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Effect of Salt Concentration on the Interfacial Solvation Structure and Early Stage of Solid–Electrolyte Interphase Formation in Ca(BH4)2/THF for Ca Batteries

  • Zhenzhen Yang*
    Zhenzhen Yang
    Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
    Joint Center for Energy Storage Research, Lemont, Illinois 60439, United States
    *Email: [email protected]
  • Noel J. Leon
    Noel J. Leon
    Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
    Joint Center for Energy Storage Research, Lemont, Illinois 60439, United States
    More by Noel J. Leon
  • Chen Liao
    Chen Liao
    Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
    Joint Center for Energy Storage Research, Lemont, Illinois 60439, United States
    More by Chen Liao
  • Brian J. Ingram
    Brian J. Ingram
    Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
    Joint Center for Energy Storage Research, Lemont, Illinois 60439, United States
  • , and 
  • Lynn Trahey*
    Lynn Trahey
    Joint Center for Energy Storage Research, Lemont, Illinois 60439, United States
    *Email: [email protected]
    More by Lynn Trahey
Cite this: ACS Appl. Mater. Interfaces 2023, 15, 20, 25018–25028
Publication Date (Web):May 12, 2023
https://doi.org/10.1021/acsami.3c01606
Copyright © 2023 UChicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society

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    Abstract

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    The Ca2+ solvation structure at the electrolyte/electrode interface is of central importance to understand electroreduction stability and solid–electrolyte interphase (SEI) formation for the novel multivalent Ca battery systems. Using an exemplar electrolyte, the concentration-dependent solvation structure of Ca(BH4)2-tetrahydrofuran on a gold model electrode has been investigated with various electrolyte concentrations via electrochemical quartz crystal microbalance with dissipation (EQCM-D) and X-ray photoelectron spectroscopy (XPS). For the first time, in situ EQCM-D results prove that the prevalent species adsorbed at the interface is CaBH4+ across all concentrations. As the salt concentration increases, the number of BH4 anions associated with Ca2+ increases, and much larger solvated complexes such as CaBH4+·4THF or Ca(BH4)3·4THF form at the interface at high concentrations prior to Ca plating. Different interfacial chemistries lead to the formation of SEIs with different components demonstrated by XPS. High electrolyte concentrations reduce the solvent decomposition and promote the formation of thick, uniform, and inorganic-rich (i.e., CaO) SEI layers, which contribute to improved Ca plating efficiency and current density in electrochemical measurements.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.3c01606.

    • In situ EQCM-D measurements during OCP monitoring; in situ EQCM-D measurement during first negative scan in CV measurement from 300–460 s; table of the molecular mass for possible solvated species; CV data of the first 3 cycles; XPS depth profiling data of the SEI composition after stripping; EDS elemental data; and cross-sectional SEM image of Ca deposit on Au (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Aaron M. Melemed, Dhyllan A. Skiba, Katherine J. Steinberg, Kyeong-Ho Kim, Betar M. Gallant. Impact of Differential Ca2+ Coordination in Borohydride-Based Electrolyte Blends on Calcium Electrochemistry and SEI Formation. The Journal of Physical Chemistry C 2023, 127 (40) , 19886-19899. https://doi.org/10.1021/acs.jpcc.3c03800