Latest ArticlesAcute 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.
In recent years, biopharmaceuticals have witnessed remarkable advancements, transforming the landscape of therapeutic interventions. Biopharmaceuticals encompassing therapeutics generated through cutting-edge biotechnological methods have shown promising therapeutic outcomes. However, their clinical success hinges significantly on overcoming drug delivery challenges related to stability, intracellular delivery, immunogenicity, and pharmacokinetic properties. Herein, we provide an overview of various marketed macromolecules, including nucleic acids, and immunotherapeutic agents such as cytokines and monoclonal antibodies, as well as other therapeutic peptides/proteins like enzymes, hormones, and coagulation factors. Our primary focus is on elucidating the delivery challenges associated with these macromolecules and highlighting the pivotal role played by drug delivery platforms in the development of currently marketed products, offering valuable insights for both scientific research and the pharmaceutical industry.
Ln-containing polyoxoniobates (PONbs) have appealing applications in luminescence, information encryption and magnetic fields, but the synthesis of PONbs containing high-nuclearity Ln-O clusters is challenging due to the easy hydrolysis of Ln3+ ions in alkaline environments. In this paper, we are able to integrate CO32− and high-nuclearity Ln-O clusters into PONb to construct an inorganic giant Eu19-embedded PONb H49K16Na13(H2O)63[Eu21O2(OH)7(H2O)5(Nb7O22)10(Nb2O6)2(CO3)18]·91H2O (1), which contains the highest nuclearity Eu-O clusters and the largest number of Eu3+ ions among PONbs. In addition, the film that was prepared by mixing 1 with gelatin and glycerol, exhibits reversible luminescence switching behavior under acid/alkali stimulation and has been used to create a fluorescence-encoded information approach. This work paves a feasible strategy for the construction of high-nuclearity Ln-O cluster-containing PONbs and the expansion of the application of Ln-containing PONbs in information encryption.
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.
Nitrogen-doping of carbon support (N-C) for platinum (Pt) nanoparticles to form Pt/N-C catalyst represents an effective strategy to promote the electrocatalysis of cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. For fundamental understanding, clearly identifying the metal-support effect on enhancement mechanisms of ORR electrocatalysis is definitely needed. In this work, the impact of Pt-support interaction via interfacial Pt-N coordination on electrocatalytic ORR activity and stability in Pt/N-C catalyst is deeply studied through structural/compositional characterizations, electrochemical measurements and theoretical DFT-calculations/AIMD-simulations. The resulting Pt/N-C catalyst exhibits a superior electrocatalytic performance compared to the commercial Pt/C catalyst in both half-cell and H2-O2 fuel cell. Experimental and theoretical results reveal that the interfacial Pt-N coordination enables electron transfer from N-C support to Pt nanoparticles, which can weaken the adsorption strength of oxygen intermediates on Pt surface to improve ORR activity and induce the strong Pt-support interaction to enhance electrochemical stability.
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.
Developing a heterostructure for alloying-based anode for sodium-ion batteries (SIBs) is an efficient solution to accommodate volume change upon sodiation/desodiation and boost sodium storage since it combines the merits of each component. Herein, we report a metallic and microphone-like Sn-Zn0.9Mn0.1O heterostructure via an in-situ Mn doping strategy. Based on theoretical calculations and experimental results, the introduction of Mn into ZnO (a small amount of Mn also diffuses into the Sn lattice) can not only enhance intrinsic electronic conductivity but also reduce the Na+ diffusion barrier inside the Sn phase. When evaluated as anode for SIBs, the obtained heterostructures show a high reversible capacity of 395.1 mAh/g at 0.1 A/g, rate capability of 332 mAh/g at 5 A/g, and capacity retention of almost 100% after 850 cycles at 5 A/g, indicating its great potential for high-power application of SIBs.
A series of heteronuclear yttrium-nickel monoxide carbonyl complexes YNiO(CO)n− (n = 1–5) were generated in a pulsed-laser vaporization source and characterized by mass-selected photoelectron velocity-map spectroscopy combined with theoretical calculations. CO ligand-mediated reactivity in CO oxidation of yttrium-nickel monoxide carbonyl complexes was experimentally and theoretically identified. During the consecutive CO adsorption, a μ2-O linear structure was most favorable for YNiO(CO)n− (n = 1, 2), then a structure in which the terminal O was bonded to the Y atom became favored for YNiO(CO)3−, and finally a structure bearing a CO2 moiety was most favorable for YNiO(CO)n− (n = 4, 5). Theoretical calculations indicated that the Ni atom acted as an electron acceptor and accumulated electron density at n ≤ 3, and then served as an electron donor along with the Y atom to contribute electron density in the rearrangement that accompanied CO oxidation at n > 3.
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.
Sensitization of metal-centered forbidden transitions is of great significance. Solid MnⅡ-based phosphors with d-d forbidden transition sensitized by CeⅢ with d-f allowed transition are promising light conversion materials, but the energy transfer mechanism in CeⅢ-MnⅡ is still in dispute for the uncertainty of distances between metal centers. Herein, for the first time, we explored the energy transfer mechanism in two well-designed luminescent heteronuclear complexes with clear crystal structures, i.e., Ce-N8-Mn and Ce-N2O6-Mn (N8 = 1,4,7,10,13,16,21,24-octaazabicyclo[8.8.8]hexacosane; N2O6 = 4,7,13,16,21,24-hexaoxa-1,10-diazabicyclo[8.8.8]hexacosane). Short distances between metal centers facilitate efficient energy transfer from CeⅢ to MnⅡ in both complexes, resulting in high photoluminescence quantum yield up to unity. After systematic study of the two heteronuclear complexes as well as two reference complexes Ce(N8)Br3 and Ce(N2O6)Br3, we concluded that dipole-quadrupole interaction is the dominant energy transfer mechanism in the heteronuclear complexes.
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