Computational Design and Preparation of Cation‐Disordered Oxides for High‐Energy‐Density Li‐Ion Batteries |
| |
| Authors: | Alexander Urban Ian Matts Aziz Abdellahi Gerbrand Ceder |
| |
| Affiliation: | 1. Department of Materials Science and Engineering, University of California, Berkeley, CA, USA;2. Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA;3. Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA |
| |
| Abstract: | Cation‐disordered lithium‐excess metal oxides have recently emerged as a promising new class of high‐energy‐density cathode materials for Li‐ion batteries, but the exploration of disordered materials has been hampered by their vast and unexplored composition space. This study proposes a practical methodology for the identification of stable cation‐disordered rocksalts. Here, it is established that the efficient method, which makes use of special quasirandom structures, correctly predicts cation‐ordering strengths in agreement with accurate Monte‐Carlo simulations and experimental observations. By applying the approach to the composition space of ternary oxides with formula unit LiA0.5B0.5O2 (A, B: transition metals), this study discovers a previously unknown cation‐disordered structure, LiCo0.5Zr0.5O2, that may function as the basis for a new class of cation‐disordered cathode materials. This computational prediction is confirmed experimentally by solid‐state synthesis and subsequent characterization by powder X‐ray diffraction demonstrating the potential of the computational screening of large composition spaces for accelerating materials discovery. |
| |
| Keywords: | lithium batteries cation disorder cluster expansion DFT calculations transition‐metal oxides |
|
|
