Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells
Solutions for improving fast charging of lithium‐ion batteries have largely focused on alleviating through‐plane lithiation gradients while little is understood about in‐plane heterogeneities and how to resolve them. Herein, high‐speed synchrotron X‐ray diffraction (XRD) resolves graphite lithiation...
| Main Authors: | , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2023-07-01
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| Series: | Small Science |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/smsc.202200067 |
| _version_ | 1797777609543647232 |
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| author | Abigale P. Monasterial Peter J. Weddle Kristen Atkinson David S. Wragg Andrew M. Colclasure Francois L. E. Usseglio-Viretta Natalie Seitzman Jun-Sang Park Jonathan Almer Kandler Smith Donal P. Finegan |
| author_facet | Abigale P. Monasterial Peter J. Weddle Kristen Atkinson David S. Wragg Andrew M. Colclasure Francois L. E. Usseglio-Viretta Natalie Seitzman Jun-Sang Park Jonathan Almer Kandler Smith Donal P. Finegan |
| author_sort | Abigale P. Monasterial |
| collection | DOAJ |
| description | Solutions for improving fast charging of lithium‐ion batteries have largely focused on alleviating through‐plane lithiation gradients while little is understood about in‐plane heterogeneities and how to resolve them. Herein, high‐speed synchrotron X‐ray diffraction (XRD) resolves graphite lithiation spatially and temporally during 6 C charging and 2 C discharging. At every point during operation, considerable differences in the state of lithiation across the pouch cell are present. Some regions are more responsive to operation than others, reaching full lithiation early during charge and full delithiation during discharge. Other regions within the cell never fully delithiate during discharge, despite a prolonged voltage hold at 2.8 V. Using time‐resolved XRD data, the calculated local current density (mA cm−2) at the graphite surface shows an unexpected occurrence of local inverted current densities where regions of graphite are observed to delithiate during charging and lithiate during discharging. A pseudo‐3D model is developed for the graphite electrode with spatially varying microstructural tortuosity to show how microstructural heterogeneity could influence spatial charge dynamics. The model could not predict the complex in‐plane charge behavior observed within the cell. Consequently physics‐based charging protocols based on homogeneous electrode assumptions may underestimate the local variations in charge dynamics and occurrence of lithium plating. |
| first_indexed | 2024-03-12T23:07:15Z |
| format | Article |
| id | doaj.art-077e2dbc34cf4f00a11ca9ab31c30691 |
| institution | Directory Open Access Journal |
| issn | 2688-4046 |
| language | English |
| last_indexed | 2024-03-12T23:07:15Z |
| publishDate | 2023-07-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Small Science |
| spelling | doaj.art-077e2dbc34cf4f00a11ca9ab31c306912023-07-18T13:22:01ZengWiley-VCHSmall Science2688-40462023-07-0137n/an/a10.1002/smsc.202200067Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch CellsAbigale P. Monasterial0Peter J. Weddle1Kristen Atkinson2David S. Wragg3Andrew M. Colclasure4Francois L. E. Usseglio-Viretta5Natalie Seitzman6Jun-Sang Park7Jonathan Almer8Kandler Smith9Donal P. Finegan10National Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USANational Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USANational Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USACentre for Materials and Nanotechnology University of Oslo 0315 Oslo NorwayNational Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USANational Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USADepartment of Chemistry Colorado School of Mines 1500 Illinois Street Golden CO 80401 USAX-ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USAX-ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USANational Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USANational Renewable Energy Laboratory 15013 Denver West Parkway Golden CO 80401 USASolutions for improving fast charging of lithium‐ion batteries have largely focused on alleviating through‐plane lithiation gradients while little is understood about in‐plane heterogeneities and how to resolve them. Herein, high‐speed synchrotron X‐ray diffraction (XRD) resolves graphite lithiation spatially and temporally during 6 C charging and 2 C discharging. At every point during operation, considerable differences in the state of lithiation across the pouch cell are present. Some regions are more responsive to operation than others, reaching full lithiation early during charge and full delithiation during discharge. Other regions within the cell never fully delithiate during discharge, despite a prolonged voltage hold at 2.8 V. Using time‐resolved XRD data, the calculated local current density (mA cm−2) at the graphite surface shows an unexpected occurrence of local inverted current densities where regions of graphite are observed to delithiate during charging and lithiate during discharging. A pseudo‐3D model is developed for the graphite electrode with spatially varying microstructural tortuosity to show how microstructural heterogeneity could influence spatial charge dynamics. The model could not predict the complex in‐plane charge behavior observed within the cell. Consequently physics‐based charging protocols based on homogeneous electrode assumptions may underestimate the local variations in charge dynamics and occurrence of lithium plating.https://doi.org/10.1002/smsc.202200067fast chargingheterogeneityLi-ion batterymodelingX-ray diffraction |
| spellingShingle | Abigale P. Monasterial Peter J. Weddle Kristen Atkinson David S. Wragg Andrew M. Colclasure Francois L. E. Usseglio-Viretta Natalie Seitzman Jun-Sang Park Jonathan Almer Kandler Smith Donal P. Finegan Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells Small Science fast charging heterogeneity Li-ion battery modeling X-ray diffraction |
| title | Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells |
| title_full | Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells |
| title_fullStr | Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells |
| title_full_unstemmed | Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells |
| title_short | Dynamic In‐Plane Heterogeneous and Inverted Response of Graphite to Fast Charging and Discharging Conditions in Lithium‐Ion Pouch Cells |
| title_sort | dynamic in plane heterogeneous and inverted response of graphite to fast charging and discharging conditions in lithium ion pouch cells |
| topic | fast charging heterogeneity Li-ion battery modeling X-ray diffraction |
| url | https://doi.org/10.1002/smsc.202200067 |
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