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Article ; Online: Highlighting the interdependence between volumetric contribution of fragility and cooperativity for polymeric segmental relaxation.

Trubert, Jules / Matkovska, Liubov / Saiter-Fourcin, Allisson / Delbreilh, Laurent

2024 Volume 160, Issue 4

Abstract: The blurring around the link between the isobaric fragility and the characteristic size of cooperative rearranging region for glass-forming liquids has been cleared up by considering volumetric and thermal contributions of the structural relaxation. The ... ...

Abstract	The blurring around the link between the isobaric fragility and the characteristic size of cooperative rearranging region for glass-forming liquids has been cleared up by considering volumetric and thermal contributions of the structural relaxation. The measurement of these contributions is carried out for three amorphous thermoplastic polymers using broadband dielectric spectroscopy under pressure, providing an understanding of the link between isobaric fragilities, glass transition temperatures, and microstructures. The cooperative rearranging region (CRR) volume is calculated as a function of pressure using the extended Donth's approach, and the values are compared with the activation volume at the glass transition under different isobaric conditions. By combining these different results, a link between the chemical structure and the influence of pressure/temperature on the molecular mobility can be established. Furthermore, this study shows also a strong correlation between the activation volume, leading to the volumetric contribution of the isobaric fragility, and the CRR volume. Finally, this work highlights the influence of inter- and intra-molecular interactions on thermal and volumetric contributions of the isobaric fragility as a function of pressure.
Language	English
Publishing date	2024-01-30
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/5.0187941
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Influence of Chemical Composition and Structure on the Cooperative Fluctuation in Supercooled Glass-Forming Liquids.

Hallavant, Kylian / Mejres, Marouane / Schawe, Jürgen E K / Esposito, Antonella / Saiter-Fourcin, Allisson

The journal of physical chemistry letters

2024 Volume 15, Issue 16, Page(s) 4508–4514

Abstract: The kinetics of the glass transition and the characteristic size of the fluctuating spatio-temporal domains in supercooled glass-forming liquids, i.e., the Cooperatively Rearranging Regions (CRR), were measured upon cooling over a broad range of cooling ... ...

Abstract	The kinetics of the glass transition and the characteristic size of the fluctuating spatio-temporal domains in supercooled glass-forming liquids, i.e., the Cooperatively Rearranging Regions (CRR), were measured upon cooling over a broad range of cooling rates using Differential Scanning Calorimetry (DSC) and chip-based Fast Scanning Calorimetry (FSC). The investigations were conducted on a selection of fragile glass formers (fragility indices between 80 and 140), with a large variance in the atomic or molecular structure but comparable thermal glass transition temperatures
Language	English
Publishing date	2024-04-18
Publishing country	United States
Document type	Journal Article
ISSN	1948-7185
ISSN (online)	1948-7185
DOI	10.1021/acs.jpclett.4c00632
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Multiscale Analysis of Segmental Relaxation in PC/PETg Multilayers: Evidence of Immiscible Nanodroplets

Rijal, Bidur / Delbreilh, Laurent / Sollogoub, Cyrille / Baer, Eric / Saiter-Fourcin, Allisson

Macromolecules. 2022 July 29, v. 55, no. 15

2022

Abstract: This work highlights the influence of layer thicknesses on glass transition and molecular mobility in polycarbonate (PC) and poly(ethylene terephthalate glycol) (PETg) multilayered films obtained by the layer-multiplying coextrusion process. By combining ...

Abstract	This work highlights the influence of layer thicknesses on glass transition and molecular mobility in polycarbonate (PC) and poly(ethylene terephthalate glycol) (PETg) multilayered films obtained by the layer-multiplying coextrusion process. By combining modulated temperature scanning calorimetry (MT-DSC) and dielectric relaxation spectroscopy (DRS) measurements, the average values of the cooperative rearranging region (CRR) size in a wide range of relaxation times and temperatures have been calculated. The size reduction from micro- to nanoscale is accompanied by a significant deviation of the structural and dynamical properties compared to the bulk. Furthermore, we have evidenced significant differences in PETg and PC behaviors: PETg plays the role of a “hard-confined” polymer, while PC behaves as a “free-confined” polymer, implying opposite variations of the glass transition temperature. The determination of the relaxation parameters for each individual polymer has been possible even for very low layer thicknesses (below 10 nm), for which the multilayer structure is not observed. This result shows that even when PETg and PC are brought into very intimate contact, they maintain their own structural behavior and segmental relaxation, suggesting the formation of immiscible nanodroplets when the multilayer structure disappears.
Keywords	calorimetry ; glass transition ; glass transition temperature ; polymers ; spectroscopy
Language	English
Dates of publication	2022-0729
Size	p. 6562-6572.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	1491942-4
ISSN	1520-5835 ; 0024-9297
ISSN (online)	1520-5835
ISSN	0024-9297
DOI	10.1021/acs.macromol.2c00691
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Distinct dynamics of structural relaxation in the amorphous phase of poly(l-lactic acid) revealed by quiescent crystallization.

