34 GHz Pulsed ENDOR Characterization of the Copper Coordination of an Amyloid β Peptide Relevant to Alzheimer’s Disease

Kim, Donghun; Kim, Nam Hee; Kim, Sun Hee

doi:10.1002/anie.201208108

Cited by 38 publications

(30 citation statements)

References 39 publications

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“…To directly confirm the location of the proton with respect to the electrochemically active Mo V species of 1T-MoS 2 , 1 H Davies ENDOR spectroscopy, which is ideal for the detection of strongly coupled nuclei ( 61 – 63 ), was performed. We could examine the presence of the exchangeable proton(s) by subtracting the 1 H ENDOR spectrum obtained in D 2 O solution from that obtained in H 2 O.…”

Section: Resultsmentioning

confidence: 99%

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS ₂

Ooka

Kim

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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Molybdenum sulfide (MoS2) is the most widely studied transition-metal dichalcogenide (TMDs) and phase engineering can markedly improve its electrocatalytic activity. However, the selectivity toward desired products remains poorly explored, limiting its application in complex chemical reactions. Here we report how phase engineering of MoS2 significantly improves the selectivity for nitrite reduction to nitrous oxide, a critical process in biological denitrification, using continuous-wave and pulsed electron paramagnetic resonance spectroscopy. We reveal that metallic 1T-MoS2 has a protonation site with a pKa of ∼5.5, where the proton is located ∼3.26 Å from redox-active Mo site. This protonation site is unique to 1T-MoS2 and induces sequential proton−electron transfer which inhibits ammonium formation while promoting nitrous oxide production, as confirmed by the pH-dependent selectivity and deuterium kinetic isotope effect. This is atomic-scale evidence of phase-dependent selectivity on MoS2, expanding the application of TMDs to selective electrocatalysis.

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Section: Resultsmentioning

confidence: 99%

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS ₂

Ooka

Kim

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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“…In Component II Cu(II) is bound to one His residue, one N atom belonging to the N-terminal, one carboxylic oxygen from the N-terminal amino acid Asp and one N atom belonging to an Ala 15,16 . Since axial oxygens are not visible in ESEEM and HYSCORE experiments, as the ones here considered 14,15 , following Kim et al 41 , we completed the preferred penta-coordinated Cu first shell by including an oxygen atom from a water molecule. A two-component model of this kind requires, besides the optimization of the structural parameter of the two metal sites, a fit of the relative weights by which each structural component contribute to the total spectrum.…”

Section: Resultsmentioning

confidence: 99%

Cu(II)–Zn(II) Cross-Modulation in Amyloid–Beta Peptide Binding: An X-ray Absorption Spectroscopy Study

et al. 2015

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In this work we analyze at a structural level the mechanism by which Cu(II) and Zn(II) ions compete for binding to the Aβ peptides that is involved in the etiology of Alzheimer’s disease. We collected X-ray Absorption Spectroscopy data on samples containing Aβ with Cu and Zn at different concentration ratios. We show that the order in which metals are added to the peptide solution matters and that, when Zn is added first, it prevents Cu from binding. On the contrary, when Cu is added first, it does not (completely) prevent Zn binding to Aβ peptides. Our analysis suggests that Cu and Zn ions are coordinated to different numbers of histidine residues depending on the [ion]:[peptide] concentration ratio.

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“…This method elucidates the hyperfine interaction of an unpaired electron with surrounding nuclei. 28−30 In particular, Mims ENDOR is useful when hyperfine interaction is relatively weak.…”

Section: Results and Discussionmentioning

confidence: 99%

Investigation of the Hydration State of Self-Assembled Peptide Nanostructures with Advanced Electron Paramagnetic Resonance Spectroscopy

et al. 2019

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Probing the intermolecular interactions and local environments of self-assembled peptide nanostructures (SPNs) is crucial for a better understanding of the underlying molecular details of self-assembling phenomena. In particular, investigation of the hydration state is important to understand the nanoscale structural and functional characteristics of SPNs. In this report, we examined the local hydration environments of SPNs in detail to understand the driving force of the discrete geometric structural self-assembling phenomena for peptide nanostructures. Advanced electron paramagnetic resonance spectroscopy was used to probe the hydrogen bond formation and geometry as well as the hydrophobicity of the local environments at various spin-labeled sites in SPNs. The experimental results supplement the sparse experimental data regarding local structures of SPNs, such as the hydrogen bonding and the hydrophobicity of the local environment, providing important information on the formation of SPNs, which have immense potential for bioactive materials.

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34 GHz Pulsed ENDOR Characterization of the Copper Coordination of an Amyloid β Peptide Relevant to Alzheimer’s Disease

Cited by 38 publications

References 39 publications

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS ₂

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS ₂

Cu(II)–Zn(II) Cross-Modulation in Amyloid–Beta Peptide Binding: An X-ray Absorption Spectroscopy Study

Investigation of the Hydration State of Self-Assembled Peptide Nanostructures with Advanced Electron Paramagnetic Resonance Spectroscopy

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34 GHz Pulsed ENDOR Characterization of the Copper Coordination of an Amyloid β Peptide Relevant to Alzheimer’s Disease

Cited by 38 publications

References 39 publications

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS 2

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS 2

Cu(II)–Zn(II) Cross-Modulation in Amyloid–Beta Peptide Binding: An X-ray Absorption Spectroscopy Study

Investigation of the Hydration State of Self-Assembled Peptide Nanostructures with Advanced Electron Paramagnetic Resonance Spectroscopy

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Product

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Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS ₂

Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS ₂