Cross-Linked Ionomer Gel Separators for Polysulfide Shuttle Mitigation in Magnesium–Sulfur Batteries: Elucidation of Structure–Property Relationships

Ford, Hunter O.; Merrill, Laura C.; He, Peng; Upadhyay, Sunil P.; Schaefer, Jennifer L.

doi:10.1021/acs.macromol.8b01717

Title: Cross-Linked Ionomer Gel Separators for Polysulfide Shuttle Mitigation in Magnesium–Sulfur Batteries: Elucidation of Structure–Property Relationships

Journal Article · Mon Oct 22 00:00:00 EDT 2018 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.8b01717· OSTI ID:1504959

Ford, Hunter O. ^[1]; Merrill, Laura C. ^[1]; He, Peng ^[1]; Upadhyay, Sunil P. ^[1];

^[1]

Univ. of Notre Dame, IN (United States)

Cross-linked ionomer networks of varying poly- (ethylene glycol) diacrylate cross-linker chain length, ionic comonomer chemistry, and comonomer ratio have been studied for their use as polysulfide shuttle inhibiting separators in magnesium–sulfur (Mg–S) batteries. Through the use of X-ray scattering, polysulfide diffusion experiments, conductivity measurements, and Mg–S cell cycling, it was determined in this work that inclusion of tethered anions in polymer networks mitigates the polysulfide shuttle effect. Polysulfide crossover through networks into a bulk electrolyte can be reduced by absorption into the polymer gel, steric rejection, and electrostatic rejection, with the predominance of these mechanisms dictated by polymer composition and structure. The best network composition allowed an initial Mg–S cell discharge capacity of 522 mAh/g compared to a discharge capacity of 365 mAh/g using a literature standard glass fiber separator. The ionomer cell saw 67% capacity retention after three cycles, whereas the glass fiber separator could not complete the first charging cycle due to the polysulfide shuttle.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC); The Society of Arthur J. Schmitt Fellows; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; CBET-1706370

OSTI ID:: 1504959

Journal Information:: Macromolecules, Vol. 51, Issue 21; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 29 works

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Title: Cross-Linked Ionomer Gel Separators for Polysulfide Shuttle Mitigation in Magnesium–Sulfur Batteries: Elucidation of Structure–Property Relationships

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