Christian Pellerin

Christian Pellerin
Université de Montréal | UdeM · Department of Chemistry

PhD in chemistry

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102
Publications
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Publications

Publications (102)
Article
Understanding interfacial interactions in polymer systems is crucial for their applicability for instance in adhesives and coatings. Enclosing polymers in a cylindrical volume provides a system for studying interactions dictated by a continuous interfacial layer and a bulk-like volume in the middle of the cylinders. Here, we describe a simple metho...
Article
Full-text available
Electrospun fibers often exhibit enhanced properties at reduced diameters, a characteristic now widely attributed to a high molecular orientation of the polymer chains along the fiber axis. A parameter that can affect the molecular organization is the type of collector onto which fibers are electrospun. In this work, we use polarized confocal Raman...
Article
Eumelanin, a macromolecular biopigment, is an attractive candidate for sustainable (green) organic electronics. Establishing structure−property relationships in eumelanin films is an essential step to exploit its technological potential. We report on the evolution from the molecular state to film after spin coating on silicon dioxide solutions of (...
Article
Large-area metal/molecule/metal junctions based on self-assembled monolayers (SAMs) of organothiolates are of interest for investigations of charge transport across ultrathin organic films and the fabrication of molecular electronic devices. Several recent reports demonstrate an odd-even dependency in the rate of charge transport through SAMs of th...
Article
Elucidating the influence of the monolayer interface versus bulk on the macroscopic properties (e.g., surface hydrophobicity, charge transport, and electron transfer) of organic self-assembled monolayers (SAMs) chemically anchored to metal surfaces is a challenge. This article reports the characterization of prototypical SAMs of n-alkanethiolates o...
Article
A challenge in glass engineering is the design of molecular glasses combining a high glass kinetic stability (GS) of the amorphous phase with a low (sub‐ambient) glass transition temperature (Tg). Triazine derivatives with arylamino substituents readily form glassy phases that can show outstanding resistance to crystallization. In the present study...
Article
Large-area metal/molecule/metal junctions based on self-assembled monolayers (SAMs) of organothiolates are of interest for the investigation of charge transport across ultrathin organic films and the fabrication of molecular electronic devices such as diodes and switches. Several reports demonstrate an odd-even dependency in the rate of charge tran...
Article
Lithium-ion batteries (LiBs) are a mature technology which has attracted much attention over the last three decades with the development of portable devices. With the increasing number of LiBs and their use in electric vehicles, there are persistent efforts to enhance their safety by identifying suitable substitutes for liquid non-aqueous electroly...
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Full-text available
Supramolecular complexation between photoresponsive azobenzene chromophores and a photopassive polymer host offers synthetic and design advantages compared to conventional covalent azo-containing polymers. In this context, it is important to understand the impact of the strength of the supramolecular interaction on the optical response. Herein, we...
Article
The rate of photomechanical formation of surface relief gratings (SRG) in thin films of azobenzene materials depends on their glass transition temperature (Tg), with an optimal Tg around 50-60 °C yielding the fastest SRG growth. Herein, the SRG growth of five analogous Disperse Red 1 molecular glasses with Tg values ranging from 9 to 71 °C was stud...
Article
With the idea of improving the mechanical properties of acrylonitrile–butadiene rubber (NBR) for potential industrial application, hybrid nanofillers prepared by hybridizing graphene oxide (GO) with halloysite nanotubes (HNT), were incorporated through mechanical blending to reinforce NBR. Graphene oxide/halloysite nanotubes (GH) hybrid filler demo...
Article
Gel polymer electrolytes (GPEs) based on polyacrylonitrile elastomer (HNBR) are investigated for lithium-ion batteries application. This study examines the acrylonitrile content, as well as the solvent used to make the GPE, in order to understand their impact on lithium solvation. To do so, we propose a three-component system comprising HNBR:solven...
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The black-brown biopigment eumelanin screens the harmful ultraviolet (UV) radiation in the human skin. In industry, the absorption in the UV range of plastics is improved by the inclusion of additives. Our work reports an evaluation of the biopigment eumelanin as a nature-inspired additive for polymers to improve their UV-absorption. Eumelanin bein...
Article
Knowledge of the thermotropic phase behavior of solid-supported bilayer lipid assemblies is essential for mimicking the molecular organization and lateral fluidity of cell membranes. The gel-to-fluid phase transitions in a homologous series of single phospholipid bilayers supported on planar silicon substrates were investigated by temperature-contr...
