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Two-dimensional (2D) MXene materials have recently been the focus of membrane research due to their unique properties, such as their single-atomic-layer thickness, flexibility, molecular filtration abilities and microstructural similarities with graphene, which is currently the most efficient precursor material for gas separation applications. In addition, the potential to process nanoscale channels has motivated investigations of parameters which can improve membrane permeability and selectivity. Interlayer spacing and defects, which are still challenging to control, are among the most crucial parameters for membrane performance. Herein, the effect of heat treatment on the d-spacing of MXene nanosheets and the surface functionalization of nanolayers was shown regarding its impact on the gas diffusion mechanism. The distance of the layers was reduced by a factor of over 10 from 0.345 nm to 0.024 nm, the defects were reduced, and the surface functionalization was maintained upon treatment of the Ti3C2 membrane at 500 °C under an Ar/H2 atmosphere as compared to 80 °C under vacuum. This led to a change from Knudsen diffusion to molecular sieving, as demonstrated by single-gas permeation tests at room temperature. Overall, this work shows a simple and promising way to improve H2/CO2 selectivity via temperature treatment under a controlled atmosphere.

Poly(ethylene oxide) (PEO)-based copolymers are at the forefront of advanced membrane materials for selective CO2 separation. In this work, free-standing composite membranes were prepared by blending imidazolium-based ionic liquids (ILs) having different structural characteristics with a PEO-based copolymer previously developed by our group, targeting CO2 permeability improvement and effective CO2/gas separation. The effect of IL loading (30 and 40 wt%), alkyl chain length of the imidazolium cation (ethyl- and hexyl- chain) and the nature of the anion (TFSI-, C(CN)3-) on physicochemical and gas transport properties were studied. Among all composite membranes, PEO-based copolymer with 40 wt% IL3-[HMIM][TFSI] containing the longer alkyl chain of the cation and TFSI- as the anion exhibited the highest CO2 permeability of 46.1 Barrer and ideal CO2/H2 and CO2/CH4 selectivities of 5.6 and 39.0, respectively, at 30 °C. In addition, almost all composite membranes surpassed the upper bound limit for CO2/H2 separation. The above membrane showed the highest water vapor permeability value of 50,000 Barrer under both wet and dry conditions and a corresponding H2O/CO2 ideal selectivity value of 1080; values that are comparable with those reported for other highly water-selective PEO-based polymers. These results suggest the potential application of this membrane in hydrogen purification and dehydration of CO2 gas streams.

Nanocomposite sodalite/ceramic membranes supported on α-Al2O3 tubular support were prepared via the pore-plugging hydrothermal (PPH) synthesis protocol using one interruption and two interruption steps. In parallel, thin-film membranes were prepared via the direct hydrothermal synthesis technique. The as-synthesized membranes were evaluated for H2/CO2 separation in the context of pre-combustion CO2 capture. Scanning electron microscopy (SEM) was used to check the surface morphology while x-ray diffraction (XRD) was used to check the crystallinity of the sodalite crystals and as-synthesized membranes. Single gas permeation of H2, CO2, N2 and mixture gas H2/CO2 was used to probe the quality of the membranes. Gas permeation results revealed nanocomposite membrane prepared via the PPH synthesis protocols using two interruption steps displayed the best performance. This was attributed to the enhanced pore-plugging effect of sodalite crystals in the pores of the support after the second interruption step. The nanocomposite membrane displayed H2 permeance of 7.97 × 10−7 mol·s−1·m−2·Pa−1 at 100 °C and 0.48 MPa feed pressure with an ideal selectivity of 8.76. Regarding H2/CO2 mixture, the H2 permeance reduced from 8.03 × 10−7 mol·s−1·m−2·Pa−1 to 1.06 × 10−7 mol·s−1·m−2·Pa−1 at 25 °C and feed pressure of 0.18 MPa. In the presence of CO2, selectivity of the nanocomposite membrane reduced to 4.24.