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  Electrochemical Lithium Alloying Behavior of Guest-Free Type II Silicon Clathrates

Dopilka, A., Childs, A., Bobev, S., & Chan, C. K. (2021). Electrochemical Lithium Alloying Behavior of Guest-Free Type II Silicon Clathrates. The Journal of Physical Chemistry C, 125(35), 19110-19118. doi:10.1021/acs.jpcc.1c04020.

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 Creators:
Dopilka, Andrew1, Author
Childs, Amanda2, Author
Bobev, Svilen2, Author
Chan, Candace K.1, 3, Author              
Affiliations:
1Materials Science and Engineering, School for Engineering of Matter, Transport and Energy, Arizona State University, P.O. Box 876106, Tempe, Arizona 85827, United States, ou_persistent22              
2Department of Chemistry and Biochemistry, University of Delaware, Newark, Delaware 19716, United States, ou_persistent22              
3Research Group Tüysüz, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1950290              

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 Abstract: The guest-free type II Si clathrate (Si136) is an open framework polymorph of Si that displays unique electrochemical reactions with Li. Li ions are first topotactically inserted into the vacant clathrate cages, followed by an alloying reaction that forms an amorphous lithium silicide phase. The alloying reaction voltage is higher than those seen in other Si electrodes, suggesting that there are structural differences in the formed amorphous phases. Synchrotron X-ray total scattering measurements and pair distribution function analysis are employed to characterize the amorphous phases formed after lithiation. The results show that the clathrate becomes completely amorphous at an earlier stage of lithiation when compared to diamond cubic Si, forming a phase with comparatively larger amounts of Si–Si bonding. The initial insertion of Li into the clathrate cages establishes important Li diffusion paths that kinetically enable the formation of an amorphous phase with lower Li content than typically seen in other silicon-based electrodes. After the initial crystalline-to-amorphous conversion reaction, lithiation takes place via solid-solution alloying. These results demonstrate how the topotactic insertion of Li into an alloying host can kinetically enable modified reaction pathways leading to more homogeneous lithiation throughout the electrode, which is beneficial for Li-ion battery applications.

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Language(s): eng - English
 Dates: 2021-05-052021-08-302021-09-09
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpcc.1c04020
 Degree: -

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Title: The Journal of Physical Chemistry C
  Abbreviation : J. Phys. Chem. C
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 125 (35) Sequence Number: - Start / End Page: 19110 - 19118 Identifier: ISSN: 1932-7447
CoNE: https://pure.mpg.de/cone/journals/resource/954926947766