Article
Dip-coating allows nanostructured block copolymer (BCP) thin film fabrication in a fast and facile one-step process. It can also be coupled with external controls, such as illumination. Herein, we expose several design principles that enable photocontrol of the nanostructured surface pattern and thickness of supramolecular BCP thin films. This is d...
Article
Full-text available
Advanced fibers revolutionized structural materials in the second half of the 20th Century. However, all high-strength fibers developed to date are brittle. Recently, pioneering simultaneous ultrahigh strength and toughness were discovered in fine (<250 nm) individual electrospun polymer nanofibers (NFs). This highly desirable combination of proper...
Article
In the human body, the black‐brown biopigment eumelanin blocks the harmful ultraviolet (UV) radiation. In the plastics industry, additives are often added to polymers to increase their UV‐absorption properties. We herein report an assessment of the biopigment eumelanin as a nature‐inspired additive for plastics to enhance their UV‐absorption. Since...
Article
Hydrogen bonding is a key element of supramolecular chemistry and is often used in crystal engineering to direct crystal packing. In particular, systems where motifs with multiple hydrogen (H) bonds are present, such as the donor- acceptor-donor – acceptor-donor-acceptor (DAD-ADA) synthon, can be used to generate various supramolecular architecture...
Article
Recent mechanical studies of ultrafine electrospun polymer nanofibers showed they can simultaneously possess high strength and toughness attributed to high degree of chain alignment coupled with low crystallinity. Quantitative analysis of macromolecular alignment in nanofibers is needed for better understanding of processing/structure/properties re...
Article
Mussels’ anchoring threads, named byssus, are collagen-rich fibers with outstanding mechanical properties. Our previous work has shown the possibility of producing a byssus protein hydrolyzate with good film-forming ability, providing a promising new avenue for the preparation of biomaterials. Materials prepared from regenerated fibrous proteins of...
Article
To optimize azobenzene-containing materials for applications such as rewritable waveguides and holographic data storage, it is imperative to understand the effect of the azobenzene structure on the photoresponse of the material. Supramolecular materials, in which a complexed photoactive azobenzene controls the motion or other properties of a passiv...
Article
Exciting new applications, from large-area nanopatterning and templating to soft light-powered robotics, are emerging from the fundamental research on light-triggered changes in macromolecular systems upon photoisomerization of azobenzene-based molecular photoswitches. The understanding of how the initial molecular-scale photoisomerization of azobe...
Article
Full-text available
Introducing photochromic or polymeric dopants into nematic liquid crystals is a well-established method to create stimuli-responsive photonic materials with the ability to “control light with light”. Herein, we demonstrate a new material design concept by showing that specific supramolecular interactions between the host liquid crystal and the gues...
Article
A star shaped poly(sulfobetaine methacrylate) (PSBMA) and its linear analogs, display upper-critical-solution-temperature (UCST) type behavior in 0.1 M NaCl. The presence of sodium dodecyl sulfate (SDS) or cetyl trimethyl ammonium bromide (CTAB) has a significant effect on the thermal transition of the polymer. The association of the polymer with t...
Article
Electrospun fibers are complex polymeric materials with a typical diameter of a few hundred nanometers that are often frozen in out-of-equilibrium states due to the fast solvent evaporation and high elongational forces during the process. Their molecular orientation, and the parameters affecting it, is a critical (although challenging) parameter to...
Article
Strong and directional non-covalent interactions stand as valuable tools in crystal engineering for influencing molecular packing. However, hydrogen (H) bonds have also been used to engineer compounds capable of forming very stable glassy phases, which they stabilize by providing molecular cohesion and limiting molecular mobility. Herein, a second...
Article
It has recently been established that physical vapor deposition (PVD) can produce organic glasses with enhanced kinetic stability, high density, and anisotropic packing, with the substrate temperature during deposition (Tsubstrate) as the key control parameter. The influence of hydrogen bonding on the formation of PVD glasses has not been fully exp...
Article
Full-text available
Several bivalve species produce byssus threads to provide attachment to substrates, with mechanical properties highly variable among species. Here, we examined the distal section of byssal threads produced by a range of bivalve species (Mytilus edulis, Mytilus trossulus, Mytilus galloprovincialis, Mytilus californianus, Pinna nobilis, Perna perna,...
Article
Irradiation of azomaterials causes various photophysical and photomechanical effects that can be exploited for the preparation of functional materials such as surface relief gratings (SRGs). Herein, we develop and apply an efficient strategy to optimize the SRG inscription process by decoupling, for the first time, the important effects of the azo...
