Metal-Oxide-Based Nucleation Process under Confined Conditions: Two Mixed-Valence V6-Type Aggregates Closing the W48 Wheel-Type Cluster Cavities
Getting together helps: The wheel‐shaped {P8W48} polyoxotungstate (see picture) provides a reaction chamber for the directed assembly of two unprecedented mixed‐valence vanadium oxide cavity‐capping groups based on linked octahedra and tetrahedra with VIV and VV centers, respectively. The magnetic a...
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| Published in: | Angewandte Chemie International Edition Vol. 46; no. 24; pp. 4477 - 4480 |
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| Main Authors: | , , , , , , , , , |
| Format: | Journal Article |
| Language: | English |
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Weinheim
WILEY-VCH Verlag
2007
WILEY‐VCH Verlag |
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| ISSN: | 1433-7851, 1521-3773 |
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| Abstract | Getting together helps: The wheel‐shaped {P8W48} polyoxotungstate (see picture) provides a reaction chamber for the directed assembly of two unprecedented mixed‐valence vanadium oxide cavity‐capping groups based on linked octahedra and tetrahedra with VIV and VV centers, respectively. The magnetic and electronic properties are controlled by the confined conditions. |
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| AbstractList | Getting together helps: The wheel‐shaped {P8W48} polyoxotungstate (see picture) provides a reaction chamber for the directed assembly of two unprecedented mixed‐valence vanadium oxide cavity‐capping groups based on linked octahedra and tetrahedra with VIV and VV centers, respectively. The magnetic and electronic properties are controlled by the confined conditions. |
| Author | Dressel, Martin Tsukerblat, Boris Pope, Michael T. Bögge, Hartmut Thouvenot, René van Slageren, Joris Todea, Ana Maria Gouzerh, Pierre Bell, Aidan Müller, Achim |
| Author_xml | – sequence: 1 givenname: Achim surname: Müller fullname: Müller, Achim email: a.mueller@uni-bielefeld.de organization: Fakultät für Chemie der Universität, Postfach 100131, 33501 Bielefeld, Germany, Fax: (+49) 521-106-6003 – sequence: 2 givenname: Michael T. surname: Pope fullname: Pope, Michael T. email: popem@georgetown.edu organization: Department of Chemistry, Georgetown University, Box 571227, Washington, DC 20057, USA, Fax: (+1) 202-687-6209 – sequence: 3 givenname: Ana Maria surname: Todea fullname: Todea, Ana Maria organization: Fakultät für Chemie der Universität, Postfach 100131, 33501 Bielefeld, Germany, Fax: (+49) 521-106-6003 – sequence: 4 givenname: Hartmut surname: Bögge fullname: Bögge, Hartmut organization: Fakultät für Chemie der Universität, Postfach 100131, 33501 Bielefeld, Germany, Fax: (+49) 521-106-6003 – sequence: 5 givenname: Joris surname: van Slageren fullname: van Slageren, Joris organization: 1. Physikalisches Institut, Universität Stuttgart, Pfaffenwaldring 57, 70550 Stuttgart, Germany – sequence: 6 givenname: Martin surname: Dressel fullname: Dressel, Martin organization: 1. Physikalisches Institut, Universität Stuttgart, Pfaffenwaldring 57, 70550 Stuttgart, Germany – sequence: 7 givenname: Pierre surname: Gouzerh fullname: Gouzerh, Pierre organization: Laboratoire de Chimie Inorganique et Matériaux Moléculaires (UMR CNRS 7071), Université Pierre et Marie Curie-Paris 6, 4 place Jussieu, 75252 Paris, France – sequence: 8 givenname: René surname: Thouvenot fullname: Thouvenot, René organization: Laboratoire de Chimie