Intermolecular N-N Coupling of a Dinitrosyl Iron Complex Induced by Hydrogen Bond Donors in the Secondary Coordination Sphere

Kayla M. Fugami; Gabriel S. Black; Tim Kowalczyk; Takele Seda; John D. Gilbertson

doi:10.1021/jacs.4c12787

Intermolecular N-N Coupling of a Dinitrosyl Iron Complex Induced by Hydrogen Bond Donors in the Secondary Coordination Sphere

Kayla M. Fugami, Gabriel S. Black, Tim Kowalczyk, Takele Seda, John D. Gilbertson

Western Washington University

Research output: Contribution to journal › Article › peer-review

Abstract

The intermolecular N-N coupling of NO in a dinitrosyl iron complex (DNIC) induced by hydrogen bond donors in the secondary coordination sphere to form N₂O is reported. A family of complexes containing pendant anilines in the secondary coordination sphere were synthesized and characterized. Reduction of the {Fe(NO)₂}⁹ complex [Fe(^PhNHPDI)(NO)₂][BPh₄] (3) to the {Fe(NO)₂}¹⁰ Fe(^PhNHPDI)(NO)₂ (4) results in intermolecular N-N coupling to form N₂O. Similar reactions of the control {Fe(NO)₂}⁹ complex [Fe(^PhNMePDI)(NO)₂][BPh₄] (7), which does not have H-bonding groups in the secondary coordination sphere, do not result in N₂O formation. The hydrogen bonding capabilities of the complexes were explored spectroscopically and computationally.

Original language	English
Pages (from-to)	7274-7281
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	147
Issue number	9
DOIs	https://doi.org/10.1021/jacs.4c12787
State	Published - Mar 5 2025

ASJC Scopus Subject Areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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title = "Intermolecular N-N Coupling of a Dinitrosyl Iron Complex Induced by Hydrogen Bond Donors in the Secondary Coordination Sphere",

abstract = "The intermolecular N-N coupling of NO in a dinitrosyl iron complex (DNIC) induced by hydrogen bond donors in the secondary coordination sphere to form N2O is reported. A family of complexes containing pendant anilines in the secondary coordination sphere were synthesized and characterized. Reduction of the {Fe(NO)2}9 complex [Fe(PhNHPDI)(NO)2][BPh4] (3) to the {Fe(NO)2}10 Fe(PhNHPDI)(NO)2 (4) results in intermolecular N-N coupling to form N2O. Similar reactions of the control {Fe(NO)2}9 complex [Fe(PhNMePDI)(NO)2][BPh4] (7), which does not have H-bonding groups in the secondary coordination sphere, do not result in N2O formation. The hydrogen bonding capabilities of the complexes were explored spectroscopically and computationally.",

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T1 - Intermolecular N-N Coupling of a Dinitrosyl Iron Complex Induced by Hydrogen Bond Donors in the Secondary Coordination Sphere

AU - Fugami, Kayla M.

AU - Black, Gabriel S.

AU - Kowalczyk, Tim

AU - Seda, Takele

AU - Gilbertson, John D.

PY - 2025/3/5

Y1 - 2025/3/5

N2 - The intermolecular N-N coupling of NO in a dinitrosyl iron complex (DNIC) induced by hydrogen bond donors in the secondary coordination sphere to form N2O is reported. A family of complexes containing pendant anilines in the secondary coordination sphere were synthesized and characterized. Reduction of the {Fe(NO)2}9 complex [Fe(PhNHPDI)(NO)2][BPh4] (3) to the {Fe(NO)2}10 Fe(PhNHPDI)(NO)2 (4) results in intermolecular N-N coupling to form N2O. Similar reactions of the control {Fe(NO)2}9 complex [Fe(PhNMePDI)(NO)2][BPh4] (7), which does not have H-bonding groups in the secondary coordination sphere, do not result in N2O formation. The hydrogen bonding capabilities of the complexes were explored spectroscopically and computationally.

AB - The intermolecular N-N coupling of NO in a dinitrosyl iron complex (DNIC) induced by hydrogen bond donors in the secondary coordination sphere to form N2O is reported. A family of complexes containing pendant anilines in the secondary coordination sphere were synthesized and characterized. Reduction of the {Fe(NO)2}9 complex [Fe(PhNHPDI)(NO)2][BPh4] (3) to the {Fe(NO)2}10 Fe(PhNHPDI)(NO)2 (4) results in intermolecular N-N coupling to form N2O. Similar reactions of the control {Fe(NO)2}9 complex [Fe(PhNMePDI)(NO)2][BPh4] (7), which does not have H-bonding groups in the secondary coordination sphere, do not result in N2O formation. The hydrogen bonding capabilities of the complexes were explored spectroscopically and computationally.

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Intermolecular N-N Coupling of a Dinitrosyl Iron Complex Induced by Hydrogen Bond Donors in the Secondary Coordination Sphere

Abstract

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