It is demonstrated that solvent-saturated graphite oxide can be considered to be solid solvate, and two phases with distinctly different solvent composition are found near room temperature. Phase transitions between these two solvated phases were observed using synchrotron powder X-ray diffraction and DSC for methanol, ethanol, acetone, and dimethylformamide (DMF) solvents. Solvate A, formed at room temperature, undergoes a reversible phase transition into expanded Solvate L at temperatures slightly below ambient due to insertion of one monolayer of solvent molecules between the GO planes. The phase transition is reversible upon heating, whereas the low-temperature expanded phase L can be quenched to room temperature for ethanol and DMF solvates.
The change of distance between individual graphene oxide sheets due to swelling is the key parameter to explain and predict permeation of multilayered graphene oxide (GO) membranes by various solvents and solutions. In situ synchrotron X-ray diffraction study shows that swelling properties of GO membranes are distinctly different compared to precursor graphite oxide powder samples. Intercalation of liquid dioxolane, acetonitrile, acetone, and chloroform into the GO membrane structure occurs with maximum one monolayer insertion (Type I), in contrast with insertion of 2-3 layers of these solvents into the graphite oxide structure. However, the structure of GO membranes expands in liquid DMSO and DMF solvents similarly to precursor graphite oxide (Type II). It can be expected that Type II solvents will permeate GO membranes significantly faster compared to Type I solvents. The membranes are found to be stable in aqueous solutions of acidic and neutral salts, but dissolve slowly in some basic solutions of certain concentrations, e.g. in NaOH, NaHCO3 and LiF. Some larger organic molecules, alkylamines and alkylammonium cations are found to intercalate and expand the lattice of GO membranes significantly, e.g. up to ∼35 Å in octadecylamine/methanol solution. Intercalation of solutes into the GO structure is one of the limiting factors for nano-filtration of certain molecules but it also allows modification of the inter-layer distance of GO membranes and tuning of their permeation properties. For example, GO membranes functionalized with alkylammonium cations are hydrophobized and they swell in non-polar solvents.
The roughness of woven fabrics strongly limits print quality, which is particularly critical in printing of conductive circuits on fabrics. This work demonstrates the use of wood-derived cellulose nanofibrils (CNFs) mixed with a plasticizer as coatings of woven cotton fabrics for inkjet printing using (i) conventional water-based pigment inks and (ii) conductive silver nanoparticle inks. CNFs, being similar in nature to cotton, introduced minimal alteration to woven cotton fabrics by preserving their visual appearance as well as their mechanical properties. We also showed that the use of CNF-based coatings facilitated ink droplet settling on the substrate, which ensured high quality with the potential of higher printing speed production. The coatings of CNFs plasticized with glycerol enabled concentrating the pigment on the surface of the fabric, preventing its penetration into the fabric depth, which allows for increasing the resolution of the printed pattern. When used for color ink printing, it enhanced the print chroma and permitted reducing the amount of deposited ink, yielding similar color lightness. The CNF coatings allowed for substantial reduction of the amount of silver ink when printing the conductive tracks on fabrics. Furthermore, the nature of the coating imparts flexibility to the conductive layer, while maintaining electric signal quality, even when folded. This study provides a platform for manufacturing sustainable and disposable e-textiles.
High-viscosity liquid cis-1,4 polyisoprene (PI), with up to 20 wt % single-wall carbon nanotubes (SWCNTs), has been cross-linked by high pressure and high temperature (HP&HT) treatment at 513 K and pressures in the range 0.5 to 1.5 GPa to yield densified network polymer composites. A composite with 5 wt % SWCNTs showed 2.2 times higher tensile strength σ UTS (σ UTS = 17 MPa), 2.3 times higher Young's modulus E (E = 220 MPa) and longer extension at break than pure PI. The improvement is attributed to SWCNT reinforcement and improved SWCNT-PI interfacial contact as a result of the HP&HT cross-linking process, and reduced brittleness despite a higher measured cross-link density than that of pure PI. The latter may originate from an effect similar to crazing, i.e., bridging of microcracks by polymer fibrils. We surmise that the higher cross-link densities of the composites are due mainly to physical cross-links/constraints caused by the SWCNT-PI interaction, which also reflects the improved interfacial contact, and that the CNTs promote material flow by disrupting an otherwise chemically cross-linked network. We also deduce that the PI density increase at HP&HT cross-linking is augmented by the presence of CNTs.
