Nondestructively Visualizing and Understanding the Mechano-Electro-chemical Origins of “Soft Short” and “Creeping” in All-Solid-State Batteries

Daxian Cao; Kena Zhang; Wei Li; Yuxuan Zhang; Tongtai Ji; Xianhui Zhao; Ercan Cakmak; Juner Zhu; Ye Cao; Hongli Zhu

doi:10.1002/adfm.202307998

Nondestructively Visualizing and Understanding the Mechano-Electro-chemical Origins of “Soft Short” and “Creeping” in All-Solid-State Batteries

Daxian Cao, Kena Zhang, Wei Li, Yuxuan Zhang, Tongtai Ji, Xianhui Zhao, Ercan Cakmak, Juner Zhu, Ye Cao, Hongli Zhu

Research output: Contribution to journal › Article › peer-review

20 Scopus citations

Abstract

All-solid-state Li-metal batteries (ASLMBs) represent a significant breakthrough in the quest to overcome limitations associated with traditional Li-ion batteries, particularly in energy density and safety aspects. However, widespread implementation is stymied due to a lack of profound understanding of the complex mechano-electro-chemical behavior of Li metal in the ASLMBs. Herein, operando neutron imaging and X-ray computed tomography (XCT) are leveraged to nondestructively visualize Li behaviors within ASLMBs. This approach offers real-time observations of Li evolutions, both pre- and post- occurrence of a “soft short”. The coordination of 2D neutron radiography and 3D neutron tomography enables charting of the terrain of Li metal deformation operando. Concurrently, XCT offers a 3D insight into the internal structure of the battery following a “soft short”. Despite the manifestation of a “soft short”, the persistence of Faradaic processes is observed. To study the elusive “soft short”, phase field modeling is coupled with electrochemistry and solid mechanics theory. The research unravels how external pressure curbs dendrite growth, potentially leading to dendrite fractures and thus uncovering the origins of both “soft” and “hard” shorts in ASLMBs. Furthermore, by harnessing finite element modeling, it dive deeper into the mechanical deformation and the fluidity of Li metal.

Original language	English
Article number	2307998
Journal	Advanced Functional Materials
Volume	33
Issue number	52
DOIs	https://doi.org/10.1002/adfm.202307998
State	Published - Dec 22 2023

Funding

This research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors acknowledge Dr. Jean Bilheux for the developed Jupyter Imaging Notebook. H.Z. acknowledges the financial support from National Science Foundation under Award Number CBET-ES-1924534. Y.C. acknowledges the financial support from the National Science Foundation under Award Number 2038083. The research performed by J.Z. and W.L. was partially supported by the NASA Ames Research Center through the 19-TTT-0103 program (No. 80NSSC21M0114). We acknowledge Dr. Arturas Adomkevicius for editing. This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The authors acknowledge Dr. Jean Bilheux for the developed Jupyter Imaging Notebook. H.Z. acknowledges the financial support from National Science Foundation under Award Number CBET‐ES‐1924534. Y.C. acknowledges the financial support from the National Science Foundation under Award Number 2038083. The research performed by J.Z. and W.L. was partially supported by the NASA Ames Research Center through the 19‐TTT‐0103 program (No. 80NSSC21M0114). We acknowledge Dr. Arturas Adomkevicius for editing. This manuscript has been authored by UT‐Battelle, LLC under Contract No. DE‐AC05‐00OR22725 with the U.S. Department of Energy. The United States Government retains the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non‐exclusive, paid‐up, irrevocable, world‐wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe‐public‐access‐plan ).

Keywords

Li metal
mechano-electrochemical reaction
operando neutron imaging
soft short
solid-state batteries

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "Nondestructively Visualizing and Understanding the Mechano-Electro-chemical Origins of “Soft Short” and “Creeping” in All-Solid-State Batteries",

abstract = "All-solid-state Li-metal batteries (ASLMBs) represent a significant breakthrough in the quest to overcome limitations associated with traditional Li-ion batteries, particularly in energy density and safety aspects. However, widespread implementation is stymied due to a lack of profound understanding of the complex mechano-electro-chemical behavior of Li metal in the ASLMBs. Herein, operando neutron imaging and X-ray computed tomography (XCT) are leveraged to nondestructively visualize Li behaviors within ASLMBs. This approach offers real-time observations of Li evolutions, both pre- and post- occurrence of a “soft short”. The coordination of 2D neutron radiography and 3D neutron tomography enables charting of the terrain of Li metal deformation operando. Concurrently, XCT offers a 3D insight into the internal structure of the battery following a “soft short”. Despite the manifestation of a “soft short”, the persistence of Faradaic processes is observed. To study the elusive “soft short”, phase field modeling is coupled with electrochemistry and solid mechanics theory. The research unravels how external pressure curbs dendrite growth, potentially leading to dendrite fractures and thus uncovering the origins of both “soft” and “hard” shorts in ASLMBs. Furthermore, by harnessing finite element modeling, it dive deeper into the mechanical deformation and the fluidity of Li metal.",

keywords = "Li metal, mechano-electrochemical reaction, operando neutron imaging, soft short, solid-state batteries",

author = "Daxian Cao and Kena Zhang and Wei Li and Yuxuan Zhang and Tongtai Ji and Xianhui Zhao and Ercan Cakmak and Juner Zhu and Ye Cao and Hongli Zhu",

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AU - Zhao, Xianhui

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Nondestructively Visualizing and Understanding the Mechano-Electro-chemical Origins of “Soft Short” and “Creeping” in All-Solid-State Batteries

Abstract

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Keywords

UN SDGs

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