The
fabrication, thickness, and structure of aerogel films composed
of covalently cross-linked cellulose nanocrystals (CNCs) and poly(oligoethylene
glycol methacrylate) (POEGMA) were optimized for use as electrolyte
absorbers in dye-sensitized solar cells (DSSCs). The aerogel films
were cast directly on transparent conducting counter electrode substrates
(glass and flexible poly(ethylene terephthalate) plastic) and then
used to absorb drop-cast liquid electrolyte, thus providing an alternative
method of filling electrolyte in DSSCs. This approach eliminates the
use of electrolyte-filling holes, which are a typical pathway of electrolyte
leakage, and furthermore enables a homogeneous distribution of electrolyte
components within the photoelectrode. Unlike typical in situ electrolyte gelation approaches, the phase inversion method used
here results in a highly porous (>99%) electrolyte scaffold with
excellent
ionic conductivity and interfacial properties. DSSCs prepared with
CNC–POEGMA aerogels reached similar power conversion efficiencies
as compared to liquid electrolyte devices, indicating that the aerogel
does not interfere with the operation of the device. These aerogels
retain their structural integrity upon bending, which is critical
for their application in flexible devices. Furthermore, the aerogels
demonstrate impressive chemical and mechanical stability in typical
electrolyte solvents because of their stable covalent cross-linking.
Overall, this work demonstrates that the DSSC fabrication process
can be simplified and made more easily upscalable by taking advantage
of CNCs, being an abundant and sustainable bio-based material.