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Article ; Online: Importance of the Electrostatic Correlations in Surface Tension of Hydrated Reline Deep Eutectic Solvent from Combined Experiments and Molecular Dynamics Simulations.

Cuvellier, Jean-Baptiste / Andanson, Jean-Michel / Ballerat-Busserolles, Karine / Hulin, Hyazann / Artzner, Franck / Malfreyt, Patrice / Ghoufi, Aziz

The journal of physical chemistry. B

2024 Volume 128, Issue 16, Page(s) 4008–4020

Abstract: In this study, the surface tension and the structure of hydrated reline are investigated by using diverse methods. Initially, the surface tension displays a nonlinear pattern as water content increases, decreasing until reaching 45 wt %, then gradually ... ...

Abstract	In this study, the surface tension and the structure of hydrated reline are investigated by using diverse methods. Initially, the surface tension displays a nonlinear pattern as water content increases, decreasing until reaching 45 wt %, then gradually matching that of pure water. This fluctuation is associated with strong electrostatic correlations present in pure reline, which decrease as more water is added. Changes in surface tension reflect a shift from charge layering in pure reline to an increased interfacial hydrogen bonding as the water content rises. This shift causes the segregation of urea molecules into the bulk phase and a gradual anchoring of water molecules to the air-reline interface. An interesting observation is the antisurfactant effect, where heightened interfacial anchoring results in an unexpected increase in real contribution of surface tension. This, along with weakened electrostatic correlations beyond 45 wt % due to reinforced interfacial hydrogen bonding, contributes to the complex behavior of surface tension observed in this study.
Language	English
Publishing date	2024-04-15
Publishing country	United States
Document type	Journal Article
ISSN	1520-5207
ISSN (online)	1520-5207
DOI	10.1021/acs.jpcb.3c08338
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Article ; Online: Improving laccase thermostability with aqueous natural deep eutectic solvents.

Delorme, Astrid E / Andanson, Jean-Michel / Verney, Vincent

International journal of biological macromolecules

2020 Volume 163, Page(s) 919–926

Abstract: The wide-spread use of laccases in industry is often limited due to the enzyme inactivation over time at conditions which exceeds the operating conditions of the enzymes, which are neutral pH and ambient temperatures (30-40 °C). Natural Deep Eutectic ... ...

Abstract	The wide-spread use of laccases in industry is often limited due to the enzyme inactivation over time at conditions which exceeds the operating conditions of the enzymes, which are neutral pH and ambient temperatures (30-40 °C). Natural Deep Eutectic Solvents (NADESs) have attracted considerable attention as reaction media in biocatalysis due to their promising compatibility with enzymes and sustainable derivation. In this contribution we demonstrate the possibility of applying aqueous NADESs as incubation media to alter the activity and inhibit thermal inactivation of laccase T. versicolor. For example we show that by incubating 0.25 g L
MeSH term(s)	Biological Products/chemistry ; Enzyme Activation ; Enzyme Stability ; Hydrogen-Ion Concentration ; Laccase/chemistry ; Solvents/chemistry ; Structure-Activity Relationship ; Thermodynamics
Chemical Substances	Biological Products ; Solvents ; Laccase (EC 1.10.3.2)
Language	English
Publishing date	2020-07-08
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	282732-3
ISSN	1879-0003 ; 0141-8130
ISSN (online)	1879-0003
ISSN	0141-8130
DOI	10.1016/j.ijbiomac.2020.07.022
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Article ; Online: Reactive sputtering onto an ionic liquid, a new synthesis route for bismuth-based nanoparticles.

Ibrahim, Sara / Ntomprougkidis, Vitalios / Goutte, Mathias / Monier, Guillaume / Traïkia, Mounir / Andanson, Jean-Michel / Bonnet, Pierre / Bousquet, Angelique

Nanoscale

2023 Volume 15, Issue 11, Page(s) 5499–5509

Abstract: Metallic bismuth and Bi-oxyfluoride nanoparticles (NPs) are successfully synthesized by non-reactive and reactive sputtering of a Bi target onto 1-butyl-3-methylimidazolium bis(trifluoro-methylsulfonyl)imide ([BMIM][TFSI]) ionic liquid (IL). Non-reactive ...

