Journal of Cluster Science, Vol. 11, No. 3, 2000 Organically Templated Vanadium Oxide Phases: Synthesis and Structures of [H 3 NCH 2 CH 2 NH 3 ][V 2 O 6 ] and [HN(CH 2 CH 2 ) 3 NH][V V 2 V IV 4 O 14 ]}H 2 O 1 M. Ishaque Khan, 2, 5 Thomas Hope, 2 Sabri Cevik, 2 Chong Zheng, 3 and Douglas Powell 4 Received March 2, 2000 The synthesis and crystal structures of [H 3 NCH 2 CH 2 NH 3 ][V 2 O 6 ]( 1) and [HN(CH 2 CH 2 ) 3 NH][V V 2 V IV 4 O 14 ]}H 2 O( 2) are described. The structure of the oxidized compound 1 consists of parallel stacks of vanadium oxide chains of corner sharing [ VO 4 ] tetrahedra. The chains are stabilized by extensive hydrogen bonding involving oxide ligands of the chains and ethylenediam- monium ions which fill the space between the stacks of chains. The structure of compound 2 consists of vanadium oxide layers separated by doubly protonated 1,4-diazabicyclo[2.2.2]octane and lattice water. The vanadium oxide layers, containing mixed-valence vanadium (V V and V IV ) centers, are composed of zigzag ribbons of edge-sharing [VO 5 ] square pyramids interconnected by [VO 4 ] tetrahedra. Crystal data.C 2 H 10 N 2 O 6 V 2 , 1: monoclinic, space group P2 1 c (No. 14), a =5.5359(5), b =12.9430(12), c =5.6856(5) A 1 , : =90, ; =97.460(2), #=90%, V=403.93(6) A 1 3 , Z=2. A total of 2506 reflections ( % max =27.89%) was collected, of which 954 were used to resolve the structure. The structure was solved by direct methods and least-squares refinement converged at R=0.0592. C 6 H 16 N 2 O 15 V 6 , 2: monoclinic, space group C2 (No. 5), a =19.303(4), b = 6.667(2), c =7.579(2) A 1 , : =90, ;=111.31(2), # =90%, V=908.4(4) A 1 3 , Z=2. A total of 1779 reflections was collected, of which 1591 unique reflections were 433 1040-7278000900-043318.000  2000 Plenum Publishing Corporation 1 Dedicated to Professor Kenneth Schug on the occasion of his 75th birthday. 2 Department of Biological, Chemical, and Physical Sciences, Illinois Institute of Technology, Chicago, Illinois 60616. 3 Department of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115. 4 Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706. 5 To whom correspondence should be addressed. E-mail: Ishaque.Khaniit.edu.