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Oligopeptides Generated by Neprilysin Degradation of β-Amyloid Have the Highest Cu(II) Affinity in the Whole Aβ Family
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    Oligopeptides Generated by Neprilysin Degradation of β-Amyloid Have the Highest Cu(II) Affinity in the Whole Aβ Family
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    • Karolina Bossak-Ahmad
      Karolina Bossak-Ahmad
      Institute of Biochemistry and Biophysics, Polish Academy of Sciences, 02-106 Warsaw, Poland
    • Mariusz Mital
      Mariusz Mital
      Institute of Biochemistry and Biophysics, Polish Academy of Sciences, 02-106 Warsaw, Poland
      Florey Department of Neuroscience and Mental Health, The University of Melbourne, Melbourne, Victoria 3010, Australia
    • Dawid Płonka
      Dawid Płonka
      Institute of Biochemistry and Biophysics, Polish Academy of Sciences, 02-106 Warsaw, Poland
    • Simon C. Drew*
      Simon C. Drew
      Institute of Biochemistry and Biophysics, Polish Academy of Sciences, 02-106 Warsaw, Poland
      Department of Medicine (Royal Melbourne Hospital), The University of Melbourne, Melbourne, Victoria 3010, Australia
      *E-mail: [email protected] (S.C.D.).
    • Wojciech Bal*
      Wojciech Bal
      Institute of Biochemistry and Biophysics, Polish Academy of Sciences, 02-106 Warsaw, Poland
      *E-mail: [email protected] (W.B.).
      More by Wojciech Bal
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2019, 58, 1, 932–943
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    https://doi.org/10.1021/acs.inorgchem.8b03051
    Published December 24, 2018
    Copyright © 2018 American Chemical Society

    Abstract

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    The catabolism of β-amyloid (Aβ) is carried out by numerous endopeptidases including neprilysin, which hydrolyzes peptide bonds preceding positions 4, 10, and 12 to yield Aβ4–9 and a minor Aβ12–x species. Alternative processing of the amyloid precursor protein by β-secretase also generates the Aβ11–x species. All these peptides contain a Xxx-Yyy-His sequence, also known as an ATCUN or NTS motif, making them strong chelators of Cu(II) ions. We synthesized the corresponding peptides, Phe-Arg-His-Asp-Ser-Gly-OH (Aβ4–9), Glu-Val-His-His-Gln-Lys-am (Aβ11–16), Val-His-His-Gln-Lys-am (Aβ12–16), and pGlu-Val-His-His-Gln-Lys-am (pAβ11–16), and investigated their Cu(II) binding properties using potentiometry, and UV–vis, circular dichroism, and electron paramagnetic resonance spectroscopies. We found that the three peptides with unmodified N-termini formed square-planar Cu(II) complexes at pH 7.4 with analogous geometries but significantly varied Kd values of 6.6 fM (Aβ4–9), 9.5 fM (Aβ12–16), and 1.8 pM (Aβ11–16). Cyclization of the N-terminal Glu11 residue to the pyroglutamate species pAβ11–16 dramatically reduced the affinity (5.8 nM). The Cu(II) affinities of Aβ4–9 and Aβ12–16 are the highest among the Cu(II) complexes of Aβ peptides. Using fluorescence spectroscopy, we demonstrated that the Cu(II) exchange between the Phe-Arg-His and Val-His-His motifs is very slow, on the order of days. These results are discussed in terms of the relevance of Aβ4–9, a major Cu(II) binding Aβ fragment generated by neprilysin, as a possible Cu(II) carrier in the brain.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.inorgchem.8b03051.

    • Additional analyses of UV–vis, CD, and potentiometric titrations (PDF)

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    Cited By

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    This article is cited by 25 publications.

