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Area of Science:

  • Materials Science
  • Electrochemistry
  • Energy Harvesting

Background:

  • Ionic thermoelectric (i-TE) materials offer potential for harvesting low-grade heat for self-powered electronics.
  • Coupling multiple i-TE effects in n-type materials is limited, hindering high-performance system development.

Purpose of the Study:

  • To uncover and characterize a novel thermogalvanic redox reaction in i-TE materials.
  • To investigate the interactive coupling effect between thermogalvanic and thermodiffusion contributions.
  • To establish a design principle for high-performance i-TE materials based on coordination chemistry.

Main Methods:

  • Operando characterization techniques to track reaction processes.
  • Quantitative analysis of ion speciation and coordination species.
  • Fabrication and testing of polyvinyl alcohol (PVA)-CuCl2 gel systems.

Main Results:

  • An overlooked thermogalvanic redox reaction between Cu2+ and Cu+ stabilized by Cl- was identified.
  • An interactive i-TE coupling effect driven by ion speciation was validated in PVA-CuCl2 gels.
  • A giant thermopower of -30.6 mV/K and power density of 0.6 mW/m2K2 were achieved by tuning ion speciation.
  • 16-cell i-TE modules generated 3.5 V and 22 µW from a 15 K temperature difference.

Conclusions:

  • Coordination chemistry plays a crucial role in the interactive thermo-diffusion/galvanic coupling effect.
  • Tuning ion speciation offers a viable strategy for enhancing i-TE material performance.
  • The discovered coupling effect provides a new design principle for advanced i-TE materials for sustainable energy harvesting.