Since the initial work of Mobil researchers on the synthesis of mesoporous silica, [1] a lot of work has been devoted to extend the composition of mesoporous materials to metal oxides other than silica for applications in acid, redox catalysis, or photocatalytic processes. [2±4] Polyhedron 1998, 17, 845 ± 850; b) V. L. Pecoraro, G. B. Wong, T. A. Kent, K. N. Raymond, J. Am. Chem. Soc. 1983, 105, 4617 ± 4623. [16] X-ray crystal data for 1: C 36 H 63 CrN 6 , M r 589.85, triclinic, P1 ≈ , a 9.9754(17), b 12.707(2), c 16.687(3) ä, a 77.228(3), b 75.734 (3), g 70.655(4)8, V 1911.5(6) ä 3 , Z 2, 1 calcd 1.025 g cm À3 , m 0.326 mm À1 , 8755 independent reflections harvested from 2450 frames of data collected at 20 s per frame and 0.28 between frames yielded 13 711 integrated intensities, R int 0.029. All data were included in the refinement. For I > 2s(I), R 1 0.0685 and wR 2 0.1856; including weak data R 1 0.1585 and wR 2 0.2141. Siemens/ Bruker P4-CCD, Mo Ka radiation (l 0.7107 ä), graphite monochromator, 2V max 56.58, T 295(2) K. Suitable crystals for single-crystal X-ray analysis were selected and mounted inside thin-walled capillaries in a dry box under nitrogen atmosphere. Data collection and integration used the Bruker SMART and SAINT software. Empirical absorption corrections were calculated using the program SA-DABS. [17] Solution and refinement used the programs SHELXS [17] and SHELXL-93. [17] All non-hydrogen atoms were described anisotropically. Hydrogen atoms were placed in calculated positions. The 3,5-di-tert-butylpyrazolato ligands typically show severe disorder in the tert-butyl groups, which results in modeling difficulties and high R values. However, other criteria of chemical and crystallographic reasonableness show these to be acceptable structural models. CCDC-175570 (1) and CCDC-175571 (2 ¥ (C 6 H 14 ) 0.5 ) contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/conts/retrieving.html (or from the Cambridge Crystallographic Data Centre, 12, Union Road, ) are gratefully acknowledged for their collaboration in NMR and Mˆssbauer experiments.