Although widely used, the most promising Li-based technologies still suffer from a lack of suitable electrodes. There is therefore a need to seek new materials concepts to satisfy the increasing demands for energy storage worldwide. Here we report on a new layered electrode material, Cu(2.33)V(4)O(11), which shows a sustainable reversible capacity of 270 mA h g(-1) at a voltage of about 2.7 V, and electrochemically reacts with Li in an unusual and spectacular way. The reaction entails a reversible Li-driven displacement process leading to the growth and disappearance of Cu dendrites with a concomitant reversible decomposition and recrystallization of the initial electrode material. We show from structural considerations that the uniqueness of Cu(2.33)V(4)O(11) is rooted in the peculiar flexibility of the stacked [V(4)O(11)](n) layers, which is due to the presence of pivot oxygen atoms. Fully reversible displacement reactions could provide a new direction for developing an alternative class of higher energy density Li storage electrodes.
The grafting reaction between a trifunctional silylating agent and two kinds of 2:1 type layered silicates was studied using FTIR, XRD, TGA, and 29Si CP/MAS NMR. XRD patterns clearly indicate the introduction of 3-aminopropyltriethoxysilane (gamma-APS) into the clay interlayer. In the natural montmorillonite, gamma-APS adopts a parallel-bilayer arrangement, while it adopts a parallel-monolayer arrangement in the synthetic fluorohectorite. These different silane arrangements have a prominent effect on the mechanism of the condensation reaction within the clay gallery. In natural montmorillonite, the parallel-bilayer arrangement of gamma-APS results in bidentate (T2) and tridendate (T3) molecular environments, while the parallel-monolayer arrangement leads to monodentate (T1), as indicated by 29Si CP/MAS NMR spectra. This study demonstrates that the silylation reaction and the interlayer microstructure of the grafting products strongly depend on the original clay materials.
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