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Title: Effect of composition on the structure of lithium- and manganese-rich transition metal oxides

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. In this, 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.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [2] ;  [2] ;  [4] ;  [5] ;  [5] ;  [5]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy, The Molecular Foundry and Energy Storage and Distributed Resources Division; SuperSTEM, Daresbury (United Kingdom)
  2. SuperSTEM, Daresbury (United Kingdom)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Center for Electron Microscopy and Molecular Foundry
  4. Austrian Academy of Sciences, Leoben (Austria). Erich Schmid Inst. of Materials Science
  5. Envia Systems, Newark, NY (United States)
Publication Date:
Grant/Contract Number:
AC02-05CH11231; EE0006443
Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 11; Journal Issue: 4; Related Information: © 2018 The Royal Society of Chemistry.; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); Engineering and Physical Science Research Council (EFRC)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1465456