Abstract	Metallic bismuth and Bi-oxyfluoride nanoparticles (NPs) are successfully synthesized by non-reactive and reactive sputtering of a Bi target onto 1-butyl-3-methylimidazolium bis(trifluoro-methylsulfonyl)imide ([BMIM][TFSI]) ionic liquid (IL). Non-reactive sputtering is realized in pure Ar plasma, where isotropic, well crystallized and dispersed Bi NPs of 3-7 nm are obtained. The diameter and the size distribution of these NPs do not significantly vary with the power, gas pressure, and sputtering time; but these sputtering parameters seem to influence the NP concentration. Then, the introduction of O
Language	English
Publishing date	2023-03-16
Publishing country	England
Document type	Journal Article
ZDB-ID	2515664-0
ISSN	2040-3372 ; 2040-3364
ISSN (online)	2040-3372
ISSN	2040-3364
DOI	10.1039/d2nr07028f
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Article ; Online: Natural deep eutectic solvents as thermostabilizer for Humicola insolens cutinase.

Romano, Angela / Varriale, Simona / Pezzella, Cinzia / Totaro, Grazia / Andanson, Jean-Michel / Verney, Vincent / Sisti, Laura

New biotechnology

2023 Volume 76, Page(s) 118–126

Abstract: As a new generation of green solvents, deep eutectic solvents (DESs) are considered a promising alternative to current harsh organic solvents and find application in many chemical processing methods such as extraction and synthesis. DESs, normally formed ...

Abstract	As a new generation of green solvents, deep eutectic solvents (DESs) are considered a promising alternative to current harsh organic solvents and find application in many chemical processing methods such as extraction and synthesis. DESs, normally formed by two or more components via various hydrogen bond interactions, offer high potential as medium for biocatalysis reactions where they can improve efficiency by enhancing substrate solubility and the activity and stability of the enzymes. In the current study, the stabilization of Humicola insolens cutinase (HiC) in natural deep eutectic solvents (NADESs) was assessed. The best hydrogen bond donor among sorbitol, xylitol, erythritol, glycerol and ethylene glycol, and the best acceptor among betaine, choline chloride, choline acetate, choline dihydrogen citrate and tetramethylammonium chloride, were selected, evaluating binding energies and molecular orientations through molecular docking simulations, and finally used to prepare NADES aqueous solutions. The effects of component ratio and NADES concentration on HiC thermostability at 90 °C were also investigated. The choline dihydrogen citrate:xylitol, in a 1:1 ratio with a 20 wt% concentration, was selected as the best combination in stabilizing HiC, increasing its half-life three-fold.
MeSH term(s)	Deep Eutectic Solvents ; Molecular Docking Simulation ; Xylitol ; Solvents/chemistry ; Choline/chemistry ; Citrates
Chemical Substances	Deep Eutectic Solvents ; cutinase (EC 3.1.1.-) ; Xylitol (VCQ006KQ1E) ; Solvents ; Choline (N91BDP6H0X) ; Citrates
Language	English
Publishing date	2023-05-29
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	2400836-9
ISSN	1876-4347 ; 1876-4347
ISSN (online)	1876-4347
ISSN	1876-4347
DOI	10.1016/j.nbt.2023.05.006
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Article ; Online: Natural deep eutectic solvents as thermostabilizer for Humicola insolens cutinase

Romano, Angela / Varriale, Simona / Pezzella, Cinzia / Totaro, Grazia / Andanson, Jean-Michel / Verney, Vincent / Sisti, Laura

New BIOTECHNOLOGY. 2023 May 29,

2023

Abstract	As a new generation of green solvents, deep eutectic solvents (DESs) are considered a promising alternative to current harsh organic solvents and find application in many chemical processing methods such as extraction and synthesis. DESs, normally formed by two or more components via various hydrogen bond interactions, offer high potential as medium for biocatalysis reactions where they can improve efficiency by enhancing substrate solubility and the activity and stability of the enzymes. In the current study, the stabilization of Humicola insolens cutinase (HiC) in natural deep eutectic solvents (NADESs) was assessed. The best hydrogen bond donor among sorbitol, xylitol, erythritol, glycerol and ethylene glycol, and the best acceptor among betaine, choline chloride, choline acetate, choline dihydrogen citrate and tetramethylammonium chloride, were selected, evaluating binding energies and molecular orientations through molecular docking simulations, and finally used to prepare NADES aqueous solutions. The effects of component ratio and NADES concentration on HiC thermostability at 90 °C were also investigated. The choline dihydrogen citrate:xylitol, in a 1:1 ratio with a 20wt% concentration, was selected as the best combination in stabilizing HiC, increasing its half-life three-fold.
Keywords	Humicola insolens ; acetates ; betaine ; biocatalysis ; biotechnology ; chlorides ; choline ; choline chloride ; citrates ; cutinase ; erythritol ; ethylene glycol ; glycerol ; half life ; hydrogen bonding ; solubility ; sorbitol ; tetramethylammonium compounds ; thermal stability ; xylitol ; Bet ; ChAc ; ChCl ; ChDHC ; Ery ; EtG ; Gly ; HDA ; HBD ; NADES ; Sor ; TMACl ; Xyl ; wt% ; enzyme stability ; Molecular docking ; Choline dihydrogencitrate
Language	English
Dates of publication	2023-0529
Publishing place	Elsevier B.V.
Document type	Article ; Online
Note	Pre-press version ; Use and reproduction
ZDB-ID	2400836-9
ISSN	1876-4347 ; 1871-6784
ISSN (online)	1876-4347
ISSN	1871-6784
DOI	10.1016/j.nbt.2023.05.006
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Article ; Online: Time-concentration profiles of tire particle additives and transformation products under natural and artificial aging

