double-layer polymer electrolyte in which one layer contacts the anode and the other polymer layer contacts the cathode.Various types of lithium-conducting polymers have been explored; lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in poly(ethylene oxide) (PEO) composites have been the most extensively studied owing to their relatively high cation conductivity, acceptable anodic stability, and good membrane-forming capability. [4] Despite these advantages, the PEO-based polymer electrolytes are slowly oxidized at voltages over 3.9 V, which has restricted their use to cells with a lower-voltage cathode such as LiFePO 4 . [5] Enlarging the polymer redox voltage window is needed to be compatible with a high-voltage cathode if a polymer solid electrolyte battery is to meet the energy density specification ΔE > 300 Wh kg −1 . Moreover, there has been no suitable single liquid electrolyte having the required redox window. [3] The high oxidation potential solvents that are stable for cathodes show high anodic reactivity at the negative side; the low oxidation potential solvents compatible with a Li-metal anode exhibit a high reactivity on the high-voltage cathode side. The mixture of a high-voltage stable solvent and a low-voltage stable solvent in liquid electrolyte systems might hurt the electrochemical performance owing to the free diffusion of liquid solvent molecules. However, separate polymer interphase layers for lowering the interfacial impedance between a ceramic electrolyte and an electrode have been demonstrated, [6] which has initiated an investigation of a bilayer polymer electrolyte with a high-voltage stable layer contacting cathode and a low-voltage stable layer contacting anode.Poly(N-methyl-malonic amide) (PMA) contains a repeating unit of high dielectric constant dimethylacetamide (DMAc) that is used as an additive to protect electrolyte oxidation by a high-voltage cathode. [7] However, DMAc is easily reduced by a metallic lithium anode, as shown in Figure S1 in the Supporting Information. [8] Therefore, PMA-LiTFSI layer was used to contact only the cathode and PEO-LiTFSI layer to contact only the anode in a double-layer polymer solid electrolyte (DLPSE) having both a wide redox window and the high flexibility and plasticity for retention of electrode/electrolyte interfaces with low interfacial resistance over a long cycle life. In this DLPSE system, the DMAc containing PMA-LiTFSI layer was well isolated from the lithium-metal anode by a PEO-LiTFSI layer and the PEO-LiTFSI layer was protected by a PMA-LiTFSI layer from a high-voltage oxidation.No single polymer or liquid electrolyte has a large enough energy gap between the empty and occupied electronic states for both dendrite-free plating of a lithium-metal anode and a Li + extraction from an oxide host cathode without electrolyte oxidation in a high-voltage cell during the charge process. Therefore, a double-layer polymer electrolyte is investigated, in which one polymer provides dendrite-free plating of a Li-metal anode and the other all...
Electrochemical reduction of CO2 to valuable fuels is appealing for CO2 fixation and energy storage. However, the development of electrocatalysts with high activity and selectivity in a wide potential window is challenging. Herein, atomically thin bismuthene (Bi‐ene) is pioneeringly obtained by an in situ electrochemical transformation from ultrathin bismuth‐based metal–organic layers. The few‐layer Bi‐ene, which possesses a great mass of exposed active sites with high intrinsic activity, has a high selectivity (ca. 100 %), large partial current density, and quite good stability in a potential window exceeding 0.35 V toward formate production. It even deliver current densities that exceed 300.0 mA cm−2 without compromising selectivity in a flow‐cell reactor. Using in situ ATR‐IR spectra and DFT analysis, a reaction mechanism involving HCO3− for formate generation was unveiled, which brings new fundamental understanding of CO2 reduction.
Mesoporous C-doped TiO2 nanomaterials with an anatase phase are prepared by a one-pot green synthetic approach using sucrose as a carbon-doping source for the first time. A facile post-thermal treatment is employed to enhance visible light photocatalytic activity of the as-prepared photocatalyst. The enhancement effect of post-thermal treatment between 100 and 300 °C is proved by the photodegradation of gas-phase toluene, and the optimum temperature is 200 °C. Physicochemical properties of the samples are characterized in detail by X-ray diffraction, Raman spectroscopy, N2 adsorption–desorption isotherms, transmission electron microscopy, Fourier transform-infrared spectroscopy, X-ray photoelectron spectroscopy, UV–vis diffuse reflectance spectroscopy, and photoluminescence. The results indicate that the promotive effect of the post-thermal treatment can be attributed to the changes of the catalysts’ surface and optical properties. The results also show that the recombination of electron–hole pairs is effectively inhibited after thermal treatment due to the reduction of surface defects. The facile post-thermal treatment provides a new route for potential industrial applications of C-doped TiO2 nanomaterials prepared by a green approach owing to its low cost and easy scale-up.
