Outstanding Low Temperature Thermoelectric Power Factor from Completely Organic Thin Films Enabled by Multidimensional Conjugated Nanomaterials

In an effort to create a paintable/printable thermoelectric material, comprised exclusively of organic components, polyaniline (PANi), graphene, and double‐walled nanotube (DWNT) are alternately deposited from aqueous solutions using the layer‐by‐layer assembly technique. Graphene and DWNT are stabilized with an intrinsically conductive polymer, poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). An 80 quadlayer thin film (≈1 μm thick), comprised of a PANi/graphene‐PEDOT:PSS/PANi/DWNT‐PEDOT:PSS repeating sequence, exhibits unprecedented electrical conductivity (σ ≈ 1.9 × 105 S m−1) and Seebeck coefficient (S ≈ 120 μV K−1) for a completely organic material. These two values yield a thermoelectric power factor (PF = S 2 σ −1) of 2710 μW m−1 K−2, which is the highest value ever reported for a completely organic material and among the highest for any material measured at room temperature. These outstanding properties are attributed to the highly ordered structure in the multilayer assembly. This water‐based thermoelectric nanocomposite is competitive with the best inorganic semiconductors (e.g., bismuth telluride) at room temperature and can be applied as a coating to any flexible surface (e.g., fibers in clothing). For the first time, there is a real opportunity to harness waste heat from unconventional sources, such as body heat, to power devices in an environmentally‐friendly way. High power factor organic thermoelectric nanocomposites are assembled via layer‐by‐layer assembly. Polyaniline, graphene, and double‐walled carbon nanotubes, stabilized with intrinsically conductive poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate), are alternately deposited from aqueous solutions. This multilayer nanocomposite thin film (≈1 μm thick) exhibits an electrical conductivity of 1880 S cm−1 and a Seebeck coefficient of 120 μV K−1, producing a thermoelectric power factor of 2710 μW m−1 K−2.