Monnier, Xavier / Delpouve, Nicolas / Saiter-Fourcin, Allisson

Soft matter

2020 Volume 16, Issue 13, Page(s) 3224–3233

Abstract: Fast scanning calorimetry (FSC) experiments were performed to investigate physical aging in amorphous and semi-crystalline poly(l-lactic acid)s (PLLAs) that were thermally crystallized under conditions leading to the α'- or α-crystalline form, and either ...

Abstract	Fast scanning calorimetry (FSC) experiments were performed to investigate physical aging in amorphous and semi-crystalline poly(l-lactic acid)s (PLLAs) that were thermally crystallized under conditions leading to the α'- or α-crystalline form, and either favouring or inhibiting the development of a rigid amorphous fraction (RAF). The enthalpy of recovery was calculated after two procedures of rescaling to the content of the whole amorphous phase and also to the only content of the mobile amorphous fraction (MAF), which helped in clarifying the contribution of the RAF. From the dependence of the structural relaxation rate on the aging temperature, two regimes were evidenced for all samples. In the aging temperature domain situated close to the glass transition, the structural relaxation occurs significantly faster in the MAF. Its rate is independent of the aging temperature and is not influenced by the microstructure. However, the distance to equilibrium is higher in samples for which the coupling is strong between crystal and amorphous, implying that the time to reach equilibrium is also higher. In contrast, at low aging temperatures, for which the whole amorphous phase can be considered as solid, MAF and RAF exhibit the same structrural relaxation rate. This convergence in the relaxation kinetics by decreasing the temperature of physical aging was interpreted as the evolution of relaxation dynamics in the MAF from segmental to local. This change is highlighted by the comparison between MAF and RAF relaxation kinetics, but it occurs similarly in a pure amorphous system.
Language	English
Publishing date	2020-03-23
Publishing country	England
Document type	Journal Article
ZDB-ID	2191476-X
ISSN	1744-6848 ; 1744-683X
ISSN (online)	1744-6848
ISSN	1744-683X
DOI	10.1039/c9sm02541c
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Quantifying morphological and mechanical properties of thermoplastics elastomers by selective localization of nanofillers with different geometries

Chandran, Nithin / C, Sarathchandran / Sivadas, Anjaly / Saiter-Fourcin, Allisson / Thomas, Sabu

Colloids and surfaces. 2021 Nov. 20, v. 629

2021

Abstract: Potential role of nanofiller in deciding their localization in polypropylene (PP)-natural rubber (NR) blend system is evaluated using experimental techniques followed by authentication using various theoretical approaches. Thermoplastic elastomers (TPEs) ...

Abstract	Potential role of nanofiller in deciding their localization in polypropylene (PP)-natural rubber (NR) blend system is evaluated using experimental techniques followed by authentication using various theoretical approaches. Thermoplastic elastomers (TPEs) of PP-NR blend-based nanocomposites with Cloisite 15A and titanium dioxide (TiO₂) were prepared by melt mixing method, using Haake rheocord-90. In pre-fixed blend composition of 70-30 (PP-NR), selective localization of nanofiller was determined by transmission electron microscopy (TEM), and quantified by Harmonic mean theoretical studies. Correlation length (ξcₗₐy) and average length of the clay layers (Lcₗₐy) measured for the dispersion of nanoclay. The dispersion efficiency of Cloisite 15A and TiO₂ in blend matrix were determined by X-ray diffraction (XRD) studies. Mechanical properties of blend nanocomposites were examined by varying the nanofiller loading and compared with theoretical approaches such as Kerner, Guth, Halpin-Tsai, Einstein and Quemada models. It was found that irrespective of the geometry, the fillers migrated to the PP phase leading to significant changes in morphological development (size reduction of dispersed phase) and increased mechanical properties of 70-30 (PP-NR) neat blend. Nevertheless, it is very important to mention that at higher loading the layers of Cloisite 15A are found to penetrate partially into the NR phase due to the anisotropic nature of the clay platelets.
Keywords	X-ray diffraction ; anisotropy ; clay ; geometry ; nanoclays ; nanocomposites ; polypropylenes ; rubber ; thermoplastics ; titanium dioxide ; transmission electron microscopy
Language	English
Dates of publication	2021-1120
Publishing place	Elsevier B.V.
Document type	Article
ZDB-ID	1500517-3
ISSN	0927-7757
ISSN	0927-7757
DOI	10.1016/j.colsurfa.2021.127365
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Impact of chirality on the amorphous state of conglomerate forming systems: a case study of

Atawa, Bienvenu / Couvrat, Nicolas / Affouard, Frédéric / Correia, Natália T / Coquerel, Gérard / Saiter-Fourcin, Allisson

Physical chemistry chemical physics : PCCP

2021 Volume 23, Issue 42, Page(s) 24282–24293

Abstract: The present work aims at addressing the issue of molecular handedness in glassy and liquid states and its impact on heterogeneous equilibrium. For this purpose, we evaluated the glass forming ability (GFA), crystallization propensity, molecular mobility ... ...