Article
Langmuir-Blodgett (LB) films of amphiphilic block copolymers (BCs) form well-defined nanostructures with long-range order useful, for instance, for nanolithography applications. Nanostructures with a 2D circular micelle ("dot") morphology are known to present a constant pressure plateau in their Langmuir isotherm (surface pressure vs molecular area...
Article
The byssus that anchors mussels to solid surfaces is a protein-based material combining strength and toughness as well as a self-healing ability. These exceptional mechanical properties are explained in part by the presence of metal ions forming sacrificial bonds with amino acids. In this study, we show that the properties of hydrogel films prepare...
Article
The influence of the supramolecular interaction type - hydrogen bonding, proton transfer, and pure ionic bonding - on photoresponsive behavior, particularly surface relief grating (SRG) inscription, has been investigated using a homopolymer with an ambient temperature glass transition (Tg). To this end, poly(dimethylaminoethyl methacrylate) (PDMAEM...
Article
The electrospinning of continuous fibers normally requires the presence of a network of topological entanglements in solution, limiting the spinnability of low molecular weight polymers. Here, we show that a supramolecular approach can improve, and even render possible, the electrospinning of low molecular weight polymers, illustrated here with pol...
Article
Mexylaminotriazine derivatives form molecular glasses with outstanding glass-forming ability (GFA), high resistance to crystallization (glass kinetic stability, GS), and a glass transition temperature (Tg) above room temperature that can be conveniently modulated by selection of the headgroup and ancillary groups. A common feature of all these comp...
Article
We demonstrate experimentally for the first time that the illumination of azobenzene derivatives leads to changes in molecular environment similar to those observed on heating but that are highly heterogeneous at the sub-molecular scale. This localized photoplasticization, which can be associated with a free volume gradient, helps to understand the...
Article
The supramolecular assembly of photoactive azobenzenes with passive polymers via halogen or hydrogen bonding is a cost-effective way to design materials for various photomechanical applications that convert light energy directly into macroscopic motion, for instance, in all-optical surface patterning and photochemical imaging of plasmonic structure...
Article
We demonstrate a unique combination of simultaneous top-down and bottom-up control of the morphology of block copolymer films by application of in situ optical irradiation during dip-coating. A light-addressable and block-selective small molecule, 4-butyl-4′-hydroxyazobenzene (BHAB), is introduced into a diblock copolymer of polystyrene and poly(4-...
Article
Recent literature has shown that the thickness of dip-coated films has a V-shaped dependence on dip-coating rate when very slow rates are included. For supramolecular block copolymer films, small molecule (SM) uptake and film morphology are also rate-dependent, as shown previously for a poly(styrene-b-4-vinylpyridine) (PS-P4VP) block copolymer in T...
Article
Electrospun fibers are versatile materials that exhibit unusual and tunable properties when studied at the single fiber level, including an exponential increase in modulus with a decreasing diameter toward the nanoscale. Understanding the detailed molecular organization giving rise to this behavior is a key for reaching the ultimate goal of control...
Article
Full-text available
Surface patterning that occurs spontaneously during the formation of a thin film is a powerful tool for controlling film morphology at the nanoscale level because it avoids the need for further processing. However, one must first learn under which conditions these patterning phenomena occur or not, and how to achieve control over the surface morpho...
Article
Electrospun fibers show a rich and complex variety of diameter-dependent properties. Chain orientation, confinement, and partial disentanglement are the three main factors that have been proposed to explain these phenomena. While molecular orientation is currently the subject of intensive study, the others are more challenging to probe experimental...
Article
The fabrication of electrospun fibers generally requires relatively concentrated solutions to have sufficient chain entanglements acting as physical crosslinks during the electrospinning process. We propose a supramolecular approach to diminish the necessary concentration. To this end, we investigated the use of a small hydrogen-bond effective cros...
Article
The byssus is a series of collagen-rich fibers securing mussels to surfaces. The complex but elegant heterogeneous assembly of the various proteins in the threads is responsible for their remarkable mechanical properties combining strength and extensibility. Along with the well-known biocompatibility and biodegradability attributed to collagen-base...
Article
To understand the characteristics of electrospun fibers of poly(4-vinyl pyridine) (P4VP) that are potentially crosslinked by hydrogen-bonding when blended with small molecules like 4,4′-biphenol (BiOH), it is necessary to determine the proportion of hydrogen-bonded pyridine rings (fb) and to contrast it with FOH, the mole percent of OH groups avail...
