A metal–organic
framework (MOF) based on a conjugated organic
ligand and a transition-metal ion was designed and used to construct
a novel multiwalled carbon nanotube (MWNT)/MOF interphase via hierarchical
assembly on the carbon fiber (CF) surface and was compared to various
interphases established by MWNT and MOF. An intertwined MWNT and MOF
“jujube core” was randomly dispersed on MWNT@CF and
MOF@CF surfaces, while interpenetrating structures with the MWNT network
and MOF jujube core were simultaneously observed on MWNT/MOF@CF due
to coordination bonds and π–π conjugation effects,
which were derived from the MWNT template with carboxyl groups and
sp2-hybridized domains as well as the secondary growth
of MOF to promote self-assembly and the connection of MOF. The transverse
fiber bundle test (TFBT) strength and interfacial shear strength (IFSS)
of the MWNT/MOF@CF composite were 36.9, 6.1, and 20.8%, 16.3% higher
than those of MWNT@CF and MOF@CF composites, which were attributed
to the smoothed modulus transition of the stiffening interphase formed
by the MWNT/MOF hybrid structure as “armor” to effectively
buffer the stress transfer between a carbon fiber and the resin matrix.
Compared to MWNT@CF and MOF@CF composites, MWNT/MOF@CF composites
had the highest EMI shielding effectiveness, which was attributed
to the combined effects of multiple reflections, conductive loss,
and interface polarization from the interpenetrating MWNT/MOF hybrid
structures, which realized the integration of the structure and function
of the carbon fiber composites.