Mechanically strong nanopapers based on lignin containing cellulose micro- and nano-hybrid fibrils: Lignin content-fibrils morphology-strengthening mechanism

Lignin-containing cellulose nanopapers are emerging multifunctional materials in the fields of coatings, films, and packaging. However, the forming mechanism and properties of nanopapers with various lignin content have not been thoroughly studied. In this work, a mechanically strong nanopaper was fabricated based on lignin-containing cellulose micro- and nano-hybrid fibrils (LCNFs). The influence of lignin content and fibrils morphology on the formation process of nanopapers was investigated to understand the strengthening mechanism of nanopapers. LCNFs with high lignin content provided nanopapers with intertwined micro- and nano-hybrid fibrils layers with small layer spacing, while LCNFs with low lignin content offered nanopapers interlaced nanofibrils layers with large layer spacing. Although lignin was expected to interfere with hydrogen bonds between fibrils, the uniformly distributed lignin contributed to the stress transfer between fibrils. Due to the good coordination between microfibrils, nanofibrils and lignin (as network skeleton, filler and natural binder, respectively), the well-designed LCNFs nanopapers with lignin content of 14.5 % showed excellent mechanical properties, including tensile strength (183.8 MPa), Young's modulus (5.6 GPa) and elongation (9.2 %). This work deeply reveals the relationship between lignin content, morphology and strengthening mechanism of nanopapers, and providing theoretical guidance for employing LCNFs as structural and reinforcing materials to design robust composites.