Thermally conductive adhesives have attracted considerable
attention
in recent years due to their dual functions in promoting interfacial
bonding and thermal transfer. A great number of strategies have been
explored for producing them. However, most of them are based on irreversible
covalent cross-linking resins, which are difficult to be recycled.
Herein, we demonstrate a strategy for in situ producing high-performance,
recyclable thermal adhesives from common stocks with a reversibly
cross-linkable hyperbranched-star copolymer, HBPE@PSF. The copolymer
possesses a hyperbranched polyethylene core covalently bearing multiple
polystyrene side chains with small amount of furan moieties, which
can be synthesized from commercially available ethylene and styrene
as the main monomers. As a stabilizer, the copolymer can effectively
promote the exfoliation of hexagonal boron nitride (h-BN) in chloroform under sonication to render high-quality boron
nanosheets (BNNSs). Moreover, some of the copolymer can be irreversibly
adsorbed on the BNNS surface based on the noncovalent CH−π
and π–π interactions. From the resultant nanofiller,
BNNS/HBPE@PSF composite adhesives have been successfully prepared
through an in situ solution cast process directly with the copolymer
as the matrix. After the cross-linking via the Diels–Alder
reaction, the resultant adhesives simultaneously exhibit excellent
interfacial bonding, thermal transfer, and recyclability, despite
their extremely low furan content, 0.30 mol %. This has been confirmed
to originate from the unique chain structure of the copolymer, which
can form a hyperbranched-star, reversibly cross-linking structure
in the composite system. The composite adhesives obtained herein may
find their important applications as thermal interface materials in
the areas of various electronic products.