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We examined a working hypothesis of sticky thermoelectric (TE) materials, which is inversely designed to mass-produce flexible TE sheets with lamination or roll-to-roll processes without electric conductive adhesives. Herein, we prepared p-type and n-type sticky TE materials via mixing antimony and bismuth powders with low-volatilizable organic solvents to achieve a low thermal conductivity. Since the sticky TE materials are additionally injected into punched polymer sheets to contact with the upper and bottom electrodes in the fabrication process, the sticky TE modules of ca. 2.4 mm in thickness maintained temperature differences of ca. 10°C and 40°C on a hot plate of 40 °C and 120°C under a natural-air cooling condition with a fin. In the single-cell resistance analysis, we found that 75~150-μm bismuth powder shows lower resistance than the smaller-sized one due to the fewer number of particle-particle interfaces in the electric pass between the upper and bottom electrodes. After adjusting the printed wiring pattern for the upper and bottom electrodes, we achieved 42 mV on a hot plate (120°C) with the 6 × 6 module having 212 Ω in the total resistance. In addition to the possibility of mass production at a reasonable cost, the sticky TE materials provide a low thermal conductivity for flexible TE modules to capture low-temperature waste heat under natural-air cooling conditions with fins for the purpose of energy harvesting.

Sticky thermoelectric (TE) materials have been inversely designed to enable the mass production of flexible TE sheets through lamination or roll-to-roll processes without using electrically conductive adhesives. They have also been demonstrated as inorganic/organic hybrid materials consisting of TE inorganic particles and low-volatilizable organic solvents to exhibit Seebeck coefficients based on the TE particles and low thermal conductivities based on the organic matrix. To achieve energy harvesting of 250 µW for driving various electric devices using voltage boosters, herein, we employ p- and n-type Bi2Te3 particles due to their high Seebeck coefficients, and cover the Bi2Te3 bodies with Au skins because the interfacial electrical resistance depends on the electrical resistance of opposing substances at the interface. After controlling the plating amount to cover the Bi2Te3 particles with Au skins, we achieve a TE power generation two orders of magnitude greater than the previous study, i.e., 255 µW on a hot plate of 110 °C with a 6 × 6 module. Overall, with input from other organic devices, like organic light-emitting diodes and dye-sensitized solar cells, this study presents a hierarchical design for TE hybrid materials that suppresses the thermal conduction by hybridizing TE particles with the organic matrix at the microscale. This reduces the electrical resistance by modifying the interfaces of the TE particles at the nanoscale and optimizes the Seebeck coefficient of TE particles at the atomic scale. To compete with solid-state TE modules with regards to power generation capacity, the hierarchical design towards a possible further two orders of magnitude improvement is also discussed.

To examine the potential of organic thermoelectrics (TEs) for energy harvesting, we fabricated an organic TE module to achieve 250 mV in the open-circuit voltage which is sufficient to drive a commercially available booster circuit designed for energy harvesting usage. We chose the π-type module structure to maintain the temperature differences in organic TE legs, and then optimized the p- and n-type TE materials’ properties. After injecting the p- and n-type TE materials into photolithographic mold, we eventually achieved 250 mV in the open-circuit voltage by a method to form the upper electrodes. However, we faced a difficulty to reduce the contact resistance in this material system. We conclude that TE materials must be inversely designed from the viewpoints of the expected module structures and mass-production processes, especially for the purpose of energy harvesting., GRAPHICAL ABSTRACT