Visualizing nanoscale 3D compositional fluctuation of lithium in advanced lithium-ion battery cathodes

Devaraj, Arun; Gu, Meng; Colby, Robert J.; Yan, Pengfei; Wang, Chong M.; Zheng, Jianming; Xiao, Jie; Genc, Arda; Zhang, Jiguang; Belharouak, Ilias; Wang, Dapeng; Amine, Khalil; Thevuthasan, Suntharampillai

doi:10.1038/ncomms9014

Title: Visualizing nanoscale 3D compositional fluctuation of lithium in advanced lithium-ion battery cathodes

Journal Article · Fri Aug 14 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms9014· OSTI ID:1212997

Devaraj, Arun ^[1]; Gu, Meng ^[1]; Colby, Robert J. ^[1]; Yan, Pengfei ^[1]; Wang, Chong M. ^[1]; Zheng, Jianming ^[1]; Xiao, Jie ^[1]; Genc, Arda ^[2]; Zhang, Jiguang ^[1]; Belharouak, Ilias ^[3]; Wang, Dapeng ^[4]; Amine, Khalil ^[4]; Thevuthasan, Suntharampillai ^[5]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
FEI Company, Hillsboro, OR (United States)
Qatar Environment and Energy Research Institute, Doha (Qatar)
Argonne National Lab. (ANL), Argonne, IL (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Qatar Environment and Energy Research Institute, Doha (Qatar)

The distribution and concentration of lithium in Li-ion battery cathodes at different stages of cycling is a pivotal factor in determining battery performance. Non-uniform distribution of the transition metal cations has been shown to affect cathode performance; however, the Li is notoriously challenging to characterize with typical high-spatial-resolution imaging techniques. Here, for the first time, laser–assisted atom probe tomography is applied to two advanced Li-ion battery oxide cathode materials—layered Li_1.2Ni_0.2Mn_0.6O₂ and spinel LiNi_0.5Mn_1.5O₄—to unambiguously map the three dimensional (3D) distribution of Li at sub-nanometer spatial resolution and correlate it with the distribution of the transition metal cations (M) and the oxygen. The as-fabricated layered Li_1.2Ni_0.2Mn_0.6O₂ is shown to have Li-rich Li₂MO₃ phase regions and Li-depleted Li(Ni_0.5Mn_0.5)O₂ regions while in the cycled layered Li_1.2Ni_0.2Mn_0.6O₂ an overall loss of Li and presence of Ni rich regions, Mn rich regions and Li rich regions are shown in addition to providing the first direct evidence for Li loss on cycling of layered LNMO cathodes. The spinel LiNi_0.5Mn_1.5O₄ cathode is shown to have a uniform distribution of all cations. These results were additionally validated by correlating with energy dispersive spectroscopy mapping of these nanoparticles in a scanning transmission electron microscope. Thus, we have opened the door for probing the nanoscale compositional fluctuations in crucial Li-ion battery cathode materials at an unprecedented spatial resolution of sub-nanometer scale in 3D which can provide critical information for understanding capacity decay mechanisms in these advanced cathode materials.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; AC02-06CH11357

OSTI ID:: 1212997

Alternate ID(s):: OSTI ID: 1224906

Report Number(s):: PNNL-SA-111262; 48658

Journal Information:: Nature Communications, Vol. 6, Issue 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 97 works

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