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A facile processing strategy to fabricate thermoelectric (TE) polymer nanocomposite foams with non-conducting polymers is reported in this study. Multilayered networks of graphene nanoplatelets (GnPs) and multi-walled carbon nanotubes (MWCNTs) are deposited on macroporous polyvinylidene fluoride (PVDF) foam templates using a layer-by-layer (LBL) assembly technique. The open cellular structures of foam templates provide a platform to form segregated 3D networks consisting of one-dimensional (1D) and/or two-dimensional (2D) carbon nanoparticles. Hybrid nanostructures of GnP and MWCNT networks synergistically enhance the material system's electrical conductivity. Furthermore, the polymer foam substrates possess high porosity to provide ultra-low thermal conductivity without compromising the electrical conductivity of the TE nanocomposites. With an extremely low GnP loading (i.e., ~1.5 vol.%), the macroporous PVDF nanocomposites exhibit a thermoelectric figure-of-merit of ~10 -3 . To the best of our knowledge, this ZT value is the highest value reported for organic TE materials using non-conducting polymers and MWCNT/GnP nanofillers. The proposed technique represents an industrially viable approach to fabricate organic TE materials with enhanced energy conversion efficiencies. The current study demonstrates the potential to develop light-weight, low-cost, and flexible TE materials for green energy generation.

Thermoelectric Nanocomposite Foams Using Non-Conducting Polymers with Hybrid 1D and 2D Nanofillers