Understanding Solid-State Synthesis of Layered Oxide Cathodes by Operando Synchrotron Characterization

The chemical and structural transformations during solid-state synthesis are crucial for developing cost-effective, durable, and high-energy inorganic battery cathodes. However, the thermodynamic and mechanic origins and their effects on synthetic reactions are yet to be fully elucidated. In this work, using a manganese (Mn)-rich precursor specifically targeted for cost-effective cathodes, we decoupled the distinct contributions of thermodynamic parameters in the solid-state synthesis of P2-type Mn-rich layered oxide cathodes for sodium-ion batteries. By utilizing operando synchrotron X-ray diffraction, full field 3D transmission X-ray tomography, high-resolution transmission electron microscopy, and density functional theory calculations, we identified the key reaction pathways that governing the transformation during solid-state synthesis. These pathways ultimately affect the crystallite size, morphology, and electrochemical properties of the resultant layered oxide materials.

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