Inorganique et Matériaux Moléculaires (UMR CNRS 7071), Université Pierre et Marie Curie-Paris 6, 4 place Jussieu, 75252 Paris, France – sequence: 9 givenname: Boris surname: Tsukerblat fullname: Tsukerblat, Boris organization: Department of Chemistry, Ben-Gurion University of the Negev, Beer Sheva, Israel – sequence: 10 givenname: Aidan surname: Bell fullname: Bell, Aidan organization: Fakultät für Chemie der Universität, Postfach 100131, 33501 Bielefeld, Germany, Fax: (+49) 521-106-6003 |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/17487914$$D View this record in MEDLINE/PubMed |
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| Notes | istex:0C8942EE4BBC9EA01E1131F25BAE956E3833B564 German-Israeli Foundation Volkswagenstiftung Deutsche Forschungsgemeinschaft European Union - No. MRTN-CT-2003-504880 Fonds der Chemischen Industrie Petroleum Research Fund A.M., J.S., and M.D. gratefully acknowledge the financial support of the Deutsche Forschungsgemeinschaft. A.M. further acknowledges the financial support of the Fonds der Chemischen Industrie, the Volkswagenstiftung, and the European Union (together with A.B.) (MRTN-CT-2003-504880). A.M. and B.T. gratefully acknowledge the financial support of the German-Israeli Foundation for Scientific Research and Development (GIF). M.T.P. acknowledges support from the Alexander von Humboldt Foundation and the Petroleum Research Fund administered by the American Chemical Society. ark:/67375/WNG-D1KPB07T-8 Alexander von Humboldt Foundation ArticleID:ANIE200700441 A.M., J.S., and M.D. gratefully acknowledge the financial support of the Deutsche Forschungsgemeinschaft. A.M. further acknowledges the financial support of the Fonds der Chemischen Industrie, the Volkswagenstiftung, and the European Union (together with A.B.) (MRTN‐CT‐2003‐504880). A.M. and B.T. gratefully acknowledge the financial support of the German–Israeli Foundation for Scientific Research and Development (GIF). M.T.P. acknowledges support from the Alexander von Humboldt Foundation and the Petroleum Research Fund administered by the American Chemical Society. ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
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| References | Other examples include equatorial W centers in [AsIII2W21O69(H2O)]6− (Y. Jeannin, J. Martin-Frère, J. Am. Chem. Soc. 1981, 103, 1664-1667) and [PV2W21O71(H2O)3]6 M. Gross, Chem. Br. 2003, (8), 18. M. B. Robin, P. Day, Adv. Inorg. Chem. Radiochem. 1967, 10, 247-422. R. Contant, A. Tézé, Inorg. Chem. 1985, 24, 4610-4614. L. Pauling, The Nature of the Chemical Bond, Ithaca, New York, 1948 A. Müller, S. Roy, in The Chemistry of Nanomaterials: Synthesis, Properties and Applications (Eds.: C. N. R. Rao, A. Müller, A. K. Cheetham), Wiley-VCH, Weinheim, 2004, 452-475). J. J. Altenau, M. T. Pope, R. A. Prados, H. So, Inorg. Chem. 1975, 14, 417-421. Examples of P8W48 complexes containing single-valence guests include [Cu20Cl(OH)24(H2O)12(P8W48O184)]25− (S. S. Mal, U. Kortz, Angew. Chem. 2005, 117, 3843-3846 H. So, M. T. Pope, Inorg. Chem. 1972, 11, 1441-1443 From molybdate solutions under reducing conditions finally a Mo37-type species is formed: A. Müller, J. Meyer, E. Krickemeyer, C. Beugholt, H. Bögge, F. Peters, M. Schmidtmann, P. Kögerler, M. J. Koop, Chem. Eur. J. 1998, 4, 1000-1006. R. L. Belford, N. D. Chasteen, H. So, R. E. Tapscott, J. Am. Chem. Soc. 1969, 91, 4675-4680. H. So, C. M. Flynn, Jr., M. T. Pope, J. Inorg. Nucl. Chem. 1974, 36, 329-332 The extinction coefficient per VIV center (ca. 1900 M−1 cm−1) in 2 is