- Hau, Han-Ming;
- Mishra, Tara;
- Ophus, Colin;
- Huang, Tzu-Yang;
- Bustilo, Karen;
- Sun, Yingzhi;
- Yang, Xiaochen;
- Holstun, Tucker;
- Zhao, Xinye;
- Wang, Shilong;
- Ha, Yang;
- Lee, Gihyeok;
- Song, Chengyu;
- Turner, John;
- Bai, Jianming;
- Ma, Lu;
- Chen, Ke;
- Wang, Feng;
- Yang, Wanli;
- Mccloskey, Bryan;
- Cai, Zijian;
- Ceder, Gerbrand
Manganese-based materials have tremendous potential to become the next-generation lithium-ion cathode as they are Earth abundant, low cost and stable. Here we show how the mobility of manganese cations can be used to obtain a unique nanosized microstructure in large-particle-sized cathode materials with enhanced electrochemical properties. By combining atomic-resolution scanning transmission electron microscopy, four-dimensional scanning electron nanodiffraction and in situ X-ray diffraction, we show that when a partially delithiated, high-manganese-content, disordered rocksalt cathode is slightly heated, it forms a nanomosaic of partially ordered spinel domains of 3-7 nm in size, which impinge on each other at antiphase boundaries. The short coherence length of these domains removes the detrimental two-phase lithiation reaction present near 3 V in a regular spinel and turns it into a solid solution. This nanodomain structure enables good rate performance and delivers 200 mAh g-1 discharge capacity in a (partially) disordered material with an average primary particle size of ∼5 µm. The work not only expands the synthesis strategies available for developing high-performance Earth-abundant manganese-based cathodes but also offers structural insights into the ability to nanoengineer spinel-like phases.