Formation of a ring-shaped reduced 'metal oxide' with the simple composition [(MoO3)176(H2O)80H32]

Angewandte Chemie - International Edition

Volumn 37, Issue 9, 1998, Pages 1220-1223

  Müller, Achim ^a   Krickemeyer, Erich ^a   Bögge, Hartmut ^a   Schmidtmann, Marc ^a   Beugholt, Christian ^a   Kögerler, Paul ^a   Lu, Canzhong ^a  

^a BIELEFELD UNIVERSITY   (Germany)

Author keywords

Inorganic rings; Molybdenum; Molybdenum blue; Polyoxometalates; Supramolecular chemistry

Indexed keywords

EID: 0037793956     PISSN: 14337851     EISSN: None     Source Type: Journal    
DOI: 10.1002/(SICI)1521-3773(19980518)37:9<1220::AID-ANIE1220>3.0.CO;2-G     Document Type: Article

References (46)

1. a) A. Müller, E. Krickemeyer, J. Meyer, H. Bögge, F. Peters, W. Plass, E. Diemann, S. Dillinger, F. Nonnenbruch, M. Randerath, C. Menke, Angew. Chem. 1995, 107, 2293-2295; Angew. Chem. Int. Ed. Engl. 1995, 34, 2122-2124 (cf. [12] there);
2. a) A. Müller, E. Krickemeyer, J. Meyer, H. Bögge, F. Peters, W. Plass, E. Diemann, S. Dillinger, F. Nonnenbruch, M. Randerath, C. Menke, Angew. Chem. 1995, 107, 2293-2295; Angew. Chem. Int. Ed. Engl. 1995, 34, 2122-2124 (cf. [12] there)
3. b) A. Müller, C. Beugholt, Nature 1996, 383, 296-297
4. c) H. Plenio, Angew. Chem. 1997, 109, 58-360; Angew. Chem. Int. Ed. Engl. 1997, 36, 348-351.
5. c) H. Plenio, Angew. Chem. 1997, 109, 58-360; Angew. Chem. Int. Ed. Engl. 1997, 36, 348-351.
6. The term (conservative) self-organization seems to be justified for an aggregation process that leads to extremely large and/or complicated molecular structures under one-pot conditions. However, the prerequisite should be that an intermediate formed during the self-aggregation process possesses such a directing effect on the following processes that the complex structure cannot be synthesized in a stepwise fashion by the chemist. In this sense, the formation of a crystal showing translation invariance from a nucleus cannot be described as complex as it is due to the operation of translation symmetry.
7. Cf. K. Wassermann, M. H. Dickman, M. T. Pope, Angew. Chem. 1997, 109, 1513-1516; Angew. Chem. Int. Ed. Engl. 1997, 36, 1445-1448.
8. Cf. K. Wassermann, M. H. Dickman, M. T. Pope, Angew. Chem. 1997, 109, 1513-1516; Angew. Chem. Int. Ed. Engl. 1997, 36, 1445-1448.
9. I. D. Brown in Structure and Bonding in Crystals, Vol. II (Ed.: M. O'Keeffe, A. Navrotsky), Academic Press, New York, 1981, pp. 1-30.
10. max = 45°). The crystals of 2 were taken directly out of the mother liquor and measured immediately to prevent weathering through loss of crystal water. The measurements of individual crystals always led to the same result. The structure was solved with the programme SHELXS-96 and refined with the programme SHELXL-93 (G. M. Sheldrick, University of Göttingen, 1996 and 1993). Further details of the structure investigations can he obtained from the Fachinformationszentrum Karlsruhe, D-76344 Eggenstein-Leopoldshafen, Germany (fax: (+49)7247-808-666; e-mail: crysdata@fiz-karlsruhe.de), on quoting the number CSD-408508.
11. A. Müller, H. Reuter, S. Dillinger, Angew. Chem. 1995, 107, 2505-2539; Angew. Chem. Int. Ed. Engl. 1995, 34, 2328-2361, and references therein.
12. A. Müller, H. Reuter, S. Dillinger, Angew. Chem. 1995, 107, 2505-2539; Angew. Chem. Int. Ed. Engl. 1995, 34, 2328-2361, and references therein.
