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941.
A facile route is presented for fabricating a new class of nanomimics that overexpress hepatitis B virus (HBV) receptor by a natural biosynthetic procedure against HBV infection. A nine‐transmembrane HBV‐specific receptor, human sodium taurocholate co‐transporting polypeptide (hNTCP), was engineered to naturally immobilize it onto the cellular surface and subsequently trigger the budding of hNTCP‐anchoring membrane vesicles (hNTCP‐MVs) that favor the HBV virion. hNTCP‐MVs could rapidly block HBV infection in cell models. Furthermore, hNTCP‐MVs treatment could effectively prevent viral infection, spreading, and replication in a human‐liver‐chimeric mouse model of HBV infection. Our findings demonstrate the receptor‐mediated antiviral effect of hNTCP‐MVs to trick HBV and offer novel opportunities for further development of antiviral strategies in nanomedicine.  相似文献   
942.
Supported vanadium oxides are one of the most promising alternative catalysts for propane dehydrogenation (PDH) and efforts have been made to improve its catalytic performance. However, unlike Pt‐based catalysts, the nature of the active site and surface structure of the supported vanadium catalysts under reductive reaction conditions still remain elusive. This paper describes the surface structure and the important role of surface‐bound hydroxyl groups on VOx / γ‐Al2O3 catalysts under reaction conditions employing in situ DRIFTS experiments and DFT calculations. It is shown that hydroxyl groups on the VOx /Al2O3 catalyst (V?OH) are produced under H2 pre‐reduction, and the catalytic performance for PDH is closely connected to the concentration of V?OH species on the catalyst. The hydroxyl groups are found to improve the catalyst that leads to better stability by suppressing the coke deposition.  相似文献   
943.
The organoborane‐catalyzed reductive carbocyclization of homoallylic alcohols has been developed by using hydrosilanes as reducing reagents to provide a range of 1,2‐disubstituted arylcyclobutanes. The reaction proceeds in a cis‐selective manner with high efficiency under mild conditions. Mechanistic studies, including deuterium scrambling and Hammett studies, and DFT calculations, suggest a dual ring‐closing pathway.  相似文献   
944.
Carbon dioxide (CO2) reduction in aqueous solutions is an attractive strategy for carbon capture and utilization. Cuprous oxide (Cu2O) is a promising catalyst for CO2 reduction as it can convert CO2 into valuable hydrocarbons and suppress the side hydrogen evolution reaction (HER). However, the nature of the active sites in Cu2O remains under debate because of the complex surface structure of Cu2O under reducing conditions, leading to limited guidance in designing improved Cu2O catalysts. This paper describes the functionality of surface‐bonded hydroxy groups on partially reduced Cu2O(111) for the CO2 reduction reaction (CO2RR) by combined density functional theory (DFT) calculations and experimental studies. We find that the surface hydroxy groups play a crucial role in the CO2RR and HER, and a moderate coverage of hydroxy groups is optimal for promotion of the CO2RR and suppression of the HER simultaneously. Electronic structure analysis indicates that the charge transfer from hydroxy groups to coordination‐unsaturated Cu (CuCUS) sites stabilizes surface‐adsorbed COOH*, which is a key intermediate during the CO2RR. Moreover, the CO2RR was evaluated over Cu2O octahedral catalysts with {111} facets and different surface coverages of hydroxy groups, which demonstrates that Cu2O octahedra with moderate coverage of hydroxy groups can indeed enhance the CO2RR and suppress the HER.  相似文献   
945.
Mn4+‐doped fluoride phosphors have been widely used in wide‐gamut backlighting devices because of their extremely narrow emission band. Solid solutions of Na2(SixGe1?x)F6:Mn4+ and Na2(GeyTi1?y)F6:Mn4+ were successfully synthesized to elucidate the behavior of the zero‐phonon line (ZPL) in different structures. The ratio between ZPL and the highest emission intensity υ6 phonon sideband exhibits a strong relationship with luminescent decay rate. First‐principles calculations are conducted to model the variation in the structural and electronic properties of the prepared solid solutions as a function of the composition. To compensate for the limitations of the Rietveld refinement, electron paramagnetic resonance and high‐resolution steady‐state emission spectra are used to confirm the diverse local environment for Mn4+ in the structure. Finally, the spectral luminous efficacy of radiation (LER) is used to reveal the important role of ZPL in practical applications.  相似文献   
946.
