Fabrication of regular macro-mesoporous reduced graphene aerogel beads with ultra-high mechanical property for efficient bilirubin adsorption.

Three-dimensional graphene materials have been widely studied in many fields for their role as potential absorbent, especially for bilirubin adsorption. In this study, we developed a simple method to prepare reduced graphene aerogel beads as hemoperfusion materials for fast bilirubin adsorption. The graphene oxide (GO) aerogel beads were produced by self-assembly of GO nanosheet that cross-linked by Ca2+ previously in a coagulation bath, then it was reduced by ascorbic acid and lyophilized to yield the reduced graphene aerogel beads. The beads had a regular macroscopic spherical structure with a diameter of about 1.3-2 mm, where the macroporosity was about 10 µm and the mesoporosity was about 12 nm. The macro-mesoporous structure also gave the reduced graphene aerogel beads ultra-high mechanical strengths and high specific surface area, which were both important for hemoperfusion materials. Moreover, the fixed-bed column adsorption revealed that the reduced graphene aerogel beads manifested excellent bilirubin adsorption (649.512 mg/g) with a rapid adsorption equilibrium time (1.5 h) under the optimized conditions. Even in the bilirubin-enriched blood, the adsorption capacity of the beads could reach 367.14 mg/g. Furthermore, the aerogel beads had a low hemolysis ratio and improved anticoagulant property showing good blood compatibility. Hence, the spherical reduced graphene aerogel beads with millimeter-level size presented a good potential for clinical applications in hemoperfusion therapy.