The direct use of graphene for potential thermoelectric material requires the opening of its bandgap without loss of its high electric conductivity. We herein demonstrate a synchronous reduction and assembly strategy to fabricate large-area reduced graphene oxide films with high electric conductivity and optimized low thermal conductivity assembly. The reduced graphene oxide films have a high electric conductivity and low thermal conductivity, which results from high longitudinal carrier mobility of the lattice domains as well as the enhanced scattering of phonons in the defects and their boundary that substantially reduces the mean phonon free path and the thermal conductivity. Flexible thermoelectric generators were prepared by assembling reduced graphene oxide film on 3D printed polydimethylsiloxane grids, demonstrating a remarkable output voltage of 57.33 mV/g at a temperature difference of 50 K. A wristband-type flexible thermoelectric generator with 7 repeating units generated a maximum power density of 4.19 µW/g at ambient temperature of 15 °C. The 3D printed generator is promising in providing power autonomy to wearable microwatt electronic devices. In addition, we believe that this work can be easily scaled up and can offer the pathway to produce large-scale manufacturing of graphene based materials for future microelectronics and large-scaled flexible and wearable energy harvesting systems.

将石墨烯直接用于潜在的热电材料需要打开其带隙而不损失其高电导率。我们在本文中演示了同步还原和组装策略，以制造具有高电导率和优化的低热导率组装的大面积还原氧化石墨烯薄膜。还原的氧化石墨烯薄膜具有高电导率和低热导率，这是由于晶格域的高纵向载流子迁移率以及缺陷和缺陷边界中声子的散射增强，从而大大降低了平均声子自由程和能级。导热系数。通过在3D打印的聚二甲基硅氧烷网格上组装还原的氧化石墨烯膜来制备柔性热电发生器，在50 K的温差下显示出57.33 mV / g的显着输出电压。具有7个重复单元的腕带式柔性热电发电机在15°C的环境温度下产生的最大功率密度为4.19 µW / g。3D打印发生器有望为可穿戴微瓦电子设备提供电源自主性。此外，我们相信这项工作可以轻松扩大规模，并且可以为大规模生产石墨烯基材料提供途径，以用于未来的微电子学和大规模的柔性和可穿戴式能量收集系统。3D打印发生器有望为可穿戴微瓦电子设备提供电源自主性。此外，我们认为这项工作可以轻松扩大规模，并且可以为大规模生产石墨烯基材料提供途径，以用于未来的微电子学和大规模的柔性和可穿戴式能量收集系统。3D打印发生器有望为可穿戴微瓦电子设备提供电源自主性。此外，我们相信这项工作可以轻松扩大规模，并且可以为大规模生产石墨烯基材料提供途径，以用于未来的微电子学和大规模的柔性和可穿戴式能量收集系统。