High areal capacity and energy density 3D-printed Li-ion battery enabled by silver nanoparticles embedded in cross-linked activated carbon/reduced graphene oxide

Abstract

Creating lithium-ion batteries (LIBs) with high areal capacity and energy density remains a significant challenge. Thick electrodes with increased thickness show a potential attitude toward improved areal capacity. However, the energy density of thick electrodes is hindered by poor electrolyte infiltration and charge/ion transportation. This study employed material extrusion (ME) technology to fabricate a thick 3D-printed electrodes incorporating highly conductive silver nanoparticles (AgNPs), cross-linked activated carbon-reduced graphene oxides (ACrGO), and Li₄Ti₅O₁₂ (LTO) particles as the functional ink. ACrGO, which is integrated with a conductive AgNP network, facilitates charge and ion transport in 3D-printed electrodes with abundant channels, and imparts high electrical conductivity. A 3D-printed AC@rGO-AgNPs-LTO anode with a thickness of 350 μm demonstrated a high discharge capacity of 197.8 mAh g⁻¹ at 0.1C, 141.9 mAh g⁻¹ at 1C, and maintained 84.3 % of its capacity after 200 cycles, and achieved an areal capacity of 7.0 mAh cm⁻² with a high mass loading of 53.25 mg cm⁻² (1112 μm). Coupled with a high-voltage 3D printed LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode, a full cell delivers energy densities of 791.40 Wh kg⁻¹ and 2131.86 Wh L⁻¹. This research offers a promising approach for developing high-performance thick electrodes for LIBS requiring high energy density.