Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers

Easley, Alexandra D.; Shaligram, Sayali V.; Echols, Ian J.; Nixon, Kevin; Regen, Steven L.; Lutkenhaus, Jodie L.

doi:10.1149/1945-7111/ac4cd9

Title: Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers

Journal Article · 31 January 2022 · Journal of the Electrochemical Society

DOI: https://doi.org/10.1149/1945-7111/ac4cd9 · OSTI ID:1864790

Easley, Alexandra D. ^[1]; Shaligram, Sayali V. ^[2]; Echols, Ian J. ^[3];

^[3]; Regen, Steven L. ^[2];

^[3]

Texas A & M Univ., College Station, TX (United States); Lehigh University
Lehigh Univ., Bethlehem, PA (United States)
Texas A & M Univ., College Station, TX (United States)

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lehigh Univ., Bethlehem, PA (United States); Texas A & M Univ., College Station, TX (United States)

Sponsoring Organization:: National Science Foundation Graduate Research Fellowship; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-05ER15720; SC0014006

OSTI ID:: 1864790

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 2 Vol. 169; ISSN 0013-4651

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Layer-by-Layer Conjugated Extension of a Semiconducting Polymer for High-Performance Organic Field-Effect Transistor Jang, Mi; Kim, Se Hyun; Lee, Han-Koo Advanced Functional Materials, Vol. 25, Issue 25 https://doi.org/10.1002/adfm.201403497	journal	May 2015
High-Performance Polymer Solar Cells with Electrostatic Layer-by-Layer Self-Assembled Conjugated Polyelectrolytes as the Cathode Interlayer Zhang, Kai; Hu, Zhicheng; Xu, Rongguo Advanced Materials, Vol. 27, Issue 24 https://doi.org/10.1002/adma.201500972	journal	May 2015
Solution‐Processable Thermally Crosslinked Organic Radical Polymer Battery Cathodes Wang, Shaoyang; Park, Albert Min Gyu; Flouda, Paraskevi ChemSusChem, Vol. 13, Issue 9 https://doi.org/10.1002/cssc.201903554	journal	March 2020
An Electroactive and Transparent Haptic Interface Utilizing Soft Elastomer Actuators with Silver Nanowire Electrodes Jun, Kiwoo; Kim, Jongnam; Oh, Il-Kwon Small, Vol. 14, Issue 35 https://doi.org/10.1002/smll.201801603	journal	July 2018
Electrochemical decomposition of layer-by-layer thin films composed of TEMPO-modified poly(acrylic acid) and poly(ethyleneimine) Takahashi, Shigehiro; Aikawa, Yu; Kudo, Tomotaka Colloid and Polymer Science, Vol. 292, Issue 3 https://doi.org/10.1007/s00396-014-3169-0	journal	February 2014
Polyelectrolyte Multilayers Studied by Electron Paramagnetic Resonance (EPR) Spin-Label Technique Lappan, Uwe; Wiesner, Brigitte; Zschoche, Stefan Applied Magnetic Resonance, Vol. 44, Issue 1-2 https://doi.org/10.1007/s00723-012-0398-6	journal	October 2012
The influence of current density, rest time and electrolyte composition on the self-discharge of organic radical polymers Gerlach, P.; Balducci, A. Electrochimica Acta, Vol. 377 https://doi.org/10.1016/j.electacta.2021.138070	journal	May 2021
Polymer ionic liquid bearing radicals as an active material for organic batteries with ultrafast charge-discharge rate Aqil, Mohamed; Ouhib, Farid; Aqil, Abdelhafid European Polymer Journal, Vol. 106 https://doi.org/10.1016/j.eurpolymj.2018.07.028	journal	September 2018
Nitroxide TEMPO-containing PILs: Kinetics study and electrochemical characterizations Aqil, Mohamed; Aqil, Abdelhafid; Ouhib, Farid European Polymer Journal, Vol. 152 https://doi.org/10.1016/j.eurpolymj.2021.110453	journal	June 2021
Synthesis and characterization of amorphous mesoporous silica using TEMPO-functionalized amphiphilic templates de Vries, Wilke; Doerenkamp, Carsten; Zeng, Zhaoyang Journal of Solid State Chemistry, Vol. 237 https://doi.org/10.1016/j.jssc.2016.01.023	journal	May 2016
Redox-active polymers: The magic key towards energy storage – a polymer design guideline progress in polymer science Rohland, Philip; Schröter, Erik; Nolte, Oliver Progress in Polymer Science, Vol. 125 https://doi.org/10.1016/j.progpolymsci.2021.101474	journal	February 2022
