Pyrophyllite solid solutions, Al2Si4−xAlxO10−x(OH2+x), have been synthesized from a gel and from lightly ground and milled natural materials. Sohd solutions crystallize from structurally degraded or amorphous starting materials due to the tendency for Al3+ to enter tetrahedral sites. The extent of sohd solution is small; synthesis from a gel yielded pyrophyllite with the formula Al2.0(Si3.8Al0.2)O9.8,(OH)2.2

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