The combination of a magnesium anode with a sulfur cathode is one of the most promising electrochemical couples because of its advantages of good safety, low cost, and a high theoretical energy density. However, magnesium sulfur batteries are still in a very early stage of research and development, and the discovery of suitable electrolytes is the key challenge for further improvement. Here, a new preparation method for non-nucleophilic electrolyte solutions using a two-step reaction in one-pot is presented, which provides a feasible way to optimize the physiochemical properties of the electrolyte for the application in magnesium sulfur batteries. The fi rst use of modifi ed electrolytes in glymes and binary solvents of glyme and ionic liquid shows benefi cial effects on the performance of magnesium sulfur batteries. New insights into the reaction mechanism of electrochemical conversion between magnesium and sulfur are also investigated.
Keywords: Li-ion batteries, intercalation cathodes, disordered rock salt, Li 2 VO 2 F Advanced cathode materials with superior energy storage capability are highly demanded for mobile and stationary applications. The inherent structural feature of Li + hosts is critical for the battery performance. High-capacity conversion cathode materials often encounter large voltage hysteresis (low energy efficiency) accompanied with the structural reconstruction.[1]The current commercial cathode materials are still dominated by intercalation materials with intrinsic structural integrity for accommodating Li + .[2] However, the known intercalation materials have limited theoretical capacity (< 300 mAh g -1 ). [3] In addition, structural transition/degradation have often been observed for the common intercalation hosts with ordered Li + / transition metal (TM) lattice sites. Antisite disorder (Li + sites/layers occupied by TM ions) in olivines can block the one-dimensional Li + diffusion path.[4] The activation barrier for Li + diffusion in layered oxides is sensitive to the Li-content, the spacing of the
Metal-free nanostructured elemental carbons and carbonbased composites (e.g. C 3 N 4 ) have proven to be attractive alternatives to conventional metal-based catalysts for several important reactions, such as dehydrogenation of aromatic hydrocarbons or alkanes, Friedel-Crafts Reaction.[1] Carbon as the catalytic substance has significant advantages over the conventional metal-supported systems owing to the unique controllability of both its surface acidity/basicity and pelectron density through surface functionalization. In a carbon material it is the short-and long-range ordering of atomic carbon that essentially determines the macroscopic properties (e.g. thermal and electronic conductivities, combustibility) and thus its long-term performance in any potential industrial process. However, the lack of basic knowledge on the nature of carbonmediated reactions remains the most critical restriction for the development of carbon-based catalysis. For oxidative dehydrogenation (ODH) reactions, surface quinone-type oxygen functional groups have been proposed as the active sites and the reaction has been assumed to proceed by a redox mechanism.[2, 3] However, no quantitative description of the elementary steps, or kinetic data can be derived from the literature. The few mechanistic studies reported were conducted either with remarkable secondary oxidation and deactivation [4] or over "impure" surfaces, for example, Pd-or Fe-coordinated polynaphthoquinone[2] or pre-coked metal phosphates or oxides.[5] More detailed and reliable information is expected to be obtained over a pure carbon surface in the kinetic reaction region. Most importantly, the Mars-van Krevelen model for redox reactions is widely accepted based on previous work on the ODH of ethylbenzene. [4, 5] However, this model is incorrect and without physical relevance.[6] Therefore there is an urgent need to describe the reaction pathway by a physically relevant model. Ordered nanocarbon is chemically homogeneous and thus could be seen as the most suitable platform for a mechanistic investigation. To date, all such investigations have been confined to pure or mostly sp 2 -hybridized carbons. [4, 7] In particular, conventional activated carbon which has long-range disorder and high porosity
Au nanoparticles are known to be a good catalyst or an effective promoter for a wide range of catalytic reactions. Bimetallic Au-Pd nanoparticles supported on activated carbon were synthesized following a twostep procedure: immobilization of Au sol onto activated carbon followed by immobilization of Pd(0). The catalysts showed superior activities compared to monometallic Pd or Au nanoparticles on the same support. A series of catalysts with Au:Pd ratios varying from 9.5:0.5 to 2:8 were prepared. These catalysts were characterized by TEM, HRTEM, EDX, and X-ray mapping techniques to obtain morphological information, particle size distributions, crystalline structure, and distribution of the two metals. Correlating with the result from catalytic tests of selective oxidation of glycerol to glyceric acid, we found that the surface configuration of Pd monomers isolated by Au atoms has a substantial effect on activity and stability. The Au:Pd ratio on the surface of the particles is the key parameter and can be finely tuned to achieve optimal catalytic performance. The segregation or inhomogeneity of Pd weakens the synergistic effect of the bimetallic catalyst
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