High-resolution Al-27 and Si-29 NMR were employed to characterize layered s
ilicates in the suite of eight Argonne Premium coals. Analyses were perform
ed on native coals directly, or fractions isolated by sink-float techniques
. Mineral phases of kaolinite, quartz, and illite-montmorillinite clays cou
ld readily be distinguished nonquantitatively by Si-29 NMR techniques using
direct detection or cross polarization. Al-27 NMR was used to determine qu
antitatively the amounts of tetrahedral and octahedral aluminum forms prese
nt. The Al-27 NMR results were consistent with mineralogical analyses by XR
D, showing that increases in tetrahedral content paralleled illitization of
the clay minerals. A remarkably good relationship also was found between t
he total amount of tetrahedral aluminum associated with the mineral matter
and degree of maturation of the organic matter in the coal. The data sugges
t that illitization of the clays can be used as a mineralogical thermal mat
urity indicator for Type II kerogens, as demonstrated for the Argonne Premi
um coals, provided that contributions from organo-chelated aluminum species
and detrital mineral matter are taken into account.