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Title: Single-crystal based studies for correlating the properties and high-voltage performance of Li[NixMnyCo1₋x₋y]O2 cathodes

Journal Article · · Journal of Materials Chemistry. A
DOI: https://doi.org/10.1039/c8ta10329a · OSTI ID:1515780
 [1]; ORCiD logo [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
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Safe and stable cycling of lithium-ion battery cathodes at high voltages is essential for meeting next-generation energy storage demands, yet the lack of fundamental understanding of the correlation of a material's properties and reactivities largely hinders current progress. Here, we demonstrate how single-crystal samples with well-controlled physical characteristics can be used to unambiguously establish the relationships among specific properties, surface chemistry and electrochemical performance, enabling rational design of better performing cathode materials. Layered Li[NixMnyCo1₋x₋y]O2 (NMC) crystals, with four different particle shapes of an octahedron (Oct), truncated octahedron (T-Oct), polyhedron (Poly) and platelet (Plate), were prepared to vary the presence of (104), (001) and (012) family facets on the surface. This represents the first experimental verification of NMC morphologies that were theoretically calculated in the past. Systematic studies on the impact of isolated physical properties reveal the important roles of the Ni content, particle size and facet on surface stability and electrochemical performance. We show that compared to (012) surface dominated samples, high-voltage cycling stability was much improved on the (001) dominated Plate sample, suggesting that replacing the (012) surface with lower energy (001) and/or (104) surfaces can be effective in stabilizing NMCs during high energy applications. Our study moreover provides insights into how tailoring a material's surface properties can be used as an important route in balancing cathode capacity and stability.

Research Organization:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Organization:
Argonne National Lab. (ANL), Lemont, IL (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515
OSTI ID:
1515780
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 10 Vol. 7; ISSN JMCAET; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (2)

Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies journal December 2019
Oriented porous LLZO 3D structures obtained by freeze casting for battery applications journal January 2019

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