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dc.contributor.author
Kashima, Keita
dc.contributor.author
Fujisaki, Tomoyuki
dc.contributor.author
Serrano-Luginbühl, Sandra Anne
dc.contributor.author
Khaydarov, Abbos
dc.contributor.author
Kissner, Reinhard
dc.contributor.author
Janošević-Ležaić, Aleksandra
dc.contributor.author
Bajuk-Bogdanović, Danica
dc.contributor.author
Ćirić-Marjanović, Gordana
dc.contributor.author
Schuler, Lukas D.
dc.contributor.author
Walde, Peter
dc.date.accessioned
2018-12-05T14:38:40Z
dc.date.available
2018-11-09T05:08:47Z
dc.date.available
2018-11-21T11:32:42Z
dc.date.available
2018-12-05T14:38:40Z
dc.date.issued
2018
dc.identifier.issn
2046-2069
dc.identifier.other
10.1039/c8ra05731a
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/302275
dc.identifier.doi
10.3929/ethz-b-000302275
dc.description.abstract
The Trametes versicolor laccase (TvL)-catalysed oligomerisation of the aniline dimer p-aminodiphenylamine (PADPA) was investigated in an aqueous medium of pH = 3.5, containing 80–100 nm-sized anionic vesicles formed from AOT, the sodium salt of bis(2-ethylhexyl)sulfosuccinic acid. If run under optimal conditions, the reaction yields oligomeric products which resemble the emeraldine salt form of polyaniline (PANI-ES) in its polaron state, known to be the only oxidation state of linear PANI which is electrically conductive. The vesicles serve as “templates” for obtaining products with the desired PANI-ES-like features. For this complex, heterogeneous, vesicle-assisted, and enzyme-mediated reaction, in which dissolved dioxygen also takes part as a re-oxidant for TvL, small changes in the composition of the reaction mixture can have significant effects. Initial conditions may not only affect the kinetics of the reaction, but also the outcome, i.e., the product distribution once the reaction reaches its equilibrium state. While a change in the reaction temperature from T ≈ 25 to 5 °C mainly influenced the rate of reaction, increase in enzyme concentration and the presence of millimolar concentrations of chloride ions were found to have significant undesired effects on the outcome of the reaction. Chloride ions, which may originate from the preparation of the pH = 3.5 solution, inhibit TvL, such that higher TvL concentrations are required than without chloride to yield the same product distribution for the same reaction runtime as in the absence of chloride. With TvL concentrations much higher than the elaborated value, the products obtained clearly were different and over-oxidised. Thus, a change in the activity of the enzyme was found to have influence not only on kinetics but also led to a change in the final product distribution, molecular structure and electrical properties, which was a surprising find. The complementary analytical methods which we used in this work were in situ UV/vis/NIR, EPR, and Raman spectroscopy measurements, in combination with a detailed ex situ HPLC analysis and molecular dynamics simulations. With the results obtained, we would like to recall the often neglected or ignored fact that it is important to describe and pay attention to the experimental details, since this matters for being able to perform experiments in a reproducible way.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
Royal Society of Chemistry
en_US
dc.rights.uri
http://creativecommons.org/licenses/by-nc/3.0/
dc.title
How experimental details matter. The case of a laccase-catalysed oligomerisation reaction
en_US
dc.type
Journal Article
dc.rights.license
Creative Commons Attribution-NonCommercial 3.0 Unported
ethz.journal.title
RSC Advances
ethz.journal.volume
8
en_US
ethz.journal.issue
58
en_US
ethz.journal.abbreviated
RSC Adv.
ethz.pages.start
33229
en_US
ethz.pages.end
33242
en_US
ethz.version.deposit
publishedVersion
en_US
ethz.grant
Soft Interfaces as Regulators of Laccase-catalyzed Oligomerization Reactions
en_US
ethz.grant
Conducting polymers synthesized by enzymatic polymerization
en_US
ethz.grant
HPLC analysis of the enzymatic oligomerization of p-aminodiphenylamine
en_US
ethz.identifier.wos
ethz.publication.place
London
en_US
ethz.publication.status
published
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02160 - Dep. Materialwissenschaft / Dep. of Materials
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02160 - Dep. Materialwissenschaft / Dep. of Materials::03763 - Niederberger, Markus / Niederberger, Markus
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02513 - Laboratorium für Anorganische Chemie / Laboratory of Inorganic Chemistry::03872 - Copéret, Christophe / Copéret, Christophe
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02160 - Dep. Materialwissenschaft / Dep. of Materials::03763 - Niederberger, Markus / Niederberger, Markus
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02513 - Laboratorium für Anorganische Chemie / Laboratory of Inorganic Chemistry::03872 - Copéret, Christophe / Copéret, Christophe
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02160 - Dep. Materialwissenschaft / Dep. of Materials::03763 - Niederberger, Markus / Niederberger, Markus
ethz.grant.agreementno
150254
ethz.grant.agreementno
152457
ethz.grant.agreementno
170360
ethz.grant.fundername
SNF
ethz.grant.fundername
SNF
ethz.grant.fundername
SNF
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.funderDoi
10.13039/501100001711
ethz.grant.program
Projektförderung in Mathematik, Natur- und Ingenieurwissenschaften (Abteilung II)
ethz.grant.program
Individuelle Kurzaufenthalte
ethz.grant.program
Joint research projects (SCOPES)
ethz.date.deposited
2018-11-09T05:08:51Z
ethz.source
WOS
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2018-11-21T11:33:01Z
ethz.rosetta.lastUpdated
2024-02-02T06:47:00Z
ethz.rosetta.versionExported
true
ethz.COinS
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