Discovering electrode
materials with exceptional capacitance, an
indicator of the ability of a material to hold charge, is critical
for developing capacitive deionization devices for water desalination.
Maganese oxides (MnO
x
) have shown promise
as capacitive electrode materials, but they exhibit a trade-off in
which a higher loading of the active MnO
x
comes at the cost of lower conductivity. To address this challenge
and achieve high salt adsorption, we fabricated electrodes comprising
vertically aligned core–shell nanostructures using atomic layer
deposition (ALD) to coat thin films of MnO
x
onto vertically aligned carbon nanotubes (VACNTs). The inherently
hierarchical, anisotropic, three-dimensional macroporous structure
of VACNTs and the tunable coating, a hallmark of ALD, enabled co-optimization
of the hybrid material’s specific capacitance with respect
to mass and geometric area. The specific capacitance was optimized
in this study to 215 ± 7 F/g and 1.1 ± 0.1 F/cm2 in a 1 M NaCl electrolyte at a scan rate of 5 mV/s. This material
exhibited a remarkable sodium ion adsorption capacity of 490 ±
30 μmol of Na/g of material (2-fold higher than that of pristine
VACNTs) at a functioning voltage of 1.2 V, which may ultimately enable
expanded desalination applications of capacitive deionization.