Abstract	The present work aims at addressing the issue of molecular handedness in glassy and liquid states and its impact on heterogeneous equilibrium. For this purpose, we evaluated the glass forming ability (GFA), crystallization propensity, molecular mobility and hydrogen bonding structure of a chiral conglomerate forming system,
Language	English
Publishing date	2021-11-03
Publishing country	England
Document type	Journal Article
ZDB-ID	1476244-4
ISSN	1463-9084 ; 1463-9076
ISSN (online)	1463-9084
ISSN	1463-9076
DOI	10.1039/d1cp03843e
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Assessment of Graphene Oxide and Nanoclay Based Hybrid Filler in Chlorobutyl-Natural Rubber Blend for Advanced Gas Barrier Applications.

Keloth Paduvilan, Jibin / Velayudhan, Prajitha / Amanulla, Ashin / Joseph Maria, Hanna / Saiter-Fourcin, Allisson / Thomas, Sabu

Nanomaterials (Basel, Switzerland)

2021 Volume 11, Issue 5

Abstract: Nanomaterials have engaged response from the scientific world in recent decades due to their exceptional physical and chemical properties counter to their bulk. They have been widely used in a polymer matrix to improve mechanical, thermal, barrier, ... ...

Abstract	Nanomaterials have engaged response from the scientific world in recent decades due to their exceptional physical and chemical properties counter to their bulk. They have been widely used in a polymer matrix to improve mechanical, thermal, barrier, electronic and chemical properties. In rubber nanocomposites, nanofillers dispersion and the interfacial adhesion between polymer and fillers influences the composites factual properties. In the present work, a comparison of the hybrid effects of carbon black with two different nanofillers (graphene oxide and nanoclay) was studied. The 70/30 composition of chlorobutyl rubber/natural rubber elastomer blend was taken as per the blend composition optimized from our previous studies. The hybrid effects of graphene oxide and nanoclay in dispersing the nanofillers were studied mainly by analyzing nanocomposite barrier properties. The results confirm that the combined effect of carbon black with graphene oxide and nanoclay could create hybrid effects in decreasing the gas permeability. The prepared nanocomposites which partially replace the expensive chlorobutyl rubber can be used for tyre inner liner application. Additionally, the reduction in the amount of carbon black in the nanocomposite can be an added advantage of considering the environmental and economic factors.
Language	English
Publishing date	2021-04-23
Publishing country	Switzerland
Document type	Journal Article
ZDB-ID	2662255-5
ISSN	2079-4991
ISSN	2079-4991
DOI	10.3390/nano11051098
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Article ; Online: Influence of reduced graphene oxide on flow behaviour, glass transition temperature and secondary crystallinity of plasticized poly(vinyl chloride).

Akhina, H / Ramya, Koduvayur A / Gopinathan Nair, M R / Saiter-Fourcin, Allisson / Garda, Marie-Rose / Deshpande, Abhijit P / Kalarikkal, Nandakumar / Thomas, Sabu

RSC advances

2020 Volume 10, Issue 49, Page(s) 29247–29256

Abstract: Understanding the rheological behaviour of thermoplastic nanocomposites is important to obtain a concrete knowledge of their processability. The viscoelastic properties of nanocomposites are a reflection of their morphology. The study of flow and ... ...

Abstract	Understanding the rheological behaviour of thermoplastic nanocomposites is important to obtain a concrete knowledge of their processability. The viscoelastic properties of nanocomposites are a reflection of their morphology. The study of flow and deformation of nanocomposites provides essential information related to prevalent interactions in the system as well as contribution from the dispersion of incorporated nanofillers. In the present study, plasticized polyvinyl chloride/reduced graphene oxide nanocomposites (PPVC/RGO) were fabricated using melt mixing technique with different filler concentration. Flow behaviour of the nanocomposites was analyzed using small amplitude oscillatory shear (SAOS) measurements and it indicated an enhancement in the storage modulus (
Language	English
Publishing date	2020-08-07
Publishing country	England
Document type	Journal Article
ISSN	2046-2069
ISSN (online)	2046-2069
DOI	10.1039/d0ra04560h
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Influence of reduced graphene oxide on flow behaviour, glass transition temperature and secondary crystallinity of plasticized poly(vinyl chloride)

