A High-Throughput Search for Functional Cathode Coatings for Lithium-Ion Batteries By First-Principles Thermodynamics
In the current framework, we consider three main thermodynamic criteria to assess the effectiveness of a compound AaBbCc…O1/2 as a coating. First criterion is the thermodynamic stability of the candidate material. We evaluate this criterion by finding whether the material is stable against decomposition to other phases in its chemical space A-B-C-…-O. The second criterion is the electrochemical stability. This criterion tests whether the material is stable against reduction and oxidation during cycling. The third criterion is the HF-scavenging tendency. We evaluate this criterion for systems where an HF-scavenging functionality is preferred, by identifying the HF-scavenging reactions and free energies. In addition, we take into account the effect of different cathode-electrolyte chemistries on these three criteria, namely, presence of common cathode materials (LiCoO2, LiMn2O4, etc.), as well as presence of HF-free or HF-bearing electrolytes.
Utilizing the HT-coating design framework described above, we screen more than ~100,000 oxide materials available in the Open Quantum Materials Database (OQMD) to find coating materials with different target properties. We suggest promising multi-component oxide cathode coatings that can prolong the cycle-lives of LIBs, and surpass the effectiveness of common coatings used such as Al2O3, MgO and ZrO2.
This work has been supported by The Dow Chemical Company.
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