and Yb and Their Relation to the Armstrongite (CaZr(Si 6O15)·3H2O) Structure. -K 7.814Sm3Si12O32(OH)0.814·0.77H2O (I), K7.04Tb3Si12O32.02·1.36H2O (II), K2GdAlSi4O12·0.25H2O (III), K2SmAlSi4O12·0.375H2O (IV), and K4Yb2Si8O21 (V) are hydrothermally synthesized from aqueous mixtures of Ln 2O3 (Ln: Yb, Sm, Tb, Gd), SiO 2, Al2O3, and KOH (autoclave equipped with either copper or nickel containers, 500 C, 30 d). The crystal structures of the compounds are determined by single crystal XRD. (I) and (II) crystallize in the triclinic space group P1 with Z = 1 and their structures contain Si 12O32 units of a single-layer type. Compounds (III), (IV), and (V) crystallize in the monoclinic space group C2/c with Z = 8 for (III) and (IV) and Z = 4 for (V). The aluminosilicates (III) and (IV) are built of AlSi 4O12 units of a double-layer type, whereas (V) contains a new tubular type of Si 8O21 unit. The relation of the silicate layers and frameworks in these compounds to the armstrongite silicate framework is discussed. -(TAROEV, V. K.; KASHAEV, A. A.; MALCHEREK, T.; GOETTLICHER*, J.; KANEVA, E. V.; VASILJEV, A. D.; SUVOROVA, L. F.; SUVOROVA, D. S.; TAUSON, V. L.; J. Solid State Chem. 227 (2015) 196-203, http://dx.