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Silicon is emerging as a very attractive anode material for lithium ion batteries due to its low discharge potential, natural abundance, and high theoretical capacity of 4200 mAh/g, more than ten times that of graphite (372 mAh/g). This high charge capacity is the result of silicon’s ability to incorporate 4.4 lithium atoms per silicon atom; however, the incorporation of lithium also leads to a 300-400% volume expansion during charging, which can cause pulverization of the material and loss of access to the silicon. The architecture of the anode must therefore be able to adapt to this volume increase. Here we present a layered carbon nanotube and silicon nanoparticle electrode structure, fabricated using directed assembly techniques. The porous carbon nanotube layers maintain electrical connectivity through the active material and increase the surface area of the current collector. Using this architecture, we obtain an initial capacity in excess of 4000 mAh/g, as well as increased power and energy density as compared to anodes fabricated using the standard procedure of slurry casting.
In this study, the multicomponent electrode approach was used in an attempt to simultaneously improve the cell's specific energy values by shifting the cathode's voltage up to the 5V-region, combined with the increased specific capacity via addition of the second electrode component. The electrode materials were prepared by variety of synthetic methods (e.g. solid state, sol-gel, mechanical mixing etc.) and tested for lithium-ion intercalation properties. Structural properties and morphology of synthesized materials were characterized by X-ray diffraction (XRD) methods. The prospective 5V cathode materials were investigated as cathodes in the cells with lithium-metal counter electrode.
6Li MAS NMR spectra of lithium manganese oxides with differing manganese oxidation states (LiMn2O4, Li4Mn5O12, Li2Mn4O9, and Li2Mn2O4) are presented. Improved understanding of the lithium NMR spectra of these model compounds is used to interpret the local structure of the LixMn2O4 cathode materials following electrochemical Li+ deintercalation to various charging levels. In situ x-ray diffraction patterns of the same material during charging are also reported for comparison. Evidence for two-phase behavior for x < 0.4 (LixMn2O4) is seen by both NMR and diffraction.
A series of electroactive spinel compounds, LiMn2-xCuxO4 (0.1 ≤ x ≤ 0.5) has been studied by crystallographic, spectroscopie and electrochemical methods and by electron-microscopy. These LiMn2-xCuxO4 spinels are nearly identical in structure to cubic LiMn2O4 and successfully undergo reversible Li intercalation. The electrochemical data show slight shifts to higher voltage for the delithiation reaction that normally occurs at 4.1 V in standard Li1−xMn2O4 electrodes (1 ≥ x ≥ 0) corresponding to the oxidation of Mn3+ to Mn4+. The data also show a remarkable reversible electrochemical process at 4.9 V which is attributed to the oxidation of Cu2+ to Cu3+. The inclusion of Cu in the spinel structure enhances the electrochemical stability of these materials upon cycling. The initial capacity of LiMn2-xCuxO4 spinels decreases with increasing x from 130 mAh/g in LiMn2O4 (x=0) to 70 mAh/g in “LiMn1.5Cu0.5O4”(x=0.5). Although the powder X-ray diffraction pattern of “LiMn1.5Cu0.5 O4” shows a single-phase spinel product, neutron diffraction data show a small, but significant quantity of an impurity phase, the composition and structure of which could not be identified. X-ray absorption spectroscopy was used to gather information about the oxidation states of the manganese and copper ions. The composition of the spinel component in the LiMn1.5Cu0.5O4 was determined from X-ray diffraction and XANES data to be Li1.01Mn1.67Cu0.32O4 suggesting, to a best approximation, that the impurity in the sample was a lithium-copper-oxide phase.
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