6,423 research outputs found

    Progress and perspective of interface design in garnet electrolyte-based all-solid-state batteries

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    Inorganic solid-state electrolytes (SSEs) are nonflammable alternatives to the commercial liquid-phase electrolytes. This enables the use of lithium (Li) metal as an anode, providing high-energy density and improved stability by avoiding unwanted liquid-phase chemical reactions. Among the different types of SSEs, the garnet-type electrolytes witness a rapid development and are considered as one of the top candidates to pair with Li metal due to their high ionic conductivity, thermal, and electrochemical stability. However, the large resistances at the interface between garnet-type electrolytes and cathode/anode are the major bottlenecks for delivering desirable electrochemical performances of all-solid-state batteries (SSBs). The electrolyte/anode interface also suffers from metallic dendrite formation, leading to rapid performance degradation. This is a fundamental material challenge due to the poor contact and wettability between garnet-type electrolytes with electrode materials. Here, we summarize and analyze the recent contributions in mitigating such materials challenges at the interface. Strategies used to address these challenges are divided into different categories with regard to their working principles. On one hand, progress has been made in the anode/garnet interface, such as the successful application of Li-alloy anode and different artificial interlayers, significantly improving interfacial performance. On the other hand, the desired cathode/garnet interface is still hard to reach due to the complex chemical and physical structure at the cathode. The common methods used are nanostructured cathode host and sintering additives for increasing the contact area. On the basis of this information, we present our views on the remaining challenges and future research of electrode/garnet interface. This review not only motivates the need for further understanding of the fundamentals, stability, and modifications of the garnet/electrode interfaces but also provides guidelines for the future design of the interface for SSB

    Selective catalytic oxidation of ammonia over nano Cu/zeolites with different topologies

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    The selective catalytic oxidation of ammonia (NH3-SCO) is the last mitigation step in exhaust treatment using a 4-way catalytic converter to convert any excess and unreacted NH3 (that was used as a reductant of NOx) into environmentally benign N2 and H2O. Here, we report a series of highly reactive and selective nano Cu/zeolites for the NH3-SCO reaction. The NH3-SCO activity was found in the order nano Cu/ZSM-5 (MFI topology) > Cu/Beta (BEA) > Cu/MCM-49 (MWW) > Cu/Y (FAU) > Cu/Mordenite (MOR) > Cu/Ferrierite (FER). The best catalyst, i.e., nano Cu/ZSM-5, achieves 98% NH3 conversion at 250 °C with the N2 yield maintained at >98% even at up to 500 °C. When assessed under practical exhaust conditions in the presence of moisture (5% H2O) as well as that after hydrothermal aging (5% H2O, 850 °C, 8 h), the nano Cu/ZSM-5 exhibited only minor deactivation as a result of its good retention of Cu dispersion, pore structure and specific surface area. Furthermore, small micropore (10-membered ring, 10-MR) topologies were found to be crucial in maintaining high N2 yields. For Cu/Y and Cu/Mordenite, composed of 12-MR pores that are non-interconnected with smaller pores, their N2 yields were compromised by forming NOx at temperatures above 400 °C. Based on the in situ DRIFTS study, the iSCR mechanism appears to be applicable for all fresh and aged Cu/zeolites with the exception of fresh Cu/MCM-49 that follows the imide mechanism

    Global behavior of cosmological dynamics with interacting Veneziano ghost

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    In this paper, we shall study the dynamical behavior of the universe accelerated by the so called Veneziano ghost dark energy component locally and globally by using the linearization and nullcline method developed in this paper. The energy density is generalized to be proportional to the Hawking temperature defined on the trapping horizon instead of Hubble horizon of the Friedmann-Robertson-Walker (FRW) universe. We also give a prediction of the fate of the universe and present the bifurcation phenomenon of the dynamical system of the universe. It seems that the universe could be dominated by dark energy at present in some region of the parameter space.Comment: 8 pages, 7 figures, accepted for publication in JHE

    Effective Activation of Strong C−Cl Bonds for Highly Selective Photosynthesis of Bibenzyl via Homo-Coupling

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    Carbon-carbon (C−C) coupling of organic halides has been successfully achieved in homogeneous catalysis, while the limitation, e.g., the dependence on rare noble metals, complexity of the metal-ligand catalylst and the poor catalyst stability and recyclability, needs to be tackled for a green process. The past few years have witnessed heterogeneous photocatalysis as a green and novel method for organic synthesis processes. However, the study on C−C coupling of chloride substrates is rare due to the extremely high bond energy of C−Cl bond (327 kJ mol−1). Here, we report a robust heterogeneous photocatalyst (Cu/ZnO) to drive the homo-coupling of benzyl chloride with high efficiency, which achieves an unprecedented high selectivity of bibenzyl (93 %) and yield rate of 92 % at room temperature. Moreover, this photocatalytic process has been validated for C−C coupling of 10 benzylic chlorides all with high yields. In addition, the excellent stability has been observed for 8 cycles of reactions. With detailed characterization and DFT calculation, the high selectivity is attributed to the enhanced adsorption of reactants, stabilization of intermediates (benzyl radicals) for the selective coupling by the Cu loading and the moderate oxidation ability of the ZnO support, besides the promoted charge separation and transfer by Cu species

