticlesThe cyclic guanosine monophosphate-adenosine monophosphate synthase and the stimulator of interferon genes (cGAS-STING) has emerged as a promising target for cancer immunotherapy. However, the development of natural STING agonists is impeded by several challenges, including limited biostability, poor pharmacokinetics, and inefficient cytosolic delivery. Herein, we meticulously designed a double-layer polyethylenimine (PEI) modified nanoscale covalent organic polymer (CPGP) for efficient delivery of 2′3′ cyclic guanosine monophosphate-adenosine monophosphate (cGAMP), a natural STING agonist. The double-layer PEI structured CPGP enhanced both the loading capacity and stability of cGAMP. Furthermore, CPGP improved the intracellular delivery efficiency and amplified the activation of STING pathway for the secretion of type-Ⅰ interferon and pro-inflammatory cytokines. In contrast, single-layered nanoparticles failed to permit stable loading and intracellular delivery of cGAMP for immune response. The nano-STING agonist also mitigated the immunosuppressive tumor microenvironment (TME) by reducing regulatory T cells and polarizing M2 macrophages to the M1 phenotype, thereby creating an immune-supportive TME to enhance adaptive immune responses. The combination of CPGP and immune checkpoint blockers showed synergistic effect, further enhancing the inhibition effect on tumor growth. This double-layer PEI modified CPGP may offer a generalizable platform for other natural dinucleotide STING agonists to overcome the cascade delivery barriers, augmenting immune activation for tumor immunotherapy.
Manganese dioxide (MnO2) electrode material possesses the advantages of high energy density, structural diversity and high modification potential. This allows it become one of the important cathodes for aqueous zinc ion battery. However, the applications are limited by the poor electrical conductivity, narrow layer spacing and the ease of dissolution. Herein, we prepare MnO2-PVP@0.03GO composites by the co-modification of polyvinylpyrrolidone (PVP) pre-insertion layer and graphene oxide (GO) self-assembly layer. The Zn//MnO2-PVP@0.03GO cells deliver a discharge specific capacity of 442 mAh/g at a current density of 0.2 A/g. It also maintains 100% capacity for 1000 times cycling at 1 A/g. The assembled soft package batteries demonstrate superior flexibility and adaptability under different bending conditions.
Efficient and stable electrocatalyst for oxygen evolution reaction (OER) in acidic environment is vital for polymer electrolyte membrane water electrolysis (PEMWE). In this work, we have devised the formation of heterostructured RuO2/MnO2 with nanoflower structure for acidic OER catalysis. Compared to commercial RuO2, the overpotential at 50 mA/cm2 is decreased by 36 mV, corresponding to a 3.7-fold better mass activity. The boosted acidic OER performance is attributed to the heterostructure inducing more electrons are filled in eg orbital of Ru atom triggering a better deprotonation of bridge oxygen atom in Ru-Obri-Mn structure evidenced by pH-independent cyclic voltammetry test. Moreover, RuO2/MnO2 sustains its acidic OER activity within 20 h, longer than commercial RuO2. The membrane electrode assembly (MEA) test suggests than only 2.18 V is required to achieve a current density of 5 A/cm2. The theoretical calculation reveals that the eg filling of Ru atom is increased from 2.18 to 2.39 after MnO2 incorporation, reducing the energy for the formation of *OOH moiety.
The cross-photodimerization often comes with the formation of undesired and competitive homo-photodimer as side products. Herein, we report a series of highly selective [4 + 4] cross-photodimerization between anthracene and 4a-azoniaanthracene derivatives within a cucurbit[10]uril (CB[10]) host in water. Heteroternary inclusion complexes were formed through encapsulation of donor (D1-D2, anthracene derivative) and acceptor (A1-A3, 4a-azoniaanthracene derivatives) pairs in CB[10]. In the presence of CB[10] (1.0 equiv.), the [4 + 4] cross-photodimerization between D1 and A1/A2/A3 efficiently gave a single racemic cross-photodimer. Furthermore, the cross-photodimerization between 9-substituted anthracene D2 and A1/A3 was catalyzed by CB[10] (0.1 equiv.) to quantitatively yield a cross-photodimer with high regioselectivity. Efficient formation of selective cross-photodimers could be attributed to the exclusive encapsulation of D-A hetero-guest pairs in CB[10] and the confinement effect of the CB[10] host cavity. Our study further proves host–guest complexation as a powerful strategy for cross-cycloaddition reactions with high efficiency.
Diabetic liver injury is a widespread complication of diabetes and carries a high risk to liver function. Therefore, early diagnosis of diabetic liver injury is of great significance for providing quality of life for diabetic patients. Most of the activated dual-modal probes are usually activated by single factor stimulation, which greatly reduces the diagnostic accuracy of liver injury. Here, a novel cysteine (Cys)/homocysteine (Hcy) and viscosity-enhanced dual-modal probe DAL was developed for the first time to monitor diabetic liver injury and its repair process. In the presence of Cys/Hcy, the near-infrared fluorescence (NIRF) and photoacoustic (PA) signals of the probe DAL were activated, with further signal enhancement in high viscosity environments. This Cys/Hcy and viscosity cascade probe exhibits heightened sensitivity and enhanced anti-interference capabilities, contributing to the advancement of liver injury diagnosis accuracy. In addition, the probe DAL shows exceptional mitochondrial targeting ability, enabling sensitive monitoring of Cys/Hcy and viscosity alterations within mitochondria. Based on NIRF/PA dual-modal imaging technology, the probe was successfully used for the first time in a mouse diabetic liver injury model to evaluate the extent of liver damage and the repair process by tracking the levels of Cys/Hcy and viscosity. Therefore, the two-factor activated dual-modal probe developed in this study provides a powerful instrument for accurate diagnosis and efficacy evaluation of complications related to diabetes.
Herein, we developed the first example of copper-catalyzed silicon radical-initiated 1,4-silylcyanation of unactivated 1,3-enynes, which provided an efficient method to access CN-bearing tri- and tetra-substituted homoallenylsilane derivatives in high yields with excellent regioselectivities. This protocol featured good functional group compatibility and broad substrate scopes, enabling the formation of C-Si bond under cheap copper catalyst with a low loading. Furthermore, this means showed potential application value in the late-stage functionalization of natural products.
A photoredox-catalyzed synthesis of α,α-difluoromethyl sulfones from sulfur dioxide with readily available gem–difluoroalkenes is reported. This protocol features mild reaction conditions, broad substrate scope and good functional group compatibility, giving rise to the target α,α-difluoromethyl sulfones in moderate to excellent yields. Mechanistic studies indicate that this reaction is initiated by an aryl radical with the insertion of sulfur dioxide.
Supramolecular prodrug vesicles (H-4⊃B-2@MB) with selective antibacterial activity have been successfully constructed. Specifically, a natural antibiotic prodrug (B-2) with glutathione (GSH)-responsiveness was synthesized. The hydrophobic interaction between B-2 and a novel water-soluble cavitand with deep cavity (H-4) resulted in the formation of a host-guest complex, which further self-assembled into supramolecular vesicles. The formed vesicles could effectively encapsulate the photosensitizer methylene blue (MB), enabling co-delivery of antibiotics and photosensitizers in the presence of GSH. Moreover, upon excitation at 630 nm, the photosensitizers generate reactive oxygen species (ROS), effectively eradicating E. coli through combined chemo-photodynamic therapy. Considering that GSH is predominantly present in Gram-negative bacteria such as E. coli, this strategy exhibits substantial potential for selectively inhibiting bacteria characterized by high GSH levels to regulate bacterial colony equilibrium.
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