Reduced-Graphene Oxide/Poly(acrylic acid) Aerogels as a Three-Dimensional Replacement for Metal-Foil Current Collectors in Lithium-Ion Batteries

We report the synthesis and properties of a low-density (∼5 mg/cm³) and highly porous (99.6% void space) three-dimensional reduced graphene oxide (rGO)/poly­(acrylic acid) (PAA) nanocomposite aerogel as the scaffold for cathode materials in lithium-ion batteries (LIBs). The rGO-PAA is both simple and starts from readily available graphite and PAA, thereby providing a scalable fabrication procedure. The scaffold can support as much as a 75 mg/cm² loading of LiFePO₄ (LFP) in a ∼430 μm thick layer, and the porosity of the aerogel is tunable by compression; the flexible aerogel can be compressed 30-fold (i.e., to as little as 3.3% of its initial volume) while retaining its mechanical integrity. Replacement of the Al foil by the rGO-PAA current collector of the slurry-cast LFP (1.45 ± 0.2 g/cm³ tap density) provides for exemplary mass loadings of 9 mg_LFP/cm² at 70 μm thickness and 1.4 g/cm³ density or 16 mg_LFP/cm² at 100 μm thickness and ∼1.6 g/cm³ density. When compared to Al foil, the distribution of LFP throughout the three-dimensional rGO-PAA framework doubles the effective LFP solution-contacted area at 9 mg/cm² loading and increases it 2.5-fold at 16 mg/cm² loading. Overall, the rGO-PAA current collector increases the volumetric capacity by increasing the effective electrode area without compromising the electrode density, which was compromised in past research where the effective electrode area has been increased by reducing the particle size.