As one of the first studied photothermal agents, eumelanin
is often
used for photothermal materials based on its broadband light absorption
ability, biocompatibility, and cheap availability. However, it is
still a challenge to conduct in-depth development of the photothermal
effect of eumelanin in flexible polymeric composites due to its dispersion
problem. Here, we report light-controlled healable and reversible
adhesive elastomers using polar liquid cross-linkers to assist eumelanin
dispersion into carboxylic styrene butadiene rubber (XSBR). The uniformly
dispersed eumelanin and the coordination between Zn2+ and
eumelanin bring the elastomer a satisfactory photothermal conversion
efficiency (80%), even if only 1 phr eumelanin is added. Under near-infrared
(NIR) laser irradiation of 0.55 W cm–2, the temperature
of the elastomer with 1 phr eumelanin sharply increases from room
temperature to 120 and ∼190 °C (the maximum temperature)
in 20 and 90 s, respectively. Benefiting from the efficient photothermal
conversion ability and transesterification, the elastomer shows excellent
NIR light-controlled healing ability, and its healing efficiency can
reach 94%. Based on noncovalent interactions (mainly hydrogen bonds),
the elastomer shows temperature-dependent reversible adhesive behavior.
The adhesion strength of the elastomer can be adjusted by changing
the temperature or irradiating light, thus facilitating the disassembly
and reuse of the elastomers. Thanks to these advantages, the obtained
elastomers have potential applications in harvesting sunlight for
electricity generation and also provide insights into the development of
sustainable reversible adhesive materials.