(Battery Division Early Career Award Sponsored by Neware Technology Limited) Spin Probes and Materials Design for Next-Generation Batteries
Authors: Nguyen Howie , Sebti Elias , Richardson Peter , Giovine Raynald , Clement Raphaele J 
Published: December 2024

While batteries have become ubiquitous in our daily lives, rapid growth in demand requires the development of higher energy density devices, and lower cost and more sustainable battery chemistries. When it comes to Li-ion batteries, despite significant research efforts over decades, we continue to rely on a limited subset of cathode materials that derive from LiCoO2 developed in 1980. The main bottleneck to advancing cathodes is the exceptional complexity of charge-discharge processes. This is compounded by the dearth of experimental techniques capable of bridging atomic-level phenomena and electrode-level performance. In the first part of this talk, I will present our work combining advanced ex situ and operando characterization and first principles calculations to better understand the working principles and sources of irreversibility in LiNiO2. [1, 2] The second part of this talk will focus on alternatives to the current Li-ion technology, including Na-based and solid-state batteries. In particular, solid electrolyte development has been hampered by the difficulty to identify materials that are chemically and electrochemically stable during normal battery operation, while also exhibiting a high ionic conductivity. I will present our recent work investigating chloride-based solid electrolytes for Li- and Na-based solid-state devices. [3-6] A common theme throughout is the combined use of solid-state NMR, magnetometry, X-ray diffraction, and first principles calculations to better understand the links between synthesis, composition/structure and electrochemical properties.
[1] Nguyen, H., Kurzhals, P., Bianchini, M., Seidel, K., Clément, R., “New insights into aging in LiNiO2 cathodes from high resolution paramagnetic NMR spectroscopy”, ChemComm, 60(35), 4707-4710 (2024).
[2] Nguyen, H., Silverstein, R., Zaveri, A., Cui, W., Kurzhals, P., Sicolo, S., Bianchini, M., Seidel, K., Clément, R., “Twin Boundaries Contribute to The First Cycle Irreversibility of LiNiO2”, Adv. Funct. Mater., 2306168 (2023).
[3] Sebti, E., Evans, H., Chen, H., Richardson, P., White, K., Giovine, R., Koirala, K., Xu, Y., Gonzalez-Correa, E., Wang, C., Brown, C., Cheetham, A., Canepa, P., Clément, R., "Stacking Faults Assist Lithium-Ion Conduction in a Halide-Based Superionic Conductor", J. Am. Chem. Soc., 144, 5795 (2022).
[4] Wu, E., Banerjee, S., Tang, H., Richardson, P., Doux, J.-M., Qi, J., Zhu, Z., Grenier, A., Li, Y., Zhao, E., Deysher, G., Sebti, E., Nguyen, H., Stephens, R., Verbist, G., Chapman, K., Clément, R., Banerjee, A., Meng, Y. S., Ong, S. P., "A Stable Cathode-Solid Electrolyte Composite for High-Voltage, Long-Cycle-Life Solid-State Sodium-Ion Batteries", Nat. Commun., 12(1), 1256 (2021).
[5] Sebti, E., Qi, J., Richardson, P., Ridley, P., Wu, E., Banerjee, S., Giovine, R., Cronk, A., Ham, S.-Y., Meng, Y. S., Ong, S. P., Clément, R., “Synthetic control of structure and conduction properties in Na-Y-Zr-Cl solid electrolytes“, J. Mater. Chem. A, 10 (40), 21565-21578 (2022).
[6] Ridley, P., Nguyen, L. H. B., Sebti, E., Duong, G., Chen, Y.-T., Sayahpour, B., Cronk, A., Deysher, G., Ham, S.-Y., Oh, J. A. S., Wu, E., Tan, D., Doux, J.-M., Clément, R., Jang, J., Meng, Y. S., “Amorphous and Nanocrystalline Halide Solid Electrolytes with Enhanced Sodium-ion Conductivity”, Matter, 7(2), 485-499 (2024).