In the quest for sustainable materials for quasi-solid-state (QS)
electrolytes in aqueous dye-sensitized solar cells (DSSCs), novel
bioderived polymeric membranes were prepared in this work by reaction
of preoxidized kraft lignin with poly(ethylene glycol)diglycidylether
(PEGDGE). The effect of the PEGDGE/lignin relative proportions on
the characteristics of the obtained membranes was thoroughly investigated,
and clear structure–property correlations were highlighted.
In particular, the glass transition temperature of the materials was
found to decrease by increasing the amount of PEGDGE in the formulation,
indicating that polyethylene glycol chains act as flexible segments
that increase the molecular mobility of the three-dimensional polymeric
network. Concurrently, their swelling ability in liquid electrolyte
was found to increase with the concentration of PEGDGE, which was
also shown to influence the ionic transport efficiency within the
membrane. The incorporation of these lignin-based cross-linked systems
as QS electrolyte frameworks in aqueous DSSCs allowed the preparation
of devices with excellent long-term stability under UV–vis
light, which were found to be superior to benchmark QS-DSSCs incorporating
state-of-the-art carboxymethylcellulose membranes. This
study provides the first demonstration of lignin-based QS electrolytes
for stable aqueous DSSCs, establishing a straightforward strategy
to exploit the potential of lignin as a functional polymer precursor
for the field of sustainable photovoltaic devices.