Thermoelectrochemical cells (thermocells) designed for harvesting human body heat can provide constant power output for wearable electronics, supplementing state‐of‐the‐art flexible power storage and conversion solutions. However, a systematic investigation into the optimization of wearable thermocells is lacking, especially with regard to device design, n‐type electrolytes, and electrode/electrolyte integration. Here, a n‐type gel electrolyte: polyvinyl alcohol‐FeCl2/3 with outstanding flexibility and elasticity and exceptional electrolyte/electrode integration into a 3D porous poly(3,4‐ethylenedioxythiophene)/polystyrenesulfonate (PEDOT/PSS) electrode, is produced via an in situ chemical crosslinking method. The integrated n‐type cell shows excellent seebeck coefficients (0.85 mV K−1) and output current density (1.74 A m−2 K−1) that are comparable with an optimized p‐type cell consisting of a carboxymethylcellulose‐K3/4Fe(CN)6 electrolyte with a 3D PEDOT/PSS‐edge functionalized graphene/carbon nanotube electrode (−1.22 mV K−1 and 1.85 A m−2 K−1). The equivalent performance of the n‐type and p‐type cells enables the effective series connection of up to 18 pairs of p–n cells that combines to give an output voltage of 0.34 V (∆T = 10 K). This in‐series device is fabricated into a proof‐of‐concept watch strap, which can harvest body heat, charge supercapacitor (up to 470 mF) as well as illuminate a green light emitting diode, demonstrating the practical applications.

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A facile synthesis of nitrogen-doped graphene with high atomic percentages of pyridinic N and graphitic N is reported. The synthesized materials show superior capacitance performance and metal-free bifunctional electrocatalysis of ORR and OER.

A novel flexible three-dimensional (3D) architecture of nitrogen and sulfur codoped graphene has been successfully synthesized via thermal treatment of a liquid crystalline graphene oxide-doping agent composition, followed by a soft self-assembly approach. The high temperature process turns the layer-by-layer assembly into a high surface area macro- and nanoporous free-standing material with different atomic configurations of graphene. The interconnected 3D network exhibits excellent charge capacitive performance of 305 F g(-1) (at 100 mV s(-1)), an unprecedented volumetric capacitance of 188 F cm(-3) (at 1 A g(-1)), and outstanding energy density of 28.44 Wh kg(-1) as well as cycle life of 10 000 cycles as a free-standing electrode for an aqueous electrolyte, symmetric supercapacitor device. Moreover, the resulting nitrogen/sulfur doped graphene architecture shows good electrocatalytic performance, long durability, and high selectivity when they are used as metal-free catalyst for the oxygen reduction reaction. This study demonstrates an efficient approach for the development of multifunctional as well as flexible 3D architectures for a series of heteroatom-doped graphene frameworks for modern energy storage as well as energy source applications.

Multifunctional cellular architecture of sulfur doped graphene paves the way for high performance flexible energy device application.

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Brain-machine interfaces are key components for the development of hands-free, brain -controlled devices. Electroencephalogram (EEG) electrodes are particularly attractive for harvesting the neural signals in a non-invasive fashion. Here, we explore the use of epitaxial graphene grown on silicon carbide on silicon for detecting the electroencephalogram signals with high sensitivity. This dry and non-invasive approach exhibits a markedly improved skin contact impedance when benchmarked to commercial dry electrodes, as well as superior robustness, allowing prolonged and repeated use also in a highly saline environment. In addition, we report the newly -observed phenomenon of surface conditioning of the epitaxial graphene electrodes. The prolonged contact of the epitaxial graphene with the skin electrolytes functionalize the grain boundaries of the graphene, leading to the formation of a thin surface film of water through physisorption and consequently reducing its contact impedance by more than 75%. This effect is primed in highly saline environments, and could be also further tailored as pre-conditioning to enhance the performance and reliability of the epitaxial graphene sensors.