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@ARTICLE{Frieg:877684,
author = {Frieg, Benedikt and Goerg, Boris and Qvartskhava, Natalia
and Jeitner, Thomas and Homeyer, Nadine and Häussinger,
Dieter and Gohlke, Holger},
title = {{M}echanism of fully-reversible, p{H}-sensitive inhibition
of human glutamine synthetase by tyrosine nitration},
journal = {Journal of chemical theory and computation},
volume = {16},
number = {7},
issn = {1549-9626},
address = {Washington, DC},
reportid = {FZJ-2020-02394},
pages = {4694–4705},
year = {2020},
abstract = {Glutamine synthetase (GS) catalyzes an ATP-dependent
condensation of glutamate and ammonia to form glutamine.
This reaction – and therefore GS – are indispensable for
the hepatic nitrogen metabolism. Nitration of tyrosine 336
(Y336) inhibits human GS activity. GS nitration and the
consequent loss of GS function are associated with a broad
range of neurological diseases. The mechanism by which Y336
nitration inhibits GS, however, is not understood. Here, we
show by means of unbiased MD simulations, binding and
configurational free energy computations that Y336 nitration
hampers ATP binding, but only in the deprotonated and
negatively-charged state of residue 336. By contrast, for
the protonated and neutral state, our computations indicate
an increased binding affinity for ATP. pKa computations of
nitrated Y336 within GS predict a pKa of ~5.3. Thus, at
physiological pH nitrated Y336 exists almost exclusively in
the deprotonated and negatively-charged state. In vitro
experiments confirm these predictions, in that, the
catalytic activity of nitrated GS is decreased at pH 7 and
pH 6, but not at pH 4. These results indicate a novel, fully
reversible, pH-sensitive mechanism for the regulation of GS
activity by tyrosine nitration.},
cin = {JSC / NIC / IBI-7},
ddc = {610},
cid = {I:(DE-Juel1)JSC-20090406 / I:(DE-Juel1)NIC-20090406 /
I:(DE-Juel1)IBI-7-20200312},
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:32551588},
UT = {WOS:000607532300058},
doi = {10.1021/acs.jctc.0c00249},
url = {https://juser.fz-juelich.de/record/877684},
}