Abstract
The redox process in a lithium-ion battery occurs when a conduction electron from the lithium anode is transferred to the redox orbital of the cathode. Understanding the nature of orbitals involved in anionic as well as cationic redox reactions is important for improving the capacity and energy density of Li-ion batteries. In this connection, we have obtained magnetic Compton profiles (MCPs) from the Li-rich cation-disordered rock-salt compound LixTi0.4Mn0.4O2 (LTMO). The MCPs, which involved the scattering of circularly polarized hard X-rays, are given by the momentum density of all the unpaired spins in the material. The net magnetic moment in the ground state can be extracted from the area under the MCP, along with a SQUID measurement. Our analysis gives insight into the role of Mn 3d magnetic electrons and O 2p holes in the magnetic redox properties of LTMO.
Highlights
IntroductionThe high capacity of the Li-rich cathode materials has been suggested to result from a combination of cationic and anionic redox processes [2], a fundamental understanding of the redox mechanism at play in Li-rich cathode materials is needed for optimizing their performance
These results can be compared to the spin magnetic moment extracted from the magnetic Compton profile using the sum rule: Z ∞
We show that magnetic Compton scattering spectra measured under a magnetic field of 2.5 T allow access to the momentum density of unpaired spins of disordered lithium-rich cathode material Lix Ti0.4 Mn0.4 O2 (LTMO) over a wide range of lithium concentrations x
Summary
The high capacity of the Li-rich cathode materials has been suggested to result from a combination of cationic and anionic redox processes [2], a fundamental understanding of the redox mechanism at play in Li-rich cathode materials is needed for optimizing their performance
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