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@ARTICLE{WienenSchmidt:866049,
author = {Wienen-Schmidt, Barbara and Schmidt, Denis and Gerber,
Hans-Dieter and Heine, Andreas and Gohlke, Holger and Klebe,
Gerhard},
title = {{S}urprising {N}on-{A}dditivity of {M}ethyl-{G}roups in
{D}rug-{K}inase {I}nteraction},
journal = {ACS chemical biology},
volume = {14},
number = {12},
issn = {1554-8937},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2019-05295},
pages = {2585-2594},
year = {2019},
abstract = {Drug optimization is guided by biophysical methods with
increasing popularity. In the context of lead structure
modifications, the introduction of methyl groups is a simple
but potentially powerful approach. Hence, it is crucial to
systematically investigate the influence of ligand
methylation on biophysical characteristics such as
thermodynamics. Here, we investigate the influence of ligand
methylation in different positions and combinations on the
drug–kinase interaction. Binding modes and complex
structures were analyzed using protein crystallography.
Thermodynamic signatures were measured via isothermal
titration calorimetry (ITC). An extensive computational
analysis supported the understanding of the underlying
mechanisms. We found that not only position but also
stereochemistry of the methyl group has an influence on
binding potency as well as the thermodynamic signature of
ligand binding to the protein. Strikingly, the combination
of single methyl groups does not lead to additive effects.
In our case, the merger of two methyl groups in one ligand
leads to an entirely new alternative ligand binding mode in
the protein ligand complex. Moreover, the combination of the
two methyl groups also resulted in a nonadditive
thermodynamic profile of ligand binding. Molecular dynamics
(MD) simulations revealed distinguished characteristic
motions of the ligands in solution explaining the pronounced
thermodynamic changes. The unexpected drastic change in
protein ligand interaction highlights the importance of
crystallographic control even for minor modifications such
as the introduction of a methyl group. For an in-depth
understanding of ligand binding behavior, MD simulations
have shown to be a powerful tool.},
cin = {JSC / NIC / ICS-6},
ddc = {540},
cid = {I:(DE-Juel1)JSC-20090406 / I:(DE-Juel1)NIC-20090406 /
I:(DE-Juel1)ICS-6-20110106},
pnm = {511 - Computational Science and Mathematical Methods
(POF3-511) / Forschergruppe Gohlke $(hkf7_20170501)$},
pid = {G:(DE-HGF)POF3-511 / $G:(DE-Juel1)hkf7_20170501$},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:31638770},
UT = {WOS:000504806100012},
doi = {10.1021/acschembio.9b00476},
url = {https://juser.fz-juelich.de/record/866049},
}