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Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption

[Image: see text] 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 electrode...

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Autores principales: Harks, Peter-Paul R. M. L., Verhallen, Tomas W., George, Chandramohan, van den Biesen, Jan Karel, Liu, Qian, Wagemaker, Marnix, Mulder, Fokko M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2019
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6876927/
https://www.ncbi.nlm.nih.gov/pubmed/31448600
http://dx.doi.org/10.1021/jacs.9b05993
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author Harks, Peter-Paul R. M. L.
Verhallen, Tomas W.
George, Chandramohan
van den Biesen, Jan Karel
Liu, Qian
Wagemaker, Marnix
Mulder, Fokko M.
author_facet Harks, Peter-Paul R. M. L.
Verhallen, Tomas W.
George, Chandramohan
van den Biesen, Jan Karel
Liu, Qian
Wagemaker, Marnix
Mulder, Fokko M.
author_sort Harks, Peter-Paul R. M. L.
collection PubMed
description [Image: see text] 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, (6)Li, 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.
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spelling pubmed-68769272019-11-27 Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption Harks, Peter-Paul R. M. L. Verhallen, Tomas W. George, Chandramohan van den Biesen, Jan Karel Liu, Qian Wagemaker, Marnix Mulder, Fokko M. J Am Chem Soc [Image: see text] 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, (6)Li, 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. American Chemical Society 2019-08-25 2019-09-11 /pmc/articles/PMC6876927/ /pubmed/31448600 http://dx.doi.org/10.1021/jacs.9b05993 Text en Copyright © 2019 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Harks, Peter-Paul R. M. L.
Verhallen, Tomas W.
George, Chandramohan
van den Biesen, Jan Karel
Liu, Qian
Wagemaker, Marnix
Mulder, Fokko M.
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
title_full Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption
title_fullStr Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption
title_full_unstemmed Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption
title_short Spatiotemporal Quantification of Lithium both in Electrode and in Electrolyte with Atomic Precision via Operando Neutron Absorption
title_sort spatiotemporal quantification of lithium both in electrode and in electrolyte with atomic precision via operando neutron absorption
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6876927/
https://www.ncbi.nlm.nih.gov/pubmed/31448600
http://dx.doi.org/10.1021/jacs.9b05993
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