Reversible control of the magnetization of spinel ferrites based electrodes by lithium-ion migration

Lithium-ion (Li-ion) batteries based on spinel transition-metal oxide electrodes have exhibited excellent electrochemical performance. The reversible intercalation/deintercalation of Li-ions in spinel materials enables not only energy storage but also nondestructive control of the electrodes' physical properties. This feature will benefit the fabrication of novel Li-ion controlled electronic devices. In this work, reversible control of ferromagnetism was realized by the guided motion of Li-ions in MnFe₂O₄ and γ-Fe₂O₃ utilizing miniature lithium-battery devices. The in-situ characterization of magnetization during the Li-ion intercalation/deintercalation process was conducted, and a reversible variation of saturation magnetization over 10% was observed in both these materials. The experimental conditions and material parameters for the control of the ferromagnetism are investigated, and the mechanism related to the magnetic ions' migration and the exchange coupling evolution during this process was proposed. The different valence states of tetrahedral metal ions were suggested to be responsible for the different performance of these two spinel materials.