Abstract
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.
Highlights
Lithium-ion batteries (LIB) based on transition-metal oxide electrodes, typically in a spinel structure, have attracted extensive research interests for their remarkable electrochemical properties[1,2,3,4,5,6,7,8,9]
As electrodes for lithium-ion batteries (LIB), TM oxides would experience a series of redox reactions during the battery cycle, which will change the state of the 3d electrons and their magnetic properties
There are few reports about the reversible control of ferromagnetism in spinel materials during lithium intercalation and deintercalation, and the explanation is mostly restricted to the change of chemical states[29,30,31,32,33]
Summary
Lithium-ion batteries (LIB) based on transition-metal oxide electrodes, typically in a spinel structure, have attracted extensive research interests for their remarkable electrochemical properties[1,2,3,4,5,6,7,8,9]. Considering that the interaction between the electrode material and the Li-ions is definitely accompanied with change in electronic structure, in-situ magnetization characterization is a promising method to achieve a deeper understanding of battery operation This would benefit research on the manipulation of magnetism via the guided motion of Li-ions. There are few reports about the reversible control of ferromagnetism in spinel materials during lithium intercalation and deintercalation, and the explanation is mostly restricted to the change of chemical states[29,30,31,32,33] This suggests that further research needs to be conducted to explore whether there are other modulating mechanisms during the battery cycle. Based on the results obtained from a variety of complementary analytical tools that were used to probe the structural, electronic, and chemical changes, a modulation mechanism focused on the magnetic ions’ migration in the lattice and induced magnetic coupling evolution during the battery operation is proposed
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