Akhina, H / Ramya, Koduvayur A / Gopinathan Nair, M. R / Saiter-Fourcin, Allisson / Garda, Marie-Rose / Deshpande, Abhijit P / Kalarikkal, Nandakumar / Thomas, Sabu

RSC advances. 2020 Aug. 07, v. 10, no. 49

2020

Abstract	Understanding the rheological behaviour of thermoplastic nanocomposites is important to obtain a concrete knowledge of their processability. The viscoelastic properties of nanocomposites are a reflection of their morphology. The study of flow and deformation of nanocomposites provides essential information related to prevalent interactions in the system as well as contribution from the dispersion of incorporated nanofillers. In the present study, plasticized polyvinyl chloride/reduced graphene oxide nanocomposites (PPVC/RGO) were fabricated using melt mixing technique with different filler concentration. Flow behaviour of the nanocomposites was analyzed using small amplitude oscillatory shear (SAOS) measurements and it indicated an enhancement in the storage modulus (G′), loss modulus (G′′) and complex viscosity (η*) with RGO content. This can be attributed to very good dispersion and reinforcing effect of RGO in PPVC matrix as supported by TEM and FTIR results. Weak gel model is used to fit the rheological parameters and is found to be in excellent agreement with the SAOS experiments. Thermal history of the prepared nanocomposites was learned using differential scanning calorimetry. A shift in glass transition temperature (Tg) to higher temperature region could be seen, that manifest the effect of RGO in the amorphous portion of PPVC. An interesting property called secondary crystallinity was also found in these materials.
Keywords	crystal structure ; deformation ; gels ; glass transition temperature ; graphene oxide ; loss modulus ; models ; nanocomposites ; poly(vinyl chloride) ; storage modulus ; thermoplastics ; viscoelasticity
Language	English
Dates of publication	2020-0807
Size	p. 29247-29256.
Publishing place	The Royal Society of Chemistry
Document type	Article
Note	NAL-AP-2-clean
ISSN	2046-2069
DOI	10.1039/d0ra04560h
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Promoting Interfacial Interactions with the Addition of Lignin in Poly(Lactic Acid) Hybrid Nanocomposites.

Patanair, Bindu / Saiter-Fourcin, Allisson / Thomas, Sabu / Thomas, Martin George / Parathukkamparambil Pundarikashan, Poornima / Gopalan Nair, Kalaprasad / Kumar, Varsha Krishna / Maria, Hanna J / Delpouve, Nicolas

Polymers

2021 Volume 13, Issue 2

Abstract: In this paper, the calorimetric response of the amorphous phase was examined in hybrid nanocomposites which were prepared thanks to a facile synthetic route, by adding reduced graphene oxide (rGO), Cloisite 30B (C30B), or multiwalled carbon nanotubes ( ... ...

Abstract	In this paper, the calorimetric response of the amorphous phase was examined in hybrid nanocomposites which were prepared thanks to a facile synthetic route, by adding reduced graphene oxide (rGO), Cloisite 30B (C30B), or multiwalled carbon nanotubes (MWCNT) to lignin-filled poly(lactic acid) (PLA). The dispersion of both lignin and nanofillers was successful, according to a field-emission scanning-electron microscopy (FESEM) analysis. Lignin alone essentially acted as a crystallization retardant for PLA, and the nanocomposites shared this feature, except when MWCNT was used as nanofiller. All systems exhibiting a curtailed crystallization also showed better thermal stability than neat PLA, as assessed from thermogravimetric measurements. As a consequence of favorable interactions between the PLA matrix, lignin, and the nanofillers, homogeneous dispersion or exfoliation was assumed in amorphous samples from the increase of the cooperative rearranging region (CRR) size, being even more remarkable when increasing the lignin content. The amorphous nanocomposites showed a signature of successful filler inclusion, since no rigid amorphous fraction (RAF) was reported at the filler/matrix interface. Finally, the nanocomposites were crystallized up to their maximum extent from the glassy state in nonisothermal conditions. Despite similar degrees of crystallinity and RAF, significant variations in the CRR size were observed among samples, revealing different levels of mobility constraining in the amorphous phase, probably linked to a filler-dimension dependence of space filling.
Language	English
Publishing date	2021-01-15
Publishing country	Switzerland
Document type	Journal Article
ZDB-ID	2527146-5
ISSN	2073-4360 ; 2073-4360
ISSN (online)	2073-4360
ISSN	2073-4360
DOI	10.3390/polym13020272
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