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It is widely believed that the origin of a significant cause for the voltageand capacity fading observed in lithium (Li)-ion batteries is related tostructural modifications occurring in the cathode material during the Li-ioninsertion/de-insertion process. The Li-ion insertion/de-insertion mechanism andthe resulting structural changes are known to exert a severe strain on thelattice, and consequently leading to performance degradation. Here, with a viewto shed more light on the effect of such strain on the structural properties ofthe cathode material, we have systematically investigated the pressuredependence of structural and transport properties of an LixCoO2 single crystal,grown using 5% excess Li in the precursors. Ambient pressure synchrotrondiffraction on these crystals reveals that, the excess Li during the growth,has facilitated the stabilization of a layered rhombohedral phase (space groupR3m) as well as a disordered rock-salt phase (space group Fm3m). The volumefraction of the rhombohedral and cubic phase is 60:40, respectively, whichremains unchanged up to 10.6 GPa. No structural phase transition has beenobserved up to 10.6 GPa. An increase in resistance with a decrease intemperature has revealed the semi-metallic nature of the sample. Further, theapplication of hydrostatic pressure up to 2.8 GPa shows the enhancement ofsemi-metallic nature. The obtained experimental results can be qualitativelyexplained via density functional theory (DFT) and thermodynamics modelling. Thecalculated density of states was reduced, and the activation energy wasincreased by applied pressure. Our investigations indicate a significant phasestability of the mixed phase crystals under externally applied high pressureand thus suggest the possible use of such mixed phase materials as a cathode inlithium-ion batteries.

Hydrostatic pressure effect on structural and transport properties of co-existing layered and disordered rock-salt phase of LixCoO2