There has been increasing interest in the emerging ionic thermoelectric materials with huge ionic thermopower. However, it’s challenging to selectively tune the thermopower of all-solid-state polymer materials because the transportation of ions in all-solid-state polymers is much more complex than those of liquid-dominated gels. Herein, this work provides all-solid-state polymer materials with a wide tunable thermopower range (+20~−6 mV K−1), which is different from previously reported gels. Moreover, the mechanism of p-n conversion in all-solid-state ionic thermoelectric polymer material at the atomic scale was presented based on the analysis of Eastman entropy changes by molecular dynamics simulation, which provides a general strategy for tuning ionic thermopower and is beneficial to understand the fundamental mechanism of the p-n conversion. Furthermore, a self-powered ionic thermoelectric thermal sensor fabricated by the developed p- and n-type polymers demonstrated high sensitivity and durability, extending the application of ionic thermoelectric materials.

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Assembling nanoparticles to spatially well-defined functional nanomaterials and sophisticated architectures has been an intriguing goal for scientists. However, maintaining a long-range order of assembly to create macrostructures remains a challenge, owing to the reliance on purely interparticle interactions. Here, we present a general strategy to synthesize a class of inorganic nanosheets via a bottom-up directional freezing method. We demonstrate that, by confining a homogeneously dispersed metal-cyano colloidal suspension at the ice–water interface, followed by removal of ice crystals, large nanosheets with a lateral scale of up to several millimeters can be produced. The formation of millimeter-sized nanosheets is attributed to balanced electrostatic forces between dispersed nanoparticles, coupled with an appropriate hydrodynamic size of nanoparticles, potentially favorable lattice matching between nanoparticles and ice crystals, and the intermediate water at the ice–particle interface. The highly anisotropic growth of ice crystals can therefore guide the 2D confined assembly of nanoparticles in a long-range order, leading to well-defined 2D nanosheets. This contribution sheds light on the potential of nanoparticle assembly at larger length scales in designing families of large 2D nanoarchitectures for practical applications.

The giant thermopower of ionic thermoelectric materials has attracted great attention for waste-heat recovery technologies. However, generating cyclic power by ionic thermoelectric modules remains challenging, since the ions cannot travel across the electrode interface. Here, we reported a reversible bipolar thermopower (+20.2 mV K−1 to −10.2 mV K−1) of the same composite by manipulating the interactions of ions and electrodes. Meanwhile, a promising ionic thermoelectric generator was proposed to achieve cyclic power generation under a constant heat course only by switching the external electrodes that can effectively realize the alternating dominated thermodiffusion of cations and anions. It eliminates the necessity to change the thermal contact between material and heat, nor does it require re-establish the temperature differences, which can favor improving the efficiency of the ionic thermoelectrics. Furthermore, the developed micro-thermal sensors demonstrated high sensitivity and responsivity in light detecting, presenting innovative impacts on exploring next-generation ionic thermoelectric devices.