Layer-by-layer coating of oriented conjugated polymer films towards anisotropic electronics Pandey, Manish; Sadakata, Shifumi; Nagamatsu, Shuichi Synthetic Metals, Vol. 227 https://doi.org/10.1016/j.synthmet.2017.02.018	journal	May 2017
Electrochemistry of Multilayer Electrodes: From the Basics to Energy Applications Gu, Minsu; Kim, Byeong-Su Accounts of Chemical Research, Vol. 54, Issue 1 https://doi.org/10.1021/acs.accounts.0c00524	journal	November 2020
Innovation in Layer-by-Layer Assembly Richardson, Joseph J.; Cui, Jiwei; Björnmalm, Mattias Chemical Reviews, Vol. 116, Issue 23 https://doi.org/10.1021/acs.chemrev.6b00627	journal	November 2016
Mixed Ionic and Electronic Conduction in Radical Polymers Yu, Ilhwan; Jeon, Daeyoung; Boudouris, Bryan Macromolecules, Vol. 53, Issue 11 https://doi.org/10.1021/acs.macromol.0c00460	journal	May 2020
Charge–Discharge with Rocking-Chair-Type Li ⁺ Migration Characteristics in a Zwitterionic Radical Copolymer Composed of TEMPO and Trifluoromethanesulfonylimide with Carbonate Electrolytes for a High-Rate Li-Ion Battery Tokue, Hiroshi; Murata, Tomoaki; Agatsuma, Haruka Macromolecules, Vol. 50, Issue 5 https://doi.org/10.1021/acs.macromol.6b02404	journal	February 2017
Odd–Even Effect on Rotational Dynamics of Spin-Labeled Polyacid Chain Segments in Polyelectrolyte Multilayers Lappan, Uwe; Rau, Cindy; Naas, Carolin Macromolecules, Vol. 52, Issue 6 https://doi.org/10.1021/acs.macromol.9b00101	journal	March 2019
Surface Self-Assembly of Functional Electroactive Nanofibers on Textile Yarns as a Facile Approach toward Super Flexible Energy Storage Tebyetekerwa, Mike; Xu, Zhen; Li, Weili ACS Applied Energy Materials, Vol. 1, Issue 2 https://doi.org/10.1021/acsaem.7b00057	journal	December 2017
Redox Properties of Polyvinylamine- g -TEMPO in Multilayer Films with Sodium Poly(styrenesulfonate) Fu, Qiang; Zoudanov, Igor; Gustafsson, Emil ACS Applied Materials & Interfaces, Vol. 9, Issue 6 https://doi.org/10.1021/acsami.6b15319	journal	February 2017
Visible-to-NIR Electrochromic Device Prepared from a Thermally Polymerizable Electroactive Organic Monomer Wałęsa-Chorab, Monika; Skene, W. G. ACS Applied Materials & Interfaces, Vol. 9, Issue 25 https://doi.org/10.1021/acsami.7b02903	journal	June 2017
Layer-by-Layer Assembly of Polyaniline Nanofibers and MXene Thin-Film Electrodes for Electrochemical Energy Storage Yun, Junyeong; Echols, Ian; Flouda, Paraskevi ACS Applied Materials & Interfaces, Vol. 11, Issue 51 https://doi.org/10.1021/acsami.9b16692	journal	November 2019
100th Anniversary of Macromolecular Science Viewpoint: Fundamentals for the Future of Macromolecular Nitroxide Radicals Wang, Shaoyang; Easley, Alexandra D.; Lutkenhaus, Jodie L. ACS Macro Letters, Vol. 9, Issue 3 https://doi.org/10.1021/acsmacrolett.0c00063	journal	February 2020
Charge Storage in Polymer Acid-Doped Polyaniline-Based Layer-by-Layer Electrodes Jeon, Ju-Won; O’Neal, Josh; Shao, Lin ACS Applied Materials & Interfaces, Vol. 5, Issue 20 https://doi.org/10.1021/am402809e	journal	October 2013
Preparation of Layer-by-Layer Thin Films Composed of DNA and Ferrocene-Bearing Poly(amine)s and Their Redox Properties Sato, Hiroshi; Anzai, Jun-ichi Biomacromolecules, Vol. 7, Issue 6 https://doi.org/10.1021/bm060222a	journal	May 2006
Electrochemical oxidation of tertiary amines. Effect of structure upon reversibility Nelsen, S. F.; Hintz, P. J. Journal of the American Chemical Society, Vol. 94, Issue 20 https://doi.org/10.1021/ja00775a041	journal	October 1972
Donnan Permselectivity in Layer-by-Layer Self-Assembled Redox Polyelectrolye Thin Films Calvo, Ernesto J.; Wolosiuk, Alejandro Journal of the American Chemical Society, Vol. 124, Issue 28 https://doi.org/10.1021/ja020107h	journal	June 2002
