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Title: Correlated X-Ray 3D Ptychography and Diffraction Microscopy Visualize Links between Morphology and Crystal Structure of Lithium-Rich Cathode Materials

Abstract

The search for higher performance, improved safety, and lifetime of lithium-ion batteries relies on the understanding of degradation mechanisms. Complementary to methods and studies on primary particles or crystalline structure on bulk materials, here we use spatially correlated ptychographic X-ray computed nanotomography with a 35 nm resolution and scanning X-ray diffraction microscopy with 1 μm resolution to visualize in 3D the hidden morphological and structural degradation processes in individual secondary particles of lithium-rich nickel, cobalt, and manganese oxides. From comparative examination of pristine and cycled particles, we suggest that morphological degradation could have radial dependency and secondary particle size dependency. The same particles were examined to correlate the degradation to crystallinity, which shows surprising core-shell structures. As a result, this study reveals the inner 3D structure of the secondary particles while opening up questions on the unexpected crystalline structural distributions, which could offer clues for future studies on this promising cathode material for lithium-ion batteries.

Authors:
ORCiD logo; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1547905
Alternate Identifier(s):
OSTI ID: 1495004
Report Number(s):
BNL-211267-2019-JAAM
Journal ID: ISSN 2589-0042; S258900421830258X; PII: S258900421830258X
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Published Article
Journal Name:
iScience
Additional Journal Information:
Journal Name: iScience Journal Volume: 11 Journal Issue: C; Journal ID: ISSN 2589-0042
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English
Subject:
25 ENERGY STORAGE; lithium-ion battery; X-ray microscopy; tomography

Citation Formats

Tsai, Esther H. R., Billaud, Juliette, Sanchez, Dario F., Ihli, Johannes, Odstrčil, Michal, Holler, Mirko, Grolimund, Daniel, Villevieille, Claire, and Guizar-Sicairos, Manuel. Correlated X-Ray 3D Ptychography and Diffraction Microscopy Visualize Links between Morphology and Crystal Structure of Lithium-Rich Cathode Materials. Netherlands: N. p., 2019. Web. doi:10.1016/j.isci.2018.12.028.
Tsai, Esther H. R., Billaud, Juliette, Sanchez, Dario F., Ihli, Johannes, Odstrčil, Michal, Holler, Mirko, Grolimund, Daniel, Villevieille, Claire, & Guizar-Sicairos, Manuel. Correlated X-Ray 3D Ptychography and Diffraction Microscopy Visualize Links between Morphology and Crystal Structure of Lithium-Rich Cathode Materials. Netherlands. doi:10.1016/j.isci.2018.12.028.
Tsai, Esther H. R., Billaud, Juliette, Sanchez, Dario F., Ihli, Johannes, Odstrčil, Michal, Holler, Mirko, Grolimund, Daniel, Villevieille, Claire, and Guizar-Sicairos, Manuel. Tue . "Correlated X-Ray 3D Ptychography and Diffraction Microscopy Visualize Links between Morphology and Crystal Structure of Lithium-Rich Cathode Materials". Netherlands. doi:10.1016/j.isci.2018.12.028.
@article{osti_1547905,
title = {Correlated X-Ray 3D Ptychography and Diffraction Microscopy Visualize Links between Morphology and Crystal Structure of Lithium-Rich Cathode Materials},
author = {Tsai, Esther H. R. and Billaud, Juliette and Sanchez, Dario F. and Ihli, Johannes and Odstrčil, Michal and Holler, Mirko and Grolimund, Daniel and Villevieille, Claire and Guizar-Sicairos, Manuel},
abstractNote = {The search for higher performance, improved safety, and lifetime of lithium-ion batteries relies on the understanding of degradation mechanisms. Complementary to methods and studies on primary particles or crystalline structure on bulk materials, here we use spatially correlated ptychographic X-ray computed nanotomography with a 35 nm resolution and scanning X-ray diffraction microscopy with 1 μm resolution to visualize in 3D the hidden morphological and structural degradation processes in individual secondary particles of lithium-rich nickel, cobalt, and manganese oxides. From comparative examination of pristine and cycled particles, we suggest that morphological degradation could have radial dependency and secondary particle size dependency. The same particles were examined to correlate the degradation to crystallinity, which shows surprising core-shell structures. As a result, this study reveals the inner 3D structure of the secondary particles while opening up questions on the unexpected crystalline structural distributions, which could offer clues for future studies on this promising cathode material for lithium-ion batteries.},
doi = {10.1016/j.isci.2018.12.028},
journal = {iScience},
issn = {2589-0042},
number = C,
volume = 11,
place = {Netherlands},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1016/j.isci.2018.12.028

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Surface geometry and electrochemical performance of Li-rich NMC. (AC) Scanning electron micrographs of (A) pristine NMC particles, (B) after first delithiation, and (C) after long-term cycling. Primary particles consist of 50- to 100-nm grains that aggregate to form the secondary particles with diameters of around 5 to 20more » µm. A crack on the surface is highlighted in yellow in (B), although the spatial extent of the crack is unknown. Onion-like layered structures are observed from broken particles in (C). (D) The evolution of the specific charge upon cycling at C/10 after the first cycle activation at C/20. The dashed line gives the specific charge obtained after the first cycle. See also Figure S1 for the first cycle activation« less

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