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@ARTICLE{Kcher:857551,
author = {Köcher, Simone S. and Düwel, Stephan and Hundshammer,
Christian and Glaser, Steffen J. and Schilling, Franz and
Granwehr, Josef and Scheurer, Christoph},
title = {{A}b {I}nitio {S}imulation of p{H}-{S}ensitive {B}iomarkers
in {M}agnetic {R}esonance {I}maging},
journal = {The journal of physical chemistry / A A, Molecules,
spectroscopy, kinetics, environment $\&$ general theory},
volume = {122},
number = {40},
issn = {1520-5215},
address = {Washington, DC},
publisher = {Soc.66306},
reportid = {FZJ-2018-06542},
pages = {7983 - 7990},
year = {2018},
abstract = {An ab initio simulation scheme is introduced as a
theoretical prescreening approach to facilitate and enhance
the research for pH-sensitive biomarkers. The proton 1H and
carbon 13C nuclear magnetic resonance (NMR) chemical shifts
of the recently published marker for extracellular pH,
[1,5–13C2]zymonic acid (ZA), and the as yet unpublished
(Z)-4-methyl-2-oxopent-3-enedioic acid (OMPD) were
calculated with ab initio methods as a function of the pH.
The influence of the aqueous solvent was taken into account
either by an implicit solvent model or by explicit water
molecules, where the latter improved the accuracy of the
calculated chemical shifts considerably. The theoretically
predicted chemical shifts allowed for a reliable NMR peak
assignment. The pKa value of the first deprotonation of ZA
and OMPD was simulated successfully whereas the
parametrization of the implicit solvent model does not allow
for an accurate description of the second pKa. The
theoretical models reproduce the pH-induced chemical shift
changes and the first pKa with sufficient accuracy to
establish the ab initio prescreening approach as a valuable
support to guide the experimental search for pH-sensitive
biomarkers.},
cin = {IEK-9},
ddc = {530},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {135 - Fuel Cells (POF3-135)},
pid = {G:(DE-HGF)POF3-135},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:30222345},
UT = {WOS:000447471400006},
doi = {10.1021/acs.jpca.8b04665},
url = {https://juser.fz-juelich.de/record/857551},
}