Deposition of functional
materials on nonplanar surfaces remains
a challenge for various applications, including three-dimensional
(3D) all-solid-state Li-ion batteries. In this Letter we present a
new process to deposit functional oxide materials on high aspect ratio
microstructures without the use of vacuum-based deposition methods.
Using ultrasonic spray deposition in combination with metal citrate
chemistry, we were able to deposit high-quality coatings on Si microcylinders
with an aspect ratio of 10. These results were achieved by controlling
the precursor chemistry, wetting properties, gel mobility, and precursor
decomposition. The versatility of the process was shown by depositing
titanium oxide (TiO2), lithium lanthanum titanate (Li0.35La0.55TiO3), and tungsten oxide (WO3) on Si microcylinders of 50 μm length with an intercylinder
distance of 5 μm. Finally, a proof of the 3D battery concept
was achieved by coating of TiN/Si microcylinders with WO3 using a minimized thermal budget to preserve the (oxidative) TiN
current collector. This led to an almost 3-fold electrode capacity
enhancement per footprint area, due to the high surface-to-bulk ratio
of the 3D coating. Therefore, these results represent a breakthrough
in the field of solution-processing of nonplanar microstructures.
In addition, the flexibility, low cost, and high scale-up potential
of this approach are very promising for various applications requiring
coated 3D microstructures.