    UV-IR luminosity functions and stellar mass functions of galaxies in the Shapley supercluster core

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    We present a panchromatic study of luminosity functions (LFs) and stellar mass functions (SMFs) of galaxies in the core of the Shapley supercluster at z=0.048, in order to investigate how the dense environment affects the galaxy properties, such as star formation (SF) or stellar masses. We find that while faint-end slopes of optical and NIR LFs steepen with decreasing density, no environment effect is found in the slope of the SMFs. This suggests that mechanisms transforming galaxies in different environments are mainly related to the quench of SF rather than to mass-loss. The Near-UV (NUV) and Far-UV (FUV) LFs obtained have steeper faint-end slopes than the local field population, while the 24μ\mum and 70μ\mum galaxy LFs for the Shapley supercluster have shapes fully consistent with those obtained for the local field galaxy population. This apparent lack of environmental dependence for the infrared (IR) LFs suggests that the bulk of the star-forming galaxies that make up the observed cluster IR LF have been recently accreted from the field and have yet to have their SF activity significantly affected by the cluster environment.Comment: 5 pages, 3 figures, JENAM 2010, Symposium 2. Conference proceeding

    Versatile Preparation of Mesoporous Single-Layered Transition-Metal Sulfide/Carbon Composites for Enhanced Sodium Storage

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    Transition metal sulfides are promise electrochemical energy storage materials due to their abundant active sites, large inter-layer space and high theoretical capacities. Especially for sodium storage. However, the low conductivity and poor cycling stability at high current densities hampered their applications. Herein, we report a versatile dual-templates method to elaborate ordered mesoporous single layered MoS2 /carbon composite with high specific area, uniform pore size and large pore volume. The single layered MoS2 is confined in the carbon matrix. The mesopores between the composite nanorods provide fast electrolyte diffusion. The obtained nanocomposite shows a high sodium storage capability, excellent rate capacity, and very good cycling performance. A 310 mAh g-1 capacity can remains at 5.0 A g-1 after 2500 cycles. Furthermore, a SIB full cell composed the MoS2 /carbon composite anode and a Na3 V2 (PO4 )3 (NVP) cathode maintains a specific capacity of 330 mA h g-1 at 1.0 A g-1 during 100 cycles. The mechanism is investigated by in situ and ex situ characterizations as well as density functional theory (DFT) calculations. This article is protected by copyright. All rights reserved

    Specific heat of MgB_2 after irradiation

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    We studied the effect of disorder on the superconducting properties of polycrystalline MgB_2 by specific-heat measurements. In the pristine state, these measurements give a bulk confirmation of the presence of two superconducting gaps with 2 Delta 0 / k_B T_c = 1.3 and 3.9 with nearly equal weights. The scattering introduced by irradiation suppresses T_c and tends to average the two gaps although less than predicted by theory. We also found that by a suitable irradiation process by fast neutrons, a substantial bulk increase of dH_{c2}/dT at T_c can be obtained without sacrificing more than a few degrees in T_c. The upper critical field of the sample after irradiation exceeds 28 T at T goes to 0 K.Comment: 11 pages text, 6 figures, accepted by Journal of Physics: Condensed Matte

    Metal-Specific Reactivity in Single-Atom Catalysts: CO Oxidation on 4d and 5d Transition Metals Atomically Dispersed on MgO

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    Understanding and tuning the catalytic properties of metals atomically dispersed on oxides are major stepping-stones toward a rational development of single-atom catalysts (SACs). Beyond individual showcase studies, the design and synthesis of structurally regular series of SACs opens the door to systematic experimental investigations of performance as a function of metal identity. Herein, a series of single-atom catalysts based on various 4d (Ru, Rh, Pd) and 5d (Ir, Pt) transition metals has been synthesized on a common MgO carrier. Complementary experimental (X-ray absorption spectroscopy) and theoretical (Density Functional Theory) studies reveal that, regardless of the metal identity, metal cations occupy preferably octahedral coordination MgO lattice positions under step-edges, hence highly confined by the oxide support. Upon exposure to O2-lean CO oxidation conditions, FTIR spectroscopy indicates the partial deconfinement of the monatomic metal centers driven by CO at precatalysis temperatures, followed by the development of surface carbonate species under steady-state conditions. These findings are supported by DFT calculations, which show the driving force and final structure for the surface metal protrusion to be metal-dependent, but point to an equivalent octahedral-coordinated M4+ carbonate species as the resting state in all cases. Experimentally, apparent reaction activation energies in the range of 96 ± 19 kJ/mol are determined, with Pt leading to the lowest energy barrier. The results indicate that, for monatomic sites in SACs, differences in CO oxidation reactivity enforceable via metal selection are of lower magnitude than those evidenced previously through the mechanistic involvement of adjacent redox centers on the oxide carrier, suggesting that tuning of the oxide surface chemistry is as relevant as the selection of the supported metal
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