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@ARTICLE{Nguyen:201294,
author = {Nguyen, Trung Hai and Arnesano, Fabio and Scintilla, Simone
and Rossetti, Giulia and Ippoliti, Emiliano and Carloni,
Paolo and Natile, Giovanni},
title = {{S}tructural {D}eterminants of {C}isplatin and
{T}ransplatin {B}inding to the {M}et-{R}ich {M}otif of
{C}tr1: {A} {C}omputational {S}pectroscopy {A}pproach},
journal = {Journal of chemical theory and computation},
volume = {8},
number = {8},
issn = {1549-9626},
address = {Washington, DC},
publisher = {American Chemical Society (ACS)},
reportid = {FZJ-2015-03599},
pages = {2912 - 2920},
year = {2012},
abstract = {The cellular uptake of cisplatin and of other
platinum-based drugs is mediated by the high-affinity copper
transporter Ctr1. The eight-residue long peptide called
Mets7 (MTGMKGMS) mimics one of extracellular methionine
(Met)-rich motifs of Ctr1. It is an excellent model for
investigating the interaction of platinum drugs with Ctr1
under in vitro and in vivo conditions. Some of us have shown
that (i) Cisplatin loses all of its ligands upon reaction
with Mets7 and the metal ion binds to the three Met residues
and completes its coordination shell with a fourth ligand
that can be a chloride or a water/hydroxyl oxygen. (ii)
Transplatin loses only the chlorido ligands, which are
replaced by Met residues. Here, we provide information on
the structural determinants of cisplatin/Mets7 and
transplatin/Mets7 adducts by computational methods. The
predictions are validated against EXAFS, NMR, and CD
spectra. While EXAFS gives information restricted to the
metal coordination shell, NMR provides information extended
to residue atoms around the coordination shell, and finally,
CD provides information about the overall conformation of
the peptide. This allows us to elucidate the different
reaction modes of cisplatin and transplatin toward the
peptide, as well as to propose the platinated peptides
[PtX]+−(M*TGM*KGM*S) (X = Cl−, OH− ) and
trans[Pt(NH3)2]2+−(M*TGM*KGMS) as the most relevant
species occurring in water solution.},
cin = {GRS / IAS-5},
ddc = {540},
cid = {I:(DE-Juel1)GRS-20100316 / I:(DE-Juel1)IAS-5-20120330},
pnm = {899 - ohne Topic (POF2-899)},
pid = {G:(DE-HGF)POF2-899},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000307478800039},
doi = {10.1021/ct300167m},
url = {https://juser.fz-juelich.de/record/201294},
}