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Novelmultifunctional poly(ε-caprolactone)-gelatin encapsulatingupconversion core/shell silica nanoparticles (NPs) composite fibersas dual drugs delivery system (DDDS), with indomethacin (IMC) anddoxorubicin (DOX) releasing in individual release properties, havebeen designed and fabricated via electrospinning process. Uniformand monodisperse upconversion (UC) luminescent NaYF4:Yb3+, Er3+nanocrystals (UCNCs) were encapsulatedwith mesoporous silica shells, resulting in the formation of core/shellstructured NaYF4:Yb3+, Er3+@mSiO2(UCNCs@mSiO2) NPs, which can be performed as DOXdelivery carriers. These UCNCs@mSiO2NPs loading DOX thenwere dispersed into the mixture of poly(ε-caprolactone) (PCL)and gelatin-based electrospinning solution containing IMC, followedby the preparation of dual drug-loaded composite fibers (DDDS) viaelectrospinning method. The drugs release profiles of the DDDS weremeasured, and the results indicated that the IMC and DOX releasedfrom the electrospun composite fibers showed distinct properties.The IMC in the composite fibers presented a fast release manner, whileDOX showed a sustained release behavior. Moreover, the UC luminescentintensity ratios of 2H11/2/4S3/2–4I15/2to 4F9/2–4I15/2from Er3+vary with the amounts of DOX in the system, and thus drug releasecan be tracked and monitored by the luminescence resonance energytransfer (LRET) mechanism. [ABSTRACT FROM AUTHOR]

Alcoholic liver disease (ALD) is one of the causes of hepatocellular carcinoma, accompanied by intestinal leakage and microbial changes. Pueraria has protective effects on liver injury. The aim of this study was to investigate the mechanism of pueraria in the treatment of ALD. UPLC-Q/TOF-MS was used to analyze the composition of the pueraria extract (PUE). Acute and chronic ALD models were established to evaluate the antialcoholic and hepatoprotective effects of PUE. As a result, PUE treatment reduced the serum levels of ALT, AST, TC, and TG and inflammatory factors and alleviated liver inflammation and drunk state. PUE decreased the gene expression of ADH1 and the serum level of acetaldehyde (ACH) to inhibit the generation of ACH from ethanol metabolism, increased the gene level of ALDH2 to accelerate the decomposition of ACH, and thereby alleviated liver inflammation and intestinal barrier damage. Meanwhile, 16 S rDNA revealed that PUE altered the microbiota composition, reduced the amount of Proteobacteria and Desulfobacterota , and thus inhibited the generation of lipopolysaccharide and its downstream-like TLR4/MyD88/NF-κB pathway. PUE also increased the abundance of Bacteroides , Ruminococcus , and Prevotella and producted short-chain fatty acids to protect the intestinal wall. Treatment with fecal microbiota transplantation further confirmed that PUE gut microbiota dependently alleviated ALD. Therefore, PUE regulated gut microbiota and inhibited ethanol metabolism to alleviate ALD through the liver-gut-brain axis. It has good prospects in the future.

Ulcerative colitis (UC) is a common chronic, relapsing inflammatory bowel condition. Procyanidins (PC) are known for their antiangiogenic, anti-inflammatory, antioxidant, and antimetastatic properties. However, there is comparatively limited information on how PC interacts with UC. In this study, 5 mg/10 mL/kg body weight of PC was administered to mice with dextran sulfate sodium (DSS)-induced colitis mice. PC treatment prolonged the survival period of mice, ameliorated UC symptoms, reduced damage to the intestinal mucosal barrier, and increased the protein expression of ZO-1 and occludin in the DSS-treated mice. Importantly, PC treatment significantly reduced gene expression related to Th17 cell differentiation, including STAT3, SMAD3, TGF-β, and JAK1. The results of the flow cytometry analysis indicated significant increase in the number of Treg cells and a concomitant decrease in the proportion of Th17 cells in the colon following PC treatment. Additionally, PC increased the abundance of gut microbiota such as Bacteroidota , Oscillospiraceae , Muribaculaceae, and Desulfovibrionaceae , as well as the concentrations of acetate acid, propionate acid, and butyrate acid in the feces. PC also activated short-chain fatty acid receptors, such as G-protein coupled receptor 43 in the colon, which promoted the proliferation of Treg cells. The depletion of gut microbiota and subsequent transplantation of fecal microbiota demonstrated that PC's effects on gut microbiota were effective in improving UC and restoring intestinal Th17/Treg homeostasis in a microbiota-dependent manner. This suggests that PC could be a promising functional food for the prevention and treatment of UC in the future.