approximately three times greater than that observed in other tungstovanadates (S. P. Harmalker, M. A. Leparulo, M. T. Pope, J. Am. Chem. Soc. 1983, 105, 4286-4292). This is attributed to the larger V-O-W angles (162-164°) in 2, which favor greater electron delocalization from VIV to WVI. M. T. Pope, Heteropoly and Isopoly Oxometalates, Springer, Berlin, 1983. F. A. Cotton, G. Wilkinson, C. A. Murillo, M. Bochmann, Advanced Inorganic Chemistry, 6th ed., Wiley, New York, 1999 O. Glemser, A. Müller, Z. Anorg. Allg. Chem. 1963, 325, 220-224 and references cited therein. Angew. Chem. Int. Ed. 2005, 44, 3777-3780) and {Ln4(H2O)28[K⊂P8W48O184(H4W4O12)2Ln2(H2O)10]13−}x (Ln=La, Ce, Pr, Nd M. Zimmermann, N. Belai, R. J. Butcher, M. T. Pope, E. V. Chubarova, M. H. Dickman, U. Kortz, Inorg. Chem. 2007, 46, 1737-1740). Kortz has also reported other Cu20-encapsulated anions as well as complexes incorporating four Ni2+, Co2+, and VVO2+ cations A. Müller, S. Roy, J. Mater. Chem. 2005, 15, 4673-4677 and C. M. Tourné, G. F. Tourné, T. J. R. Weakley, J. Chem. Soc. Dalton Trans. 1986, 2237-2242). The problem is of basic importance for larger species such as Mo132, Mo72Fe30, and Mo154. In the first two species, the MoO bonds are preferably directed outwards (ca. 80 %), but according to a disorder also approximately 20 % Mo(OH2) groups are directed outwards. In the latter ring-type species, the situation is more complicated because of the presence of more (different) building units. In any case, there is a preference for H2O ligands on the outer periphery (for compound types, see, for example D. P. Smith, H. So, J. Bender, M. T. Pope, Inorg. Chem. 1973, 12, 685-688 A. Müller, S. Q. N. Shah, H. Bögge, M. Schmidtmann, Nature 1999, 397, 48-50. 1983; 105 2005 2005 2007; 117 44 46 1974; 36 1969; 91 1967; 10 1973; 12 1963; 325 1975; 14 1983 1999; 397 1981 1986 2005 2004; 103 15 2003 1948 1998; 4 1972; 11 1985; 24 1999 |
| References_xml | – reference: L. Pauling, The Nature of the Chemical Bond, Ithaca, New York, 1948; – reference: Other examples include equatorial W centers in [AsIII2W21O69(H2O)]6− (Y. Jeannin, J. Martin-Frère, J. Am. Chem. Soc. 1981, 103, 1664-1667) and [PV2W21O71(H2O)3]6− ( – reference: H. So, M. T. Pope, Inorg. Chem. 1972, 11, 1441-1443; – reference: M. B. Robin, P. Day, Adv. Inorg. Chem. Radiochem. 1967, 10, 247-422. – reference: R. L. Belford, N. D. Chasteen, H. So, R. E. Tapscott, J. Am. Chem. Soc. 1969, 91, 4675-4680. – reference: From molybdate solutions under reducing conditions finally a Mo37-type species is formed: A. Müller, J. Meyer, E. Krickemeyer, C. Beugholt, H. Bögge, F. Peters, M. Schmidtmann, P. Kögerler, M. J. Koop, Chem. Eur. J. 1998, 4, 1000-1006. – reference: J. J. Altenau, M. T. Pope, R. A. Prados, H. So, Inorg. Chem. 1975, 14, 417-421. – reference: R. Contant, A. Tézé, Inorg. Chem. 1985, 24, 4610-4614. – reference: A. Müller, S. Roy, in The Chemistry of Nanomaterials: Synthesis, Properties and Applications (Eds.: C. N. R. Rao, A. Müller, A. K. Cheetham), Wiley-VCH, Weinheim, 2004, 452-475). – reference: C. M. Tourné, G. F. Tourné, T. J. R. Weakley, J. Chem. Soc. Dalton Trans. 