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Designing n-Type Thermogalvanic TEMPO-Substituted Polyacrylamide via Conformational Entropic Modulation
Ching-Chieh Hsu1, Kohei Ishigami2, Ryo Shirakawa2
1Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan.
None:
This work pioneers the use of TEMPO-substituted polyacrylamide (PTAm) for n-type thermogalvanic (TG) systems, uniquely harnessing redox-induced conformational entropy changes to enhance the thermoelectric performance. Through the electrochemical oxidation of low-molecular-weight PTAm, which is initially water-insoluble, a water-soluble polyelectrolyte (ox-PTAm) is formed, containing both TEMPO and oxoammonium species, as indicated by cyclic voltammetry. The redox transitions induce conformational entropy changes, which are corroborated by electrochemical and thermoelectric measurements, leading to an observed n-type thermopower (α) of -0.76 mV K-1. A maximum power output of 1.18 mW m-2 K-2 is achieved under a thermal gradient of 3.8 K. This work highlights the potential of entropy modulation in redox-active polymers as a strategy for advancing organic thermoelectric materials targeting low-grade waste heat recovery.
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