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Hyperbranched TEMPO-based polymers as catholytes for redox flow battery applications.

Koosha Ehtiati1,2, Ilya Anufriev1,3, Christian Friebe4

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Hyperbranched polymers reduce redox flow battery electrolyte viscosity and improve charge transfer. However, side reactions and TEMPO deactivation limit performance, requiring further research for practical applications.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Polymer Chemistry

Background:

  • Redox-active polymers (RAPs) offer potential cost reduction in redox flow batteries (RFBs) by enabling the use of size-exclusion membranes.
  • High electrolyte viscosity and slow diffusion/electron transfer rates in RAPs hinder their performance compared to small molecules.
  • The relationship between RAP structure and hydrodynamic properties remains underexplored.

Purpose of the Study:

  • To synthesize and investigate hyperbranched 2,2,6,6-tetramethylpiperidinyloxyl (TEMPO)-based polymers as low-viscosity catholytes for RFBs.
  • To elucidate the influence of polymer structure and molar mass distribution on hydrodynamic properties.
  • To evaluate the potential of these RAPs in RFB applications.

Main Methods:

  • Synthesis of TEMPO-based polymers via step-growth polymerization (aza-Michael addition) and post-polymerization modification.
  • Characterization of polymer structure and molar mass distribution using size-exclusion chromatography (SEC) with viscometric detection.
  • Viscometric and crossover investigations to determine optimal molar mass and hydrodynamic properties.
  • Electrochemical testing in RFB configurations.

Main Results:

  • Successfully synthesized hyperbranched TEMPO-based polymers with a compact structure and reduced viscosity (approx. 21 mPas at 1 M TEMPO units).
  • Demonstrated faster diffusion and higher charge transfer rates for hyperbranched polymers compared to linear counterparts.
  • Observed poor RFB performance attributed to side reactions of oxidized TEMPO moieties and partial deactivation of TEMPO units.

Conclusions:

  • Hyperbranched polymer architecture effectively reduces viscosity and enhances mobility in TEMPO-based RAPs for RFBs.
  • Challenges remain, including material loss during dialysis (crossover), TEMPO deactivation, and side reactions under battery conditions.
  • Further research is needed to address these challenges for practical implementation of these promising RAPs.