1986, 2237-2242). The problem is of basic importance for larger species such as Mo132, Mo72Fe30, and Mo154. In the first two species, the MoO bonds are preferably directed outwards (ca. 80 %), but according to a disorder also approximately 20 % Mo(OH2) groups are directed outwards. In the latter ring-type species, the situation is more complicated because of the presence of more (different) building units. In any case, there is a preference for H2O ligands on the outer periphery (for compound types, see, for example: – reference: The extinction coefficient per VIV center (ca. 1900 M−1 cm−1) in 2 is approximately three times greater than that observed in other tungstovanadates (S. P. Harmalker, M. A. Leparulo, M. T. Pope, J. Am. Chem. Soc. 1983, 105, 4286-4292). This is attributed to the larger V-O-W angles (162-164°) in 2, which favor greater electron delocalization from VIV to WVI. – reference: F. A. Cotton, G. Wilkinson, C. A. Murillo, M. Bochmann, Advanced Inorganic Chemistry, 6th ed., Wiley, New York, 1999; – reference: M. Gross, Chem. Br. 2003, (8), 18. – reference: Examples of P8W48 complexes containing single-valence guests include [Cu20Cl(OH)24(H2O)12(P8W48O184)]25− (S. S. Mal, U. Kortz, Angew. Chem. 2005, 117, 3843-3846; – reference: Angew. Chem. Int. Ed. 2005, 44, 3777-3780) and {Ln4(H2O)28[K⊂P8W48O184(H4W4O12)2Ln2(H2O)10]13−}x (Ln=La, Ce, Pr, Nd) ( – reference: O. Glemser, A. Müller, Z. Anorg. Allg. Chem. 1963, 325, 220-224 and references cited therein. – reference: H. So, C. M. Flynn, Jr., M. T. Pope, J. Inorg. Nucl. Chem. 1974, 36, 329-332; – reference: M. T. Pope, Heteropoly and Isopoly Oxometalates, Springer, Berlin, 1983. – reference: A. Müller, S. Roy, J. Mater. Chem. 2005, 15, 4673-4677 and – reference: A. Müller, S. Q. N. Shah, H. Bögge, M. Schmidtmann, Nature 1999, 397, 48-50. – reference: M. Zimmermann, N. Belai, R. J. Butcher, M. T. Pope, E. V. Chubarova, M. H. Dickman, U. Kortz, Inorg. Chem. 2007, 46, 1737-1740). Kortz has also reported other Cu20-encapsulated anions as well as complexes incorporating four Ni2+, Co2+, and VVO2+ cations ( – reference: D. P. Smith, H. So, J. Bender, M. T. Pope, Inorg. Chem. 1973, 12, 685-688; – volume: 14 start-page: 417 year: 1975 end-page: 421 publication-title: Inorg. Chem. – year: 1983 – volume: 397 start-page: 48 year: 1999 end-page: 50 publication-title: Nature – volume: 10 start-page: 247 year: 1967 end-page: 422 publication-title: Adv. Inorg. Chem. Radiochem. – volume: 4 start-page: 1000 year: 1998 end-page: 1006 publication-title: Chem. Eur. J. – volume: 36 start-page: 329 year: 1974 end-page: 332 publication-title: J. Inorg. Nucl. Chem. – volume: 11 start-page: 1441 year: 1972 end-page: 1443 publication-title: Inorg. Chem. – volume: 24 start-page: 4610 year: 1985 end-page: 4614 publication-title: Inorg. Chem. – year: 1948 – volume: 103 15 start-page: 1664 2237 4673 452 year: 1981 1986 2005 2004 end-page: 1667 2242 4677 publication-title: J. Am. Chem. Soc. J. Chem. Soc. Dalton Trans. J. Mater. Chem. – volume: 91 start-page: 4675 year: 1969 end-page: 4680 publication-title: J. Am. Chem. Soc. – volume: 117 44 46 start-page: 3843 3777 1737 year: 2005 2005 2007 end-page: 3846 3780 1740 publication-title: Angew. Chem. Angew. Chem. Int. Ed. Inorg. Chem. – volume: 325 start-page: 220 year: 1963 end-page: 224 publication-title: Z. Anorg. Allg. Chem. – volume: 12 start-page: 685 year: 1973 end-page: 688 publication-title: Inorg. Chem. – volume: 105 start-page: 4286 year: 1983 end-page: 4292 publication-title: J. Am. Chem. Soc. – start-page: 8 year: 2003 publication-title: Chem. Br. – year: 1999 |
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| SubjectTerms | confined geometries directed‒assembly electronic structure mixed‒valent compounds polyoxometalates |
| Title | Metal-Oxide-Based Nucleation Process under Confined Conditions: Two Mixed-Valence V6-Type Aggregates Closing the W48 Wheel-Type Cluster Cavities |
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