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A Multiple-Electron Reaction in Rechargeable Lithium Batteries with a Positive Electrode Li9V3P8-δO29-δ'

The oxygen and phosphorus deficient material of monodiphosphate Li 9 V 3 (P 2 O 7 ) 3 (PO 4 ) 2 with a trigonal layered structure, or Li 9 V 3 P 8-δ O 29-δ' has been synthesized, where the lattice constants are a = 9.7422(4) and c = 13.6145(8) A in the hexagonal basis. The electrochemical characteristics using this material with δ≈0.4 and δ' ≈1 as a positive electrode exhibit a double-electron reaction with a capacity 170 A h kg -1 and an energy density 670 W h kg -1 . The V atoms are ionized significantly to reduce the V–O electronic admixture and are in a state with the orbital singlet–doublet separation 1370 cm -1 within the Γ 4 manifold. The Li ionic motion at 295 K is suggested from a microscopic viewpoint.