Binder-jet powder-bed additive manufacturing (3D printing) of thick graphene-based electrodes

Additive manufacturing (AM), also known as 3D printing, is emerging as a promising method for the fabrication of complex 3D structures and has the potential to replace the conventional techniques used in the manufacture of commercial devices based on advanced materials. Graphene has shown superior performance in various electronic devices such as electrochemical supercapacitors. However, it remains challenging to produce the thick, high loading graphene-based electrodes required to achieve a high practical energy density in full devices. Herein, we introduce a powder-bed AM technique for the fabrication of crack-free, mm-thick graphene-based electrodes, with high surface area that can be printed in complex shapes. While this technology has the potential to be used in many application areas including energy storage, conversion, and sensing, in this work, we demonstrate their use as high performance supercapacitors. Devices fabricated using thermally exfoliated graphene oxide powder had gravimetric and areal capacitance of ∼260 F g⁻¹ and ∼700 mF cm⁻², respectively at 5 mV s⁻¹ in 1 M H₂SO₄ electrolyte. The supercapacitors retained 80% of their capacity over 1000 cycles. This technique provides a promising route for the fabrication and commercialization of thick, porous graphene-based devices.