The exploration of substrate materials to construct electrochemical biosensors for glucose monitoring in the field of clinical diagnosis, especially for diabetes is still being investigated extensively. In this paper, NiO/Fe2O3 nanocomposites are designed and synthesized by two-step hydrothermal approach in combination with calcinations. The morphology and microstructure are studied by SEM, XRD, XPS, and TEM systematically. Optimized NiO/Fe2O3 nanocomposites are employed as substrate to construct glucose biosensors, and the electrochemical properties are carried out by cyclic voltammetric and chronoamperometric techniques. The results indicate as-prepared biosensors achieve a high sensitivity of 230.5 μA cm?2 mM?1, wide linear range between 50 and 2867 μM, and low detection limit of 3.9 μM towards glucose detection. The synergistic effect between NiO and Fe2O3 as substrate to construct glucose biosensors is elucidated. The selectivity is acceptable based on the detection of glucose concentration for diabetics.  相似文献   
947.
In contrast to the traditional multistep synthesis, we demonstrate herein a two‐step synthesis shortcut to triphenylamine‐based hole‐transporting materials (HTMs) through sequential direct C?H arylations. These hole‐transporting molecules are fabricated in perovskite‐based solar cells (PSCs) that exhibit promising efficiencies up to 17.69 %, which is comparable to PSCs utilizing commercially available 2,2′,7,7′‐tetrakis[N,N‐di(4‐methoxyphenyl)amino]‐9,9′‐spirobifluorene (spiro‐OMeTAD) as the HTM. This is the first report describing the use of step‐saving C?H activations/arylations in the facile synthesis of small‐molecule HTMs for perovskite solar cells.  相似文献   
948.
In this paper, we consider the knot placement problem in B-spline curve approximation. A novel two-stage framework is proposed for addressing this problem. In the first step, the $l_{\infty, 1}$-norm model is introduced for the sparse selection of candidate knots from an initial knot vector. By this step, the knot number is determined. In the second step, knot positions are formulated into a nonlinear optimization problem and optimized by a global optimization algorithm — the differential evolution algorithm (DE). The candidate knots selected in the first step are served for initial values of the DE algorithm. Since the candidate knots provide a good guess of knot positions, the DE algorithm can quickly converge. One advantage of the proposed algorithm is that the knot number and knot positions are determined automatically. Compared with the current existing algorithms, the proposed algorithm finds approximations with smaller fitting error when the knot number is fixed in advance. Furthermore, the proposed algorithm is robust to noisy data and can handle with few data points. We illustrate with some examples and applications.  相似文献   
949.
Leukemia cell and melanoma tumor tissue extracts were studied for small (mostly m/z?<?250) polar metabolites by LC-ESI-HRMSn analysis powered by a hybrid Quadrupole-Orbitrap. MS data were simultaneously acquired in fast polarity switching mode operating in MS1 and MS/MS (All Ion Fragmentation, AIF) full-scan analyses at high mass resolution. Positive metabolite assignments were achieved by AIF analysis considering at least two characteristic transitions. Targeted metabolite profiling was achieved by the relative quantification of 18 metabolites through spiking of their respective deuterated counterparts. Manual data processing of MS1 and AIF scans were compared for the accurate determination of natural metabolites and their deuterated analogs by chromatographic alignment and peak area integration. Evaluation of manual and automated (MetaboList R package) AIF data processing yielded comparable results. The versatility of AIF analysis also enabled the untargeted metabolite profiling of leukemia and melanoma samples in which 22 and 53 compounds were, respectively, identified outside those studied by labeling. The main limitation of this method was that low abundance metabolites with scan rates below 8 scans/peak could not be accurately quantified by AIF analysis. The combination of AIF analysis with MetaboList R package represents an opportunity to move towards automated, faster, and more global metabolomics approaches supported by an entirely flexible open source data processing platform freely available from Comprehensive R Archive Network (CRAN, https://CRAN.R-project.org/package=MetaboList).  相似文献   
950.
The authors introduce an arc ion plating method for the deposition of chromium oxide (Cr2O3) on a steel wire substrate, and its use as a coating for solid phase microextraction. The coating has a micro- and nano-scaled structure after annealing at 700 °C. It is found that Cr2O3 exhibits a good extraction capability for the aromatic hydrocarbons naphthalene, anthracene, fluorene, fluoranthene, and biphenyl. Following desorption by high temperature at 300 °C, the analytes were quantified by gas chromatography (GC). The limits of detection are in the range between 20 and 200 ng·L?1, and calibration plots are linear within a wide range (0.2 to 400 μg·L?1). The coating has excellent mechanical properties, with a hardness is as high as 31.7 GPa, and the adhesion strength between coating and substrate reaches 20.1 N (corresponding to the critical Hertzian contact stress of 10 GPa). This, along with the chemical and thermal stability of the Cr2O3 coating, endows the wire with a long operational life. It was used for at least 100 times without any obvious decline of extraction capability.
Graphical abstract An arc ion plating method was introduced for the deposition of chromium oxide (Cr2O3) on a steel wire substrate, and its use as a coating for solid phase microextraction with high mechanical strength, stability, and long operational lifetime.
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