13. [8b] but generally speaking cause a change in reactivity.
14. a) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, F. Peters, C. Menke, J. Meyer, Angew. Chem. 1997, 109, 500-502; Angew.Chem. Int. Ed. Engl. 1997, 36, 484-486;
15. a) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, F. Peters, C. Menke, J. Meyer, Angew. Chem. 1997, 109, 500-502; Angew.Chem. Int. Ed. Engl. 1997, 36, 484-486;
16. b) A. Müller, E. Krickemeyer, H. Bögge, M. Schmidtmann, F. Peters, C. Lu, C. Beugholt, unpublished results;
17. c) A. Müller, F. Peters, M. T. Pope, D. Gatteschi, Chem. Rev. 1998, 98, 239-271.
18. The EHMO calculations are based on the positions of the atoms obtained from the X-ray structure analysis. Standard atomic parameters of the program were used (G. A. Landrum, YAeHMOP 2.0: "Yet Another Extended Hückel Molecular Orbital Package(Matrix Presented); URL: http://overlap.chem.cornell.edu/yaehmop). The positions of the H atoms were obtained on the basis of bond valence sums of the oxygen positions by molecular modeling calculations (generic UFF-plus force-field) using the CERIUS 3.2 software (CERIUS 3.2, Molecular Simulations, Cambridge 1993).
19. [8]
20. a) K. von der Heide, K. A. Hoffmann, Z. Anorg. Chem. 1896, 12, 279-292; V. Kohlschlüter, K. A. Hoffmann, Justus Liebigs Ann. Chem. 1898, 307, 323; Übersicht: E. Lassner, J. Less Common. Met. 1968, 15, 143-150;
21. a) K. von der Heide, K. A. Hoffmann, Z. Anorg. Chem. 1896, 12, 279-292; V. Kohlschlüter, K. A. Hoffmann, Justus Liebigs Ann. Chem. 1898, 307, 323; Übersicht: E. Lassner, J. Less Common. Met. 1968, 15, 143-150;
22. a) K. von der Heide, K. A. Hoffmann, Z. Anorg. Chem. 1896, 12, 279-292; V. Kohlschlüter, K. A. Hoffmann, Justus Liebigs Ann. Chem. 1898, 307, 323; Übersicht: E. Lassner, J. Less Common. Met. 1968, 15, 143-150;
23. b) see, for example, A. Müller, S. Sarkar, Angew. Chem. 1977, 89, 189-190; Angew. Chem. Int. Ed. Engl. 1977, 16, 183-184; ibid. 1977, 89, 479-480 or 1977, 16, 468-469; A. Müller, W. Eltzner, S. Sarkar, H. Bögge, P. J. Aymonino, N. Mohan, U. Seyer, P. Subramanian, Z. Anorg. Allg. Chem. 1983, 503, 22-36, and references therein;
24. b) see, for example, A. Müller, S. Sarkar, Angew. Chem. 1977, 89, 189-190; Angew. Chem. Int. Ed. Engl. 1977, 16, 183-184; ibid. 1977, 89, 479-480 or 1977, 16, 468-469; A. Müller, W. Eltzner, S. Sarkar, H. Bögge, P. J. Aymonino, N. Mohan, U. Seyer, P. Subramanian, Z. Anorg. Allg. Chem. 1983, 503, 22-36, and references therein;
25. b) see, for example, A. Müller, S. Sarkar, Angew. Chem. 1977, 89, 189-190; Angew. Chem. Int. Ed. Engl. 1977, 16, 183-184; ibid. 1977, 89, 479-480 or 1977, 16, 468-469; A. Müller, W. Eltzner, S. Sarkar, H. Bögge, P. J. Aymonino, N. Mohan, U. Seyer, P. Subramanian, Z. Anorg. Allg. Chem. 1983, 503, 22-36, and references therein;
26. b) see, for example, A. Müller, S. Sarkar, Angew. Chem. 1977, 89, 189-190; Angew. Chem. Int. Ed. Engl. 1977, 16, 183-184; ibid. 1977, 89, 479-480 or 1977, 16, 468-469; A. Müller, W. Eltzner, S. Sarkar, H. Bögge, P. J. Aymonino, N. Mohan, U. Seyer, P. Subramanian, Z. Anorg. Allg. Chem. 1983, 503, 22-36, and references therein;
27. b) see, for example, A. Müller, S. Sarkar, Angew. Chem. 1977, 89, 189-190; Angew. Chem. Int. Ed. Engl. 1977, 16, 183-184; ibid. 1977, 89, 479-480 or 1977, 16, 468-469; A. Müller, W. Eltzner, S. Sarkar, H. Bögge, P. J. Aymonino, N. Mohan, U. Seyer, P. Subramanian, Z. Anorg. Allg. Chem. 1983, 503, 22-36, and references therein;
