Advancements in electrochemical double-layer capacitor (EDLC) technology require the concomitant use of novel efficient electrode materials and viable electrode manufacturing methods. Cost-effectiveness, scalability and sustainability are key-drivers for fulfilling product development chain accepted by worldwide legislations. Herein, we report a scalable and sprayable “green” electrode material-based ink based on activated carbon and single-/few-layer graphene (SLG/FLG) flakes. We show that, contrary to commercial reduced graphene oxide, defect-free and flat SLG/FLG flakes reduce the friction of ions over the electrode films, while spray coating deposition of our ink maximises the electrolyte accessibility to the electrode surface area. Sprayed SLG/FLG flakes-based EDLCs display superior rate capability performance (e.g., specific energies of 31.5, 23.7 and 12.5 Wh kg⁻¹ at specific powers of 150, 7500 and 30000 W kg⁻¹, respectively) compared to both SLG/FLG flakes-free devices and commercial-like EDLCs produced by slurry-coating method. The use of SLG/FLG flakes enables our sprayed EDLCs to operate in a wide range of temperature (−40/+100°C) compatible with ionic liquid/organic solvent-based electrolytes, overcoming the specific power limits of AC-based EDLCs. A prototype EDLCs stack consisting of multiple large-area EDLCs, each one displaying a capacitance of 25 F, demonstrates the industrial potential of our technology.

电化学双层电容器（EDLC）技术的进步要求同时使用新型高效电极材料和可行的电极制造方法。成本效益，可扩展性和可持续性是实现全球立法所接受的产品开发链的关键驱动力。本文中，我们报告了一种基于活性炭和单层/几层石墨烯（SLG / FLG）薄片的可缩放且可喷涂的“绿色”电极材料基油墨。我们发现，与商业化的氧化石墨烯还原相反，无缺陷且平坦的SLG / FLG薄片可减少离子在电极膜上的摩擦，而我们的油墨的喷涂沉积可最大程度地提高电解质对电极表面积的可及性。喷涂的基于SLG / FLG薄片的EDLC显示出卓越的速率性能（例如，与分别通过浆涂法生产的SLG / FLG无鳞片装置和类似商业的EDLC相比，分别在150、7500和30000 W kg ^-1的比功率下分别具有31.5、23.7和12.5 Wh kg ^-1的比能。 。SLG / FLG薄片的使用使我们的喷涂EDLC能够在与离子液体/有机溶剂基电解质兼容的宽温度范围（−40 / + 100°C）中运行，从而克服了AC基EDLC的特定功率限制。原型EDLC堆栈由多个大面积EDLC组成，每一个都显示25 F的电容，证明了我们技术的工业潜力。