Fohet, Loélia / Andanson, Jean-Michel / Charbouillot, Tiffany / Malosse, Lucie / Leremboure, Martin / Delor-Jestin, Florence / Verney, Vincent

Science of the Total Environment. 2023 Feb., v. 859 p.160150-

2023

Abstract: Tire and road wear particles (TRWP) are polymer-based microparticles that are emitted into the environment during tire usage. Growing efforts are currently being made to quantify these emissions, characterize the leachates and assess their environmental ... ...

Abstract	Tire and road wear particles (TRWP) are polymer-based microparticles that are emitted into the environment during tire usage. Growing efforts are currently being made to quantify these emissions, characterize the leachates and assess their environmental impact. This study aimed to investigate the effect of aging on TRWP composition. Cryomilled tire tread particles (CMTTP) and TRWP were exposed for different durations to three aging conditions: accelerated thermal and photochemical aging and natural outdoor aging. Particles were then extracted with cyclohexane/ethanol. The time-concentration profiles of 23 additives and transformation products present in these extracts were determined by UHPLC-HRMS. Several chemicals, such as N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine (6-PPD) or 1,3-diphenylguanidine (DPG), decayed exponentially under all aging conditions, with half-lives of a few days under artificial photoaging versus dozens of days under pure thermal aging at 60 °C. The natural aging profiles lie between those 2 laboratory aging conditions. Other chemicals, such as 6PPD-quinone, presented bell-shaped concentration profiles within CMTTP when particles were exposed to UV light. 6PPD-quinone reached a maximal concentration within a month under natural aging. For TRWP, the initial load of 6PPD-quinone had already reached a maximum prior to the aging experiments and decreased exponentially under natural aging with a half-life below one month. Pure thermal aging induced a significantly slower decay of 6PPD-quinone within TRWP (half-life of half a year), emphasizing a greater stability and persistence in environmental compartments without light. This study highlighted that the more readily accessible CMTTP could be considered a reasonable proxy of TRWP to investigate the fate of chemicals within rubber particles, at least from a qualitative standpoint. Overall, the concentrations of 20 of the evaluated chemicals decreased by >50 % within 50 days under natural aging.
Keywords	cyclohexanes ; environment ; environmental impact ; ethanol ; half life ; photoaging ; photochemistry ; rubber ; ultraviolet radiation ; 6QDI ; 6PPD ; 6PPD-quinone ; BR ; BT ; CBS ; CMTTP ; DPG ; DT50 ; ESI ; NR ; PM2.5 ; PM10 ; RT ; SBR ; TMQ ; TRWP ; UHPLC-HRMS ; Tire and road wear particles (TRWP) ; Aging ; N,N′-diphenylguanidine (DPG) ; N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine (6PPD)
Language	English
Dates of publication	2023-02
Publishing place	Elsevier B.V.
Document type	Article ; Online
ZDB-ID	121506-1
ISSN	1879-1026 ; 0048-9697
ISSN (online)	1879-1026
ISSN	0048-9697
DOI	10.1016/j.scitotenv.2022.160150
Database	NAL-Catalogue (AGRICOLA)

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Article: Improving laccase thermostability with aqueous natural deep eutectic solvents

