Histidine pK(a) shifts and changes of tautomeric states induced by the binding of gallium-protoporphyrin IX in the hemophore HasA(SM)

Protein Science : a Publication of the Protein Society
Nicolas WolffA Lecroisey

Abstract

The HasA(SM) hemophore, secreted by Serratia marcescens, binds free or hemoprotein bound heme with high affinity and delivers it to a specific outer membrane receptor, HasR. In HasA(SM), heme is held by two loops and coordinated to iron by two residues, His 32 and Tyr 75. A third residue His 83 was shown recently to play a crucial role in heme ligation. To address the mechanistic issues of the heme capture and release processes, the histidine protonation states were studied in both apo- and holo-forms of HasA(SM) in solution. Holo-HasA(SM) was formed with gallium-protoporphyrin IX (GaPPIX), giving rise to a diamagnetic protein. By use of heteronuclear correlation NMR spectroscopy, the imidazole side-chain (15)N and (1)H resonances of the six HasA(SM) histidines were assigned and their pKa values and predominant tautomeric states according to pH were determined. We show that protonation states of the heme pocket histidines can modulate the nucleophilic character of the two axial ligands and, consequently, control the heme binding. In particular, the essential role of the His 83 is emphasized according to its direct interaction with Tyr 75.

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Citations

Jul 12, 2012·The Journal of Physical Chemistry. B·Gurusamy BalakrishnanThomas G Spiro
Jan 16, 2009·Proceedings of the National Academy of Sciences of the United States of America·Stefanie KriegWolfram Welte
Oct 24, 2012·Proceedings of the National Academy of Sciences of the United States of America·Wei LüOliver Einsle
Jun 16, 2012·The Journal of Biological Chemistry·Célia Caillet-SaguyAnne Lecroisey
May 23, 2015·IEEE Transactions on Nanobioscience·Milan SasmalTarun Kanti Bhattacharyya
Dec 26, 2006·Biophysical Journal·Maria Teresa Neves-PetersenEduardo Pinho e Melo
Jan 23, 2009·Journal of the American Chemical Society·Célia Caillet-SaguyAnne Lecroisey
May 21, 2013·FEBS Letters·Marco Antonio González-LópezJosé de Jesús Olivares-Trejo
May 8, 2013·Protein Science : a Publication of the Protein Society·Nhuan T VuKouhei Tsumoto
Nov 10, 2009·Proteins·Damien FarrellJens Erik Nielsen
Dec 29, 2007·The Journal of Biological Chemistry·Célia Caillet-SaguyAnne Lecroisey
Nov 16, 2019·Scientific Reports·Amelie WißbrockDiana Imhof
Jan 30, 2021·Inorganic Chemistry·Christopher M Lemon, Michael A Marletta
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Jan 5, 2006·Journal of the American Chemical Society·Célia Caillet-SaguyPaola Turano
Mar 4, 2010·Biophysical Journal·Boris AguilarAlexey V Onufriev

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