Shukla, A. K., Ramasse, Q. M., Ophus, C., Kepaptsoglou, D. M., Hage, F. S., Gammer, C., Bowling, C., Gallegos, P. A. H. and Venkatachalam, S. (2018) Effect of composition on the structure of lithium- and manganese-rich transition metal oxides. Energy and Environmental Science, 11(4), pp. 830-840. (doi: 10.1039/C7EE02443F)
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Abstract
The choice of chemical composition of lithium- and manganese-rich transition metal oxides used as cathode materials in lithium-ion batteries can significantly impact their long-term viability as storage solutions for clean energy automotive applications. Their structure has been widely debated: conflicting conclusions drawn from individual studies often considering different compositions have made it challenging to reach a consensus and inform future research. Here, complementary electron microscopy techniques over a wide range of length scales reveal the effect of lithium-to-transition metal-ratio on the surface and bulk structure of these materials. We found that decreasing the lithium-to-transition metal-ratio resulted in a significant change in terms of order and atomic-level local composition in the bulk of these cathode materials. However, throughout the composition range studied, the materials consisted solely of a monoclinic phase, with lower lithium content materials showing more chemical ordering defects. In contrast, the spinel-structured surface present on specific crystallographic facets exhibited no noticeable structural change when varying the ratio of lithium to transition metal. The structural observations from this study warrant a reexamination of commonly assumed models linking poor electrochemical performance with bulk and surface structure.
| Item Type: | Articles |
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| Additional Information: | This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy under Contract No. DE-EE0006443 under the Applied Battery Research (ABR) program. We also acknowledge financial support f rom Envia Systems and US Depart- ment of Energy’s Small Business Voucher Pilot program. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The authors also acknowledge support SuperSTEM, Daresbury, UK, which is the National Facility for Aberration-Corrected Scanning Transmission Electron Microscopy, supported by the Engineering and Physical Science Research Council. |
| Status: | Published |
| Refereed: | Yes |
| Glasgow Author(s) Enlighten ID: | Hage, Dr Fredrik Sydow |
| Authors: | Shukla, A. K., Ramasse, Q. M., Ophus, C., Kepaptsoglou, D. M., Hage, F. S., Gammer, C., Bowling, C., Gallegos, P. A. H., and Venkatachalam, S. |
| College/School: | College of Science and Engineering > School of Physics and Astronomy |
| Journal Name: | Energy and Environmental Science |
| Publisher: | Royal Society of Chemistry |
| ISSN: | 1754-5692 |
| ISSN (Online): | 1754-5706 |
| Published Online: | 10 January 2018 |
| Copyright Holders: | Copyright © 2018 The Authors |
| First Published: | First published in Energy and Environmental Science 11(4):830-840 |
| Publisher Policy: | Reproduced under a Creative Commons License |
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