Print Email Facebook Twitter Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption Title Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption Author Harks, P.P.R.M.L. (TU Delft ChemE/Materials for Energy Conversion and Storage) Verhallen, T.W. (TU Delft RST/Storage of Electrochemical Energy) George, C. (TU Delft RST/Storage of Electrochemical Energy) van den Biesen, Jan Karel (Student TU Delft) Liu, Q. (TU Delft ChemE/Advanced Soft Matter) Wagemaker, M. (TU Delft RST/Storage of Electrochemical Energy) Mulder, F.M. (TU Delft ChemE/Materials for Energy Conversion and Storage) Date 2019 Abstract The commercial uptake of lithium-sulfur (Li-S) batteries is undermined by their rapid performance decay and short cycle life. These problems originate from the dissolution of lithium polysulfide in liquid electrolytes, causing charge and active material to shuttle between electrodes. The dynamics of intractable polysulfide migration at different length scales often tend to escape the probing ability of many analytical techniques. Spatial and temporal visualization of Li in Li-S electrodes and direct mechanistic understanding of how polysulfides are regulated across Li-S batteries starting from current collector and active layer coating to electrode-electrolyte interface are still lacking. To address this we employ neutron depth profiling across Li-S electrodes using the naturally occurring isotope, 6Li, which yields direct spatial information on Li-S electrochemistry. Using three types of Li-S electrodes, namely, carbon-sulfur, carbon-sulfur with 10% lithium titanium oxide (LTO), and carbon-sulfur with LTO membrane, we provide direct evidence for the migration, adsorption, and confinement of polysulfides in Li-S cells at work. Our findings further provide insights into the dynamics of polysulfide dissolution and re-utilization in relation to Li-S battery capacity and longevity to aid rational electrode designs toward high-energy, safe, and low-cost batteries. To reference this document use: http://resolver.tudelft.nl/uuid:70424a00-b1ce-4089-a03b-de6d9bd75ff6 DOI https://doi.org/10.1021/jacs.9b05993 ISSN 0002-7863 Source Journal of the American Chemical Society, 141 (36), 14280-14287 Part of collection Institutional Repository Document type journal article Rights © 2019 P.P.R.M.L. Harks, T.W. Verhallen, C. George, Jan Karel van den Biesen, Q. Liu, M. Wagemaker, F.M. Mulder Files PDF jacs.9b05993.pdf 4 MB Close viewer /islandora/object/uuid:70424a00-b1ce-4089-a03b-de6d9bd75ff6/datastream/OBJ/view