Soil salinity is a major abiotic stress that limits agriculture productivity worldwide. Salicornia europaea is a succulent annual euhalophyte and one of the most salt tolerant plant species. The elucidation of its salt tolerance mechanism is of significance for generating salt-tolerant crops. In this study, we provided high resolution of proteome reference maps of S. europaea shoot and obtained evidence on the salt tolerance mechanism by analyzing the proteomic responses of this plant to high salinity. Our results demonstrated significant variations existed in 196 out of 1880 protein spots detected on CBB stained 2-DE gels. Of these, 111 proteins were identified by mass spectrometry. Among them, the majority was energy production and conversion related proteins, followed by photosynthesis and carbohydrate metabolism associated enzymes. Analysis of protein expression patters revealed that energy production and ion homeostasis associated proteins played important roles for this plant salt tolerance ability. Hierarchical clustering results revealed many proteins were involved in S. europaea salt tolerance mechanism as a dynamic network. Finally, based on our proteomic results, we brought forward a possible schematic representation of mechanism associated with the systematic salt tolerance phenotype in S. europaea.
We have isolated a novel cDNA clone from rat cerebral cortex encoding a protein of 670 amino acids (NCKX2) that has significant similarity to the 1199-amino acidlong Na/Ca-K exchanger of bovine rod outer segment (NCKX1). NCKX2 transcripts are 10.5 kilobase pairs in length and are expressed abundantly in neurons throughout the brain and with much lower abundance in selected other tissues. The predicted topology of the rat NCKX2 protein is very similar to that of bovine NCKX1, beginning with a solitary transmembrane segment (M0), which is removed as a "signal peptide" in bovine NCKX1, an extracellular loop, a cluster of five transmembrane spanning segments (M1 to M5), a long cytoplasmic loop, and a final hydrophobic cluster (M6 to M11). Within the hydrophobic clusters, rat NCKX2 shares 80% identity and 91% similarity with bovine NCKX1. The two larger hydrophilic loops are much shorter in NCKX2 than in NCKX1, accounting largely for the difference in length between the two proteins, and are dissimilar in sequence except for a 32-amino acid stretch with 69% identity in the cytosolic loop. NCKX2 was epitope-tagged in the extracellular domain and was shown to be expressed at the surface of transfected HEK cells. Analysis of NCKX2 function by fluorescent imaging of fura-2-loaded transfected cells demonstrated that NCKX2 is a potassium-dependent sodium/calcium exchanger.
The acid-base reactions between the scandium trialkyl complex Sc(CH(2)SiMe(3))(3)(THF)(2) and 1 equiv of Cp'-H afforded straightforwardly the corresponding mono(cyclopentadienyl)scandium dialkyl complexes Cp'Sc(CH(2)SiMe(3))(2)(THF) (Cp' = C(5)H(5) (1), C(5)MeH(4) (2), C(5)Me(4)H (3), C(5)Me(5) (4), C(5)Me(4)SiMe(3) (5)) in 65-80% isolated yields. The analogous half-sandwich complexes having a heteroatom-containing side arm, (C(5)Me(4)R)Sc(CH(2)SiMe(3))(2) (R = CH(2)CH(2)PPh(2) (6), C(6)H(4)OMe-omicron (7)), were obtained by the one-pot metathetical reactions of ScCl(3)(THF)(3) with 1 equiv of the potassium salts of the ligands and 2 equiv of LiCH(2)SiMe(3). The similar reactions of ScCl(3)(THF)(3) with KC(5)Me(4)(C(6)H(4)NMe(2)-omicron) and LiCH(2)SiMe(3) gave a methylene-bridged binuclear complex [{C(5)Me(4)(omicron-C(6)H(4)N(Me)CH(2)-mu}Sc(CH(2)SiMe(3))](2) (8). Complexes 1-8 were fully characterized by (1)H, (13)C NMR, X-ray, and microelemental analyses. The reactions of 5 and 7 with 1 equiv of [PhMe(2)NH][B(C(6)F(5))(4)] in THF afforded quantitatively the structurally characterizable cationic monoalkyl complexes [(C(5)Me(4)SiMe(3))Sc(CH(2)SiMe(3))(THF)(2)][B(C(6)F(5))(4)] (10) and [(C(5)Me(4)C(6)H(4)OMe-omicron)Sc(CH(2)SiMe(3))(THF)(2)][B(C(6)F(5))(4)] (11), respectively. In the presence of an activator such as [Ph(3)C][B(C(6)F(5))(4)], [PhMe(2)NH][B(C(6)F(5))(4)], or B(C(6)F(5))(3), all of the half-sandwich dialkyl complexes 1-7 were active for isoprene polymerization and isoprene-ethylene copolymerization, with the activity and selectivity being significantly dependent on the substituents at the cyclopentadienyl ligands to yield the corresponding homo- and copolymer materials with different microstructures and compositions. In the homopolymerization of isoprene, the less sterically demanding complexes 1 and 2 showed high cis-1,4 selectivity (up to 95%), whereas the more sterically demanding complexes 3-5 yielded 3,4-polyisoprene (51-65%) as a major product. The ether side arm coordinated complex 7 preferred trans-1,4-polyisoprene formation (60-79%), whereas the phosphine analogue 6 showed high cis-1,4 selectivity (84-90%) under the same conditions. In the copolymerization of isoprene and ethylene, complexes 1 and 2 afforded the random copolymers with high isoprene contents (85-92 mol %) and predominant cis-1,4-microstructures (up to 90%), thus constituting the first example of cis-1,4-selective copolymerization of isoprene with ethylene. In contrast, the copolymerization of isoprene and ethylene by 3, 4, 6, and 7 gave, for the first time, almost perfect alternating isoprene-ethylene copolymers. Possible mechanisms of the polymerization and copolymerization processes were proposed on the basis of the DFT calculations.
