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<p>Solid-state synthesis involves a web of coupled chemical reactions and physical changes that unfold across multiple scales. Efforts to fine-tune its parameters have historically followed heuristic, trial-driven workflows that demand significant time and resources. In this study, we aimed to open this black box by employing multiscale in situ synchrotron imaging and diffraction. Using LiNi<sub>0.5</sub>Mn<sub>0.3</sub>Co<sub>0.2</sub>O<sub>2</sub> battery positive electrode material as a model system and Ba-based sintering aids, we reveal dopant segregation, intergranular mass transport, and porosity evolution as key drivers of single-crystalline particle formation. Notably, we uncovered a dynamic competition between particle-level grain coalescence and atomic-scale cation disordering, both of which are thermally activated yet have opposing impacts on battery performance. These findings highlight the coupled, multiscale nature of structure development and offer a mechanistic basis for optimizing the solid-state synthesis process. This framework provides a path toward more controlled, efficient, and scalable production of high-performance battery positive electrode materials.</p>

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Revealing multiscale competing processes in the solid-state synthesis of single-crystalline layered oxide positive electrodes

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月15日

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  • Zhichen Xue,
  • Tianxiao Sun,
  • Sreevishnu Oruganti,
  • Xiaojing Huang,
  • Dilworth Y. Parkinson,
  • Yong S. Chu,
  • Piero Pianetta,
  • Mingyuan Ge,
  • Yijin Liu

摘要

Solid-state synthesis involves a web of coupled chemical reactions and physical changes that unfold across multiple scales. Efforts to fine-tune its parameters have historically followed heuristic, trial-driven workflows that demand significant time and resources. In this study, we aimed to open this black box by employing multiscale in situ synchrotron imaging and diffraction. Using LiNi0.5Mn0.3Co0.2O2 battery positive electrode material as a model system and Ba-based sintering aids, we reveal dopant segregation, intergranular mass transport, and porosity evolution as key drivers of single-crystalline particle formation. Notably, we uncovered a dynamic competition between particle-level grain coalescence and atomic-scale cation disordering, both of which are thermally activated yet have opposing impacts on battery performance. These findings highlight the coupled, multiscale nature of structure development and offer a mechanistic basis for optimizing the solid-state synthesis process. This framework provides a path toward more controlled, efficient, and scalable production of high-performance battery positive electrode materials.