A Green Synthesis of Controllable Shear-Assisted Catalytically Graphitized Biomass-Derived Carbon and Its Multi-Scale Reinforcement Mechanism in Natural Rubber

Carbon black (CB) serves as the most crucial reinforcing filler in natural rubber (NR) applications. However, conventional CB production relies on petroleum or coal resources, raising concerns about non-renewability and unsustainable resource consumption. Although biomass-derived carbon materials have been explored as alternatives for natural rubber reinforcement, their practical application remains constrained by inherent limitations such as large particle size and low graphitic structure, which compromise reinforcement efficiency. This study presents a novel walnut shell biochar (WSB) for natural rubber enhancement. The biochar was prepared via conventional pyrolysis and subsequently subjected to an environmentally friendly physical ball-milling process. This treatment effectively increased graphitized domains while enriching surface functional groups. Systematic investigations were conducted on the effects of ball-milling duration and biochar loading on rubber reinforcement performance. Results demonstrate that the biochar-reinforced vulcanizates achieved a 22% improvement in tensile strength compared to unfilled rubber. Notably, at 10 phr loading, the tensile strength of biochar-filled vulcanizates reached 98% of that achieved by CB(N330)-filled counterparts. The study further revealed that biochar incorporation effectively reduced hysteresis loss and enhanced elastic recovery in rubber composites. This work proposes a facile method to develop sustainable biochar-based reinforcing agents with significant potential for natural rubber applications.