▎ 摘　　要

Peptide-mediated exfoliation and suspension of graphene in aqueous media is a promising strategy for bioapplications such as drug delivery, tissue engineering, and biosensors. A few peptide sequences are known as graphene exfoliators/dispersants in water, but the mechanisms underpinning this process remain underexplored. Here, molecular simulations investigate two key steps: sheet exfoliation and subsequent sheet reunification, in aqueous media. Umbrella sampling simulations predict the energy required to separate a graphene sheet from a graphite stack in both the presence/absence of the graphene-exfoliant peptide, P1. The free-energy barrier for reunification of two P1-coated graphene sheets is similarly calculated. Under sonication, the benefit from the relatively lower free-energy barrier associated with exfoliation in the absence of the peptide is negated by its facile reunification postsonication. In contrast, although P1 slightly increases the energy barrier to exfoliation under sonication, the peptides confer high-energy barriers to sheet reunification, thus ensuring stable aqueous graphene dispersions.