Template Cooperation Effect Leading to the New Layered Aluminophosphate CN3H6·Al(HPO4)2·2H2O

CN 3 H 6 ·Al(HPO 4 ) 2 ·2H 2 O, prepared by hydrothermal methods at 120 °C, contains infinite stacks of guanidinium cations (intermolecule C···C separation ∼3.5 Å) interleaving a distinctive anionic aluminophosphate layer topology based on polyhedral eight-rings of vertex-sharing AlO 4 (OH 2 ) 2 octahedra and HPO 4 tetrahedra. Crystal data: CN 3 H 6 ·Al(HPO 4 ) 2 ·2H 2 O, M r = 315.05, orthorhombic, Pnma (No. 62), a = 6.965(2) Å, b = 20.624(4) Å, c = 7.168(2) Å, V = 1029.7(5) Å 3, Z = 4, R = 3.42%, R w = 3.40% [85 parameters, 829 observed reflections with I > 3σ( I )].