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Carbon nanotube (CNTs) networks embedded in polymer matrix have beenextensively studied over the recent years as a flexible thermoelectric (TE)transport medium. However, their power factor has been largely limited by therelatively inefficient tunneling transport at junctions between CNTs and thelow density of conducting channels through the networks. In this work, wedemonstrate that significant enhancement of power factor is possible by addingelectrically insulating microscale particles in CNT networks. When silicaparticles of a few micrometer diameters were co-embedded in single-walledCNT-polydimethylsiloxane (PDMS) composites, both the electrical conductivityand the Seebeck coefficient were simultaneously enhanced, thereby boosting thepower factor by more than a factor of six. We find that the silicamicroparticles excluded a large volume of the composite from the access of CNTsand caused CNT networks to form around them using the polymer as a binder,which in turn resulted in improved connectivity and alignment of CNTs. Ourtheoretical calculations based on junction tunneling transport show that thelarge power factor enhancement can be attributed to the enhanced tunneling withreduced junction distance between CNTs and the increased geometric factor dueto better CNT alignment. Additional enhancement of power factor by more than afactor of two was achieved by sample compression due to the further improvementof CNT alignment.

Boosting Thermoelectric Power Factor of Carbon Nanotube Networks with Excluded Volume by Co-embedded Microparticles