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Rapid progress in the performance of organic devices has increased the demand for advances in the technology of thin-film permeation barriers and understanding the failure mechanisms of these material systems. Herein, we report the extensive study of mechanical and gas barrier properties of Al2O3/ZnO nanolaminate films prepared on organic substrates by atomic layer deposition (ALD). Nanolaminates of Al2O3/ZnO and single compound films of around 250 nm thickness were deposited on polyethylene terephthalate (PET) foils by ALD at 90 °C using trimethylaluminium (TMA) and diethylzinc (DEZ) as precursors and H2O as the co-reactant. STEM analysis of the nanolaminate structure revealed that steady-state film growth on PET is achieved after about 60 ALD cycles. Uniaxial tensile strain experiments revealed superior fracture and adhesive properties of single ZnO films versus the single Al2O3 film, as well as versus their nanolaminates. The superior mechanical performance of ZnO was linked to the absence of a roughly 500 to 900 nm thick sub-surface growth observed for single Al2O3 films as well as for the nanolaminates starting with an Al2O3 initial layer on PET. In contrast, the gas permeability of the nanolaminate coatings on PET was measured to be 9.4 × 10−3 O2 cm3 m−2 day−1. This is an order of magnitude less than their constituting single oxides, which opens prospects for their applications as gas barrier layers for organic electronics and food and drug packaging industries. Direct interdependency between the gas barrier and the mechanical properties was not established enabling independent tailoring of these properties for mechanically rigid and impermeable thin film coatings.
Vipin Chawla; Mikko Ruoho; Matthieu Weber; Adib Abou Chaaya; Aidan A. Taylor; Christophe Charmette; Philippe Miele; Mikhael Bechelany; Johann Michler; Ivo Utke. Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition. Nanomaterials 2019, 9, 88 .
AMA StyleVipin Chawla, Mikko Ruoho, Matthieu Weber, Adib Abou Chaaya, Aidan A. Taylor, Christophe Charmette, Philippe Miele, Mikhael Bechelany, Johann Michler, Ivo Utke. Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition. Nanomaterials. 2019; 9 (1):88.
Chicago/Turabian StyleVipin Chawla; Mikko Ruoho; Matthieu Weber; Adib Abou Chaaya; Aidan A. Taylor; Christophe Charmette; Philippe Miele; Mikhael Bechelany; Johann Michler; Ivo Utke. 2019. "Fracture Mechanics and Oxygen Gas Barrier Properties of Al2O3/ZnO Nanolaminates on PET Deposited by Atomic Layer Deposition." Nanomaterials 9, no. 1: 88.
This experimental study explores the potential of supported ionic liquid membranes (SILMs) based on protic imidazolium ionic liquids (ILs) and randomly nanoporous polybenzimidazole (PBI) supports for CH4/N2 separation. In particular, three classes of SILMs have been prepared by the infiltration of porous PBI membranes with different protic moieties: 1-H-3-methylimidazolium bis (trifluoromethane sulfonyl)imide; 1-H-3-vinylimidazolium bis(trifluoromethane sulfonyl)imide followed by in situ ultraviolet (UV) polymerization to poly[1-(3H-imidazolium)ethylene] bis(trifluoromethanesulfonyl)imide. The polymerization process has been monitored by Fourier transform infrared (FTIR) spectroscopy and the concentration of the protic entities in the SILMs has been evaluated by thermogravimetric analysis (TGA). Single gas permeability values of N2 and CH4 at 313 K, 333 K and 363 K were obtained from a series of experiments conducted in a batch gas permeance system. The results obtained were assessed in terms of the preferential cavity formation and favorable solvation of methane in the apolar domains of the protic ionic network. The most attractive behavior exhibited poly[1-(3H-imidazolium)ethylene]bis(trifluoromethanesulfonyl)imide polymeric ionic liquid (PIL) cross-linked with 1% divinylbenzene supported membranes, showing stable performance when increasing the upstream pressure. The CH4/N2 permselectivity value of 2.1 with CH4 permeability of 156 Barrer at 363 K suggests that the transport mechanism of the as-prepared SILMs is solubility-dominated.
Parashuram Kallem; Christophe Charmette; Martin Drobek; Anne Julbe; Reyes Mallada; Maria Pilar Pina. Exploring the Gas-Permeation Properties of Proton-Conducting Membranes Based on Protic Imidazolium Ionic Liquids: Application in Natural Gas Processing. Membranes 2018, 8, 75 .
AMA StyleParashuram Kallem, Christophe Charmette, Martin Drobek, Anne Julbe, Reyes Mallada, Maria Pilar Pina. Exploring the Gas-Permeation Properties of Proton-Conducting Membranes Based on Protic Imidazolium Ionic Liquids: Application in Natural Gas Processing. Membranes. 2018; 8 (3):75.
