Heme/non-heme diiron(II) complexes and O2, CO, and NO adducts as reduced and substrate-bound models for the active site of bacterial nitric oxide reductase

Ian M. Wasser; Hong Wei Huang; Pierre Moënne-Loccoz; Kenneth D. Karlin

doi:10.1021/ja0458773

Heme/non-heme diiron(II) complexes and O₂, CO, and NO adducts as reduced and substrate-bound models for the active site of bacterial nitric oxide reductase

Ian M. Wasser, Hong Wei Huang, Pierre Moënne-Loccoz, Kenneth D. Karlin

Center for Coastal Margins

Research output: Contribution to journal › Article

60 Scopus citations

Abstract

As a first generation model for the reactive reduced active-site form of bacterial nitric oxide reductase, a heme/non-heme diiron(II) complex [( ⁶L)Fe^II-Fe^II-(CI)]⁺ (2) {where ⁶L = partially fluorinated tetraphenylporphyrin with a tethered tetradentate TMPA chelate; TMPA = tris(2-pyridyl)amine} was generated by reduction of the corresponding μ-oxo diferric compound [(⁶L) Fe^III-O-Fe^III-CI]⁺ (1). Coordination chemistry models for reactions of reduced NOR with O₂, CO, and NO were also developed. With O₂ and CO, adducts are formed, [(⁶L) Fe^III(O₂^-)(thf)⋯Fe^II-Cl] B(C₆F₅)₄ (2a·O₂) {λ_max 418 (Soret), 536 nm; ν_O-O = 1176 cm ^-1, ν_Fe-O = 574 cm^-1 and [( ⁶L)Fe^II(CO)(thf)Fe^II-Cl]B(C₆F ₅)₄ (2a·CO) {ν_CO 1969 cm ^-1}, respectively. Reaction of purified nitric oxide with 2 leads to the dinitrosyl complex [(⁶L)Fe(NO)Fe(NO)-Cl]B(C₆F ₅)₄ (2a·(NO)₂) with ν_NO absorptions at 1798 cm^-1 (non-heme Fe-NO) and 1689 cm^-1 (heme-NO).

Original language	English (US)
Pages (from-to)	3310-3320
Number of pages	11
Journal	Journal of the American Chemical Society
Volume	127
Issue number	10
DOIs	https://doi.org/10.1021/ja0458773
State	Published - Mar 16 2005

ASJC Scopus subject areas

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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Wasser, I. M., Huang, H. W., Moënne-Loccoz, P., & Karlin, K. D. (2005). Heme/non-heme diiron(II) complexes and O₂, CO, and NO adducts as reduced and substrate-bound models for the active site of bacterial nitric oxide reductase. Journal of the American Chemical Society, 127(10), 3310-3320. https://doi.org/10.1021/ja0458773

Heme/non-heme diiron(II) complexes and O₂, CO, and NO adducts as reduced and substrate-bound models for the active site of bacterial nitric oxide reductase. / Wasser, Ian M.; Huang, Hong Wei; Moënne-Loccoz, Pierre; Karlin, Kenneth D.

In: Journal of the American Chemical Society, Vol. 127, No. 10, 16.03.2005, p. 3310-3320.

Research output: Contribution to journal › Article

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title = "Heme/non-heme diiron(II) complexes and O2, CO, and NO adducts as reduced and substrate-bound models for the active site of bacterial nitric oxide reductase",

abstract = "As a first generation model for the reactive reduced active-site form of bacterial nitric oxide reductase, a heme/non-heme diiron(II) complex [( 6L)FeII-FeII-(CI)]+ (2) {where 6L = partially fluorinated tetraphenylporphyrin with a tethered tetradentate TMPA chelate; TMPA = tris(2-pyridyl)amine} was generated by reduction of the corresponding μ-oxo diferric compound [(6L) FeIII-O-FeIII-CI]+ (1). Coordination chemistry models for reactions of reduced NOR with O2, CO, and NO were also developed. With O2 and CO, adducts are formed, [(6L) FeIII(O2-)(thf)⋯FeII-Cl] B(C6F5)4 (2a·O2) {λmax 418 (Soret), 536 nm; νO-O = 1176 cm -1, νFe-O = 574 cm-1 and [( 6L)FeII(CO)(thf)FeII-Cl]B(C6F 5)4 (2a·CO) {νCO 1969 cm -1}, respectively. Reaction of purified nitric oxide with 2 leads to the dinitrosyl complex [(6L)Fe(NO)Fe(NO)-Cl]B(C6F 5)4 (2a·(NO)2) with νNO absorptions at 1798 cm-1 (non-heme Fe-NO) and 1689 cm-1 (heme-NO).",

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AU - Wasser, Ian M.

AU - Huang, Hong Wei

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AU - Karlin, Kenneth D.

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N2 - As a first generation model for the reactive reduced active-site form of bacterial nitric oxide reductase, a heme/non-heme diiron(II) complex [( 6L)FeII-FeII-(CI)]+ (2) {where 6L = partially fluorinated tetraphenylporphyrin with a tethered tetradentate TMPA chelate; TMPA = tris(2-pyridyl)amine} was generated by reduction of the corresponding μ-oxo diferric compound [(6L) FeIII-O-FeIII-CI]+ (1). Coordination chemistry models for reactions of reduced NOR with O2, CO, and NO were also developed. With O2 and CO, adducts are formed, [(6L) FeIII(O2-)(thf)⋯FeII-Cl] B(C6F5)4 (2a·O2) {λmax 418 (Soret), 536 nm; νO-O = 1176 cm -1, νFe-O = 574 cm-1 and [( 6L)FeII(CO)(thf)FeII-Cl]B(C6F 5)4 (2a·CO) {νCO 1969 cm -1}, respectively. Reaction of purified nitric oxide with 2 leads to the dinitrosyl complex [(6L)Fe(NO)Fe(NO)-Cl]B(C6F 5)4 (2a·(NO)2) with νNO absorptions at 1798 cm-1 (non-heme Fe-NO) and 1689 cm-1 (heme-NO).

AB - As a first generation model for the reactive reduced active-site form of bacterial nitric oxide reductase, a heme/non-heme diiron(II) complex [( 6L)FeII-FeII-(CI)]+ (2) {where 6L = partially fluorinated tetraphenylporphyrin with a tethered tetradentate TMPA chelate; TMPA = tris(2-pyridyl)amine} was generated by reduction of the corresponding μ-oxo diferric compound [(6L) FeIII-O-FeIII-CI]+ (1). Coordination chemistry models for reactions of reduced NOR with O2, CO, and NO were also developed. With O2 and CO, adducts are formed, [(6L) FeIII(O2-)(thf)⋯FeII-Cl] B(C6F5)4 (2a·O2) {λmax 418 (Soret), 536 nm; νO-O = 1176 cm -1, νFe-O = 574 cm-1 and [( 6L)FeII(CO)(thf)FeII-Cl]B(C6F 5)4 (2a·CO) {νCO 1969 cm -1}, respectively. Reaction of purified nitric oxide with 2 leads to the dinitrosyl complex [(6L)Fe(NO)Fe(NO)-Cl]B(C6F 5)4 (2a·(NO)2) with νNO absorptions at 1798 cm-1 (non-heme Fe-NO) and 1689 cm-1 (heme-NO).

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