28. c) see, for example, A. Müller, W. Eltzner, H. Bögge, S. Sarkar, Angew. Chem. 1982, 94, 555-556; Angew. Chem. Int. Ed. Engl. 1982, 21, 535-536; A. Müller, W. Eltzner, N. Mohan, ibid. 1979, 91, 158-159 or 1979, 18, 168-169;
29. c) see, for example, A. Müller, W. Eltzner, H. Bögge, S. Sarkar, Angew. Chem. 1982, 94, 555-556; Angew. Chem. Int. Ed. Engl. 1982, 21, 535-536; A. Müller, W. Eltzner, N. Mohan, ibid. 1979, 91, 158-159 or 1979, 18, 168-169;
30. c) see, for example, A. Müller, W. Eltzner, H. Bögge, S. Sarkar, Angew. Chem. 1982, 94, 555-556; Angew. Chem. Int. Ed. Engl. 1982, 21, 535-536; A. Müller, W. Eltzner, N. Mohan, ibid. 1979, 91, 158-159 or 1979, 18, 168-169;
31. c) see, for example, A. Müller, W. Eltzner, H. Bögge, S. Sarkar, Angew. Chem. 1982, 94, 555-556; Angew. Chem. Int. Ed. Engl. 1982, 21, 535-536; A. Müller, W. Eltzner, N. Mohan, ibid. 1979, 91, 158-159 or 1979, 18, 168-169;
32. d) P. Gouzerh, Y. Jeannin, A. Proust, F. Robert, ibid. 1989, 101, 1377-1378 and 1989, 28, 1363-1364; S. Zhang, Y. Wei, Q. Yu, M. Shao, Y. Tang, J. Am. Chem. Soc. 1997, 119, 6440-6441, and references therein;
33. d) P. Gouzerh, Y. Jeannin, A. Proust, F. Robert, ibid. 1989, 101, 1377-1378 and 1989, 28, 1363-1364; S. Zhang, Y. Wei, Q. Yu, M. Shao, Y. Tang, J. Am. Chem. Soc. 1997, 119, 6440-6441, and references therein;
34. d) P. Gouzerh, Y. Jeannin, A. Proust, F. Robert, ibid. 1989, 101, 1377-1378 and 1989, 28, 1363-1364; S. Zhang, Y. Wei, Q. Yu, M. Shao, Y. Tang, J. Am. Chem. Soc. 1997, 119, 6440-6441, and references therein;
35. e) W. F. Jakob, B. Jezowska, Roczniki, Chem. 1931, 11, 229-253;
36. f) K. Wieghardt, G. Backes-Dahmann, W. Swiridoff, J. Weiss, Inorg. Chem. 1983, 22, 1221-1224; A. Müller, W. Eltzner, unpublished results.
37. f) K. Wieghardt, G. Backes-Dahmann, W. Swiridoff, J. Weiss, Inorg. Chem. 1983, 22, 1221-1224; A. Müller, W. Eltzner, unpublished results.
38. [3] though the determination of the charge of their particular cluster anion - as was also pointed out - is not so difficult. This is due to the fact that the oxidation states of the metal centers are clearly known.
39. [14b] This simplifies of course the proof of functional groups on the one hand, but on the other complicates the differentiation of species with different numbers of these fragments, as in the case of 1 and 2.
40. A. Müller, J. Meyer, E. Krickemeyer, E. Diemann, Angew. Chem. 1996, 108, 1296-1299; Angew. Chem. Int. Ed. Engl. 1996, 35, 1206-1208;
41. A. Müller, J. Meyer, E. Krickemeyer, E. Diemann, Angew. Chem. 1996, 108, 1296-1299; Angew. Chem. Int. Ed. Engl. 1996, 35, 1206-1208;
42. b) A. Müller, M. Ohm, H. Bögge, unpublished results.
43. A. Müller, E. Diemann, B. Hollmann, H. Ratajczak, Naturwissenschaften 1996, 83, 321-322.
44. o)).
45. 2O ligands. (A. Müller, M. J. Koop, H. Bogge, M. Schmidtmann, Chem. Commun. submitted; A. Müller, E. Krickemeyer, M. J. Koop, S. Q. N. Shah, H. Bogge, M. Schmidtmann, Z. Anorg. Allg. Chem. submitted.).
46. 2O ligands. (A. Müller, M. J. Koop, H. Bogge, M. Schmidtmann, Chem. Commun. submitted; A. Müller, E. Krickemeyer, M. J. Koop, S. Q. N. Shah, H. Bogge, M. Schmidtmann, Z. Anorg. Allg. Chem. submitted.).