Graphite oxide is selectively intercalated by methanol when exposed to liquid water/methanol mixtures with methanol fraction in the range 20–100%. Insertion of water into the GO structure occurs only when the content of water in the mixture with methanol is increased up to 90%. This conclusion is confirmed by both ambient temperature XRD data and specific temperature variations of the GO structure due to insertion/deinsertion of an additional methanol monolayer observed upon cooling/heating. The composition of GO–methanol solvate phases was determined for both low temperature and ambient temperature phases. Understanding of graphite oxide structural properties in binary water/methanol mixtures is important for understanding the unusual permeation properties of graphene oxide membranes for water and alcohols. It is suggested that graphite oxide prepared by Brodie’s method can be used for purification of water using selective extraction of methanol from water/alcohol mixtures.
Polyisoprene (PI)/single-wall carbon nanotube (SWCNT) composites and pure PI have been cross-linked by high-pressure treatment to yield densified elastomeric states. Simultaneously, the SWCNT and cross-linked-induced changes of the thermal conductivity, heat capacity per unit volume, and glass transition were investigated by in situ measurements. The thermal conductivity of both the elastomeric and liquid PI improves ∼120% by the addition of 5 wt % SWCNT filler. The SWCNT filler (5 wt %) increases the glass-transition temperature of liquid PI by ∼7 K and that of the elastomeric state by as much as 12 K, which is due to a filler-induced increase in the cross-link density. Moreover, the 5 wt % filler yields a heat capacity decrease by ∼30% in both the glassy and liquid/elastomeric states, which indicates that SWCNTs cause a remarkably large reduction of both the vibrational and configurational heat capacity of PI. Finally, the consequences of high-pressure densification and the possibilities this provides to help elucidating the nature of the heat conduction in polymer/carbon nanotube composites are discussed.
We report thermal conductivity (κ) of low-density, high-density and ultra-high density polyethylene (PE) with different crystallinity and microstructures. PE was crystallized under high-pressure and high-temperature conditions which produce extended chain crystals. By applying a two-phase model, we estimate κ of 100% crystallized PE as a function of pressure and temperature. The increased crystallinity and lamellar thickness (fold length) reduce the thermal resistance, which is reflected not only in the absolute value of κ but also in more pronounced pressure and temperature dependencies approaching those of polycrystalline low-molecular weight materials. The results suggest that it is crucial to increase the lamellar thickness to significantly improve κ of PE with randomly oriented lamellae.
The transition behavior and thermal properties of nylon-6 at elevated pressure, p, have been established by in-situ thermal conductivity, κ, and heat capacity measurements. The glass transition temperature, T g , of virgin nylon-6 is described well by the empirical equation T g (p)=319.60(1 þ 1.90 p) 0.24 (p in GPa and T g in K). Moreover, isobaric heating in the 1-1.2 GPa range causes a cold-crystallization transition near 500 K. As a result, κ increased ∼15% whereas the heat capacity per unit volume decreased ∼7% slowly with time during 4 h annealing at ∼530 K. The transformation is associated with a significantly increased crystallinity, from ∼35% to 55-60%, and a pressure-induced preferred orientation and increased size for the lamellae of monoclinic R crystalline structure. This state has 8-10 K higher melting temperature and better formic acid resistance than that of virgin nylon-6. However, the results show no indication of crosslinking, as reported for similarly treated nylon-1010 and nylon-11, but instead chain scissoring.
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