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@ARTICLE{Mikhnevich:180977,
author = {T. A. Mikhnevich and V. G. Grigorenko and M. Y. Rubtsova
and G. Rukhovich and M. A. Letarova and D. S. Kravtsova and
S. A. Vladimirov and A. A. Orlov and E. N. Nikolaev and A.
Zherebker and I. V. Perminova},
othercontributors = {A. V. Vyatkina},
title = {{I}nhibition of {C}lass {A} β-{L}actamase ({TEM}-1) by
{N}arrow {F}ractions of {H}umic {S}ubstances},
journal = {ACS omega},
volume = {6},
number = {37},
issn = {2470-1343},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {DKFZ-2022-01702},
pages = {23873 - 23883},
year = {2021},
abstract = {Antimicrobial resistance is a global threat. The use of
biologically active natural products alone or in combination
with the clinically proven antimicrobial agents might be a
useful strategy to fight the resistance. The scientific
hypotheses of this study were twofold: (1) the natural humic
substances rich in dicarboxyl, phenolic, heteroaryl, and
other fragments might possess inhibitory activity against
β-lactamases, and (2) this inhibitory activity might be
linked to the molecular composition of the humic ensemble.
To test these hypotheses, we used humic substances (HS) from
different sources (coal, peat, and soil) and of different
fractional compositions (humic acids, hymatomelanic acids,
and narrow fractions from solid-phase extraction) for
inhibiting serine β-lactamase TEM-1. Fourier transform ion
cyclotron resonance mass spectrometry (FTICR MS) was used to
characterize the molecular composition of all humic
materials used in this study. The kinetic assay with
chromogenic substrate CENTA was used for assessment of
inhibitory activity. The inhibition data have shown that
among all humic materials tested, a distinct activity was
observed within apolar fractions of hymatomelanic acid
isolated from lignite. The decrease in the hydrolysis rate
in the presence of most active fractions was $42\%$ (with
$sulbactam—87\%).$ Of particular importance is that these
very fractions caused a synergistic effect (2-fold) for the
combinations with sulbactam. Linking the observed inhibition
effects to molecular composition revealed the preferential
contribution of low-oxidized aromatic and acyclic components
such as flavonoid-, lignin, and terpenoid-like molecules.
The binding of single low-molecular-weight components to the
cryptic allosteric site along with supramolecular
interactions of humic aggregates with the protein surface
could be considered as a major contributor to the observed
inhibition. We believe that fine fractionation of
hydrophobic humic materials along with molecular modeling
studies on the interaction between humic molecules and
β-lactamases might contribute to the development of novel
β-lactamase inhibitors of humic nature.},
ddc = {660},
typ = {PUB:(DE-HGF)16},
doi = {10.1021/acsomega.1c02841},
url = {https://inrepo02.dkfz.de/record/180977},
}