Unravelling structural ambiguities in lithium- and manganese-rich transition metal oxides

Shukla, Alpesh Khushalchand; Ramasse, Quentin M.; Ophus, Colin; Duncan, Hugues; Hage, Fredrik; Chen, Guoying

doi:10.1038/ncomms9711

Title: Unravelling structural ambiguities in lithium- and manganese-rich transition metal oxides

Journal Article · Thu Oct 29 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms9711· OSTI ID:1256042

Shukla, Alpesh Khushalchand ^[1]; Ramasse, Quentin M. ^[2]; Ophus, Colin ^[1]; Duncan, Hugues ^[1]; Hage, Fredrik ^[2]; Chen, Guoying ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
SciTech Daresbury Campus, Daresbury (United Kingdom). SuperSTEM Laboratory

Although Li- and Mn-rich transition metal oxides have been extensively studied as high-capacity cathode materials for Li-ion batteries, the crystal structure of these materials in their pristine state is not yet fully understood. Here we apply complementary electron microscopy and spectroscopy techniques at multi-length scale on well-formed Li 1.2 (Ni 0.13 Mn 0.54 Co 0.13)O 2 crystals with two different morphologies as well as two commercially available materials with similar compositions, and unambiguously describe the structural make-up of these samples. Systematically observing the entire primary particles along multiple zone axes reveals that they are consistently made up of a single phase, save for rare localized defects and a thin surface layer on certain crystallographic facets. More specifically, we show the bulk of the oxides can be described as an aperiodic crystal consisting of randomly stacked domains that correspond to three variants of monoclinic structure, while the surface is composed of a Co- and/or Ni-rich spinel with antisite defects.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1256042

Alternate ID(s):: OSTI ID: 1378613

Journal Information:: Nature Communications, Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 158 works

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