Dinitrogen reduction via photochemical activation of heteroleptic tris(cyclopentadienyl) rare-earth complexes

Megan E. Fieser; Jefferson E. Bates; Joseph W. Ziller; Filipp Furche; William J. Evans

doi:10.1021/ja400664s

Dinitrogen reduction via photochemical activation of heteroleptic tris(cyclopentadienyl) rare-earth complexes

Megan E. Fieser, Jefferson E. Bates, Joseph W. Ziller, Filipp Furche, William J. Evans

Chemistry (Twin Cities)

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Abstract

Dinitrogen can be reduced by photochemical activation of the Ln ³⁺ mixed-ligand tris(cyclopentadienyl) rare-earth complexes (η⁵-C₅Me₅)_3-x(C ₅Me₄H)_xLn (Ln = Y, Lu, Dy; x = 1, 2). [(C ₅Me₄R)₂Ln]₂(μ-η²: η²-N₂) products (R = H, Me) are formed in reactions in which N₂ is reduced to (Nî - N)^2- and (C ₅Me₄H)^- is oxidized to (C₅Me ₄H)₂. Density functional theory indicates that this unusual example of rare-earth photochemistry can be rationalized by absorptions involving the (η³-C₅Me₄H)^- ligands.

Original language	English (US)
Pages (from-to)	3804-3807
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	135
Issue number	10
DOIs	https://doi.org/10.1021/ja400664s
State	Published - Mar 13 2013

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title = "Dinitrogen reduction via photochemical activation of heteroleptic tris(cyclopentadienyl) rare-earth complexes",

abstract = "Dinitrogen can be reduced by photochemical activation of the Ln 3+ mixed-ligand tris(cyclopentadienyl) rare-earth complexes (η5-C5Me5)3-x(C 5Me4H)xLn (Ln = Y, Lu, Dy; x = 1, 2). [(C 5Me4R)2Ln]2(μ-η2: η2-N2) products (R = H, Me) are formed in reactions in which N2 is reduced to (N{\^i} - N)2- and (C 5Me4H)- is oxidized to (C5Me 4H)2. Density functional theory indicates that this unusual example of rare-earth photochemistry can be rationalized by absorptions involving the (η3-C5Me4H)- ligands.",

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T1 - Dinitrogen reduction via photochemical activation of heteroleptic tris(cyclopentadienyl) rare-earth complexes

AU - Fieser, Megan E.

AU - Bates, Jefferson E.

AU - Ziller, Joseph W.

AU - Furche, Filipp

AU - Evans, William J.

PY - 2013/3/13

Y1 - 2013/3/13

N2 - Dinitrogen can be reduced by photochemical activation of the Ln 3+ mixed-ligand tris(cyclopentadienyl) rare-earth complexes (η5-C5Me5)3-x(C 5Me4H)xLn (Ln = Y, Lu, Dy; x = 1, 2). [(C 5Me4R)2Ln]2(μ-η2: η2-N2) products (R = H, Me) are formed in reactions in which N2 is reduced to (Nî - N)2- and (C 5Me4H)- is oxidized to (C5Me 4H)2. Density functional theory indicates that this unusual example of rare-earth photochemistry can be rationalized by absorptions involving the (η3-C5Me4H)- ligands.

AB - Dinitrogen can be reduced by photochemical activation of the Ln 3+ mixed-ligand tris(cyclopentadienyl) rare-earth complexes (η5-C5Me5)3-x(C 5Me4H)xLn (Ln = Y, Lu, Dy; x = 1, 2). [(C 5Me4R)2Ln]2(μ-η2: η2-N2) products (R = H, Me) are formed in reactions in which N2 is reduced to (Nî - N)2- and (C 5Me4H)- is oxidized to (C5Me 4H)2. Density functional theory indicates that this unusual example of rare-earth photochemistry can be rationalized by absorptions involving the (η3-C5Me4H)- ligands.

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Dinitrogen reduction via photochemical activation of heteroleptic tris(cyclopentadienyl) rare-earth complexes

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