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Title: Revealing Anisotropic Spinel Formation on Pristine Li- and Mn-Rich Layered Oxide Surface and Its Impact on Cathode Performance

Journal Article · · Advanced Energy Materials
 [1];  [1];  [1];  [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
+ Show Author Affiliations

Surface properties of cathode particles play important roles in the transport of ions and electrons and they may ultimately dominate cathode's performance and stability in lithium-ion batteries. Through the use of carefully prepared Li1.2Ni0.13Mn0.54Co0.13O2crystal samples with six distinct morphologies, surface transition-metal redox activities and crystal structural transformation are investigated as a function of surface area and surface crystalline orientation. Complementary depth-profiled core-level spectroscopy, namely, X-ray absorption spectroscopy, electron energy loss spectroscopy, and atomic-resolution scanning transmission electron microscopy, are applied in the study, presenting a fine example of combining advanced diagnostic techniques with a well-defined model system of battery materials. The present study reports the following findings: (1) a thin layer of defective spinel with reduced transition metals, similar to what is reported on cycled conventional secondary particles in the literature, is found on pristine oxide surface even before cycling, and (2) surface crystal structure and chemical composition of both pristine and cycled particles are facet dependent. Oxide structural and cycling stabilities improve with maximum expression of surface facets stable against transition-metal reduction. The intricate relationships among morphology, surface reactivity and structural transformation, electrochemical performance, and stability of the cathode materials are revealed.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
OSTI ID:
1369400
Alternate ID(s):
OSTI ID: 1400810; OSTI ID: 1458496
Journal Information:
Advanced Energy Materials, Vol. 7, Issue 11; ISSN 1614-6832
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 46 works
Citation information provided by
Web of Science

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Cited By (8)

Enhanced structural stability and overall conductivity of Li-rich layered oxide materials achieved by a dual electron/lithium-conducting coating strategy for high-performance lithium-ion batteries journal January 2019
Surface and Subsurface Reactions of Lithium Transition Metal Oxide Cathode Materials: An Overview of the Fundamental Origins and Remedying Approaches journal September 2018
Cracks Formation in Lithium-Rich Cathode Materials for Lithium-Ion Batteries during the Electrochemical Process journal October 2018
Defects in Li 4 Ti 5 O 12 induced by carbon deposition: an analysis of unidentified bands in Raman spectra journal January 2019
Spinel/Lithium‐Rich Manganese Oxide Hybrid Nanofibers as Cathode Materials for Rechargeable Lithium‐Ion Batteries journal August 2019
Injection of oxygen vacancies in the bulk lattice of layered cathodes journal April 2019
Effect of composition on the structure of lithium- and manganese-rich transition metal oxides journal January 2018
High-discharge-voltage lithium-rich layered-oxide cathode materials based on low oxygen vacancy journal January 2019

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