Pseudocapacitive Conjugated Polyelectrolyte/2D Electrolyte Hydrogels with Enhanced Physico‐Electrochemical Properties

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  • Glenn Quek
    Departments of Chemistry and Chemical & Biomolecular Engineering National University of Singapore Singapore 119077 Singapore
  • Yude Su
    Departments of Chemistry and Chemical & Biomolecular Engineering National University of Singapore Singapore 119077 Singapore
  • Ricardo K. Donato
    Departments of Chemistry and Chemical & Biomolecular Engineering National University of Singapore Singapore 119077 Singapore
  • Ricardo J. Vázquez
    Departments of Chemistry and Chemical & Biomolecular Engineering National University of Singapore Singapore 119077 Singapore
  • Valeria S. Marangoni
    Centre for Advanced 2D Materials National University of Singapore Singapore 117546 Singapore
  • Pei Rou Ng
    Centre for Advanced 2D Materials National University of Singapore Singapore 117546 Singapore
  • Mariana C. F. Costa
    Centre for Advanced 2D Materials National University of Singapore Singapore 117546 Singapore
  • Binu Kundukad
    Singapore Centre for Environmental Life Sciences Engineering Nanyang Technological University Singapore 639798 Singapore
  • Konstantin S. Novoselov
    Centre for Advanced 2D Materials National University of Singapore Singapore 117546 Singapore
  • Antonio H. Castro Neto
    Centre for Advanced 2D Materials National University of Singapore Singapore 117546 Singapore
  • Guillermo C. Bazan
    Departments of Chemistry and Chemical & Biomolecular Engineering National University of Singapore Singapore 119077 Singapore

Description

<jats:title>Abstract</jats:title><jats:p>Conducting polymer hydrogels (CPHs) are an attractive class of materials that synergize the electrical properties of organic semiconductors with the physical properties of hydrogels. Of particular interest is the implementation of CPHs as electrode materials for electrochemical energy storage by taking advantage of redox‐tunable conjugated backbones and the large electroactive surface area. Herein, the use of 2D electrolytes as an effective post‐polymerization additive to enhance the pseudocapacitive performance of CPHs, is demonstrated. By using the self‐doped conjugated polyelectrolyte CPE‐K hydrogel as a model system, improvements in cycling stability, specific capacitance and working voltage window upon addition of the 2D electrolytes, are shown. Furthermore, positively charged 2D electrolytes to be more effective than their negatively charged counterparts are revealed. Rheology measurements and SEM imaging indicate that the 2D electrolytes serve as non‐covalent cross‐linkers that help in forming a mechanically more robust and highly percolated conducting network. These results provide a new and simple to execute post‐polymerization strategy to optimize the electrochemical performance of CPH‐based pseudocapacitors.</jats:p>

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