As one of the most attractive inorganics to improve the thermoelectric (TE) performance of the conducting polymers, tellurium (Te) has received intense concern due to its superior Seebeck coefficient (). However, far less attention has been paid to polypyrrole (PPy)/Te TE composites to date. In this work, we present an innovative full-electrochemical method to architect PPy/Te TE composite films by sequentially depositing Te with large and PPy with high electrical conductivity (σ). Consequently, the PPy/Te composite films achieved excellent TE performance, with the largest power factor (PF) reaching up to 234.3 ± 4.1 μW m K. To the best of our knowledge, this value approaches the reported highest PF record (240.3 ± 5.0 μW m K) for PPy-based composites. This suggests that the modified full-electrochemical method is a feasible and effective strategy for achieving high-performance TE composite films, which would probably provide a general guideline for the design and preparation of excellent TE materials in the future.
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