Diffusion-Cooperative Model for Charge Transport by Redox-Active Nonconjugated Polymers Sato, Kan; Ichinoi, Rieka; Mizukami, Ryusuke Journal of the American Chemical Society, Vol. 140, Issue 3 https://doi.org/10.1021/jacs.7b11272	journal	January 2018
Relationship between Molecular Structure and Electron Transfer in a Polymeric Nitroxyl-Radical Energy Storage Material Kemper, Travis W.; Larsen, Ross E.; Gennett, Thomas The Journal of Physical Chemistry C, Vol. 118, Issue 31 https://doi.org/10.1021/jp501628z	journal	July 2014
Roughness and Salt Annealing in a Polyelectrolyte Multilayer Ghostine, Ramy A.; Jisr, Rana M.; Lehaf, Ali Langmuir, Vol. 29, Issue 37 https://doi.org/10.1021/la401632x	journal	September 2013
Interdiffusion in Polyelectrolyte Multilayers Soltwedel, Olaf; Ivanova, Oxana; Nestler, Peter Macromolecules, Vol. 43, Issue 17 https://doi.org/10.1021/ma101279q	journal	September 2010
Real-time insight into the doping mechanism of redox-active organic radical polymers Wang, Shaoyang; Li, Fei; Easley, Alexandra D. Nature Materials, Vol. 18, Issue 1 https://doi.org/10.1038/s41563-018-0215-1	journal	November 2018
Synthesis and electrochemical behaviour of nitroxidepolymer brush thin-film electrodes for organic radical batteries Hung, Miao-Ken; Wang, Yu-Hsuan; Lin, Chun-Hao J. Mater. Chem., Vol. 22, Issue 4 https://doi.org/10.1039/C1JM13911H	journal	January 2012
Polyaniline nanofiber/electrochemically reduced graphene oxide layer-by-layer electrodes for electrochemical energy storage Jeon, Ju-Won; Kwon, Se Ra; Lutkenhaus, Jodie L. Journal of Materials Chemistry A, Vol. 3, Issue 7 https://doi.org/10.1039/C4TA04697H	journal	January 2015
Nanostructured organic radical cathodes from self-assembled nitroxide-containing block copolymer thin films Hauffman, G.; Vlad, A.; Janoschka, T. Journal of Materials Chemistry A, Vol. 3, Issue 38 https://doi.org/10.1039/C5TA05823F	journal	January 2015
Layer-by-layer assembly for rapid fabrication of thick polymeric films Li, Yang; Wang, Xu; Sun, Junqi Chemical Society Reviews, Vol. 41, Issue 18 https://doi.org/10.1039/c2cs35107b	journal	January 2012
Effect of polyelectrolyte interdiffusion on electron transport in redox-active polyelectrolyte multilayers Zahn, Raphael; Coullerez, Géraldine; Vörös, János Journal of Materials Chemistry, Vol. 22, Issue 22 https://doi.org/10.1039/c2jm30469d	journal	January 2012
There is still plenty of room for layer-by-layer assembly for constructing nanoarchitectonics-based materials and devices Ariga, Katsuhiko; Lvov, Yuri; Decher, Gero Physical Chemistry Chemical Physics, Vol. 24, Issue 7 https://doi.org/10.1039/d1cp04669a	journal	January 2022
Electrochemical Oxidation of Amines Using a Nitroxyl Radical Catalyst and the Electroanalysis of Lidocaine Sato, Katsuhiko; Ono, Tetsuya; Sasano, Yusuke Catalysts, Vol. 8, Issue 12 https://doi.org/10.3390/catal8120649	journal	December 2018

Similar Records

Diffusional Response of Layer-by-Layer Assembled Polyelectrolyte Chains to Salt Annealing

Journal Article · 2015 · Macromolecules · OSTI ID:1426594

Selin, Victor; Ankner, John F.; Sukhishvili, Svetlana A.

Facile Strategy to Prepare Poly(ionic liquid)-Coated Solid Polymer Electrolytes through Layer-by-Layer Assembly

Journal Article · 2023 · ACS Applied Materials and Interfaces · OSTI ID:2217709

Wang, Zongyu; Thapaliya, Bishnu P.; Popovs, Ilja; +6 more

Layer-by-Layer Assembly Strategy for Reinforcing the Mechanical Strength of an Ionogel Electrolyte without Affecting Ionic Conductivity

Journal Article · 2019 · ACS Applied Energy Materials · OSTI ID:1657987

Thapaliya, Bishnu Prasad; Popov, Ivan; Dai, Sheng

Related Subjects

25 ENERGY STORAGE
batteries
energy storage
polymer
thin film

Title: Layer-by-Layer Nanoarchitectonics of Electrochemically Active Thin Films Comprised of Radical-Containing Polymers

Citation Formats

References (38)

Similar Records

Related Subjects