The
macromolecular evolution of coal in proximity to intrusion
zones provides a means of exploring the coal to coal-derived natural
graphite (CDNG) transitions. Here, samples with different metamorphic
grades from anthracite to CDNG were examined based on X-ray diffraction
(XRD), Raman spectroscopy, and high-resolution transmission electron
microscopy (HRTEM) image analyses. The anthracite aromatic layers
were limited with the average layers in a stack being ∼10,
with a height and width of ∼4 and ∼5 nm, respectively.
The CDNG had higher crystallinity with the number of layers in a stack
being ∼120, with a height and width of ∼40 and ∼70
nm, respectively. The D1/G area ratios (Raman) decreased from 6.5
to 0.3 (from anthracite to graphite). The short fringe length (0.3–1.14
nm) distributions account for >90% of anthracite, while meta-anthracite
and semi-graphite had lower contributions of 88.5 and 81.5%. The fringe
orientation value (the frequency of the total fringe length within
the most prominent 15° bin) increased from 22.1 (anthracite)
to 29.4% (meta-anthracite). For semi-graphite, the orientation was
high reaching 72.5%. The high-grade CDNG had essentially 100% of fringes
oriented within 15°. The fringe curvature was high in the initial
anthracite (90.9% of the fringes) but this decreased to 85.5% in the
anthracite of higher metamorphic grade. In meta-anthracite, the curvature
decreased to 80.1% as the fringe length further increased. The fringe
curvature became less frequent (51.5%) in the highly ordered CDNG.
The structural evolution from anthracite to meta-anthracite followed
the general coalification characteristics: fringes are increasingly
longer, oriented, and linear but limited to small stacks. An extensive
molecular amalgamation occurs, forming fringe curvature and dislocations
in the meta-anthracite to semi-graphite transitions. With graphitization,
the curvature and the dislocations decrease forming the well-ordered
graphite.