In the realm of organic synthesis, the catalytic and stereoselective formation of C-glycosidic bonds is a pivotal process, bridging carbohydrates with aglycones. However, the inherent chirality of the saccharide scaffold often has a substantial impact on the stereoinduction imposed by a chiral ligand. In this study, we have established an unprecedented zirconaaziridine-mediated asymmetric nickel catalysis, enabling the diastereoselective coupling of bench-stable glycosyl phosphates with a range of (hetero)aromatic and glycal iodides as feasible coupling electrophiles. Our developed method showcases a broad scope and a high tolerance for various functional groups. More importantly, precise stereocontrol toward both anomeric configurations of forming C(sp 2 )-glycosides can be realized by simply utilizing the popular chiral bioxazoline (biOx) ligands in this reductive Ni catalysis. Regarding the operating mechanism, both experimental and computational studies support the occurrence of a redox transmetalation process, leading to the formation of a transient, bimetallic Ni-Zr species that acts as a potent and efficient single-electron reductant in the catalytic process.

Molten MgCl 2 -based chlorides have emerged as potential thermal storage and heat transfer materials due to high thermal stabilities and lower costs. In this work, deep potential molecular dynamics (DPMD) simulations by a method combination of the first principle, classical molecular dynamics, and machine learning are performed to systemically study the relationships of structures and thermophysical properties of molten MgCl 2 -NaCl (MN) and MgCl 2 -KCl (MK) eutectic salts at the temperature range of 800-1000 K. The densities, radial distribution functions, coordination numbers, potential mean forces, specific heat capacities, viscosities, and thermal conductivities of these two chlorides are successfully reproduced under extended temperatures by DPMD with a larger size (5.2 nm) and longer timescale (5 ns). It is concluded that the higher specific heat capacity of molten MK is originated from the strong potential mean force of Mg-Cl bonds, whereas the molten MN performs better in heat transfer due to the larger thermal conductivity and lower viscosity, attributed to the weak interaction between Mg and Cl ions. Innovatively, the plausibility and reliability of microscopic structures and macroscopic properties for molten MN and MK verify the extensibilities of these two deep potentials in temperatures, and these DPMD results also provide detailed technical parameters to the simulations of other formulated MN and MK salts.

Effective protective coatings are an essential component of lightweight engineering materials in a large variety of applications as they ensure structural integrity of the base material throughout its whole service life. Layered double hydroxides (LDHs) loaded with corrosion inhibitors depict a promising approach to realize an active corrosion protection for aluminum and magnesium. In this work, we employed a combination of density functional theory and molecular dynamics simulations to gain a deeper understanding of the influence of intercalated water content on the structure, the stability, and the anion-exchange capacity of four different LDH systems containing either nitrate, carbonate, or oxalate as potential corrosion inhibiting agents or chloride as a corrosion initiator. To quantify the structural change, we studied the atom density distribution, radial distribution function, and orientation of the intercalated anions. Additionally, we determined the stability of the LDH systems by calculating their respective hydration energies, hydrogen-bonded network connected to the intercalated water molecules, as well as the self-diffusion coefficients of the intercalated anions to provide an estimate for the probability of their release after intercalation. The obtained computational results suggest that the hydration state of LDHs has a significant effect on their key properties like interlayer spacing and self-diffusion coefficients of the intercalated anions. Furthermore, we conclude from our simulation results that a high self-diffusion coefficient which is linked to the mobility of the intercalated anions is vital for its release via an anion-exchange mechanism and to subsequently mitigate corrosion reactions. Furthermore, the presented theoretical study provides a robust force field for the computer-assisted design of further LDH-based active anticorrosion coatings., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

We develop a method to prepare hollow FeP/Fe 3 O 4 hybrid nanoparticles supported on carbon nanotubes (CNTs), which could be used as highly active and efficient electrocatalysts. The Fe@Fe 3 O 4 /CNT hybrids were first synthesized by annealing the CNTs adsorbed with Fe(NO 3 ) 3 , followed by controlled phosphorization treatment. They exhibit an outstanding catalytic activity for oxygen evolution reaction (OER) with a low overpotential of 229 mV at a current density of 10 mA cm -2 , a high turnover frequency value of 0.35 s -1 at an overpotential of 300 mV, and an ultralow Tafel slope of 27.6 mV dec -1 , which is much better than that of FeP/Fe 3 O 4 , FeP/CNTs, Fe 3 O 4 /CNTs, and the commercial RuO 2 electrocatalyst. More importantly, the Tafel slope is much lower than most non-noble metal-based OER electrocatalysts reported in the previous literature studies as far as we know. The excellent OER performance benefits from the electron transfer from Fe 3 O 4 to FeP confirmed by X-ray photoelectron spectroscopy, together with good conductivity of CNTs. This hybrid structure supported on conductive CNTs may offer an efficient method to design earth-abundant and low-cost electrocatalysts for OER in practical applications.

