Unraveling
the interaction mechanisms of type I collagen with various
inorganic nanoparticles is of pivotal importance to construct collagen-based
bionanocomposites with hierarchical structures for biomedical, pharmaceutical,
and other industrial applications. In this study, synthetic two-dimensional
Laponite nanoplatelets (LAP NPs) are surface-functionalized with tetrakis(hydroxymethyl)
phosphonium sulfate (THPS) for reinforcing their incorporation with
type I collagen matrix by focusing on the influences of the interactions
on the hierarchical structures of the collagen. Our results indicate
that the LAP NPs can be successfully surface-functionalized with THPS
via covalent bonds between the amine-functionalized NPs and the hydroxymethyl
groups of THPS. Moreover, the resulting NPs can be well dispersed
into the collagen matrix and evenly bound onto the collagen fiber
strands and between the collagen fibrils, preserving the native D-periodic banding patterns of the collagen fibrils. The
formation of covalent and hydrogen bonds between the collagen and
the functionalized NPs can stabilize the intrinsic triple-helical
conformation of the collagen, conferring the resulting collagen-based
nanocomposites with improved thermal stability and enhanced mechanical
properties. We anticipate that a fundamental understanding of the
interactions between the collagen and functionalized inorganic nanoparticles
would contribute to the design, fabrication, and further application
of hierarchical collagen-based bionanocomposites with multifunctions.