Chicago/Turabian StyleParashuram Kallem; Christophe Charmette; Martin Drobek; Anne Julbe; Reyes Mallada; Maria Pilar Pina. 2018. "Exploring the Gas-Permeation Properties of Proton-Conducting Membranes Based on Protic Imidazolium Ionic Liquids: Application in Natural Gas Processing." Membranes 8, no. 3: 75.
In this work we report on a novel concept for the preparation of gas selective composite membranes by a simple and robust synthesis protocol involving a controlled in-situpolycondensation of functional alkoxysilanes within the pores of a mesoporous ceramic matrix. This innovative approach targets the manufacture of thin nanocomposite membranes, allowing good compromise between permeability, selectivity and thermomechanical strength. Compared to simple infiltration, the synthesis protocol allows a controlled formation of gas separation membranes from size-adjusted functional alkoxysilanes by a chemical reaction within the mesopores of a ceramic support, without any formation of a thick and continuous layer on the support top-surface. Membrane permeability can thus be effectively controlled by the thickness and pore size of the mesoporous layer, and by the oligomers chain length. The as-prepared composite membranes are expected to possess a good mechanical and thermomechanical resistance and exhibit a thermally activated transport of He and H2 up to 150 °C, resulting in enhanced separation factors for specific gas mixtures e.g. FH2/CO ∼ 10; FH2/CO2 ∼ 3; FH2/CH4 ∼ 62.
M. Drobek; A. Ayral; Julius Motuzas; C. Charmette; C. Loubat; E. Louradour; D. Dhaler; A. Julbe. Novel concept for the preparation of gas selective nanocomposite membranes. The European Physical Journal Special Topics 2015, 224, 1921 -1933.
AMA StyleM. Drobek, A. Ayral, Julius Motuzas, C. Charmette, C. Loubat, E. Louradour, D. Dhaler, A. Julbe. Novel concept for the preparation of gas selective nanocomposite membranes. The European Physical Journal Special Topics. 2015; 224 (9):1921-1933.
Chicago/Turabian StyleM. Drobek; A. Ayral; Julius Motuzas; C. Charmette; C. Loubat; E. Louradour; D. Dhaler; A. Julbe. 2015. "Novel concept for the preparation of gas selective nanocomposite membranes." The European Physical Journal Special Topics 224, no. 9: 1921-1933.
Martin Drobek; Mikhael Bechelany; Cyril Vallicari; Adib Abou Chaaya; Christophe Charmette; Claudia Salvador-Levehang; Philippe Miele; Anne Julbe. An innovative approach for the preparation of confined ZIF-8 membranes by conversion of ZnO ALD layers. Journal of Membrane Science 2015, 475, 39 -46.
AMA StyleMartin Drobek, Mikhael Bechelany, Cyril Vallicari, Adib Abou Chaaya, Christophe Charmette, Claudia Salvador-Levehang, Philippe Miele, Anne Julbe. An innovative approach for the preparation of confined ZIF-8 membranes by conversion of ZnO ALD layers. Journal of Membrane Science. 2015; 475 ():39-46.
Chicago/Turabian StyleMartin Drobek; Mikhael Bechelany; Cyril Vallicari; Adib Abou Chaaya; Christophe Charmette; Claudia Salvador-Levehang; Philippe Miele; Anne Julbe. 2015. "An innovative approach for the preparation of confined ZIF-8 membranes by conversion of ZnO ALD layers." Journal of Membrane Science 475, no. : 39-46.
In this study, a membrane bioreactor (MBR) was developed for efficient, safe microbial methane hydroxylation with Methylosinus trichosporium OB3b. This innovative MBR, which couples a bioreactor with two gas/liquid macroporous membrane contactors supplying the two gaseous substrates (methane and oxygen) was operated in fed-batch mode. The feasibility and the reproducibility of this new biohydroxylation process were first demonstrated. The mass transfer within this MBR was twice that observed in a batch reactor in similar conditions. The productivity reached with this MBR was 75±25mgmethanol(gdrycell)(-1)h(-1). Compared to the literature, this value is 35times higher than that obtained with the only other fed-batch membrane bioreactor reported, which was run with dense membranes, and is comparable to those obtained with bioreactors fed by bubble-spargers. However, in the latter case, an explosive gas mixture can be formed, a problem that is avoided with the MBR.
N. Pen; L. Soussan; Marie-Pierre Belleville; J. Sanchez; Christophe Charmette; D. Paolucci-Jeanjean. An innovative membrane bioreactor for methane biohydroxylation. Bioresource Technology 2014, 174, 42 -52.
AMA StyleN. Pen, L. Soussan, Marie-Pierre Belleville, J. Sanchez, Christophe Charmette, D. Paolucci-Jeanjean. An innovative membrane bioreactor for methane biohydroxylation. Bioresource Technology. 2014; 174 ():42-52.
Chicago/Turabian StyleN. Pen; L. Soussan; Marie-Pierre Belleville; J. Sanchez; Christophe Charmette; D. Paolucci-Jeanjean. 2014. "An innovative membrane bioreactor for methane biohydroxylation." Bioresource Technology 174, no. : 42-52.
