In-plane
anisotropic thermoelectric (TE) films with TE properties
optimized in preferred orientation can establish a good match between
the direction with optimal property for materials and the direction
of temperature difference. Based on the highly conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)
(PEDOT:PSS) fibers previously produced via wet-spinning, in this work,
we further developed flexible and self-supporting PEDOT:PSS thick
films with evident TE property anisotropy by a wet-winding approach.
The as-obtained films were mainly composed of orderly tiled PEDOT:PSS
fibers, thus possessing intrinsically highly oriented and ordered
PEDOT:PSS chain packing. On the basis of their Raman spectra, a large
portion of expanded chain conformation of quinoids was also evidenced,
which thereby greatly facilitated intra-chain charge transport along
the PEDOT-conjugated backbones. As a result, the as-obtained anisotropic
films delivered a power factor of up to 35.8 μW m–1 K–2, which was 2.4 times that of the isotropic
counterpart prepared via drop-casting and also superior over that
of many binary inorganic–organic TE composite films reported
previously. Besides, the fiber-wound PEDOT:PSS films also showed high
mechanical strength and excellent stability upon cyclic bending. With
five stripes of the anisotropic films, a prototype TE generator was
further assembled, for which a good match between the optimal property
direction and temperature difference direction was achieved. This
work may pave the way for the development of anisotropic TE materials
and devices that can be of interest for the design of next-generation
wearable electronics and energy harvesters.