    1. Dawid Płonka, Radosław Kotuniak, Katarzyna Dąbrowska, Wojciech Bal. Electrospray-Induced Mass Spectrometry Is Not Suitable for Determination of Peptidic Cu(II) Complexes. Journal of the American Society for Mass Spectrometry 2021, 32 (12) , 2766-2776. https://doi.org/10.1021/jasms.1c00206
    2. Ewelina Stefaniak, M. Jake Pushie, Catherine Vaerewyck, David Corcelli, Chloe Griggs, Whitney Lewis, Emma Kelley, Noreen Maloney, Madison Sendzik, Wojciech Bal, Kathryn L. Haas. Exploration of the Potential Role for Aβ in Delivery of Extracellular Copper to Ctr1. Inorganic Chemistry 2020, 59 (23) , 16952-16966. https://doi.org/10.1021/acs.inorgchem.0c02100
    3. Nina E. Wezynfeld, Aleksandra Tobolska, Mariusz Mital, Urszula E. Wawrzyniak, Magdalena Z. Wiloch, Dawid Płonka, Karolina Bossak-Ahmad, Wojciech Wróblewski, Wojciech Bal. Aβ5–x Peptides: N-Terminal Truncation Yields Tunable Cu(II) Complexes. Inorganic Chemistry 2020, 59 (19) , 14000-14011. https://doi.org/10.1021/acs.inorgchem.0c01773
    4. Ewelina Stefaniak, Dawid Płonka, Paulina Szczerba, Nina E. Wezynfeld, Wojciech Bal. Copper Transporters? Glutathione Reactivity of Products of Cu–Aβ Digestion by Neprilysin. Inorganic Chemistry 2020, 59 (7) , 4186-4190. https://doi.org/10.1021/acs.inorgchem.0c00427
    5. Ewelina Stefaniak, Wojciech Bal. CuII Binding Properties of N-Truncated Aβ Peptides: In Search of Biological Function. Inorganic Chemistry 2019, 58 (20) , 13561-13577. https://doi.org/10.1021/acs.inorgchem.9b01399
    6. Klaudia Głowacz, Weronika Tokarska, Anita Olechowska, Nina E. Wezynfeld, Patrycja Ciosek-Skibińska. Tuning multispectral fluorescence quantum dot–based identification of short-length amyloid β peptides by applying Cu(II) ions. Microchimica Acta 2024, 191 (11) https://doi.org/10.1007/s00604-024-06764-9
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    9. Ruwini S. K. Ekanayake, Victor A. Streltsov, Stephen P. Best, Christopher T. Chantler. Nanostructure and dynamics of N-truncated copper amyloid-β peptides from advanced X-ray absorption fine structure. IUCrJ 2024, 11 (3) , 325-346. https://doi.org/10.1107/S2052252524001830
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    13. Magdalena Z. Wiloch, Martin Jönsson-Niedziółka. Very small changes in the peptide sequence alter the redox properties of Aβ(11–16)-Cu(II) and pAβ(11–16)-Cu(II) β-amyloid complexes. Journal of Electroanalytical Chemistry 2022, 922 , 116746. https://doi.org/10.1016/j.jelechem.2022.116746
    14. Paulina Gonzalez, Laurent Sabater, Emilie Mathieu, Peter Faller, Christelle Hureau. Why the Ala-His-His Peptide Is an Appropriate Scaffold to Remove and Redox Silence Copper Ions from the Alzheimer’s-Related Aβ Peptide. Biomolecules 2022, 12 (10) , 1327. https://doi.org/10.3390/biom12101327
    15. Kamila Stokowa-Sołtys, Klaudia Szczerba, Magdalena Pacewicz, Robert Wieczorek, Nina E. Wezynfeld, Wojciech Bal. Interactions of neurokinin B with copper( ii ) ions and their potential biological consequences. Dalton Transactions 2022, 51 (37) , 14267-14276. https://doi.org/10.1039/D2DT02033E
    16. Magdalena Wiloch, Martin Jönsson-Niedziółka. How Very Smallchanges in the Peptide Sequence of β‑Amyloids Influence Their Redox Properties. Electrochemical Studies of Aβ(11-16) and pAβ(11-16). SSRN Electronic Journal 2022, 14 https://doi.org/10.2139/ssrn.4094540
    17. Thomas A. Bayer. N-Truncated Aβ Starting at Position Four—Biochemical Features, Preclinical Models, and Potential as Drug Target in Alzheimer’s Disease. Frontiers in Aging Neuroscience 2021, 13 https://doi.org/10.3389/fnagi.2021.710579
    18. Chiara Bacchella, Simone Dell’Acqua, Stefania Nicolis, Enrico Monzani, Luigi Casella. Oxidase Reactivity of CuII Bound to N-Truncated Aβ Peptides Promoted by Dopamine. International Journal of Molecular Sciences 2021, 22 (10) , 5190. https://doi.org/10.3390/ijms22105190
    19. Enrico Falcone, Michael Okafor, Nicolas Vitale, Laurent Raibaut, Angélique Sour, Peter Faller. Extracellular Cu2+ pools and their detection: From current knowledge to next-generation probes. Coordination Chemistry Reviews 2021, 433 , 213727. https://doi.org/10.1016/j.ccr.2020.213727
    20. Ewelina Stefaniak, Elena Atrian‐Blasco, Wojciech Goch, Laurent Sabater, Christelle Hureau, Wojciech Bal. The Aggregation Pattern of Aβ 1–40 is Altered by the Presence of N ‐Truncated Aβ 4–40 and/or Cu II in a Similar Way through Ionic Interactions. Chemistry – A European Journal 2021, 27 (8) , 2798-2809. https://doi.org/10.1002/chem.202004484
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2019, 58, 1, 932–943
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.8b03051
    Published December 24, 2018
    Copyright © 2018 American Chemical Society

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