Article
Electrospinning was applied to DMF solution mixtures of poly(methyl methacrylate) (PMMA) and MO/PVP, which is an azo‐containing liquid crystalline complex between methyl orange (MO) and methylated poly(4‐vinyl pyridine) (PVP), to obtain composite light‐responsive fibers. The average diameter of the fibers, which ranged from 700 nm to 1.5 µm, increa...
Data
Full-text available
The byssus is a series of collagen-rich fibers securing mussels to surfaces. The complex but elegant heterogeneous assembly of the various proteins in the threads is responsible for their remarkable mechanical properties combining strength and extensibility. Along with the well-known biocompatibility and biodegradability attributed to collagen-base...
Article
Full-text available
Mexylaminotriazine derivatives are known to spontaneously form long-lived glassy phases. The role played by various structural elements in their glass formation has been studied, but the effect of substituting both arylamino substituents remains largely unknown. A library of 4,6-bis(arylamino)-or 4,6-bis(alkylamino)-1,3,5-triazine derivatives with...
Article
Electrospinning is the most versatile and popular technique for preparing nanofibers from a very broad range of polymer systems. In spite of more than 20 years of studies, our understanding of the relationships between the microstructure and the properties of these fibers, and how they are influenced by the electrospinning conditions, remains fragm...
Article
Full-text available
The physical properties of polymers are strongly affected by their molecular orientation. In this paper, we demonstrate for the first time a new and improved Raman spectroscopy method to characterize this key parameter. In recent years, Raman spectroscopy has emerged as an indispensable tool for this purpose, but its widespread use is still largely...
Article
The blue mussels Mytilus edulis are widely cultured in the coastal regions of Canada. However, their production on sleeves attached to long lines in the water column suffers from fall-offs due to byssus weakening, especially during the spawning period. Thus, we tested in laboratory the hypothesis that the spawning event changes the chemical and bio...
Article
Polarized Raman spectroscopy is widely used to quantify the level of molecular orientation of various types of materials. By using a simplified procedure we call the depol (depolarization) constant (DC) method, since it assumes that the depolarization ratio is a constant. However, our ability to quantify orientation by using the DC method is often...
Article
The molecular structure of the blue mussel Mytilus edulis whole anchoring threads was studied by two-dimensional 13C solid-state NMR on fully labeled fibers. This unique material proves to be well ordered at a molecular level despite its heterogeneous composition as evidenced by the narrow measured linewidths below 1.5 ppm. The spectra are dominate...
Article
The simultaneous orientation of poly(1,4-butylene)succinate (PBS) and 4,4′-bis(2-benzoxazolyl)stilbene (BBS) or 2,5-bis(5-tert-butyl-benzoxazol-2-yl)thiophene (BBT) in PBS–BBS and PBS–BBT films was investigated during stretching at 80 °C, about 33 °C below the PBS melting temperature. The PBS orientation was first investigated using the 3430 cm−1 i...
Article
The molecular structure of the blue mussel Mytilus edulis whole anchoring threads was studied by twodimensional 13C solid-state NMR on fully labeled fibers. This unique material proves to be well ordered at a molecular level despite its heterogeneous composition as evidenced by the narrow measured linewidths below 1.5 ppm. The spectra are dominated...
Article
Mexylaminotriazines are an exciting new class of small molecules capable of forming glassy phases (molecular glasses) that have shown outstanding glass-forming properties and resistance to crystallization. The effect of the structure of the ‘headgroup’ at the 2-position of the triazine ring on glass-forming properties has been studied, but the role...
Article
In dip-coated thin films of supramolecular block copolymers where a small molecule (SM) preferentially interacts with one of the blocks, an important issue is whether or not the SM content in the films is the same as that in the dip-coating solution. Here, we quantitatively determined the SM content, using infrared spectroscopy in the attenuated to...
Article
The ability to characterize individual electrospun fibers is essential in order to understand and control this complex process. In this paper, we demonstrate that confocal Raman microscopy is a powerful method to quantify molecular orientation and structure at the individual fiber level using poly(ethylene terephthalate) as a model system. Highly r...
Article
Full-text available
Supramolecular polymer complexes with small molecules are self-assembled through non-covalent interactions and have been proposed for a wide variety of applications in materials science and nanoscience. Our research group has recently shown the possibility of forming highly ordered nanofibers of supramolecular complexes in their thermodynamically s...
Article
Full-text available
The morphology of freeze-dried silk fibroin 3D-scaffolds was modified by varying both the NaCl concentration and the freezing temperature of the silk fibroin solution prior to lyophilization. Scanning electron micrographs showed that slow freezing at −22°C generated sponge-like interconnected porous networks, whereas fast freezing at −73°C formed s...