This work evaluates a new eco-friendly strategy for preparing ultrathin gas selective membranes on top of a microporous support. The method involves the dissolution of small amounts of fluorinated oligomers with alkoxysilane functional groups in supercritical CO2 (scCO2) and their transport to the substrate followed by the subsequent deposition/filtration under high pressure using a MFI zeolite membrane support (silicalite-1 (S-1), channel size ∼0.55 nm. During the deposition process, the oligomers are compressed on the zeolite surface and potentially forced in the intercrystalline defects of the zeolite membrane, if any. The performance of this new type of polymer/zeolite composite membranes has been evaluated for both single gas permeation and gas mixture separations. Attractive results were obtained applying oligomers with short molecular chains (∼1.2–2 nm; ∼300–600 g mol−1), easily forming an interpenetrated compact network during the deposition process at ΔP=6 MPa and 50 °C. High permselectivities were obtained at 25 °C (αHe/N2⁎=85–135 and αCO2/N2⁎=50–80 with the He and CO2 permeance in the range 1–2.7⁎10−8 mol m−2 s−1 Pa−1) together with attractive separation factors (FHe/N2FHe/N2=49 and FCO2/N2FCO2/N2=18).
Martin Drobek; Julius Motuzas; Véronique Durand; Maxime Duchateau; Christophe Charmette; Audrey Hertz; Cédric Loubat; Anne Julbe. Evaluation of a new supercritical CO2-assisted deposition method for preparing gas selective polymer/zeolite composite membranes. Journal of Membrane Science 2013, 429, 428 -435.
AMA StyleMartin Drobek, Julius Motuzas, Véronique Durand, Maxime Duchateau, Christophe Charmette, Audrey Hertz, Cédric Loubat, Anne Julbe. Evaluation of a new supercritical CO2-assisted deposition method for preparing gas selective polymer/zeolite composite membranes. Journal of Membrane Science. 2013; 429 ():428-435.
Chicago/Turabian StyleMartin Drobek; Julius Motuzas; Véronique Durand; Maxime Duchateau; Christophe Charmette; Audrey Hertz; Cédric Loubat; Anne Julbe. 2013. "Evaluation of a new supercritical CO2-assisted deposition method for preparing gas selective polymer/zeolite composite membranes." Journal of Membrane Science 429, no. : 428-435.
J. Biscarat; C. Charmette; C. Pochat-Bohatier; J. Sánchez. Novel Cross-Linked Gelatine Membranes for Gas Separation: Enhancement of Carbon Dioxide Permeability by Addition of Polyethylene Glycol and Ferulic Acid. Procedia Engineering 2012, 44, 1507 -1509.
AMA StyleJ. Biscarat, C. Charmette, C. Pochat-Bohatier, J. Sánchez. Novel Cross-Linked Gelatine Membranes for Gas Separation: Enhancement of Carbon Dioxide Permeability by Addition of Polyethylene Glycol and Ferulic Acid. Procedia Engineering. 2012; 44 ():1507-1509.
Chicago/Turabian StyleJ. Biscarat; C. Charmette; C. Pochat-Bohatier; J. Sánchez. 2012. "Novel Cross-Linked Gelatine Membranes for Gas Separation: Enhancement of Carbon Dioxide Permeability by Addition of Polyethylene Glycol and Ferulic Acid." Procedia Engineering 44, no. : 1507-1509.
In this work the growth of both a zeolite (MFI) and a zeolite-like material (SOD) were investigated in/on αAl2O3 tubular support, using hydrothermal conditions and microwave (MW) heating. The method reveals efficient for the rapid synthesis of MFI/αAl2O3 membranes although gentle conditions were required in order to limit the thermal degradation of the template. Promising results were also obtained for directly growing SOD in/on the support. In both MFI and SOD MW synthesis the chemical dissolution of the αAl2O3 support influences the final membrane characteristics. In the case of SOD synthesis, this phenomena which increases with both temperature and support size, alters the membrane homogeneity (composition and structure). In order to get round it, MWs were used to prepare SOD small crystals which were deposited on/in the αAl2O3 support and submitted to a secondary growth. Homogeneous membranes were then obtained whose ideal selectivities αH2/N2 and αHe/N2 reaches respectively 4.5 at 20°C and 6.2 at 115°C (these selectivities are lower than 2 for a ZSM-5 membrane in similar conditions).
Anne Julbe; Julius Motuzas; Christophe Charmette; Christian Guizard. How can Microwave Heating Contribute to the Development of Zeolite Membranes. MRS Proceedings 2002, 752, 1 .
AMA StyleAnne Julbe, Julius Motuzas, Christophe Charmette, Christian Guizard. How can Microwave Heating Contribute to the Development of Zeolite Membranes. MRS Proceedings. 2002; 752 ():1.
Chicago/Turabian StyleAnne Julbe; Julius Motuzas; Christophe Charmette; Christian Guizard. 2002. "How can Microwave Heating Contribute to the Development of Zeolite Membranes." MRS Proceedings 752, no. : 1.