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The Si-Al distribution in the tetrahedral sheet of phyllosilicates having Si:Al ratios near 3:1 has been analyzed by a combination of magic angle spinning-nuclear magnetic resonance spectroscopy, Monte Carlo simulation, and calculations of electrostatic energies. The results of this analysis indicate that Si-Al distribution is mainly controlled by electrostatic requirements of homogeneous dispersion of Al and local balance of interlayer charges. Long- and short-range ordered Si-Al distribution models, complying with the above requirements, differ little in energy, and no evidence for long-range order has been found. In muscovite-2M1, phlogopite-lM, and Llano vermiculite, meta and para dispositions for Al in hexagonal rings of tetrahedral cations occur in a ratio meta: para of about 2:1.

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