Extending lithium–sulfur battery
(LSB) electrode architecture
into three dimensions (3D) has been proposed for more than a decade.
A 3D lightweight and porous current collector that is capable of holding
high amounts of sulfur (S) without any significant decrease in performance
has been elusive. Although many material solutions (such as sulfurized
polyacrylonitrile or SPAN) have been identified for alleviating polysulfide
formation and the so-called shuttle effect, their incorporation into
3D current collectors with high capacity at the electrode level has
not yet been realized. Here, we show that graphene foams (GFs) are
ideally suited as 3D lightweight current collectors for LSBs and outperform
the conventional carbon-coated Al (Al/C) foils at the electrode level.
Specifically, we demonstrate that the open framework of GFs facilitates
high mass loading of SPAN without any deterioration in capacity at
the active material level even at high S loading. At the electrode
level, GF-SPAN cathodes exhibited capacities of ∼200 mAh gelectrode
–1 at 0.1C even with low S loadings (∼1.1 mg cm–2), which is at least 3 times higher than conventional Al/C electrodes.
More importantly, we fabricated cells with a high mass loading of
26.5 mg cm–2 S by stacking multiple GFs to achieve
an areal capacity as high as ∼20 mAh cm–2 (at a current density of 3.0 mA cm–2 up to 50
cycles), which is at least 3 times higher than LSB areal capacity
(6 mAh cm–2) needed to displace LIBs.