Article
We demonstrate that spin coating is an efficient method for preparing pure complexes between polymers and small molecules. Samples of the α and β complexes between poly(ethylene oxide) and urea were prepared as proof-of-concept examples since they show congruent and incongruent fusion, respectively. Infrared spectroscopy showed that pure complex of...
Article
We demonstrate that miscible and phase-separated fibers of the blend between polystyrene (PS) and poly(vinyl methyl ether) (PVME) can be electrospun by appropriate selection of the solvent. Solutions in benzene allow preparing miscible fibers with composition ranging from pure PS to PS/PVME 70/30. Results indicate that the rapid solvent evaporation...
Article
In this work, we demonstrate that electrospray is a simple and efficient method for preparing pure supramolecular complexes between a polymer and a small molecule. Such complexes are often difficult to prepare by conventional methods because of the kinetically favored crystallization of the small molecules. However, the fast solvent evaporation inv...
Article
We demonstrate that electrospinning is a simple and efficient method of preparing pure polymer complexes. Such complexes are often difficult to prepare by conventional methods because of the kinetically favored crystallization of small molecules. As proof-of-concept examples, nanofibers of the complexes of poly(ethylene oxide) with hydroquinone and...
Article
Electrospinning was used for the first time to prepare nanofibers of the host/guest complex between poly(ethylene oxide) (PEO) and thiourea. It is shown by differential scanning calorimetry (DSC) and wide-angle X-ray diffraction (WAXD) that the stoichiometry of the complex is (EO)(12)-(thiourea)(8), settling a series of conflicting values in litera...
Article
Bis(mexylamino)triazines have been identified as a family of compounds showing an exceptional propensity to form glassy phases as opposed to crystals. The particularities of this family of compounds are their ability to self-assemble through hydrogen bonding in well-defined patterns to form supramolecular aggregates which pack poorly and the wide r...
Article
Polarized planar array infrared (PA-IR) spectroscopy is shown for the first time to be a powerful approach to study the mechanical deformation of polymers. A dual-beam PA-IR spectrometer was built to enable the simultaneous recording of parallel- and perpendicular-polarized spectra at the same sample spot. The technique provides orientation and str...
Chapter
IntroductionConcept and InstrumentationPA-IR SpectroscopyApplicationsConclusions References
Article
The poly(ethylene oxide)–urea binary system forms a stable (α) complex that can be melt-quenched into a mixture of urea and a second (β) complex with a different stoichiometry. Our results confirm that this mixture is metastable, but that the β–α solid–solid transition is much slower than previously reported. In contrast with the melt-quenched mixt...
Article
Full-text available
Diaminotriazine derivatives with 3,5-dimethylphenyl groups have been shown to be capable of readily forming extremely stable glassy phases under ambient conditions, and self-assembly through hydrogen bonding has been thought to be a key element in this process. Herein, we probed the role played by hydrogen bonding in glass formation in this family...
Chapter
This chapter describes how different physical techniques can provide useful quantitative data for the evaluation of molecular orientation to emphasize their possibilities and limitations. It discusses the theory and procedures for orientation measurements and its quantitative characterization. The methods described in the chapter provide very accur...
Article
Full-text available
Polarization modulation infrared linear dichroism (PM-IRLD) is often used for measurements of molecular orientation with high sensitivity and good time resolution. However, PM-IRLD is unable to provide the structural absorbance spectrum because it does not measure separately the parallel and perpendicular spectra. Here we propose a new method, name...
Article
Solution electrospinning was used for the first time to prepare nanofibers of the stable (α) and metastable (β) complexes between poly(ethylene oxide) (PEO) and urea. Both types of fibers were highly crystalline and presented a large level of molecular orientation. Detailed characterization of the ill-studied β complex was performed using wide angl...
Article
Planar array infrared spectroscopy (PA-IR) was used for the first time to record transient infrared (TIRS) spectra. In proof-of-concept experiments, it was demonstrated that PA-TIRS can record high quality spectra of common polymeric samples. It was shown the this new technique allows acquiring spectra in as little as 17 ms, opening the door to hig...
Article
Self-assembled thin films of block copolymers constitute an elegant means to obtain nanopatterns and nanotemplates on surfaces. Here, we demonstrate how interacting small molecules can be used to control the morphology of dip-coated block copolymer films. Such films obtained from THF solutions of styrene-4-vinylpyridine block copolymers (PS-b-PVP,...