Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides
Citations Over TimeTop 1% of 2017 papers
Abstract
Lithium-rich layered transition metal oxide positive electrodes offer access to anion redox at high potentials, thereby promising high energy densities for lithium-ion batteries. However, anion redox is also associated with several unfavorable electrochemical properties, such as open-circuit voltage hysteresis. Here we reveal that in Li1.17-x Ni0.21Co0.08Mn0.54O2, these properties arise from a strong coupling between anion redox and cation migration. We combine various X-ray spectroscopic, microscopic, and structural probes to show that partially reversible transition metal migration decreases the potential of the bulk oxygen redox couple by > 1 V, leading to a reordering in the anionic and cationic redox potentials during cycling. First principles calculations show that this is due to the drastic change in the local oxygen coordination environments associated with the transition metal migration. We propose that this mechanism is involved in stabilizing the oxygen redox couple, which we observe spectroscopically to persist for 500 charge/discharge cycles.
Related Papers
- → Review on Anionic/Cationic Surfactant Mixtures(2007)299 cited
- → New sequential treatment for mature landfill leachate by cationic/anionic and anionic/cationic processes: Optimization and comparative study(2010)63 cited
- → A new metal–organic framework constructed from cationic nodes and cationic linkers for highly efficient anion exchange(2018)41 cited
- → Cationic Domino Reactions(2006)
- Influence of Gemini Cationic Surfactants for the Dyeing Property of Modified Polyester Fibers(2010)