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Functionalized Silicon Particles for Enhanced Half- and Full-Cell Cycling of Si-Based Li-Ion Batteries

  • Khryslyn G. Araño*
    Khryslyn G. Araño
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *Email: [email protected]
  • Beth L. Armstrong
    Beth L. Armstrong
    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Ethan Boeding
    Ethan Boeding
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Guang Yang
    Guang Yang
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Guang Yang
  • Harry M. Meyer III
    Harry M. Meyer, III
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Evelyna Wang
    Evelyna Wang
    Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
    More by Evelyna Wang
  • Rachel Korkosz
    Rachel Korkosz
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Katie L. Browning
    Katie L. Browning
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Thomas Malkowski
    Thomas Malkowski
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Baris Key
    Baris Key
    Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
    More by Baris Key
  • , and 
  • Gabriel M. Veith*
    Gabriel M. Veith
    Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *Email: [email protected]
Cite this: ACS Appl. Mater. Interfaces 2023, 15, 8, 10554–10569
Publication Date (Web):February 15, 2023
https://doi.org/10.1021/acsami.2c16978
Copyright © 2023 American Chemical Society

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    Abstract

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    Vinylene carbonate (VC) and polyethylene oxide (PEO) have been investigated as functional agents that mimic the solid electrolyte interphase (SEI) chemistry of silicon (Si). VC and PEO are known to contribute to the stability of Si-based lithium-ion batteries as an electrolyte additive and as a SEI component, respectively. In this work, covalent surface functionalization was achieved via a facile route, which involves ball-milling the Si particles with sacrificial VC and PEO. Thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS), and magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy indicate that the additives are strongly bound to Si. In particular, MAS NMR shows Si–R or Si–O–R groups, which confirm functionalization of the Si after milling in VC or PEO. Particle size analysis by dynamic light scattering reveals that the additives facilitate particle size reduction and that the functionalized particles result in more stable dispersions based on zeta potential measurements. Raman mapping of the electrodes fabricated from the VC and PEO-coated active material with a polyacrylic acid (PAA) binder reveals a more homogenous distribution of Si and the carbon conductive additive compared to the electrodes prepared from the neat Si. Furthermore, the VC-milled Si strikingly exhibited the highest capacity in both half- and full-cell configurations, with more than 200 mAh g–1 measured capacity compared to the neat Si in the half-cell format. This is linked to an improved electrode processing based on the Raman and zeta potential measurements as well as a thinner SEI (with more organic components for the functionalized Si relative to the neat Si) based on XPS analysis of the cycled electrodes. The effect of binder was also investigated by comparing PAA with P84 (polyimide type), where an increased capacity is observed in the latter case.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.2c16978.

    • Effect of Spex-milling time on the average particle size and the corresponding polydispersity index of Si; plot showing the bimodal particle size distribution of the Spex-milled Si; additional Si particle size data; TGA curves of the milled Si powders; Raman spectrum of a silicon electrode showing the Si and carbon peaks; Raman map showing the distribution of Si and carbon in the electrode; half-cell performance of neat Si using VC as an electrolyte additive and its comparison with the electrodes presented in Figure 7a; comparison of the Nyquist plots of neat Si, VC-milled Si (denoted as Si-VC), and neat Si using VC as an electrolyte additive (denoted as Si-VCelectrolyte); comparison of the Nyquist plots of the electrodes prepared using PAA and P84 binder; table of post-cycling surface composition of the Si electrodes obtained using XPS; and additional XPS spectrum (PDF)

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    Cited By

    This article is cited by 4 publications.

    1. Sohyun Park, Haoyu Liu, Joseph Quinn, Saul H. Lapidus, Yunya Zhang, Stephen E. Trask, Chongmin Wang, Baris Key, Fulya Dogan. Surface and Bulk Stabilization of Silicon Anodes with Mixed-Multivalent Additives: Ca(TFSI)2 and Mg(TFSI)2. ACS Applied Materials & Interfaces 2024, 16 (16) , 20341-20351. https://doi.org/10.1021/acsami.3c17578
    2. Khryslyn G. Araño, Beth L. Armstrong, Guang Yang, Chanaka Kumara, Thomas Zac Ward, Harry M. Meyer, III, Alexander M. Rogers, Elena Toups, Gabriel M. Veith. Elucidating the Role of Carbon Conductive Additive in the Processing and Electrochemical Behavior of Surface-Modified Si Anodes. Energy & Fuels 2024, 38 (7) , 6446-6458. https://doi.org/10.1021/acs.energyfuels.4c00039
    3. Khryslyn G. Araño, Guang Yang, Beth L. Armstrong, Tolga Aytug, Matthew S. Chambers, Ethan C. Self, Harry M. Meyer, III, Joseph Quinn, James F. Browning, Chongmin Wang, Gabriel M. Veith. Carbon Coating Influence on the Formation of Percolating Electrode Networks for Silicon Anodes. ACS Applied Energy Materials 2023, 6 (21) , 11308-11321. https://doi.org/10.1021/acsaem.3c02205
    4. Lulu Zhou, Yujia Huo, Yajun Cheng, Wei Guang, Xinyi Sun, Weijun Deng, Jing Hu. One-Pot Controllable Synthesis of Silica Nanocapsules with Encapsulated Osmanthus Fragrance for Durable Odor Improvement of Leather. ACS Sustainable Chemistry & Engineering 2023, 11 (32) , 11799-11810. https://doi.org/10.1021/acssuschemeng.3c01412