Selective Charge Carrier Transport and Bipolar Conduction in an Inorganic/Organic Bulk-Phase Composite: Optimization...

Abundant conducting polymers are promising organic substances for low-temperature thermoelectric applications due to their inherently low thermal conductivities. By introducing a conducting polymer filler (PEDOT:PSS─poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonic acid)) into a representative inorganic thermoelectric matrix (Bi₂Te₃), a bulk-phase composite (i.e., inorganic matrix/organic filler) for low-temperature thermoelectric applications is proposed. This composite hosts an interfacial energy barrier between the inorganic and organic components, facilitating controlled carrier transport based on its energy level, known as the energy filtering effect, and thus the composite exhibits a highly improved Seebeck coefficient compared to pristine Bi₂Te₃. The composite also displays a completely different temperature dependence on the Seebeck coefficient from Bi₂Te₃ due to its distinct bipolar conduction tendency. By regulation of the energy filtering effect and bipolar conduction tendency, the composite undergoes noticeable variations in the Seebeck coefficient, resulting in a significantly enhanced power factor. Furthermore, the composite shows a substantially reduced thermal conductivity compared to Bi₂Te₃ because it has lower carrier/lattice thermal contributions, possibly attributed to its high carrier/phonon scattering probabilities. Owing to the superior power factor and reduced thermal conductivity, the composite exhibits markedly enhanced thermoelectric performance, achieving a maximum figure of merit of approximately 1.26 at 380 K and an average figure of merit of approximately 1.23 in the temperature range of 323-423 K. The performance of the composite is competitive with previously reported n-type Bi₂Te₃ binary or ternary analogues. Therefore, the composite is highly expected to be a promising n-type counterpart of p-type Bi₂Te₃-based alloys for various low-temperature thermoelectric applications.