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Article: Synthesis, Identification, and Reactivity Properties of Symmetrical MoFe3S4 Double Cubanes with Fe-S-Fe and Fe-O-Fe Bridges
Title | Synthesis, Identification, and Reactivity Properties of Symmetrical MoFe3S4 Double Cubanes with Fe-S-Fe and Fe-O-Fe Bridges |
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Authors | |
Issue Date | 1998 |
Publisher | American Chemical Society. The Journal's web site is located at http://pubs.acs.org/ic |
Citation | Inorganic Chemistry, 1998, v. 37 n. 9, p. 2247-2254 How to Cite? |
Abstract | Singly bridged double cubane clusters containing Fe4S4 and/or MoFe3S4 cores and linked by an Fe-S-Fe unit bear an interesting compositional similarity to the cofactor of nitrogenase and constitute a nearly unexplored class of clusters. We have expanded recently our investigation of the prototypic cluster {[(Meida)MoFe3S4Cl2]2-(μ 2-S)}4- (6) (Huang et al.; J. Am. Chem. Soc. 1997, 119, 8662) to other types {[(Meida)MoFe3S4L2l2(μ 2-S)}4- (L = EtS-, ArO- (8-10)) (Meida = N-methylimidodiacetate(2-)). Clusters are formed by coupling reactions of the single cubanes [(Meida)MoFe3S4L3]2- (L = Cl- (1), ArO- (3-5) at their substitutionally labile iron sites with primarily Li2S. Using 2 NaOEt/H2O as an oxide source in Me2SO, the oxo-bridged clusters {[(Meida)-MoFe3S4L2l2(μ 2-O)}4- (L = Cl- (13), ArO- (14, 15)) have been prepared. All double cubanes were obtained as a mixture of as many as four diastereomers. Double cubane structures were established by NMR and electrochemical criteria. Both the sulfido- and oxo-bridged clusters undergo terminal ligand substitution reactions with bridge retention. Oxo bridges are much more susceptible than sulfido bridges to protic cleavage with water, (Et3NH)Cl, ArOH, and HS-. Reaction of 13 with hydrosulfide affords a second route to 6. These and other results define a set of reactions that are regiospecific at either the terminal ligand or bridge sites and provide a basis for future reactivity manipulation of symmetrical and unsymmetrical bridged double cubanes. |
Persistent Identifier | http://hdl.handle.net/10722/167324 |
ISSN | 2023 Impact Factor: 4.3 2023 SCImago Journal Rankings: 0.928 |
ISI Accession Number ID | |
References |
DC Field | Value | Language |
---|---|---|
dc.contributor.author | Huang, J | en_US |
dc.contributor.author | Holm, RH | en_US |
dc.date.accessioned | 2012-10-08T03:05:40Z | - |
dc.date.available | 2012-10-08T03:05:40Z | - |
dc.date.issued | 1998 | en_US |
dc.identifier.citation | Inorganic Chemistry, 1998, v. 37 n. 9, p. 2247-2254 | en_US |
dc.identifier.issn | 0020-1669 | en_US |
dc.identifier.uri | http://hdl.handle.net/10722/167324 | - |
dc.description.abstract | Singly bridged double cubane clusters containing Fe4S4 and/or MoFe3S4 cores and linked by an Fe-S-Fe unit bear an interesting compositional similarity to the cofactor of nitrogenase and constitute a nearly unexplored class of clusters. We have expanded recently our investigation of the prototypic cluster {[(Meida)MoFe3S4Cl2]2-(μ 2-S)}4- (6) (Huang et al.; J. Am. Chem. Soc. 1997, 119, 8662) to other types {[(Meida)MoFe3S4L2l2(μ 2-S)}4- (L = EtS-, ArO- (8-10)) (Meida = N-methylimidodiacetate(2-)). Clusters are formed by coupling reactions of the single cubanes [(Meida)MoFe3S4L3]2- (L = Cl- (1), ArO- (3-5) at their substitutionally labile iron sites with primarily Li2S. Using 2 NaOEt/H2O as an oxide source in Me2SO, the oxo-bridged clusters {[(Meida)-MoFe3S4L2l2(μ 2-O)}4- (L = Cl- (13), ArO- (14, 15)) have been prepared. All double cubanes were obtained as a mixture of as many as four diastereomers. Double cubane structures were established by NMR and electrochemical criteria. Both the sulfido- and oxo-bridged clusters undergo terminal ligand substitution reactions with bridge retention. Oxo bridges are much more susceptible than sulfido bridges to protic cleavage with water, (Et3NH)Cl, ArOH, and HS-. Reaction of 13 with hydrosulfide affords a second route to 6. These and other results define a set of reactions that are regiospecific at either the terminal ligand or bridge sites and provide a basis for future reactivity manipulation of symmetrical and unsymmetrical bridged double cubanes. | en_US |
dc.language | eng | en_US |
dc.publisher | American Chemical Society. The Journal's web site is located at http://pubs.acs.org/ic | en_US |
dc.relation.ispartof | Inorganic Chemistry | en_US |
dc.title | Synthesis, Identification, and Reactivity Properties of Symmetrical MoFe3S4 Double Cubanes with Fe-S-Fe and Fe-O-Fe Bridges | en_US |
dc.type | Article | en_US |
dc.identifier.email | Huang, J:jshuang@hkucc.hku.hk | en_US |
dc.identifier.authority | Huang, J=rp00709 | en_US |
dc.description.nature | link_to_subscribed_fulltext | en_US |
dc.identifier.doi | 10.1021/ic971353a | - |
dc.identifier.scopus | eid_2-s2.0-0001140422 | en_US |
dc.relation.references | http://www.scopus.com/mlt/select.url?eid=2-s2.0-0001140422&selection=ref&src=s&origin=recordpage | en_US |
dc.identifier.volume | 37 | en_US |
dc.identifier.issue | 9 | en_US |
dc.identifier.spage | 2247 | en_US |
dc.identifier.epage | 2254 | en_US |
dc.identifier.isi | WOS:000073506700024 | - |
dc.publisher.place | United States | en_US |
dc.identifier.scopusauthorid | Huang, J=7407192639 | en_US |
dc.identifier.scopusauthorid | Holm, RH=7202326371 | en_US |
dc.identifier.issnl | 0020-1669 | - |