A possible structure for kaolinite was first put forward by Pauling (1930) in a paper dealing generally with the structures of layer-type minerals, chlorites, micas, &c. He suggested that the structure consisted of a sheet of Si–O tetrahedra arranged in a hexagonal network with a superposed sheet of Al–(O,OH) octahedra, the two together forming a layer of composition Al2Si2O5(OH)4 (fig. 2). Ross and Kerr (1931), from a detailed microscopic study of the kaolin minerals, concluded that the symmetry of kaolinite is ‘probably monoclinic’. The first attempt at a detailed structure analysis was made by Gruner (1932a) from X-ray powder photographs. The reflections, some 40 altogether, were indexed on the basis of a monoclinic cell with a 5·14, b 8·90, c 14·51Å., β 100° 12′.

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