Developing electrode materials with high-energy densities is important for the development of lithium-ion batteries. Here, we demonstrate a mesoporous molybdenum dioxide material with abnormal lithium-storage sites, which exhibits a discharge capacity of 1,814 mAh g−1 for the first cycle, more than twice its theoretical value, and maintains its initial capacity after 50 cycles. Contrary to previous reports, we find that a mechanism for the high and reversible lithium-storage capacity of the mesoporous molybdenum dioxide electrode is not based on a conversion reaction. Insight into the electrochemical results, obtained by in situ X-ray absorption, scanning transmission electron microscopy analysis combined with electron energy loss spectroscopy and computational modelling indicates that the nanoscale pore engineering of this transition metal oxide enables an unexpected electrochemical mass storage reaction mechanism, and may provide a strategy for the design of cation storage materials for battery systems.
Noble Gemini surfactants containing a siloxane moiety have been designed and successfully synthesized in the present study and are utilized as structure-directing agents for mesoporous metal oxides such as zirconia, titania, and vanadia. The siloxane moiety is believed to play an important nano-propping role during the surfactant removal by direct calcination, yielding thermally stable mesoporous metal oxides. It is also believed that the synthesis strategy described here can be applied to the synthesis of robust nanostructured materials such as nanoparticles and nanorods in addition to mesoporous materials.
Highly ordered periodic mesoporous organosilica (PMO) materials with various mesostructures, including lamellar, bicontinuous cubic Ia3d, 2D hexagonal (P6mm), 3D hexagonal (P6 3 /mmc) and cubic Pm3n, have been synthesized using Gemini surfactants with general formulas of [C n H 2n+1 N(CH 3 ) 2 (CH 2 ) s N (CH 3 ) 2 C n H 2n+1 ]Br 2 (n 5 6-18 and s 5 3-12, C n-s-n ). The nature of the Gemini surfactant such as alkyl chain length (n) and spacer length (s), and the synthetic conditions such as reaction temperatures and molar compositions are controlling parameters for desired mesostructures. The PMO materials, synthesized at room temperature from C n-6-n , exhibit phase transition from lamellar to bicontinuous cubic Ia3d, 2D hexagonal, 3D hexagonal and cubic Pm3n as the chain length decreases, whereas only the lamellar and 2D hexagonal PMO materials with different lattice parameters depending on the chain length are obtained at high reaction temperature (373 K). The C n-8-n and C n-10-n surfactants also yield 2D hexagonal PMO material in a very wide range of synthetic condition at 373 K. The PMO materials with various mesostructures thus obtained exhibit high BET surface areas in the range of 900-1500 m 2 g 21 and total pore volumes of about 0.5-1.4 cm 3 g 21 .
Mesoporous transition metal dichalcogenides with 2D layered crystallinity, synthesized through a melting-infiltration assisted nano-replication, exhibit excellent electrochemical performances for lithium-storage.
Lithiation–delithiation reactions in Li‐ion batteries do exhibit a huge electrochemically driven volume change of the anode material between the lithium‐free and lithiated‐host states, which results in a gradually fading capacity. Minimizing this volume change of the electrode during cycling is essential to achieve stable electrochemical behavior and thus for innovating design of electrode materials for Li storage. Here, ordered mesoporous CoSn intermetallic anode materials with various Co/Sn atomic ratios are developed. A dual‐buffer effect is discovered that accommodates the volume changes in the electrode material by not only repeatedly generating void nanospaces but also by incorporating electrochemically inactive elements. Novel insights into the nanostructural changes of electrode materials during the lithiation–delithiation process are obtained by in operando small angle X‐ray scattering. The degrees of volume change and nanoscopic order are found to be highly dependent on the Co contents in the mesoporous CoSn intermetallic anode materials, being possible to achieve a durable nanostructured electrode upon prolonged cycling.
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