Three-dimensional operando optical imaging of particle and electrolyte heterogeneities inside Li-ion batteries
Year: 2023
Type: article
Abstract: Understanding (de)lithiation heterogeneities in battery materials is key to ensuring optimal electrochemical performance and developing better energy storage devices. However, this remains challenging due to the complex three dimensional morphology of microscopic electrode particles, the involvement of both solid and liquid phase reactants, and range of relevant timescales (seconds to hours). Here, we overcome this problem and demonstrate the use of bench-top laser scanning confocal microscopy for simultaneous three-dimensional operando measurement of lithium ion dynamics in single particles, and the electrolyte, in batteries. We examine two technologically important cathode materials that are known to suffer from intercalation heterogeneities: LixCoO2 and LixNi0.8Mn0.1Co0.1O2. The single-particle surface-to-core transport velocity of Li-phase fronts, and volume changes – as well as their inter-particle heterogeneity – are captured as a function of C-rate, and benchmarked to previous ensemble measurements. Additionally, we visualise heterogeneities in the bulk and at the surface of particles during cycling, and image the formation of spatially non-uniform concentration gradients within the liquid electrolyte. Importantly, the conditions under which optical imaging can be performed inside absorbing and multiply scattering materials such as battery intercalation compounds are outlined.
Source: Nature Nanotechnology
Institutions: Centre National de la Recherche Scientifique, Collège de France, University of Cambridge, Université Paris Sciences et Lettres, Laboratoire Kastler Brossel, École Normale Supérieure - PSL, Sorbonne Université, Réseau sur le Stockage Electrochimique de l'énergie, Chimie du Solide et Energie, Inserm, Centre Interdisciplinaire de Recherche en Biologie, Université Paris Cité, Interfaces Traitements Organisation et Dynamique des Systèmes, University College London, Boston College
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: green
Funders: National Science Foundation, École Normale Supérieure, Research Councils UK, University of Cambridge, Agence Nationale de la Recherche, Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, Engineering and Physical Sciences Research Council, Clare College, University of Cambridge, Department of Physics and Astronomy, University College London
OpenAlex ID: W4385955193