Advancing MR Methods to Track Processes in Battery Electrodes | Prof. Raphaële Clément | Session 109

During the 109th session of the Global NMR Discussion Meetings held on October 28th, 2025, via Zoom, Prof. Raphaële Clément from the University of California, Santa Barbara, USA, gave a talk on the topic "Advancing Magnetic (Resonance) Methods to Track Processes in Paramagnetic Battery Electrodes". The recording serves as a tutorial. Find out more about Prof. Raphaële Clément's research : https://clement.materials.ucsb.edu Abstract: Solid-state NMR has become an indispensable tool for quantifying defects and tracking the nature and reversibility of local structure changes in battery electrode materials during charge and discharge. Yet, probing paramagnetically concentrated systems with NMR remains extremely challenging. Achieving sufficient spectral resolution requires low magnetic fields and ultrafast spinning—conditions that are currently incompatible with real-time operando studies. At the same time, improved theoretical methodologies for predicting paramagnetic NMR shifts are needed to unravel the complexity of spectra acquired at different stages of cycling. In this talk, I will first present our development of operando magnetometry and EPR approaches that complement high-resolution ex situ solid-state NMR, offering new insights into the interplay between cation disorder and redox processes in LixNi1-yMnyO2 cathodes.1,2 In the second part, I will introduce an ab initio cluster expansion Monte Carlo framework for computing finite-temperature Fermi contact shifts with significantly improved accuracy compared to methods to date.3,4 Together, these developments move us closer to fully exploiting magnetic resonance for tracking battery processes in action. [1] Nguyen, H., Bassey, E., Foley, E., Kitchaev, D., Giovine, R., Clément, R., J. Magn. Reson., 2024, 368, 107772. [2] Nguyen, H., Zaveri, A., Cui, W., Silverstein, R., Kurzhals, P., Sicolo, S., Bianchini, M., Seidel, K., Clément, R., 2023, Adv. Funct. Mater., 2306168. [3] Garcia Ponte, G., Behara, S., Bassey, E., Clément, R., Van der Ven, A., Chem. Mater. 2025, 37, 5, 1835–1846. [4] Bassey, E., Sebti, E., Van der Ven, A., Clément, R., in preparation. Content of this video : 00:00 - 01:58 Introduction 01:59 - 22:31 Background 22:32 - 26:34 Operando EPR cell designs 26:35 - 34:09 Ex situ NMR and operando EPR for LiNiO2 cathode studies 34:10 - 39:16 Ex situ NMR and operando EPR for Ni redox processes study 39:17 - 55:33 Advancing computational predictions of MR properties of paraM materials 55:34 - 01:03:25 Q&A Current organizers: Adrian Draney (Creighton Uni.) Amrit Venkatesh (University of Virginia) Asif Equbal (New York Uni., Abu Dhabi) Charlotte Bocquelet (HMRLab, CRMN Lyon) Diganta Sarkar (Alberta Uni.) Julie Buhl (Uni. JKU Linz) Marcel Levien (Emsley Lab, EPFL) Mengshan Ye (Miller Institute, UC Berkeley) Mouzhe Xie (Arizona State Uni.) Nikita Rao (Indian Institute of Science, Bangalore) Nesreen Elathram (Debelouchina Lab, UCSD) Tamali Nag (Uni. of Lille/Grenoble)