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In layered LiNixMnyCozO2 cathode material for lithium-ion batteries, thespins of transition metal (TM) ions construct a two-dimensional triangularnetworks, which can be considered as a simple case of geometrical frustration.By performing neutron powder diffraction experiments and magnetizationmeasurements, we find that long-range magnetic order cannot be established inLiNixMnyCozO2 even at low temperature of 3 K. Remarkably, the frustrationparameters of these compounds are estimated to be larger than 30, indicatingthe existence of strongly frustrated magnetic interactions between spins of TMions. As frustration will inevitably give rise to lattice instability, theformation of Li/Ni exchange in LiNixMnyCozO2 will help to partially relieve thedegeneracy of the frustrated magnetic lattice by forming a stableantiferromagnetic state in hexagonal sublattice with nonmagnetic ions locatedin centers of the hexagons. Moreover, Li/Ni exchange will introduce 180{\deg}superexchange interaction, which further relieves the magnetic frustrationthrough bringing in new exchange paths. Thus, the variation of Li/Ni exchangeratio vs. TM mole fraction in LiNixMnyCozO2 with different compositions can bewell understood and predicted in terms of magnetic frustration andsuperexchange interactions. This provides a unique viewpoint to study the Li/Niions exchange in layered Li(NixMnyCoz)O2 cathode materials.

Insight into the origin of Lithium/Nickel ions exchange in layered Li(NixMnyCoz)O2 cathode materials