Free-standing electrode (FSE) architectures hold the
potential
to dramatically increase the gravimetric and volumetric energy density
of lithium-ion batteries (LIBs) by eliminating the parasitic dead
weight and volume associated with traditional metal foil current collectors.
However, current FSE fabrication methods suffer from insufficient
mechanical stability, electrochemical performance, or industrial adoptability.
Here, we demonstrate a scalable camphene-assisted fabrication method
that allows simultaneous casting and templating of FSEs comprising
common LIB materials with a performance superior to their foil-cast
counterparts. These porous, lightweight, and robust electrodes simultaneously
enable enhanced rate performance by improving the mass and ion transport
within the percolating conductive carbon pore network and eliminating
current collectors for efficient and stable Li+ storage
(>1000 cycles in half-cells) at increased gravimetric and areal
energy
densities. Compared to conventional foil-cast counterparts, the camphene-derived
electrodes exhibit ∼1.5× enhanced gravimetric energy density,
increased rate capability, and improved capacity retention in coin-cell
configurations. A full cell containing both a free-standing anode
and cathode was cycled for over 250 cycles with greater than 80% capacity
retention at an areal capacity of 0.73 mA h/cm2. This active-material-agnostic
electrode fabrication method holds potential to tailor the morphology
of flexible, current-collector-free electrodes, thus enabling LIBs
to be optimized for high power or high energy density Li+ storage. Furthermore, this platform provides an electrode fabrication
method that is applicable to other electrochemical technologies and
advanced manufacturing methods.