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
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.
|Journal series||Angewandte Chemie-International Edition, [Angewandte Chemie - International Edition], ISSN 1433-7851, e-ISSN 1521-3773|
|Publication size in sheets||0.5|
|Score||= 200.0, 07-08-2020, ArticleFromJournal|
|Publication indicators||= 0; : 2018 = 2.132; : 2018 = 12.257 (2) - 2018=12.359 (5)|
* presented citation count is obtained through Internet information analysis and it is close to the number calculated by the Publish or Perish system.