Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements

Abstract A key challenge for solid-state-batteries development is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. However, while the solid-electrolyte/electrode interfacial area should be maximized to facilitate the tra...

Full description

Bibliographic Details
Main Authors: Ming Liu, Chao Wang, Chenglong Zhao, Eveline van der Maas, Kui Lin, Violetta A. Arszelewska, Baohua Li, Swapna Ganapathy, Marnix Wagemaker
Format: Article
Language:English
Published: Nature Portfolio 2021-10-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-021-26190-2
_version_ 1797836342349004800
author Ming Liu
Chao Wang
Chenglong Zhao
Eveline van der Maas
Kui Lin
Violetta A. Arszelewska
Baohua Li
Swapna Ganapathy
Marnix Wagemaker
author_facet Ming Liu
Chao Wang
Chenglong Zhao
Eveline van der Maas
Kui Lin
Violetta A. Arszelewska
Baohua Li
Swapna Ganapathy
Marnix Wagemaker
author_sort Ming Liu
collection DOAJ
description Abstract A key challenge for solid-state-batteries development is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. However, while the solid-electrolyte/electrode interfacial area should be maximized to facilitate the transport of high electrical currents on the one hand, on the other hand, this area should be minimized to reduce the parasitic interfacial reactions and promote the overall cell stability. To improve these aspects simultaneously, we report the use of an interfacial inorganic coating and the study of its impact on the local Li-ion transport over the grain boundaries. Via exchange-NMR measurements, we quantify the equilibrium between the various phases present at the interface between an S-based positive electrode and an inorganic solid-electrolyte. We also demonstrate the beneficial effect of the LiI coating on the all-solid-state cell performances, which leads to efficient sulfur activation and prevention of solid-electrolyte decomposition. Finally, we report 200 cycles with a stable capacity of around 600 mAh g−1 at 0.264 mA cm−2 for a full lab-scale cell comprising of LiI-coated Li2S-based cathode, Li-In alloy anode and Li6PS5Cl solid electrolyte.
first_indexed 2024-04-09T15:08:23Z
format Article
id doaj.art-438be270da434405b982d387a8011ff5
institution Directory Open Access Journal
issn 2041-1723
language English
last_indexed 2024-04-09T15:08:23Z
publishDate 2021-10-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj.art-438be270da434405b982d387a8011ff52023-04-30T11:21:57ZengNature PortfolioNature Communications2041-17232021-10-0112111010.1038/s41467-021-26190-2Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurementsMing Liu0Chao Wang1Chenglong Zhao2Eveline van der Maas3Kui Lin4Violetta A. Arszelewska5Baohua Li6Swapna Ganapathy7Marnix Wagemaker8Section Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologySection Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologySection Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologySection Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologyKey Laboratory on Power Battery Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate School, Tsinghua UniversitySection Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologyKey Laboratory on Power Battery Research and Shenzhen Geim Graphene Center, Tsinghua Shenzhen International Graduate School, Tsinghua UniversitySection Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologySection Storage of Electrochemical Energy, Radiation Science and Technology, Faculty of Applied Sciences, Delft University of TechnologyAbstract A key challenge for solid-state-batteries development is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. However, while the solid-electrolyte/electrode interfacial area should be maximized to facilitate the transport of high electrical currents on the one hand, on the other hand, this area should be minimized to reduce the parasitic interfacial reactions and promote the overall cell stability. To improve these aspects simultaneously, we report the use of an interfacial inorganic coating and the study of its impact on the local Li-ion transport over the grain boundaries. Via exchange-NMR measurements, we quantify the equilibrium between the various phases present at the interface between an S-based positive electrode and an inorganic solid-electrolyte. We also demonstrate the beneficial effect of the LiI coating on the all-solid-state cell performances, which leads to efficient sulfur activation and prevention of solid-electrolyte decomposition. Finally, we report 200 cycles with a stable capacity of around 600 mAh g−1 at 0.264 mA cm−2 for a full lab-scale cell comprising of LiI-coated Li2S-based cathode, Li-In alloy anode and Li6PS5Cl solid electrolyte.https://doi.org/10.1038/s41467-021-26190-2
spellingShingle Ming Liu
Chao Wang
Chenglong Zhao
Eveline van der Maas
Kui Lin
Violetta A. Arszelewska
Baohua Li
Swapna Ganapathy
Marnix Wagemaker
Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
Nature Communications
title Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
title_full Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
title_fullStr Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
title_full_unstemmed Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
title_short Quantification of the Li-ion diffusion over an interface coating in all-solid-state batteries via NMR measurements
title_sort quantification of the li ion diffusion over an interface coating in all solid state batteries via nmr measurements
url https://doi.org/10.1038/s41467-021-26190-2
work_keys_str_mv AT mingliu quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT chaowang quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT chenglongzhao quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT evelinevandermaas quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT kuilin quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT violettaaarszelewska quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT baohuali quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT swapnaganapathy quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements
AT marnixwagemaker quantificationoftheliiondiffusionoveraninterfacecoatinginallsolidstatebatteriesvianmrmeasurements