The dynamic fluctuation of the U 3+ coordination structure in a molten LiCl-KCl mixture was studied using first principles molecular dynamics (FPMD) simulations. The radial distribution function, probability distribution of coordination numbers, fluctuation of coordination number and cage volume, self-diffusion coefficient and solvodynamic mean radius of U 3+ , dynamics of the nearest U-Cl distances, and van Hove function were evaluated. It was revealed that fast exchange of Cl - occurred between the first and second coordination shells of U 3+ accompanied with fast fluctuation of coordination number and rearrangement of coordination structure. It was concluded that 6-fold coordination structure dominated the coordination structure of U 3+ in the molten LiCl-KCl-UCl 3 mixture and a high temperature was conducive to the formation of low coordinated structure.

Near-infrared light is an attractive stimulus due to its noninvasive and deep tissue penetration. Particularly, NIR light is utilized for cancer thermotherapy and on-demand release of drugs by the disruption of the delivery carriers. Here we have prepared a novel NIR-responsive DNA-hybrid-gated nanocarrier based on mesoporous silica-coated Cu1.8S nanoparticles. Cu1.8S nanoparticles, possessing high photothermal conversion efficiency under a 980 nm laser, were chosen as photothermal agents. The mesoporous silica structure could be used for drug storage/delivery and modified with aptamer-modified GC-rich DNA-helix as gatekeepers, drug vectors, and targeting ligand. Simultaneously, the as-produced photothermal effect caused denaturation of DNA double strands, which triggered the drug release of the DNA-helix-loaded hydrophilic drug doxorubicin and mesopore-loaded hydrophobic drug curcumin, resulting in a synergistic therapeutic effect. The Cu1.8S@mSiO2 nanocomposites endocytosed by cancer cells through the aptamer-mediated mode are able to generate rational release of doxorubicin/curcumin under NIR irradiation, strongly enhancing the synergistic growth-inhibitory effect of curcumin against doxorubicin in MCF-7 cells, which is associated with a strong mitochondrial-mediated cell apoptosis progression. The underlying mechanism of apoptosis showed a strong synergistic inhibitory effect both on the expression of Bcl-2, Bcl-xL, Mcl-1, and upregulated caspase 3/9 activity and on the expression level of Bak and Bax. Therefore, Cu1.8S@mSiO2 with efficient synergistic therapeutic efficiency is a potential multifunctional cancer therapy nanoplatform.

Photodynamic therapy (PDT) is a promising antitumor treatment that is based on the photosensitizers that inhibit cancer cells by yielding reactive oxygen species (ROS) after irradiation of light with specific wavelengths. As a potential photosensitizer, titanium dioxide (TiO2) exhibits minimal dark cytotoxicity and excellent ultraviolet (UV) light triggered cytotoxicity, but is challenged by the limited tissue penetration of UV light. Herein, a novel near-infrared (NIR) light activated photosensitizer for PDT based on TiO2-coated upconversion nanoparticle (UCNP) core/shell nanocomposites (UCNPs@TiO2 NCs) is designed. NaYF4:Yb(3+),Tm(3+)@NaGdF4:Yb(3+) core/shell UCNPs can efficiently convert NIR light to UV emission that matches well with the absorption of TiO2 shells. The UCNPs@TiO2 NCs endocytosed by cancer cells are able to generate intracellular ROS under NIR irradiation, decreasing the mitochondrial membrane potential to release cytochrome c into the cytosol and then activating caspase 3 to induce cancer cell apoptosis. NIR light triggered PDT of tumor-bearing mice with UCNPs@TiO2 as photosensitizers can suppress tumor growth efficiently due to the better tissue penetration than UV irradiation. On the basis of the evidence of in vitro and in vivo results, UCNPs@TiO2 NCs could serve as an effective photosensitizer for NIR light mediated PDT in antitumor therapy.

In this article, Eu-activated CaYAlO4 aluminate phosphors were synthesized by a solid-state reaction. Under UV light excitation, characteristic red line emission of Eu(3+) was detected in the range of 570-650 nm. In addition, we introduced crystal-site engineering approach into the CaYAlO4 host through incorporation of Si(4+)-Ca(2+) to replace Al(3+)-Y(3+), which would shrink the AlO6 octahedrons, accompanied by the expansion of CaO9 polyhedron, and then enable the partial reduction of Eu(3+) to Eu(2+). The crystal structure and underlying mechanism have been clarified on the basis of the Rietveld refinement analysis. The PL spectra of Ca0.99+xY1-xAl1-xSixO4:Eu0.01 (x = 0-0.30) exhibit both green emission of Eu(2+) (4f(6)5d(1)-4f(7), broadband around 503 nm) and red-orange emission of Eu(3+) ((5)D0-(7)F1,2, 593 and 624 nm) under UV light excitation with a quantum yield of 38.5%. The CIE coordinates of Ca0.99+xY1-xAl1-xSixO4:Eu0.01 (x = 0-0.30) phosphors are regularly shifted from (0.482, 0.341) to (0.223, 0.457) with increasing x, which would expand the application of Eu. Furthermore, this investigation reveals the correlations of structure and property of luminescent materials, which would shed light on the development of novel phosphors suitable for lighting and display applications.

