Bio-inspired
approaches represent potentially transformational
methods to fabricate and activate non-natural materials for applications
ranging from biomedical diagnostics to energy harvesting platforms.
Recently, bio-based methods for the exfoliation of graphene in water
have been developed, resulting in peptide-capped nanosheets; however,
a clear understanding of the reaction system and peptide ligand structure
remains unclear, limiting the advance of such approaches. Here the
effects of reaction solution conditions and peptide ligand structure
were systematically examined for graphene exfoliation, identifying
key parameters to optimize material production. For this, the P1 peptide,
identified with affinity for graphene, was exploited to drive exfoliation
of bulk graphite to generate the final materials. The peptide was
modified at both the N- and C-terminus with a 10-carbon chain fatty
acid to explore the effects of a hydrophobic domain on the exfoliation
process. The system was examined as a function of sonication time,
pH, reagent concentration, and graphite source, where the final materials
were fully characterized using a suite of approaches. Collectively,
these results demonstrated that maximum graphene production was achieved
using the parent P1 peptide after 12 h of sonication under basic conditions.
While the exfoliation efficiency was slightly lower for the fatty
acid modified peptides, the graphene produced using these biomolecules
had fewer defects incorporated, potentially from the wrapping of the
nanosheet edge by the aliphatic domain. Such results are important
to provide key reaction designs to optimize the reproducibility of
graphene exfoliation using biomimetic approaches.