Positron Annihilation Lifetime Spectroscopy Measurements Research Articles

Effect of the electric field on the free volume investigated from positron annihilation lifetime and dielectric properties of sulfonated PVC/PMMA

AbstractPolymer electrolyte membranes (PEMs) play a vital role in electrochemical devices, facilitating ion conduction while blocking gases and electrons. Their effectiveness is closely linked to their microstructural properties, especially the free volume, which impacts ionic conductivity, mechanical strength, and overall device performance. This study examines the behavior of PVC/PMMA/SSA blends under electric fields, using Positron Annihilation Lifetime Spectroscopy (PALS) to assess free volume and dielectric properties. The study involved preparing and characterizing membranes through x‐ray diffraction (XRD), thermogravimetric analysis (TGA), and PALS. XRD results indicated semi‐crystalline structures with changes in intensity due to temperature variations, while TGA highlighted changes in thermal stability under different electric fields. PALS measurements showed that free volume varied with temperature and electric field strength, influencing the material's dielectric and mechanical characteristics. The results revealed that higher electric fields reduced free volume while enhancing dielectric properties. The dielectric constant and loss were found to depend on frequency, which was affected by the polar SO3H groups. Impedance spectroscopy provided further insights into the electrical properties, showing increased dc conductivity with stronger electric fields. A correlation between the free volume investigated from PAL and the electrical properties was observed. This study emphasizes the significance of free volume and external electric field in optimizing PEMs for advanced energy applications.

Comparative analysis of parent and modified ZSM-5 zeolites: Insights from positron annihilation lifetime spectroscopy

Modified zeolite ZSM-5 samples were prepared by synthesis in the presence of the organics acting as mesoporogens: cationic surfactant, hexadecyltrimethylammonium bromide (CTAB) and cationic polymer, polydiallyldimethylammonium chloride (PDADMAC), as well as by alkali etching of the parent zeolite. Properties of modified zeolites were compared to the parent ZSM-5 zeolite. X-ray diffractograms demonstrate that the obtained modified zeolite ZSM-5 samples in all cases have preserved parent crystalline zeolite framework of the MFI-type. However, scanning electron micrographs of the same samples show morphology variations of the modified samples as compared to the starting zeolite. Thermogravimetric analyses show distinct weight loss curves of the samples. Differences have been also noted in the hydroxyl stretching range of the infrared spectra, and in the results of positron annihilation lifetime spectroscopy (PALS) measurements, which indicated dissimilarities by probing free volume in parent and modified zeolite ZSM-5 samples. In that way, PALS as scarcely used technique in zeolite studies, proved its applicability in structural investigation of this kind.

Defects and magnetic studies of nanocrystalline cobalt substituted manganese ferrite probed by positron annihilation lifetime spectroscopy and magnetic measurement

Cobalt substituted manganese ferrite nanoparticles, Mn1-xCoxFe2O4 (x = 0.0, 0.1, 0.25 and 0.5) were prepared by co-precipitation procedure. The structural and magnetic properties of ferrite nanoparticles were measured by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and vibrating sample magnetometry (VSM). The lattice constant and cation distribution of ferrite samples were extracted from XRD patterns using the software package MAUD. The crystallite size of the samples was determined by the Scherrer equation and indicated that all of the ferrite samples were nanocrystalline. The defects in the samples were studied by employing positron annihilation lifetime spectroscopy (PALS). From the analysis of the positron lifetime spectrum, three components τ1, τ2, and τ3 with corresponding intensities I1, I2, and I3 were obtained. The mean lifetime of the annihilated positrons is maximum in the case of x = 0.25. This means that the defect concentration for this sample is greater than that for other samples. Magnetic measurements show a significant increase in the saturation magnetization from 20.62 to 36.03 emu/g, as the cobalt content (x) increased. The coercivity (Hc) of ferrite nanoparticles increased with the increasing cobalt ion substitution up to x = 0.25, and decreased for x = 0.5. This behavior of the Hc variation in samples is similar to the variation of average concentration of defects, as indicated by the mean positron lifetime τm, Therefore, it is concluded that the variation in the defect concentration affects the coercivity of the samples.

