Organic conducting polymers are promising materials for thermoelectric applications due to their high electrical conductivity and intrinsic low thermal conductivity. Among them, poly(3,4-ethylenedioxythiophene) (PEDOT) has a positive Seebeck coefficient (p-type) and is commercially available. It has therefore gained a lot of attention in the field. However, it remains challenging to process a large amount of organic thermocouples to produce an efficient thermoelectric generator (TEG). In addition, finding a way to use bidimensional (2D) printed thermocouples in a tridimensional (3D) TEG structure is not straightforward. In this article, we propose the use of ultrasonic spray-coating as a straightforward large-scale printing technique to prepare highly conducting and in situ polymerized PEDOT:OTf. The spray-coated material can reach an electrical conductivity as high as 2215 ± 665 S cm⁻¹ at 132 ± 10 nm film thickness. We studied the influence of several parameters, such as co-solvent addition, thickness control and rinsing procedure on the conduction properties. GIWAXS and low temperature electrical conductivity measurements on films of different thicknesses allowed us to elucidate the structures of the as-prepared materials and the charge transport mechanisms. Finally, a fully printed and rolled TEG containing 156 thermocouples was prepared as a proof of concept, generating a power output of 1 μW with a 48 °C thermal gradient.

中文翻译：

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喷涂PEDOT：OTf膜：热电性能并集成到印刷热电发生器中

有机导电聚合物由于其高电导率和固有的低热导率而成为有前途的热电应用材料。其中，聚（3，4-乙撑二氧噻吩）（PEDOT）的塞贝克系数（p型）为正，可以商购。因此，它在该领域引起了很多关注。然而，处理大量的有机热电偶以产生有效的热电发电机（TEG）仍然具有挑战性。此外，找到在三维（3D）TEG结构中使用二维（2D）打印热电偶的方法并不简单。在本文中，我们建议使用超声喷涂作为直接的大规模印刷技术来制备高导电性和原位聚合的PEDOT：OTf。喷涂材料在132±10 nm的膜厚下可达到2215±665 S cm ^-1的电导率。我们研究了几种参数的影响，例如助溶剂添加，厚度控制和冲洗程序对导电性能的影响。GIWAXS和在不同厚度的薄膜上的低温电导率测量结果使我们能够阐明所制备材料的结构和电荷传输机制。最后，准备了包含156个热电偶的完整印刷和卷制的TEG，作为概念证明，在48°C的热梯度下产生了1μW的功率输出。