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@ARTICLE{Zuo:943415,
author = {Zuo, Ke and Capelli, Riccardo and Rossetti, Giulia and
Nechushtai, Rachel and Carloni, Paolo},
title = {{P}redictions of the {P}oses and {A}ffinity of a {L}igand
over the {E}ntire {S}urface of a {NEET} {P}rotein: {T}he
{C}ase of {H}uman {M}ito{NEET}},
journal = {Journal of chemical information and modeling},
volume = {63},
number = {2},
issn = {0095-2338},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2023-01001},
pages = {643 - 654},
year = {2023},
abstract = {Human NEET proteins contain two [2Fe–2S] iron–sulfur
clusters, bound to three Cys residues and one His residue.
They exist in two redox states. Recently, these proteins
have revealed themselves as attractive drug targets for
mitochondrial dysfunction-related diseases, such as type 2
diabetes, Wolfram syndrome 2, and cancers. Unfortunately,
the lack of information and mechanistic understanding of
ligands binding to the whole functional, cytoplasmatic
domain has limited rational drug design approaches. Here, we
use an enhanced sampling technique, volume-based
metadynamics, recently developed by a team involving some of
us, to predict the poses and affinity of the
2-benzamido-4-(1,2,3,4-tetrahydronaphthalen-2-yl)-thiophene-3-carboxylate
ligand to the entire surface of the cytoplasmatic domain of
the human NEET protein mitoNEET (mNT) in an aqueous
solution. The calculations, based on the recently published
X-ray structure of the complex, are consistent with the
measured affinity. The calculated free energy landscape
revealed that the ligand can bind in multiple sites and with
poses other than the one found in the X-ray. This difference
is likely to be caused by crystal packing effects that allow
the ligand to interact with multiple adjacent NEET protein
copies. Such extra contacts are of course absent in the
solution; therefore, the X-ray pose is only transient in our
calculations, where the binding free energy correlates with
the number of contacts. We further evaluated how the
reduction and protonation of the Fe-bound histidine, as well
as temperature, can affect ligand binding. Both such
modifications introduce the possibility for the ligand to
bind in an area of the protein other than the one observed
in the X-ray, with no or little impact on affinity. Overall,
our study can provide insights on the molecular recognition
mechanisms of ligand binding to mNT in different oxidative
conditions, possibly helping rational drug design of NEET
ligands.},
cin = {IAS-5 / INM-9 / JSC},
ddc = {540},
cid = {I:(DE-Juel1)IAS-5-20120330 / I:(DE-Juel1)INM-9-20140121 /
I:(DE-Juel1)JSC-20090406},
pnm = {5241 - Molecular Information Processing in Cellular Systems
(POF4-524) / 5111 - Domain-Specific Simulation $\&$ Data
Life Cycle Labs (SDLs) and Research Groups (POF4-511)},
pid = {G:(DE-HGF)POF4-5241 / G:(DE-HGF)POF4-5111},
typ = {PUB:(DE-HGF)16},
pubmed = {36623826},
UT = {WOS:000914450700001},
doi = {10.1021/acs.jcim.2c01280},
url = {https://juser.fz-juelich.de/record/943415},
}