A bio-based, self-healable, conductive rubber film with oxidized cellulose nanofiber segregated network

Rubber composites are indispensable in all areas of our daily lives. However, the formation of permanent crosslinked networks in rubber materials makes it difficult to recycle, resulting in a non-negligible waste of resources. In this paper, a vulcanization-free, fully bio-sourced rubber composite was prepared by using oxidized natural rubber (oNR) and oxidized cellulose nanofibers (TOCFs). TOCFs are selectively dispersed between the latex particles to form a segregated network. Meanwhile, the formation of hydrogen-bonding between oxygenated polar groups of oNR and abundant hydroxyl and carboxyl groups of TOCFs improves their interfacial interactions. This special structure promotes strain-induced crystallization (SIC) behavior of oNR matrix, giving its tensile strength up to 14.7 MPa. Furthermore, the oNR/TOCFs film shows excellent self-healing efficiency (96 %) at 40 °C for 5 h. The hygroscopicity of the TOCFs segregated network can turn the oNR/TOCFs film to be a conductive film by regulating the absorbed water content. The film has high conductivity (0.05 S/m) at a water content of 8.99 wt%, and the resistance change (R_V/R₀) can be varied between 1-5.9 × 10^-6 at a water content range of 0-8.99 wt%, which makes it have potential for a wide range of humidity monitoring applications.