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Correlating lithium-ion transport and interfacial lithium microstructure evolution in solid-state batteries during the first cycle

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Abstract
The formation of heterogeneous Li structures at the anode/solid polymer electrolyte (SPE) membrane interphase of solid-state Li-metal batteries (SSLMBs) is one of the key factors that impede SSLMB performance. The relationship between Li+-ion transport kinetics and Li0 structural evolution at the buried interphase is critical but challenging to characterize. Here, we report an operando correlative X-ray Compton scattering and computed tomography imaging technique that quantifies the changes of Li+-ion concentrations in the bulk cathode, SPE membrane, and anode of the SSLMB full cell using a commercially standard configuration. We then visualize Li+-ion concentration distributions as well as Li0 microstructures at the buried anode/SPE interphase. Mechanistic analyses show that the Li-stripping step forms more irregular interfacial Li morphologies at the expense of bulk anode volume shrinkage compared to the Li-plating step during the first cycle.
Keywords
X-RAY-DIFFRACTION, CATHODES, DIFFUSION, CAPACITY, DYNAMICS, GROWTH

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MLA
Huang, Chun, et al. “Correlating Lithium-Ion Transport and Interfacial Lithium Microstructure Evolution in Solid-State Batteries during the First Cycle.” CELL REPORTS PHYSICAL SCIENCE, vol. 5, no. 6, 2024, doi:10.1016/j.xcrp.2024.101995.
APA
Huang, C., Wilson, M. D., Cline, B., Sivarajah, A., Stolp, W., Boone, M., … Leung, C. L. A. (2024). Correlating lithium-ion transport and interfacial lithium microstructure evolution in solid-state batteries during the first cycle. CELL REPORTS PHYSICAL SCIENCE, 5(6). https://doi.org/10.1016/j.xcrp.2024.101995
Chicago author-date
Huang, Chun, Matthew D. Wilson, Ben Cline, Abeiram Sivarajah, Wiebe Stolp, Matthieu Boone, Thomas Connolley, and Chu Lun Alex Leung. 2024. “Correlating Lithium-Ion Transport and Interfacial Lithium Microstructure Evolution in Solid-State Batteries during the First Cycle.” CELL REPORTS PHYSICAL SCIENCE 5 (6). https://doi.org/10.1016/j.xcrp.2024.101995.
Chicago author-date (all authors)
Huang, Chun, Matthew D. Wilson, Ben Cline, Abeiram Sivarajah, Wiebe Stolp, Matthieu Boone, Thomas Connolley, and Chu Lun Alex Leung. 2024. “Correlating Lithium-Ion Transport and Interfacial Lithium Microstructure Evolution in Solid-State Batteries during the First Cycle.” CELL REPORTS PHYSICAL SCIENCE 5 (6). doi:10.1016/j.xcrp.2024.101995.
Vancouver
1.
Huang C, Wilson MD, Cline B, Sivarajah A, Stolp W, Boone M, et al. Correlating lithium-ion transport and interfacial lithium microstructure evolution in solid-state batteries during the first cycle. CELL REPORTS PHYSICAL SCIENCE. 2024;5(6).
IEEE
[1]
C. Huang et al., “Correlating lithium-ion transport and interfacial lithium microstructure evolution in solid-state batteries during the first cycle,” CELL REPORTS PHYSICAL SCIENCE, vol. 5, no. 6, 2024.
@article{01HZSDB759WSF3M9MSE7A43Q81,
  abstract     = {{The formation of heterogeneous Li structures at the anode/solid polymer electrolyte (SPE) membrane interphase of solid-state Li-metal batteries (SSLMBs) is one of the key factors that impede SSLMB performance. The relationship between Li+-ion transport kinetics and Li0 structural evolution at the buried interphase is critical but challenging to characterize. Here, we report an operando correlative X-ray Compton scattering and computed tomography imaging technique that quantifies the changes of Li+-ion concentrations in the bulk cathode, SPE membrane, and anode of the SSLMB full cell using a commercially standard configuration. We then visualize Li+-ion concentration distributions as well as Li0 microstructures at the buried anode/SPE interphase. Mechanistic analyses show that the Li-stripping step forms more irregular interfacial Li morphologies at the expense of bulk anode volume shrinkage compared to the Li-plating step during the first cycle.}},
  articleno    = {{101995}},
  author       = {{Huang, Chun and Wilson, Matthew D. and Cline, Ben and Sivarajah, Abeiram and Stolp, Wiebe and Boone, Matthieu and Connolley, Thomas and Leung, Chu Lun Alex}},
  issn         = {{2666-3864}},
  journal      = {{CELL REPORTS PHYSICAL SCIENCE}},
  keywords     = {{X-RAY-DIFFRACTION,CATHODES,DIFFUSION,CAPACITY,DYNAMICS,GROWTH}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{19}},
  title        = {{Correlating lithium-ion transport and interfacial lithium microstructure evolution in solid-state batteries during the first cycle}},
  url          = {{http://doi.org/10.1016/j.xcrp.2024.101995}},
  volume       = {{5}},
  year         = {{2024}},
}

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