A series of Ln(3+) (Ln(3+) = Eu(3+)/Tb(3+)/Dy(3+)/Sm(3+)) ion doped CaNb2O6 (CNO) phosphors have been prepared via the conventional high-temperature solid-state reaction route. The X-ray diffraction (XRD) and structure refinement, diffuse reflection, photoluminescence (PL), and fluorescent decay curves were used to characterize the as-prepared samples. Under UV radiation, the CNO host present a broad emission band from about 355 to 605 nm centered around 460 nm originating from the NbO6 octahedral groups, which has spectral overlaps with the excitation of f-f transitions of Eu(3+)/Tb(3+)/Dy(3+)/Sm(3+) in CNO:Eu(3+)/Tb(3+)/Dy(3+)/Sm(3+) samples. They show both host emission and respective emission lines derived from the characteristic f-f transitions of activators, which present different emission colors owing to the energy transfer from the NbO6 group in the host to Eu(3+)/Tb(3+)/Dy(3+)/Sm(3+) with increasing activator concentrations. The decreases of decay lifetimes of host emissions in CNO:Eu(3+)/Tb(3+)/Dy(3+)/Sm(3+) demonstrate the energy transfer from the hosts to Eu(3+)/Tb(3+)/Dy(3+)/Sm(3+). The energy transfer mechanisms in CNO:Eu(3+)/Tb(3+)/Dy(3+) phosphors have been determined to be a resonant type via dipole-dipole mechanisms. For CNO:Sm(3+), the metal-metal charge transfer transition (MMCT) might contribute to the different variations of decay lifetimes and emission intensity from CNO:Eu(3+)/Tb(3+)/Dy(3+) samples. The best quantum efficiency is 71.2% for CNO:0.01/0.02Dy(3+). The PL properties of as-prepared materials indicate the promising application in UV-pumped white-emitting lighting diodes field.

Porous hydroxyapatite (HAp) composite fibers functionalized with up-conversion (UC) luminescent and magnetic Na(Y/Gd)F4:Yb(3+),Er(3+) nanocrystals (NCs) have been fabricated via electrospinning. After transferring hydrophobic oleic acid-capped Na(Y/Gd)F4:Yb(3+),Er(3+) NCs into aqueous solution, these water-dispersible NCs were dispersed into precursor electrospun solution containing CTAB. Na(Y/Gd)F4:Yb(3+),Er(3+)@HAp composite fibers were fabricated by the high temperature treatment of the electrospun Na(Y/Gd)F4:Yb(3+),Er(3+) NCs decorated precursor fibers. The biocompatibility test on MC 3T3-E1 cells using MTT assay shows that the HAp composite fibers have negligible cytotoxity, which reveals the HAp composite fibers could be a drug carrier for drug delivery. Because the contrast brightening is enhanced at increased concentrations of Gd(3+), the HAp composite fibers can serve as T1 magnetic resonance imaging contrast agents. In addition, the composites uptaken by MC 3T3-E1 cells present the UC luminescent emission of Er(3+) under the excitation of a 980 nm near-infrared laser. The above findings reveal Na(Y/Gd)F4:Yb(3+),Er(3+)@HAp composite fibers have potential applications in drug storage/release and magnetic resonance/UC luminescence imaging.

YOF:Ln(3+) (Ln = Tb, Eu, Tm, Dy, Ho, Sm) nano-/microstructures with a variety of novel and well-defined morphologies, including nanospheres, nanorod bundles, and microspindles, have been prepared through a convenient modified urea-based homogeneous precipitation (UBHP) technique followed by a heat treatment. The sizes and morphologies of the YOF products could be easily modulated by changing the pH values and fluoride sources. XRD, TG-DTA, FT-IR, SEM, and TEM, as well as photoluminescence (PL) and cathodoluminescence (CL) spectra, were used to characterize the prepared samples. The YOF:Ln(3+) nanospheres show the characteristic f-f transitions of Ln(3+) (Ln = Tb, Eu, Tm, Dy, Ho, Sm) ions and give bright green, red, blue, yellow, blue-green, and yellow-orange emission, respectively, under UV light and low-voltage electron beam excitation. Furthermore, YOF:0.03Tb(3+) phosphors exhibit green luminescence with superior properties in comparison with the commercial phosphor ZnO:Zn to a degree, which is advantageous for improving display quality. Because of the simultaneous luminescence of Ln(3+) in the YOF host, the luminescence colors of YOF:Ln(3+) phosphors can be precisely adjusted by changing the doped Ln(3+) ions and corresponding concentrations, which makes these materials hold great promise for applications in field-emission displays.