The
typically poor ductility of cellulosic fibers and ensuing bonded
networks and paper webs set limits on any effort to produce associated
three-dimensional structures without relying on chemical, often unsustainable,
approaches. To address this challenge, we report on a facile and green
method that combines mechanical and biopolymer treatment: in-plane
compression and aqueous solution permeation via spraying. The first
enabled network extensibility while the second, which relied on the
use of either food-grade gelatin, guar gum, or polylactic acid, improved
network strength and stiffness. As a result, an unprecedented elongation
of ∼30% was achieved after unrestrained drying of the fiber
web. At the same time, the structures experienced a significant increase
in tensile strength and stiffness (by ∼306% and ∼690%,
respectively). Such simultaneous property improvement, otherwise very
difficult to achieve, represents a substantial gain in the material’s
toughness, which results from the synergistic effects associated with
the mechanical response of the network under load, fiber intrinsic
strength, and interfiber bonding. The level of plasticity developed
in fiber webs upon biaxial compaction (longitudinal followed by lateral
compaction), which was performed to reduce property anisotropy, allowed
the synthesis of 3-D packaging materials via direct thermoforming.
Moreover, the formability was found to be temperature and humidity
dependent (strain and creep compliance after creep/recovery cycles
in dynamic mechanical analyses). Overall, an inexpensive, green, and
scalable approach is introduced to expand the properties spaces for
paper and related non-wovens that allows 2-D and 3-D formability of
in-plane compacted fiber networks.