Computational design and preparation of cation-disordered oxides for high-energy-density Li-ion batteries

Alexander Urban, Ian Matts, Aziz Abdellahi, Gerbrand Ceder*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

71 Citations (Scopus)


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.

Original languageEnglish
Article number1600488
JournalAdvanced Energy Materials
Issue number15
Early online date10 Aug 2016
Publication statusPublished - 10 Aug 2016


  • Cation disorder
  • Cluster expansion
  • DFT calculations
  • Lithium batteries
  • Transition-metal oxides


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