Ion Exchange Induced Efficient N-Type Thermoelectrics in Solid-State

Y Zhou and CL Yao and XX Lin and J Oh and JJ Tian and WZ Yang and YJ He and YH Ma and K Yang and B Ai and K Sun and ZP Fu and YL Lu and F Li and CD Yang and SS Chen, ADVANCED FUNCTIONAL MATERIALS, 33 (2023).

DOI: 10.1002/adfm.202214563

High-performance n-type solid-state ionic thermoelectrics (SS i-TEs) for low-grade heat harvesting are highly desired and challenging. Here, the design and synthesis of an efficient n-type mixed conductor via ion pair modulation is demonstrated, which consists of biguanide hydrochloride (MfmCl) and a poly(3,4-ethylenedioxythiophene) (PEDOT): poly(styrenesulfonate) (PSS) polymeric complex in a solid film. Theoretical calculations and nano/microstructure characterization reveal that the binding preference of ion pairs offers energetically favorable ion exchange in the matrix, which induces not only tightly bound Mfm PSS species but also favorable anion diffusion channels. Consequently, an enhanced ionic conductivity of 1.40 S m(-1) with a record highest negative thermopower of -46.97 mV K-1 is achieved for the n-type mixed conductor thus far.

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