Bestimmung der Substratposition in der Nickel‐Superoxiddismutase: eine Modellstudie

Tietze, Daniel; Voigt, Stephan; Mollenhauer, Doreen; Tischler, Marco; Imhof, Diana; Gutmann, Torsten; González, Leticia; Ohlenschläger, Oliver; Breitzke, Hergen; Görlach, Matthias; Buntkowsky, Gerd

doi:10.1002/ange.201005027

Cited by 4 publications

(3 citation statements)

References 39 publications

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“…Superoxonickel species are proposed to be key reaction intermediates in the catalytic cycle of nickel superoxide dismutase . This is also a plausible formulation for the nickel–dioxygen species which was recently crystallographically characterized in nickel‐dependent quercetin 2,4‐dioxygenase (Figure ) …”

Section: Well‐defined Nickel–oxygen Speciesmentioning

confidence: 94%

Spectroscopically Characterized Synthetic Mononuclear Nickel–Oxygen Species

Corona

2016

Chemistry A European J

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Iron, copper, and manganese are the predominant metals found in oxygenases that perform efficient and selective hydrocarbon oxidations and for this reason, a large number of the corresponding metal-oxygen species has been described. However, in recent years nickel has been found in the active site of enzymes involved in oxidation processes, in which nickel-dioxygen species are proposed to play a key role. Owing to this biological relevance and to the existence of different catalytic protocols that involve the use of nickel catalysts in oxidation reactions, there is a growing interest in the detection and characterization of nickel-oxygen species relevant to these processes. In this Minireview the spectroscopically/structurally characterized synthetic superoxo, peroxo, and oxonickel species that have been reported to date are described. From these studies it becomes clear that nickel is a very promising metal in the field of oxidation chemistry with still unexplored possibilities.

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Section: Well‐defined Nickel–oxygen Speciesmentioning

confidence: 94%

Spectroscopically Characterized Synthetic Mononuclear Nickel–Oxygen Species

Corona

2016

Chemistry A European J

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“…3) If no direct coordination to the Ni center occurs then is the Ni site required to have at least one vacant substrate binding site for its SOD activity? Biochemical evidence, both in favor4e,f,h–k and against4b, 5f, 6 substrate binding to the nickel center, exists, in support of either an inner‐ or outer‐sphere electron‐transfer (ET) mechanism. Most of this evidence, including the low prevalence of S‐oxygenation and very high rate (of an order of approximately 10 9 ) of catalytic O 2 .− disproportion, suggest an outer‐sphere ET mechanism, although this is still somewhat ambiguous.…”

Section: Methodsmentioning

confidence: 99%

“…Most of this evidence, including the low prevalence of S‐oxygenation and very high rate (of an order of approximately 10 9 ) of catalytic O 2 .− disproportion, suggest an outer‐sphere ET mechanism, although this is still somewhat ambiguous. Recent investigations support the binding of a CN − moiety to the Ni center in a peptide‐ligand environment, giving impetus to the ongoing debate 4h. Indeed, the native NiSOD active site itself and all existing model complexes have one or more empty binding sites around the nickel center.…”

Section: Methodsmentioning

confidence: 99%

Hexacoordinate Nickel(II)/(III) Complexes that Mimic the Catalytic Cycle of Nickel Superoxide Dismutase

et al. 2014

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A functional model complex of nickel superoxide dismutase (NiSOD) with a non-peptide ligand which mimics the full catalytic cycle of NiSOD is unknown. Similarly, it has not been fully elucidated whether NiSOD activity is a result of an outer-or inner-sphere electron-transfer mechanism. With this in mind, two octahedral nickel(II)/(III) complexes of a bistridentate N 2 S donor carboxamide ligand, N-2-phenylthiophenyl-2'-pyridinecarboxamide (HL Ph ), have been synthesized, structurally characterized, and their SOD activities examined. These complexes mimic the full catalytic cycle of NiSOD. Electrochemical experiments support an outer-sphere electron-transfer mechanism for their SOD activity. Scheme 1. Coordination geometry of oxidized (left) and reduced (right) forms of NiSOD active sites.

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Hexacoordinate Nickel(II)/(III) Complexes that Mimic the Catalytic Cycle of Nickel Superoxide Dismutase

Chatterjee¹,

Maji²,

Barman³

et al. 2014

Angew Chem Int Ed

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A functional model complex of nickel superoxide dismutase (NiSOD) with a non-peptide ligand which mimics the full catalytic cycle of NiSOD is unknown. Similarly, it has not been fully elucidated whether NiSOD activity is a result of an outer- or inner-sphere electron-transfer mechanism. With this in mind, two octahedral nickel(II)/(III) complexes of a bis-tridentate N2 S donor carboxamide ligand, N-2-phenylthiophenyl-2'-pyridinecarboxamide (HL(Ph)), have been synthesized, structurally characterized, and their SOD activities examined. These complexes mimic the full catalytic cycle of NiSOD. Electrochemical experiments support an outer-sphere electron-transfer mechanism for their SOD activity.

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Bestimmung der Substratposition in der Nickel‐Superoxiddismutase: eine Modellstudie

Cited by 4 publications

References 39 publications

Spectroscopically Characterized Synthetic Mononuclear Nickel–Oxygen Species

Spectroscopically Characterized Synthetic Mononuclear Nickel–Oxygen Species

Hexacoordinate Nickel(II)/(III) Complexes that Mimic the Catalytic Cycle of Nickel Superoxide Dismutase

Hexacoordinate Nickel(II)/(III) Complexes that Mimic the Catalytic Cycle of Nickel Superoxide Dismutase

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