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Fiber-based thermoelectric (TE) generators have arose significant attention in recent years for portable energy supply devices. However, it is still a great challenge to fabricate integral p-n type connected graphene fibers (GFs) at present. Herein, we prepared p-type GFs by a simple process of chemical reduction. An integral p-n connected all-graphene fiber without additional adhesive was obtained with discontinuous doping with electron-donating polyethyleneimine ethoxylated (PEIE). The integral p-n connected GFs displayed a steady electrical conductivity, excellent flexibility and acceptable tensile properties. Furthermore, a flexible wearable TE generator was fabricated through integrating as-prepared integral p-n connected GFs into flexible polydimethylsiloxane (PDMS) substrate, exhibiting a stable output power at the temperature difference between human body and air temperature, which may provide a good reference for fiber-based wearable TE energy supply.

The organic/inorganic composites are considered as a promising strategy to gain high thermoelectric (TE) performance. Although many efforts have been focused on composites, complicated methods are real hindrance to the development of TE materials. Here, we demonstrate a potential TE thin film comprising highly conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and chemically exfoliated MoS2 (ce-MoS2) nanosheets by layer-by-layer (LbL) assembly method. This work achieves the effective integration of composite, treatment, and electron transfer based on the advantages of PEDOT:PSS and ce-MoS2. On the one hand, the negative charged ce-MoS2 nanosheets facilitate the formation of heterostructure TE films with positive charged PEDOT and reduce the oxidation level of PEDOT, which would favor an enhanced thermopower (21.9 μV K–1). On the other hand, the simultaneous enhancement in the electrical conductivity (867 S cm–1) of PEDOT:PSS/ce-MoS2 composite film is caused by dimethyl sulfoxid...