Jee, Woongkyu;
Sokol, Alexey A;
Xu, Cyril;
Camino, Bruno;
Zhang, Xingfan;
Woodley, Scott M;
(2024)
Discharging of Ramsdellite MnO2 Cathode in a Lithium-Ion Battery.
Chemistry of Materials
10.1021/acs.chemmater.4c01417.
(In press).
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Abstract
We report an application of our unbiased Monte Carlo approach to investigate thermodynamic and electrochemical properties of lithiated manganese oxide in the ramsdellite phase (R-MnO2) to uncover the mechanism of lithium intercalation and understand charging/discharging of R-MnO2 as a cathode material in lithium-ion batteries. The lithium intercalation reaction was computationally explored by modeling thermodynamically significant distributions of lithium and reduced manganese in the R-MnO2 framework for a realistic range of lithium molar fractions 0 < x < 1 in LixMnO2. We employed interatomic potentials and analyzed the thermodynamics of the resultant grand canonical ensemble. We found ordered or semiordered phases at x = 0.5 and 1.0 in LixMnO2, verified by configurational entropy changes and simulated X-ray diffraction patterns of partially lithiated R-MnO2. The radial distribution functions show the preference of lithium for homogeneous distributions across the one-dimensional 2 × 1 ramsdellite channels accompanied by alternating reduced/oxidized manganese ions. The occupation of the interstitial sites in the channels is correlated with the calculated voltage profile, showing a sharp voltage drop at x = 0.5, which is explained by the energy penalty of shifting lithium ions from stable tetrahedral to unstable octahedral sites. To facilitate this work, our in-house software, Knowledge Led Master Code (KLMC) was extended to support massive parallelism on high-performance computers.
| Type: | Article |
|---|---|
| Title: | Discharging of Ramsdellite MnO2 Cathode in a Lithium-Ion Battery |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.chemmater.4c01417 |
| Publisher version: | http://dx.doi.org/10.1021/acs.chemmater.4c01417 |
| Language: | English |
| Additional information: | This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10196496 |
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