The massive depletion of fossil fuels has led to severe energy and environmental crisis, which urgently needs an in-depth research on the exploration of sustainable energy. Among various energy sources, hydrogen (H 2) is considered to be one of the most potential alternatives to traditional fossil fuels owing to its high energy density and environmental friendliness. [1] Electrochemical hydrogen evolution reaction (HER) is an attracting and scalable technology to split water into H 2 , which can use the renewable electricity as power to realize a hydrogen-based economy. [2] Metals with good conductivity and proton activation are promising electrocatalysts for HER. The past years have witnessed the great progress on metal-based catalysts for HER, where the noble metals, such as platinum (Pt) with near-zero overpotential and a very low Tafel slope for HER, are well known to meet the requirements in terms of commercial application. [3] However, the cherish scarcity and poor stability The electrochemical hydrogen evolution reaction (HER) is an attractive technology for the mass production of hydrogen. Ru-based materials are promising electrocatalysts owing to the similar bonding strength with hydrogen but much lower cost than Pt catalysts. Herein, an ordered macroporous superstructure of N-doped nanoporous carbon anchored with the ultrafine Ru nanoclusters as electrocatalytic micro/nanoreactors is developed via the thermal pyrolysis of ordered macroporous single crystals of ZIF-8 accommodating Ru(III) ions. Benefiting from the highly interconnected reticular macro-nanospaces, this superstrucure affords unparalleled performance for pH-universal HER, with order of magnitude higher mass activity compared to the benchmark Pt/C. Notably, an exceptionally low overpotential of only 13 mV@10 mA cm −2 is required for HER in alkaline solution, with a low Tafel slope of 40.41 mV dec −1 and an ultrahigh turnover frequency value of 1.6 H 2 s −1 at 25 mV, greatly outperforming Pt/C. Furthermore, the hydrogen generation rates are almost twice those of Pt/C during practical overall alkaline water splitting. A solar-to-hydrogen system is also demonstrated to further promote the application. This research may open a new avenue for the development of advanced electrocatalytic micro/nanoreactors with controlled morphology and excellent performance for future energy applications.
Objectives Scutellaria baicalensis Georgi. (Lamiaceae) is a plant of the genus Lamiaceae, and its root is the main part used as a medicine. In China, Scutellaria baicalensis is still an important traditional Chinese medicine with the functions of clearing away heat and dampness, purging fire and detoxification. This medicinal plant is widely distributed in China, Russia, Mongolia, North Korea and Japan. The purpose of this paper was to provide a systematic and comprehensive overview on the traditional usages, botany, phytochemistry, pharmacology, pharmacokinetics and toxicology of this plant. Furthermore, the possible development trends and perspectives for future research on this medicinal plant are also discussed. Key findings So far, over 40 compounds have been isolated and identified from Scutellaria baicalensis, including flavonoids, terpenoids, volatile oils and polysaccharides. The compounds and extracts isolated from Scutellaria baicalensis exhibit a wide range of pharmacological activities, including the effects on the nervous system, effects on the immune system, liver protection, antitumour effects, antibacterial and antiviral effects, antioxidant effects and other pharmacological effects. Summary As a traditional Chinese herbal medicine, Scutellaria baicalensis has shown significant effects on the treatment of various diseases, especially hepatitis, diarrhoea, vomiting and high blood pressure. Numerous traditional uses of Scutellaria baicalensis have been confirmed by current investigations. However, it is also necessary to further study the drug-forming properties and pharmacokinetics of the active constituents of Scutellaria baicalensis, as well as to establish quality control standards for different areas of Scutellaria baicalensis, and to carry out the research at the cellular and molecular levels. Preparation nameMain compositions Traditional and clinical usages Ref.Inducing sweat to dispel heat, soothing liver and harmonizing stomach and treating hypochondriac pain, liver and treating stomach disharmony, influenza and acute upper respiratory tract infection [12] Clearing the heat and transforming phlegm, calming the liver and tranquilization and treating vertigo, liver fire flaming, insomnia and hypertension [12]
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