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Lithium metal orthosilicates with general formula Li2MSiO4 (M = Mn, Fe and Co) are among the most attractive new materials as potential high-specific-energy cathodes for lithium batteries. All the members of this family present a rich polymorphism with at least three clearly identified crystal structures of each Li2MSiO4 compound. Several theoretical investigations have highlighted that the energy stability of the different polymorphs is very close to each other irrespective of their average crystal structures. At the same time, the calculated and experimental electrochemical performances are again very similar among different polymorphs. By means of neutron total scattering investigation of different polymorphs (monoclinic and orthorhombic) of Li2FeSiO4 and Li2MnSiO4 orthosilicates coupled to Pair Distribution Function (PDF) analysis we showed that, at the local scale, all the polymorphs have the same structure (in particular the structure of the monoclinic polymorph) irrespective of the average structure they possess. This experimental evidence of a strong similarity at the local scale can be correlated with the observed electrochemical similarity (such as the lithium extraction voltages) among the different orthosilicate polymorphs, thus providing an approach to elucidate the relevance of local versus long-range structure.

Correlation between the local scale structure and the electrochemical properties in lithium orthosilicate cathode materials