In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics

Lu, Xiaotang; Bogart, Timothy D.; Gu, Meng; Wang, Chong M.; Korgel, Brian

doi:10.1021/acs.jpcc.5b06386

Title: In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics

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Abstract

In situ transmission electron microscopy (TEM) studies were carried out to observe directly in real time the lithiation and delithiation of silicon (Si) nanowires with significant amounts of tin (Sn). The incorporation of Sn significantly enhances the lithiation rate compared to typical Si nanowires. For instance, surface diffusion is enhanced by two orders of magnitude and the bulk lithiation rate by one order of magnitude, resulting in a sequential surface-then-core lithiation mechanism. Pore formation was observed in the nanowires during delithiation, most likely as a result of the fast delithiation kinetics of the nanowires. Pore formation was reversible and the pores disappeared during subsequent lithiation. When an amorphous Si shell was applied to the nanowires, pore formation was not observed during the in situ TEM experimences. Ex situ TEM analysis of Sn-containing Si nanowires cycled in coin cell batteries also showed that the application of an a-Si shell significantly retards pore formation in these nanowires.

Authors:: Lu, Xiaotang; Bogart, Timothy D.; Gu, Meng; Wang, Chong M.; Korgel, Brian

Publication Date:: Thu Sep 03 00:00:00 EDT 2015

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Understanding Charge Separation and Transfer at Interfaces in Energy Materials (CST); Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1229968

Report Number(s):: PNNL-SA-111276
Journal ID: ISSN 1932-7447; 48266; KP1704020

DOE Contract Number:: AC05-76RL01830

Resource Type:: Journal Article

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 119; Journal Issue: 38; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: Environmental Molecular Sciences Laboratory

Citation Formats


                    Lu, Xiaotang, Bogart, Timothy D., Gu, Meng, Wang, Chong M., and Korgel, Brian. In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics.  United States: N. p., 2015. 
        Web.  doi:10.1021/acs.jpcc.5b06386.

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                    Lu, Xiaotang, Bogart, Timothy D., Gu, Meng, Wang, Chong M., & Korgel, Brian. In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics.  United States.  https://doi.org/10.1021/acs.jpcc.5b06386

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                    Lu, Xiaotang, Bogart, Timothy D., Gu, Meng, Wang, Chong M., and Korgel, Brian. 2015.  
        "In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics".  United States.  https://doi.org/10.1021/acs.jpcc.5b06386.

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@article{osti_1229968,

  title        = {In Situ TEM Observations of Sn-Containing Silicon Nanowires Undergoing Reversible Pore Formation Due to Fast Lithiation/Delithiation Kinetics},

  author       = {Lu, Xiaotang and Bogart, Timothy D. and Gu, Meng and Wang, Chong M. and Korgel, Brian},

  abstractNote = {In situ transmission electron microscopy (TEM) studies were carried out to observe directly in real time the lithiation and delithiation of silicon (Si) nanowires with significant amounts of tin (Sn). The incorporation of Sn significantly enhances the lithiation rate compared to typical Si nanowires. For instance, surface diffusion is enhanced by two orders of magnitude and the bulk lithiation rate by one order of magnitude, resulting in a sequential surface-then-core lithiation mechanism. Pore formation was observed in the nanowires during delithiation, most likely as a result of the fast delithiation kinetics of the nanowires. Pore formation was reversible and the pores disappeared during subsequent lithiation. When an amorphous Si shell was applied to the nanowires, pore formation was not observed during the in situ TEM experimences. Ex situ TEM analysis of Sn-containing Si nanowires cycled in coin cell batteries also showed that the application of an a-Si shell significantly retards pore formation in these nanowires.},

  doi          = {10.1021/acs.jpcc.5b06386},

  url          = {https://www.osti.gov/biblio/1229968},
  journal      = {Journal of Physical Chemistry. C},

  issn         = {1932-7447},

  number       = 38,

  volume       = 119,

  place        = {United States},

  year         = {Thu Sep 03 00:00:00 EDT 2015},

  month        = {Thu Sep 03 00:00:00 EDT 2015}

}

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