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Synthetic pathway determines the nonequilibrium crystallography of Li- and Mn-rich layered oxide cathode materials

DOI: 10.1021/acsaem.0c03027 DOI Help

Authors: Ashok S. Menon (Uppsala University) , Seda Ulusoy (Uppsala University) , Dickson O. Ojwang (Uppsala University) , Lars Riekehr (Uppsala University) , Christophe Didier (University of New South Wales) , Vanessa K. Peterson (Australian Centre for Neutron Scattering, Australian Nuclear Science and Technology Organization; University of Wollongong) , German Salazar-Alvarez (Uppsala University) , Peter Svedlindh (Uppsala University) , Kristina Edström (Uppsala University) , Cesar Pay Gomez (Uppsala University) , William R. Brant (Uppsala University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Applied Energy Materials

State: Published (Approved)
Published: February 2021
Diamond Proposal Number(s): 21804

Open Access Open Access

Abstract: 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.

Journal Keywords: Li- and Mn-rich layered oxides; Li-ion battery cathodes; synthesis−structure relationships; anionic redox materials; stacking

Diamond Keywords: Batteries; Lithium-ion

Subject Areas: Materials, Chemistry, Energy

Instruments: I11-High Resolution Powder Diffraction

Other Facilities: Australian Synchrotron


Discipline Tags:

Inorganic Chemistry Physical Chemistry Energy Energy Storage Material Sciences Energy Materials Chemistry

Technical Tags:

Diffraction X-ray Powder Diffraction