η5↔η3Hapticity interconversion in cycloheptadienyl molybdenum complexes

Abstract
A series of reactions of the general type [Mo(CO)2L25-C7H9)]++ L′→[Mo(CO)2(L′)L23-C7H9)]+, involving η5→η3 hapticity conversion at a molybdenum co-ordinated Cycloheptadienyl ring, have been examined. The specific examples investigated comprise reactions of [Mo(CO)2L25-C7H9)]+[L2= 2,2′-bipyridyl (bipy)1, Ph2PCH2PPh2(dppm)6, Ph2PCH2CH2PPh2(dppe)7; L = CNBut17 or PPh318] with NCMe or CNBut. Complex 1 reacts reversibly with NCMe to give [Mo(CO)2(NCMe)(bipy)(η3-C7H9)]+2 and, in NCMe, 7 exists as an equilibrium mixture with [Mo(CO)2(NCMe)(dppe)(η3-C7H9)]+8. The complexes 6, 17 and 18 do not react with NCMe at ambient temperature. Treatment of 1, 6 and 7 with CNBut affords [Mo(CO)2(CNBut)L23-C7H9)]+(L2= bipy 4, dppm 9 or dppe 11) although 4 is better prepared by reaction of [Mo(CO)2(CNBut)(NCMe)23-C7H9)]+5 with bipy. Complex 4 is resistant to carbonyl elimination but 9 and 11 undergo facile loss of CO to give [Mo(CO)(CNBut)L25-C7H9)]+(L2= dppm 10 or dppe 12) so establishing examples of associative ligand-substitution processes which proceed with η5→η3→η5 hapticity interconversion at the C7H9 dienyl ligand. The reaction between 17 and CNBut affords [Mo(CO)(CNBut)35-C7H9)]+19 with no observable η3-C7H9 intermediate but 19 reacts with further CNBut to yield [Mo(CO)(CNBut)43-C7H9)]+20. The crystal structures of complexes 1 and 4 have been determined. Complex 1 adopts an asymmetric ligand arrangement similar to that previously described for 6. Complex 4 has a pseudo-octahedral molecular geometry in which CNBut is located trans to the η3-bonded C7H9 ligand.

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