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@ARTICLE{Banco:826421,
author = {Banco, Michael T. and Mishra, Vidhi and Ostermann, Andreas
and Schrader, Tobias E. and Evans, Gary B. and Kovalevsky,
Andrey and Ronning, Donald R.},
title = {{N}eutron structures of the {H}elicobacter pylori
5′-methylthioadenosine nucleosidase highlight proton
sharing and protonation states},
journal = {Proceedings of the National Academy of Sciences of the
United States of America},
volume = {113},
number = {48},
issn = {1091-6490},
address = {Washington, DC},
publisher = {National Acad. of Sciences},
reportid = {FZJ-2017-00649},
pages = {13756 - 13761},
year = {2016},
abstract = {MTAN (5′-methylthioadenosine nucleosidase) catalyzes the
hydrolysis of the N-ribosidic bond of a variety of
adenosine-containing metabolites. The Helicobacter pylori
MTAN (HpMTAN) hydrolyzes 6-amino-6-deoxyfutalosine in the
second step of the alternative menaquinone biosynthetic
pathway. Substrate binding of the adenine moiety is mediated
almost exclusively by hydrogen bonds, and the proposed
catalytic mechanism requires multiple proton-transfer
events. Of particular interest is the protonation state of
residue D198, which possesses a pKa above 8 and functions as
a general acid to initiate the enzymatic reaction. In this
study we present three corefined neutron/X-ray crystal
structures of wild-type HpMTAN cocrystallized with
S-adenosylhomocysteine (SAH), Formycin A (FMA), and
(3R,4S)-4-(4-Chlorophenylthiomethyl)-1-[(9-deaza-adenin-9-yl)methyl]-3-hydroxypyrrolidine
(p-ClPh-Thio-DADMe-ImmA) as well as one neutron/X-ray
crystal structure of an inactive variant (HpMTAN-D198N)
cocrystallized with SAH. These results support a mechanism
of D198 pKa elevation through the unexpected sharing of a
proton with atom N7 of the adenine moiety possessing
unconventional hydrogen-bond geometry. Additionally, the
neutron structures also highlight active site features that
promote the stabilization of the transition state and slight
variations in these interactions that result in 100-fold
difference in binding affinities between the DADMe-ImmA and
ImmA analogs.},
cin = {JCNS (München) ; Jülich Centre for Neutron Science JCNS
(München) ; JCNS-FRM-II / Neutronenstreuung ; JCNS-1},
ddc = {000},
cid = {I:(DE-Juel1)JCNS-FRM-II-20110218 /
I:(DE-Juel1)JCNS-1-20110106},
pnm = {6G15 - FRM II / MLZ (POF3-6G15) / 6G4 - Jülich Centre for
Neutron Research (JCNS) (POF3-623) / 6215 - Soft Matter,
Health and Life Sciences (POF3-621)},
pid = {G:(DE-HGF)POF3-6G15 / G:(DE-HGF)POF3-6G4 /
G:(DE-HGF)POF3-6215},
experiment = {EXP:(DE-MLZ)BIODIFF-20140101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000388835700068},
pubmed = {pmid:27856757},
doi = {10.1073/pnas.1609718113},
url = {https://juser.fz-juelich.de/record/826421},
}