Delorme, Astrid E / Andanson, Jean-Michel / Verney, Vincent

International journal of biological macromolecules. 2020 Nov. 15, v. 163

2020

Abstract	The wide-spread use of laccases in industry is often limited due to the enzyme inactivation over time at conditions which exceeds the operating conditions of the enzymes, which are neutral pH and ambient temperatures (30–40 °C). Natural Deep Eutectic Solvents (NADESs) have attracted considerable attention as reaction media in biocatalysis due to their promising compatibility with enzymes and sustainable derivation. In this contribution we demonstrate the possibility of applying aqueous NADESs as incubation media to alter the activity and inhibit thermal inactivation of laccase T. versicolor. For example we show that by incubating 0.25 g L⁻¹ laccase in an aqueous 25 wt% betaine-xylitol based NADES at 70 °C for 15 min, the measured residual activity of laccase is a near 10 fold greater than the measured residual activity of laccase when incubated without the NADES. Moreover, the comparison of the residual activities of the enzyme in presence betaine, xylitol or NADES is clearly showing the advantage of using a NADES over its individual components. The drastic enhancement of the enzyme thermostability by pre-incubation of laccase in NADES media showcases a facile, cheap and green method of boosting the stability laccase.
Keywords	betaine ; biocatalysis ; enzyme inactivation ; heat inactivation ; industry ; laccase ; pH ; thermal stability ; xylitol
Language	English
Dates of publication	2020-1115
Size	p. 919-926.
Publishing place	Elsevier B.V.
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	282732-3
ISSN	1879-0003 ; 0141-8130
ISSN (online)	1879-0003
ISSN	0141-8130
DOI	10.1016/j.ijbiomac.2020.07.022
Database	NAL-Catalogue (AGRICOLA)

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Zs.B 2374: Show issues

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Article ; Online: Time-concentration profiles of tire particle additives and transformation products under natural and artificial aging.

Fohet, Loélia / Andanson, Jean-Michel / Charbouillot, Tiffany / Malosse, Lucie / Leremboure, Martin / Delor-Jestin, Florence / Verney, Vincent

The Science of the total environment

2022 Volume 859, Issue Pt 1, Page(s) 160150

Abstract	Tire and road wear particles (TRWP) are polymer-based microparticles that are emitted into the environment during tire usage. Growing efforts are currently being made to quantify these emissions, characterize the leachates and assess their environmental impact. This study aimed to investigate the effect of aging on TRWP composition. Cryomilled tire tread particles (CMTTP) and TRWP were exposed for different durations to three aging conditions: accelerated thermal and photochemical aging and natural outdoor aging. Particles were then extracted with cyclohexane/ethanol. The time-concentration profiles of 23 additives and transformation products present in these extracts were determined by UHPLC-HRMS. Several chemicals, such as N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine (6-PPD) or 1,3-diphenylguanidine (DPG), decayed exponentially under all aging conditions, with half-lives of a few days under artificial photoaging versus dozens of days under pure thermal aging at 60 °C. The natural aging profiles lie between those 2 laboratory aging conditions. Other chemicals, such as 6PPD-quinone, presented bell-shaped concentration profiles within CMTTP when particles were exposed to UV light. 6PPD-quinone reached a maximal concentration within a month under natural aging. For TRWP, the initial load of 6PPD-quinone had already reached a maximum prior to the aging experiments and decreased exponentially under natural aging with a half-life below one month. Pure thermal aging induced a significantly slower decay of 6PPD-quinone within TRWP (half-life of half a year), emphasizing a greater stability and persistence in environmental compartments without light. This study highlighted that the more readily accessible CMTTP could be considered a reasonable proxy of TRWP to investigate the fate of chemicals within rubber particles, at least from a qualitative standpoint. Overall, the concentrations of 20 of the evaluated chemicals decreased by >50 % within 50 days under natural aging.
MeSH term(s)	Benzoquinones/analysis ; Polymers/chemistry ; Phenylenediamines/analysis ; Guanidines/analysis ; Rubber/chemistry ; Half-Life
Chemical Substances	Benzoquinones ; Polymers ; N-(1,3-dimethylbutyl)-N'-phenyl-1,4-phenylenediamine (HJD0U67PS1) ; N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine quinone ; Phenylenediamines ; diphenylguanidine (6MRZ85RNHQ) ; Guanidines ; Rubber (9006-04-6)
Language	English
Publishing date	2022-11-13
Publishing country	Netherlands
Document type	Journal Article
ZDB-ID	121506-1
ISSN	1879-1026 ; 0048-9697
ISSN (online)	1879-1026
ISSN	0048-9697
DOI	10.1016/j.scitotenv.2022.160150
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Article: Fluorination effect on the solubility of C60 in a bis(trifluoromethimide based)imide based ionic liquid

Ahmad, Yasser / Andanson, Jean-Michel / Bonnet, Pierre / Batisse, Nicolas / Claves, Daniel / Dubois, Marc / Padua, Agilio

Colloids and surfaces. 2022 Apr. 29,

2022

Abstract: Highly fluorinated fullerenes with a chemical composition of C₆₀F₄₈ have been prepared and characterized. Their solubility of the new nanomaterials in the ionic liquid (IL) has been compared with raw fullerenes C₆₀. Fluorination may appear as a ... ...

