Axial coordination of monodentate ligands with nickel(III) peptide complexes

Murray, Carl K.; Margerum, Dale W.

doi:10.1021/ic00139a046

Cited by 22 publications

(19 citation statements)

References 5 publications

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“…Studies have shown that in water the apparent equilibrium constant for the binding of polar substrates to transition-metal complexes can be several orders of magnitude larger (approx. 105 times) in frozen solution than it is in room-temperature solution (Murray & Margerum, 1982). Although this phenomenon is not well understood, changes in solvation as a function of temperature may be involved.…”

Section: Resultsmentioning

confidence: 97%

Multi-frequency e.p.r. studies of a mercury-containing mixed-metal derivative of laccase

Morie-Bebel¹,

McMillin²,

Antholine³

1986

Biochemical Journal

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Multi-frequency e.p.r. studies of a derivative of laccase containing one mercury atom and three of copper were carried out at -150 degrees C. The e.p.r. signal of the mercury derivative and fluoride-binding studies establish that a type-2-like copper centre is present. The signal suffers broadening, owing to g-strain, but at low frequencies (S-band) ligand hyperfine splitting can be resolved, and it can be explained in terms of coupling to three nitrogen atoms. The g values and the effect of solvent deuteration on the line width suggest that the fourth ligand in the equatorial plane is a water molecule. Simulations of the e.p.r. spectrum reveal that the site is slightly rhombic at -150 degrees C, a finding in accord with the proposed N3O donor set. Finally, it is emphasized that a structural reorganization of the type-2 copper site occurs with the binding of fluoride at low temperature. The reorganization may be linked to a conformational change which has previously been claimed to occur on cooling; however, this transition is not necessarily relevant to the temperature-dependence of fluoride binding.

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Section: Resultsmentioning

confidence: 97%

Multi-frequency e.p.r. studies of a mercury-containing mixed-metal derivative of laccase

Morie-Bebel¹,

McMillin²,

Antholine³

1986

Biochemical Journal

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“…In Ni-KGHK derivative, the side chain amine groups of Lys residues (at second and fourth positions) interact at the axial site of Ni III center, leading to more stabilization of Ni III . Similarly, incorporation of two Lys at first and second positions in Ni-KKH sequence, the Ni III is effectively stabilized relative to the first or second position alone ( Bossu et al., 1977 ; Murray and Margerum, 1982 ). So, stabilization of Cu III and Ni III in ATCUN derivatives depends not only on electrostatic interaction but also on the spatial orientation of the amino acid residues.…”

Section: Redox Chemistry Of M-atcun Derivativesmentioning

confidence: 99%

Designed Metal-ATCUN Derivatives: Redox- and Non-redox-Based Applications Relevant for Chemistry, Biology, and Medicine

et al. 2020

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Summary The designed “ATCUN” motif (amino-terminal copper and nickel binding site) is a replica of naturally occurring ATCUN site found in many proteins/peptides, and an attractive platform for multiple applications, which include nucleases, proteases, spectroscopic probes, imaging, and small molecule activation. ATCUN motifs are engineered at periphery by conjugation to recombinant proteins, peptides, fluorophores, or recognition domains through chemically or genetically, fulfilling the needs of various biological relevance and a wide range of practical usages. This chemistry has witnessed significant growth over the last few decades and several interesting ATCUN derivatives have been described. The redox role of the ATCUN moieties is also an important aspect to be considered. The redox potential of designed M-ATCUN derivatives is modulated by judicious choice of amino acid (including stereochemistry, charge, and position) that ultimately leads to the catalytic efficiency. In this context, a wide range of M-ATCUN derivatives have been designed purposefully for various redox- and non-redox-based applications, including spectroscopic probes, target-based catalytic metallodrugs, inhibition of amyloid-β toxicity, and telomere shortening, enzyme inactivation, biomolecules stitching or modification, next-generation antibiotic, and small molecule activation.

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“…[66] The absence of any pH dependence for the [Ni(ditame)] 3ϩ/2ϩ couple at pH Ͻ 11 is a clear indication that deprotonation of an acidic aqua ligand in the Ni III species does not occur. [67,68] This could be attributable to the JahnϪTeller distortion caused by the low-spin d 7 -electron configuration. The drastic drop in the potential at higher pH is coupled with decomposition.…”

Section: Cyclic Voltammograms Of [Co(ditame)(h 2 O)]mentioning

confidence: 99%

The Coordination Chemistry of the Pentadentate 2,2,6,6‐Tetrakis(aminomethyl)‐4‐azaheptane (ditame)

et al. 2003

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Axial coordination of monodentate ligands with nickel(III) peptide complexes

Cited by 22 publications

References 5 publications

Multi-frequency e.p.r. studies of a mercury-containing mixed-metal derivative of laccase

Multi-frequency e.p.r. studies of a mercury-containing mixed-metal derivative of laccase

Designed Metal-ATCUN Derivatives: Redox- and Non-redox-Based Applications Relevant for Chemistry, Biology, and Medicine

The Coordination Chemistry of the Pentadentate 2,2,6,6‐Tetrakis(aminomethyl)‐4‐azaheptane (ditame)

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