The first designed syntheses of bis-dimetal molecules in which the bridges are diamidate ligands |
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Authors: | Cotton F Albert Daniels Lee M Donahue James P Liu Chun Y Murillo Carlos A |
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Institution: | Department of Chemistry and Laboratory for Molecular Structure and Bonding, P.O. Box 30012, Texas A&M University, College Station, Texas 77842-3012, USA. cotton@tamu.edu |
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Abstract: | The first deliberate syntheses of molecules in which pairs of quadruply bonded Mo2 units are bridged by N,N'-diarylterephthaloyldiamidate (aryl = Ph, m-CF3Ph) ligands are described. The addition of neutral N,N'-diarylterephthaloyldiamide to 2 equiv of Mo2(DAniF)3(MeCN)2]+ (DAniF = N,N'-di-p-anisylformamidinate) followed by the introduction of excess H3CO- in MeCN results in the formation of (DAniF)3Mo2(C6H5)NC(O)C6H4(O)CN(C6H5)]Mo2(DAniF)3 (1) and (DAniF)3Mo2(m-CF3)C6H5]NC(O)C6H4(O)CN(m-CF3)C6H5]]Mo2(DAniF)3 (2). The DeltaE1/2 for the oxidation of each Mo2 unit is greater for these terephthaloyldiamidate-bridged molecules (approximately 100 mV) than for the analogous terephthalate-bridged compound (approximately 60 mV). Variation in the nature of the substituents on the diamidate nitrogen atoms offers a means to fine-tune the oxidation potentials of the Mo2 units. |
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