Abstract	Highly fluorinated fullerenes with a chemical composition of C₆₀F₄₈ have been prepared and characterized. Their solubility of the new nanomaterials in the ionic liquid (IL) has been compared with raw fullerenes C₆₀. Fluorination may appear as a convenient method to enhance the solubility of carbonaceous nanomaterials in a fluorinated based anion IL. Indeed, the ability of 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([BmIm][NTf₂]), to solubilize C₆₀ and C₆₀F₄₈ was investigated using optical microscopy and UV-vis spectroscopy. While C₆₀ has very poor solubility in this IL (below 0.07mmol/L), the solubility increases at least eightfold, i.e. more than 1.0mg/mL (or 0.61mmol/L) for C₆₀F₄₈ samples. The presence of fluorine atoms on fullerene seems to enhance the stability of the solvated molecules in IL thanks to the limitation of the aggregation of C₆₀F₄₈ in [BmIm][NTf₂]. This improvement of the solubility could be explained by the beneficial effect of the fluorination that induces a decrease of the π-π interaction between carbonaceous solutes as the carbon hybridization changes from sp² to sp³ through the formation of C-F covalent bonds and thus enhances the interaction between the solvent and the solute. Fluorination appears as an efficient approach to limit the use of volatile organic compounds usually used as co-solvent to enhance the dispersion mechanism.
Keywords	chemical composition ; fluorine ; fullerene ; ionic liquids ; light microscopy ; solubility ; solutes ; ultraviolet-visible spectroscopy ; volatile organic compounds
Language	English
Dates of publication	2022-0429
Publishing place	Elsevier B.V.
Document type	Article
Note	Pre-press version
ZDB-ID	1500517-3
ISSN	0927-7757
ISSN	0927-7757
DOI	10.1016/j.colsurfa.2022.129140
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Article: Enhancing the Thermostability of Engineered Laccases in Aqueous Betaine-Based Natural Deep Eutectic Solvents.

Varriale, Simona / Delorme, Astrid E / Andanson, Jean-Michel / Devemy, Julien / Malfreyt, Patrice / Verney, Vincent / Pezzella, Cinzia

ACS sustainable chemistry & engineering

2021 Volume 10, Issue 1, Page(s) 572–581

Abstract: In recent years, natural deep eutectic solvents (NADESs) have gained increasing attention as promising nontoxic solvents for biotechnological applications, due to their compatibility with enzymes and ability to enhance their activity. Betaine-based ... ...

Abstract	In recent years, natural deep eutectic solvents (NADESs) have gained increasing attention as promising nontoxic solvents for biotechnological applications, due to their compatibility with enzymes and ability to enhance their activity. Betaine-based NADESs at a concentration of 25 wt % in a buffered aqueous solution were used as media to inhibit thermal inactivation of POXA1b laccase and its five variants when incubated at 70 and 90 °C. All the tested laccases showed higher residual activity when incubated in NADES solutions, with a further enhancement achieved also for the most thermostable variant. Furthermore, the residual activity of laccases in the presence of NADESs showed a clear advantage over the use of NADESs' individual components. Molecular docking simulations were performed to understand the role of NADESs in the stabilization of laccases toward thermal inactivation, evaluating the interaction between each enzyme and NADESs' individual components. A correlation within the binding energies between laccases and NADES components and the stabilization of the enzymes was demonstrated. These findings establish the possibility of preincubating enzymes in NADESs as a facile and cost-effective solution to inhibit thermal inactivation of enzymes when exposed to high temperatures. This computer-aided approach can assist the tailoring of NADES composition for every enzyme of interest.
Language	English
Publishing date	2021-12-29
Publishing country	United States
Document type	Journal Article
ISSN	2168-0485
ISSN	2168-0485
DOI	10.1021/acssuschemeng.1c07104
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