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@ARTICLE{Cui:904475,
author = {Cui, Haiyang and Pramanik, Subrata and Jaeger, Karl-Erich
and Davari, Mehdi D. and Schwaneberg, Ulrich},
title = {{C}ompass{R}-guided recombination unlocks design principles
to stabilize lipases in {IL}s with minimal experimental
efforts},
journal = {Green chemistry},
volume = {23},
number = {9},
issn = {1463-9262},
address = {Cambridge},
publisher = {RSC},
reportid = {FZJ-2021-06045},
pages = {3474 - 3486},
year = {2021},
abstract = {Biocatalysis in ionic liquids (ILs) has gained enormous
attention for the production of biodiesel, sugar esters, and
pharmaceuticals. However, hydrophilic IL interaction with
enzymes often results in reduced activity or even
inactivation. In this report, we prove that intrinsic lipase
stability and preservation of hydration shells of Bacillus
subtilis lipase A (BSLA) are two synergistic design
principles to retain enzymatic activity in ILs. After in
silico screening of nine beneficial amino acid positions by
the CompassR rule (in total, 172 variants), we rationally
designed two variants, to be constructed by site-directed
mutagenesis, and three libraries by site-saturation
mutagenesis. With minimal experiment effort, we identified
three all-around variants towards four [BMIM]-based ILs.
Remarkably, the variant M1a F17S/V54K/D64N/D91E/G155N had
6.7-fold higher resistance against $40\%$ (v/v) [BMIM]Cl,
5.6-fold in $80\%$ (v/v) [BMIM]Br, 5.0-fold in $30\%$ (v/v)
[BMIM][TfO], and 2.7-fold in $10\%$ (v/v) [BMIM]I compared
to wild-type BSLA, respectively, while showing 1.9-fold
improvement in specific activity. Computational analysis of
molecular dynamics and thermodynamic stability analysis of
the variants revealed the molecular basis for the resistant
variants M1a and M1b as the synergistic enhancement of
protein stability (ΔΔGfold ranging from −4.26 to −4.80
kcal mol−1) and increased hydration shells around the
substitutions in the four ILs (up to 1.7-fold). These design
principles and the gained molecular knowledge not only open
the door to direct experimentalists for rationally designing
promising IL-resistant enzymes, but also provide new
insights into enzymatic catalysis in ILs.},
cin = {IBG-1 / IMET},
ddc = {540},
cid = {I:(DE-Juel1)IBG-1-20101118 / I:(DE-Juel1)IMET-20090612},
pnm = {2172 - Utilization of renewable carbon and energy sources
and engineering of ecosystem functions (POF4-217)},
pid = {G:(DE-HGF)POF4-2172},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000644497200001},
doi = {10.1039/D1GC00763G},
url = {https://juser.fz-juelich.de/record/904475},
}