Origin of voltage decay in high-capacity layered oxide electrodes.
By M. Sathiya, A. Abakumov, Dominique Foix, G. Rousse, K. Ramesha, Matthieu Saubanère, M. Doublet, H. Vezin, C. P. Laisa, A. S. Prakash and 3 more. Nature Materials, 2015
815 citations recorded by the source corpus.
Although Li-rich layered oxides (Li1+xNiyCozMn1-x-y-zO2 > 250 mAh g(-1)) are attractive electrode materials providing energy densities more than 15% higher than today's commercial Li-ion cells, they suffer from voltage decay on cycling. To elucidate the origin of this phenomenon, we employ chemical substitution in structurally related Li2RuO3 compounds. Li-rich layered Li2Ru1-yTiyO3 phases with capacities of ~240 mAh g(-1) exhibit the characteristic voltage decay on cycling. A combination of transmission electron microscopy and X-ray photoelectron spectroscopy studies reveals that the migration of cations between metal layers and Li layers is an intrinsic feature of the charge-discharge process that increases the trapping of metal ions in interstitial tetrahedral sites. A correlation between these trapped ions and the voltage decay is established by expanding the study to both Li2Ru1-ySnyO3 and Li2RuO3; the slowest decay occurs for the cations with the largest ionic radii. This effect is robust, and the finding provides insights into new chemistry to be explored for developing high-capacity layered electrodes that evade voltage decay.
Subfields: Electrical and Electronic Engineering, Electronic, Optical and Magnetic Materials
View Paper: https://www.semanticscholar.org/paper/b8b46b0c7b44800e8296f22abff98f9dfac3848b
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Citations in the corpus
- Li-Rich Layered Oxides and Their Practical Challenges: Recent Progress and Perspectives (2019, result): “Moreover, recent studies have also shown that there is a close coupling between TM migration and the anion redox reactions of O [27, 97, 181, 185, 186] and this was further supported by first-principles calculations (Fig.”
- Voltage Decay in Layered Li-Rich Mn-Based Cathode Materials (2019, background): “[36] also addressed the importance of ionic radii on ion migration based on Ti4+ migration and purposed that ion migration can be suppressed through doping with larger and more electroactive ions such as Nb and Mo.”