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Title: Substitution of [sup [6,4]]Al in phlogopite: High-temperature solution calorimetry, heat capacities, and thermodynamic properties of the phlogopite-eastonite join

Journal Article · · American Mineralogist; (United States)
OSTI ID:6789435
;  [1]
  1. Princeton Univ., NJ (United States)

Enthalpies of solution of synthetic magnesium aluminum phlogopite samples K(Mg[sub 3[minus]x]Al[sub x])(Al[sub 1+x]Si[sub 3[minus]x])O[sub 10](OH)[sub 2] with 0.00 [le] X[sub East] [le] 0.92 were measured in molten 2PbO-B[sub 2]O[sub 3] at 977 K. The enthalpy of mixing for the phlogopite-eastonite join is large, asymmetric, and endothermic. The solid solution is destabilized more by [sup [6]]Mg,[sup [4]]Si substitution into eastonite than by [sup [6]]Al,[sup [4]]Al substitution into phlogopite, reflecting the increased strain in the mica structure at high [sup [6,4]]Al content that arises from increased lateral misfit between the smaller octahedral and larger tetrahedral sheets. The entropy of mixing has been calculated assuming a random distribution of Mg and Al on one octahedral site and a short-range ordered distribution of Al and Si on four tetrahedral sites. The calculated activity-composition relations predict a large region of immiscibility up to [approximately] 1,500 K that is consistent with observed limits of [sup [6,4]]Al substitution in naturally occurring Fe-poor phlogopite. The thermodynamic data for phlogopite and eastonite are assessed using the metastable reaction Phl + 3 Qtz = San + 3 En + H[sub 2]O, in which the breakdown of magnesium aluminum phlogopite also produces spinel. A standard enthalpy of formation of phlogopite from the elements at 298 K of [minus]6215.0 [plus minus] 3.5 kJ/mol is consistent with both data from high-temperature solution calorimetry and results from phase equilibria experiments. The standard enthalpy of formation of eastonite from the elements at 298 K is between [minus]6352 and [minus]6363 kJ/mol; the large uncertainty arises from estimating the heat capacity of eastonite. The P,T stability of phlogopite increases with increasing [sup [6,4]]Al content., 7 figs., 5 tabs.

DOE Contract Number:
FG02-85ER13437
OSTI ID:
6789435
Journal Information:
American Mineralogist; (United States), Vol. 77:11-12; ISSN 0003-004X
Country of Publication:
United States
Language:
English