4.7 Article

Synthetic Pathway Determines the Nonequilibrium Crystallography of Li- and Mn-Rich Layered Oxide Cathode Materials

Journal

ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 2, Pages 1924-1935

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.0c03027

Keywords

Li- and Mn-rich layered oxides; Li-ion battery cathodes; synthesis-structure relationships; anionic redox materials; stacking faulted materials

Funding

  1. Swedish Foundation for Strategic Research (SSF) within the Swedish national graduate school in neutron scattering (SwedNess)
  2. Strategic Research Area StandUp for Energy
  3. Swedish Energy Agency
  4. Swedish research council, VR [349-2014-3946, 2016-06959]
  5. Swedish Research Council [2016-06959] Funding Source: Swedish Research Council

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Li- and Mn-rich layered oxides hold promise as electrode materials for future Li-ion batteries, but their crystallography remains inaccurately described, with the synthetic route having a direct impact on the crystal structure. Clarifying structural ambiguities is crucial for understanding electrochemical performance and anionic redox behavior.
Li- and Mn-rich layered oxides show significant promise as electrode materials for future Li-ion batteries. However, an accurate description of its crystallography remains elusive, with both single-phase solid solution and multiphase structures being proposed for high performing materials such as Li1.2Mn0.54Ni0.13Co0.13O2. Herein, we report the synthesis of single- and multiphase variants of this material through sol-gel and solid-state methods, respectively, and demonstrate that its crystallography is a direct consequence of the synthetic route and not necessarily an inherent property of the composition, as previously argued. This was accomplished via complementary techniques that probe the bulk and local structure followed by in situ methods to map the synthetic progression. As the electrochemical performance and anionic redox behavior are often rationalized on the basis of the presumed crystal structure, clarifying the structural ambiguities is an important step toward harnessing its potential as an electrode material.

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