共 25 条
[Cu3(μ-S)2]3+ clusters supported by N-donor ligands:: Progress toward a synthetic model of the catalytic site of nitrous oxide reductase
被引:78
作者:

Brown, EC
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机构: Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

York, JT
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机构: Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

Antholine, WE
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机构: Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

Ruiz, E
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机构: Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

Alvarez, S
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h-index: 0
机构: Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

Tolman, WB
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h-index: 0
机构: Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
机构:
[1] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
[2] Univ Minnesota, Ctr Metals Biocatalysis, Minneapolis, MN 55455 USA
[3] Med Coll Wisconsin, Dept Biophys, Milwaukee, WI 53226 USA
[4] Univ Barcelona, Dept Quim Inorgan, Barcelona 08028, Spain
关键词:
D O I:
10.1021/ja053971t
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
By treating Cu(I) complexes of neutral, bidentate N-donor ligands with S8, clusters with novel delocalized mixed-valence [Cu3(μ-S)2]3+ cores have been isolated. X-ray crystal structures and UV-vis and resonance Raman spectral features of these clusters reveal similarities to the tetracopper-sulfide "CuZ" site in nitrous oxide reductase. A delocalized S = 1 ground state for the mixed-valent CuIIICu2II cores is supported by the observation of high symmetry in the X-ray structures and 10-line hyperfine features arising from coupling to three equivalent Cu ions in EPR spectra obtained at room temperature (shown) and 10 K. The delocalization we observe contrasts with the localization reported previously for a [Cu3(μ-O)2]3+ analogue (Root, D. E.; Henson, M. J.; Machonkin, T.; Mukherjee, P.; Stack, T. D. P.; Solomon, E. I. J. Am. Chem. Soc. 1998, 120, 4982), which we rationalized through DFT calculations. Copyright © 2005 American Chemical Society.
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页码:13752 / 13753
页数:2
相关论文
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