Water-coupled monovalent and divalent ion transport in polyviologen networks

Easley, Alexandra D.; Mohanty, Khirabdhi; Lutkenhaus, Jodie L.

doi:10.1039/d3ta00289f

Water-coupled monovalent and divalent ion transport in polyviologen networks

Journal Article · Tue Apr 11 00:00:00 EDT 2023 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/d3ta00289f· OSTI ID:2420314

Easley, Alexandra D. ^[1]; Mohanty, Khirabdhi ^[2]; ^[2]

Texas A & M Univ., College Station, TX (United States); OSTI
Texas A & M Univ., College Station, TX (United States)

Redox-active polymers (RAPs) are of interest as environmentally friendly and earth-abundant energy storage materials. Polyviologens are promising RAPs, but they tend to dissolve during operation. Further, the two-electron redox reaction for polyviologens in various electrolytes is not always reversible, highlighting the need for a deeper understanding of the redox mechanism. Here, the energy storage mechanism for a cross-linked viologen (PTPM) is demonstrated using electrochemical quartz crystal microbalance with dissipation monitoring (EQCM-D), comparing NaCl and Na2SO4 aqueous electrolytes. E-QCMD reveals that the ion-electron transport mechanism is strongly dependent on the valency of the anion. More sudden and dramatic changes in the electrode's mass were observed for the divalent sulfate ion as compared to the smooth mass transitions associated with the monovalent chloride ion. Meanwhile, there was marked hysteresis in the mass transfer profile for NaCl, but little hysteresis for Na2SO4. Our results demonstrate that electrolyte design, and specifically ion valency, will have a large impact on the nature of mass transport in polymer-based electrodes. This work enables electrolyte selection for the next generation polymer batteries with improved performance.

View Accepted Manuscript (DOE)

Research Organization:: Texas A & M Univ., College Station, TX (United States). Texas A & M Engineering Experiment Station

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0014006

OSTI ID:: 2420314

Alternate ID(s):: OSTI ID: 1969578

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 16 Vol. 11; ISSN JMCAET; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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