Illite/smectite (I/S) and illite samples that appear to be 1Md polytypes on the basis of the lack of diagnostic reflections can be resolved as partly either 1M or 2M1 or both by either vapor solvation in ethylene glycol for 40 to 80 hr at ambient temperatures or for 4 hr at 80°C, or by heating to 375°C for 2 hr. If samples are so treated, a distinct narrowing of the I/S 003/005 peak occurs and diagnostic hkl reflections are revealed. These treatments, however, do not seem to affect diagnostic polytypic peak intensities, but rather the adjacent background. We propose that the 1Md term be restricted to its original definition—the disordered polytype associated with only the 1M ordered polytype. For illites in which disorder exists with a mixture of polytypes, the generic term Ad (disordered group A micas) should be used. Correct polytype determination of illitic material is significant because it reveals thermal history of the sediments and allows greater understanding of the depositional and diagenetic history of sedimentary basins.

Study of the transformation of smectite to illite, chlorite or vermiculite via interstratified clay minerals needs precise qualitative and quantitative determinations of the different layers in the mixed-layer clays and is generally based on X-ray diffraction (XRD) patterns after specific treatments of the clay samples. Saturation with K or Mg followed by ethylene glycol (EG) solvation are classical methods used to identify high-charge smectite and vermiculite. These procedures have been applied to two experimental clays, one composed of smectite layers and the second, a mixture of vermiculite and smectite layers. Different methods of glycolation (EG vapor or liquid EG) produce significant differences in the XRD patterns. Comparison with literature data indicates that K-saturated, high-charge smectite (≈0.8 < total charge <1/unit-cell) and Mg-vermiculite (whatever its charge) do not expand in ethylene glycol vapor (d values ≈14–15 Å). Expansion to 17 Å in liquid ethylene glycol occurs for Mg-vermiculite with a total charge of <~1.2/unit-cell and for K-saturated, high-charge smectite, when the tetrahedral charge is <≈0.7/unit-cell. This study shows that: (1) glycolation procedures need to be standardized; (2) the use of saturation protocols using both liquid ethylene glycol and ethylene glycol vapor yields useful additional information about the distribution of charges in clay minerals.