Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers
Abstract
Electroactive coatings based on non-conjugated redox-active polymers have increased in popularity with the development of thin film organic batteries. Here, control over coating deposition, redox-activity, and ion transport are key to improving their energy storage performance. In this work, the synthesis, solution state electrochemical characterization, and layer-by-layer (LbL) assembly of a nitroxide-based polycation and polyanion are presented. Solution state electrochemical characterization indicates that the rate of electron transfer for the nitroxide polyanion is much higher as compared to the nitroxide polycation. LbL thin films of the nitroxide polyanion and nitroxide polycation are assembled, demonstrating linear growth and tunable thickness (28 nm/layer pair). This work confirms that the ion transport mechanism of the LbL films during the redox reaction is influenced depending on the charge of the terminating layer, where the nitroxide polyanion can participate in self-doping, which leads to a contribution from cation transport. The nitroxide polyanion-terminated film also exhibits a higher capacity and a slightly reduced charge transfer resistance. However, it was also observed that a more pronounced capacity fade occurred for the polyanion-terminated film than the polycation-terminated film. Taken together, this highlights how oppositely charged radical-containing polyelectrolytes can form electroactive coatings for possible applications in energy storage ormore »
- Authors:
-
[1];
[1]
- Texas A & M Univ., College Station, TX (United States)
- Lehigh Univ., Bethlehem, PA (United States)
- Publication Date:
- Research Org.:
- Texas A & M Univ., College Station, TX (United States); Lehigh Univ., Bethlehem, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation Graduate Research Fellowship
- OSTI Identifier:
- 1871681
- Alternate Identifier(s):
- OSTI ID: 1864790; OSTI ID: 1864795
- Grant/Contract Number:
- SC0014006; FG02-05ER15720; DGE-1746932
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Volume: 169; Journal Issue: 2; Journal ID: ISSN 0013-4651
- Publisher:
- IOP Publishing
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; polymer; thin film; batteries; energy storage
Citation Formats
Easley, Alexandra D., Shaligram, Sayali V., Echols, Ian J., Nixon, Kevin, Regen, Steven L., and Lutkenhaus, Jodie L. Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers. United States: N. p., 2022.
Web. doi:10.1149/1945-7111/ac4cd9.
Easley, Alexandra D., Shaligram, Sayali V., Echols, Ian J., Nixon, Kevin, Regen, Steven L., & Lutkenhaus, Jodie L. Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers. United States. https://doi.org/10.1149/1945-7111/ac4cd9
Easley, Alexandra D., Shaligram, Sayali V., Echols, Ian J., Nixon, Kevin, Regen, Steven L., and Lutkenhaus, Jodie L. Tue .
"Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers". United States. https://doi.org/10.1149/1945-7111/ac4cd9. https://www.osti.gov/servlets/purl/1871681.
@article{osti_1871681,
title = {Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers},
author = {Easley, Alexandra D. and Shaligram, Sayali V. and Echols, Ian J. and Nixon, Kevin and Regen, Steven L. and Lutkenhaus, Jodie L.},
abstractNote = {Electroactive coatings based on non-conjugated redox-active polymers have increased in popularity with the development of thin film organic batteries. Here, control over coating deposition, redox-activity, and ion transport are key to improving their energy storage performance. In this work, the synthesis, solution state electrochemical characterization, and layer-by-layer (LbL) assembly of a nitroxide-based polycation and polyanion are presented. Solution state electrochemical characterization indicates that the rate of electron transfer for the nitroxide polyanion is much higher as compared to the nitroxide polycation. LbL thin films of the nitroxide polyanion and nitroxide polycation are assembled, demonstrating linear growth and tunable thickness (28 nm/layer pair). This work confirms that the ion transport mechanism of the LbL films during the redox reaction is influenced depending on the charge of the terminating layer, where the nitroxide polyanion can participate in self-doping, which leads to a contribution from cation transport. The nitroxide polyanion-terminated film also exhibits a higher capacity and a slightly reduced charge transfer resistance. However, it was also observed that a more pronounced capacity fade occurred for the polyanion-terminated film than the polycation-terminated film. Taken together, this highlights how oppositely charged radical-containing polyelectrolytes can form electroactive coatings for possible applications in energy storage or sensing.},
doi = {10.1149/1945-7111/ac4cd9},
journal = {Journal of the Electrochemical Society},
number = 2,
volume = 169,
place = {United States},
year = {Tue Feb 01 00:00:00 EST 2022},
month = {Tue Feb 01 00:00:00 EST 2022}
}
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