Electrochemical synthesis
has emerged as a promising
approach for
the large-scale production of graphene-based two-dimensional (2D)
materials. Electrochemical intercalation of ions and molecules between
graphite layers plays a key role in the synthesis of graphene with
controllable thickness. However, there is still a limited understanding
regarding the impact of intercalant molecules. Herein, we investigated
a series of anionic species (i.e., ClO4
–, PF6
–, BF4
–, HSO4
–, CH3SO3
–, and TsO–) and examined their
wedging process between the weakly bonded layered materials driven
by electrochemistry. By combining cyclic voltammetry, X-ray diffraction
(XRD), and Raman spectroscopy, along with density functional theory
(DFT) calculations, we found that stage-2 graphite intercalation compounds
(GICs) can be obtained through intercalation of ClO4
–, PF6
–, or BF4
– anions into the adjacent graphene bilayers. The
anodic exfoliation step based on ClO4
––GIC in (NH4)2SO4 (aq.) resulted
in the formation of bilayer-rich (>57%) electrochemically exfoliated
graphene oxide (EGO), with a high yield (∼85 wt %). Further,
the physicochemical properties of these EGO can be readily customized
through electrochemical reduction and modification with different
surfactants. This versatility allows for precise tailoring of EGO,
making it feasible for energy and electronic applications such as
electrodes in electrochemical capacitors and functional composites
in wearable electronics.