The development of all-biomass materials to replace conventional
plastics has been gradually becoming a focus. However, all-biomass
plastics, especially those fabricated from agricultural and forestry
wastes, have the obstacles of poor formability and/or low toughness.
Herein, we demonstrated a facile, efficient, and easy-to-scale method
to significantly improve the formability and toughness of biomass
materials via constructing an aggregate of hydrogen-bonding networks,
where the relatively weak hydrogen bonding could be sacrificed during
stretching. After a continuous preparation process that combined a
paper-making process with an in situ welding process,
the regenerated cellulose material with a layered microstructure was
spontaneously formed. The interlayer hydrogen-bonding interactions
could dissipate energy during stretching. As a result, the cellulose
plastics were tough and strong. The tensile strength, strain, and
toughness reached 154.9 MPa, 57.7%, and 81.76 MJ/m3, respectively,
which were markedly higher than those of previous cellulose-based
materials. The corresponding cellulose hydrogel exhibited an excellent
strength of 9.5 MPa and a high strain of 171.4% also. During this
scalable process, a 1-ethyl-3-methylimidazolium acetate (EmimAc) aqueous
solution worked as a dispersant and a solvent, and a high solid content
of cellulose/EmimAc (20 wt %) was used. Based on such an effective
method, various agricultural and forestry wastes, including corn straw,
wheat straw, grass, and wood powder, could be directly processed into
high-tough all-biomass films, indicating a huge potential in ecofriendly
materials, environmental protection, and bioresource utilization.