Key Intermediate Species Reveal the Copper(II)-Exchange Pathway in Biorelevant ATCUN/NTS Complexes

Radosław Kotuniak , Marc J. F. Strampraad , Karolina Bossak-Ahmad , Urszula Wawrzyniak , Iwona Ufnalska , Peter-Leon Hagedoorn , Wojciech Bal

Abstract

The amino-terminal copper and nickel/N-terminal site (ATCUN/NTS) present in proteins and bioactive peptides exhibits high affinity towards CuII ions and have been implicated in human copper physiology. Little is known, however, about the rate and exact mechanism of formation of such complexes. We used the stopped-flow and microsecond freeze-hyperquenching (MHQ) techniques supported by steady-state spectroscopic and electrochemical data to demonstrate the formation of partially coordinated intermediate CuII complexes formed by glycyl–glycyl–histidine (GGH) peptide, the simplest ATCUN/NTS model. One of these novel intermediates, characterized by two-nitrogen coordination, t1/2≈100 ms at pH 6.0 and the ability to maintain the CuII/CuI redox pair is the best candidate for the long-sought reactive species in extracellular copper transport.

Author Radosław Kotuniak - [Institute of Biochemistry and Biophysics of the Polish Academy of Sciences]
Radosław Kotuniak,,
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, Marc J. F. Strampraad - [Delft University of Technology]
Marc J. F. Strampraad,,
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, Karolina Bossak-Ahmad - [Institute of Biochemistry and Biophysics of the Polish Academy of Sciences]
Karolina Bossak-Ahmad,,
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, Urszula Wawrzyniak (FC / CMB)
Urszula Wawrzyniak,,
- Chair of Medical Biotechnology
, Iwona Ufnalska (FC / CMB)
Iwona Ufnalska,,
- Chair of Medical Biotechnology
, Peter-Leon Hagedoorn - [Delft University of Technology]
Peter-Leon Hagedoorn,,
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, Wojciech Bal
Wojciech Bal,,
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Journal seriesAngewandte Chemie-International Edition, [Angewandte Chemie - International Edition], ISSN 1433-7851, e-ISSN 1521-3773
Issue year2020
Vol59
Pages1-6
Publication size in sheets0.5
ASJC Classification1503 Catalysis; 1600 General Chemistry
DOIDOI:10.1002/anie.202004264
URL https://onlinelibrary.wiley.com/doi/full/10.1002/anie.202004264
Languageen angielski
File
wdpb_publikacje_pliki_plik_publikacja_3989_org.pdf 2.21 MB
Score (nominal)200
Score sourcejournalList
ScoreMinisterial score = 200.0, 07-08-2020, ArticleFromJournal
Publication indicators Scopus Citations = 0; Scopus SNIP (Source Normalised Impact per Paper): 2018 = 2.132; WoS Impact Factor: 2018 = 12.257 (2) - 2018=12.359 (5)
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