1. To advanced high capacity layered electrode materials for lithium-ion batteries through the understanding of oxidation-reduction processes at the atomic level.

The project is aimed at solving the urgent problem of creating high-capacity secondary electrochemical current sources of the next generation with cathodes based on Li-enriched transition metal oxides. But they have a number of disadvantages, which creates obstacles to their practical use. To solve this problem, the project proposes a combined approach, including modern methods of preparative chemistry, advanced characterization methods and computer modeling within the framework of density functional theory

The project was funded by Russian Science Foundation Project No. 20-43-01012 FWO. https://www.rscf.ru/project/20-43-01012/

Publications:

1) Abakumov, A. M., Fedotov, S. S., Antipov, E. V., & Tarascon, J. M. (2020). Solid state chemistry for developing better metal-ion batteries. Nature Communications, 11(1), 4976. https://doi.org/10.1038/s41467-020-18736-7 

2) Morozov, A. V., Moiseev, I. A., Savina, A. A., Boev, A. O., Aksyonov, D. A., Zhang, L., ... & Abakumov, A. M. (2022). Retardation of structure densification by increasing covalency in Li-rich layered oxide positive electrodes for Li-ion batteries. Chemistry of Materials, 34(15), 6779-6791.  https://doi.org/10.1021/acs.chemmater.2c00921

3) Abakumov, A. M., Li, C., Boev, A., Aksyonov, D. A., Savina, A. A., Abakumova, T. A., ... & Bals, S. (2021). Grain Boundaries as a Diffusion-Limiting Factor in Lithium-Rich NMC Cathodes for High-Energy Lithium-Ion Batteries. ACS Applied Energy Materials, 4(7), 6777-6786. https://doi.org/10.1021/acsaem.1c00872

4) Savina, A. A., Saiutina, V. V., Morozov, A. V., Boev, A. O., Aksyonov, D. A., Dejoie, C., ... & Abakumov, A. M. (2022). Chemistry, Local Molybdenum Clustering, and Electrochemistry in the Li2+ x Mo1–x O3 Solid Solutions. Inorganic Chemistry, 61(14), 5637-5652. https://doi.org/10.1021/acs.inorgchem.2c00420

2. Atomic-level Understanding of Interface Structure Evolution and Engineering Guidelines for Next Li-ion Solid State Batteries

We explored the correlation of interface structure with Li-ion transport across the interface and phase stability. We studied the effect of introducing barrier layers at the cathode interface to the Li-transport and phase stability. We also studied the Li dendrites growth at the Li-metal anode interface.

The work was a part of The Skoltech – MIT Joint Next Generation Program (NGP).

https://www.skoltech.ru/research/en/opportunities-partnerships/next-generation-skoltech-mit-partnership-program/

Publications:

1) Morozov, A. V., Paik, H., Boev, A. O., Aksyonov, D. A., Lipovskikh, S. A., Stevenson, K. J., ... & Abakumov, A. M. (2022). Thermodynamics as a Driving Factor of LiCoO2 Grain Growth on Nanocrystalline Ta-LLZO Thin Films for All-Solid-State Batteries. ACS Applied Materials & Interfaces, 14(35), 39907-39916. https://doi.org/10.1021/acsami.2c07176

3. Search for new materials for gas electrodes of lithium- and sodium-oxygen current sources: predictive computer simulation and experimental testing

Using density functional theory we performed high-throughput screening of cathode material depending on their stability, band gap, surface energies and resistance towards oxidation and passivation and found out a row of potential compounds.

The project was funded by Russian Science Foundation Project No. 19-73-00321 https://www.rscf.ru/project/19-73-00321/

Publications:

1) Boev, A. O., Fedotov, S. S., Stevenson, K. J., & Aksyonov, D. A. (2021). High-throughput computational screening of cathode materials for Li-O2 battery. Computational Materials Science, 197, 110592. https://doi.org/10.1016/j.commatsci.2021.110592

Computational Materials Group (CMG) lead by Prof. D. Aksyonov is developing new electrode materials for metal-ion batteries using computational methods. The supreme ingredient of success is a deep understanding of the material’ properties on the atomic and electronic level, which can be achieved with modeling. 

Main directions:

1. Computational design of solid/solid and solid/liquid interfaces for metal-ion batteries (Applied Surface Science 537 (2021) 147750)
2. Advanced study of defects in electrodes for metal-ion batteries (Inorg. Chem. 2021, 60, 5497−5506)
3. Understanding cation migration barriers in oxide and phosphate based cathode materials with DFT calculations (Computational Materials Science 154 (2018) 449–458)
4. Development of computational framework SIMAN for high-throughput DFT calculations (https://github.com/dimonaks/siman)

Current projects:

1. Development of advanced electrochemical energy storage systems with the help of directional design of local structure and microstructure of electrode materials.

2. Effect of the electrode/electrolyte interface structure on the charge transfer kinetics: сomputer simulation and experimental verification

Finished projects:

1. To advanced high capacity layered electrode materials for lithium-ion batteries through the understanding of oxidation-reduction processes at the atomic level
2. Atomic-level Understanding of Interface Structure Evolution and Engineering Guidelines for Next Li-ion Solid State Batteries
3. Search for new materials for gas electrodes of lithium- and sodium-oxygen current sources: predictive computer simulation and experimental testing

Figure 1. Easier formation of surface antisite defect in layered oxides discovered with DFT+U oxides. From Applied Surface Science 537 (2021) 147750

Figure 2. Combined DFT + X-Ray + Neutron diffraction refined hydrogen defects in LiFePO₄ cathode material. From Inorg. Chem. 2021, 60, 5497−5506

Figure 3. Li diffusion pathways for three classes of crystal structures: (a) spinel, (b) olivine, and (c) tavorite. From Computational Materials Science 154 (2018) 449–458

Figure 4. Change of charge density in Na₂FePO₄ after extraction of sodium (black spheres). From J. Am. Chem. Soc. 2018, 140, 3994−4003.