This
article presents a systematic work on the graphitization behavior
of graphene (Gr)–pitch composites. Two commercial pitches of
varying composition and sources (coal tar pitch and petroleum pitch)
and their Gr composites were subjected to a broad series of heat treatment
temperatures750, 1000, 1500, 2000, and 2500 °C. The trajectory
of the crystallite parameter growth was analyzed using X-ray diffraction
(XRD) with both in situ and ex situ heating. Incorporating a small
amount of Gr into the pitch yielded remarkable improvements in the
interplanar spacing, accompanied by increases of up to 60% and 200%
in the in-plane crystallite diameter and stacking height, correspondingly.
Thermogravimetric analysis/differential scanning calorimetry indicated
that Gr acts as a catalyst to lower the onset temperature of stabilizing
polymerization reactions, reduce devolatilization, and improve concatenation
reactions during carbonization. A qualitative assessment of the mesophase
was performed using scanning electron microscopy imaging. High-resolution
transmission electron microscopy (TEM) with in situ heating revealed
three mechanismschemical templating, physical templating,
and self-templating in the Gr–pitch composite. A noteworthy
feature of G peak splitting observed in the Raman spectrum for the
pitch composite provided supplementary evidence of templating. Raman
spectroscopy and TEM have been employed on graphitized samples to
acquire supplementary insights in conjunction with XRD-based crystallite
analysis.