Effect of the Presence of Structural Defects on the Superconducting Properties of (NbTa)0.67(MoHfW)0.33 and Nb-47wt%Ti

A comparison of the results of studies on the influence of structural defects on the critical parameters of superconductivity has been made for the high-entropy alloy (NbTa)0.67(MoHfW)0.33 and for the conventional superconducting magnet material Nb-47wt%Ti. Positron annihilation lifetime spectroscopy (PALS), electrical resistivity, magnetization and magnetic susceptibility measurements were used. In addition, X-ray powder diffraction studies were performed on the high-entropy alloy (NbTa)0.67(MoHfW)0.33. Due to the rapid cooling of the materials after melting in the arc furnace, they contain a higher concentration of structural defects compared to the heat-treated materials. Magnetic property measurements showed that both the critical temperatures Tc and the upper critical fields μ0Hc2 of bulk superconductivity-related materials are improved in the presence of structural defects.

Mapping positron annihilation lifetime spectroscopy data of a polymer to classical molecular dynamics simulations without shifting the glass transition temperature.

Positron annihilation lifetime spectroscopy (PALS) enables the nondestructive measurement of nanoscale cavities in materials. In this study, a strategy was proposed for mapping PALS measurement data of isotactic polypropylene to classical molecular dynamics (CMD) simulations. The discrepancy between simulated and experimental glass transition temperatures was resolved by shortening the polymer chains, rather than adjusting for the temperature, using the Williams-Landel-Ferry (WLF) equation. The effective probe radii of ortho-positronium (o-Ps), determined by comparing PALS data with CMD simulations, were ∼0.8nm, which was consistent with the o-Ps size given by the solution of the Schrödinger equation. The free-volume fraction corresponding to the effective probe radius was 12.3% at the glass transition temperature, close to the value estimated using Simha-Boyer theory. The cavity number density was proportional to the effective probe radius and decreased with temperature. The o-Ps effective probe radius was proportional to both the critical probe radius and the -1/3 power of the monomer number density, and increased with increasing temperature. These findings suggest that combining PALS measurements with CMD simulations may provide insight into cavities in polymeric materials without relying on the WLF equation.

Fine-Tuning of the Pore Aperture and Framework Flexibility of Mixed-Metal (Zn/Co) Zeolitic Imidazolate Framework-8: An In Situ Positron Annihilation Lifetime Spectroscopy Study under CO2 Gas Pressure.

The mixed-metal (Zn/Co) strategy has been used to enhance the gas separation selectivity of zeolitic imidazolate framework-8 (ZIF-8)-based membranes. The enhancement in selectivity has been attributed to possible modifications in the grain boundary structure, pore architecture, and flexibility of the frameworks. In the present study, we used in situ positron annihilation lifetime spectroscopy (PALS) under varying CO2 pressure to investigate the tuning of the pore architecture and framework flexibility of mixed-metal (Zn/Co) ZIF-8 frameworks with varying Co contents. The random distribution of Zn and Co metal nodes within the highly crystalline frameworks having an SOD topology was established using electron microscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy. The inherent aperture as well as cavity size of the frameworks, and the pore interconnectivity to the outer surface, were observed to vary with the Co content in ZIF-8 due to the random distribution of Zn and Co metal nodes in the frameworks. The aperture size is reduced with the incorporation of an additional metal (Zn or Co) in ZIF-67 or ZIF-8, respectively. The aperture size remains the smallest for a lower Co content (∼0.20) in ZIF-8. The framework flexibility determined by in situ PALS measurements under CO2 pressure continuously reduces with increasing Co content in ZIF-8. A smaller aperture size as well as low flexibility of ZIF-8 with a low Co content is seen to be directly correlated to a higher separation selectivity of membranes prepared with this mixed-metal composition.

Correlating the diffusion of water to performance in model reverse osmosis polyamides with controlled crosslink densities

We systematically reduce the crosslink density of a PA network based on m-phenylene diamine by substituting a fraction of the trifunctional trimesoyl chloride crosslinking agent with a difunctional isophthaloyl analog that promotes chain extension, in order to elucidate robust design cues for improving the polyamide (PA) separation layer in reverse osmosis (RO) membranes for desalination. Thin films of these model PA networks are fully integrated into a composite membrane and evaluated in terms of their water flux and salt rejection. By incorporating 15 mol % of the difunctional chain extender, we reduce the crosslink density of the network by a factor of two, which leads to an 80% increase in the free or unreacted amine content. The resulting swelling of the PA network in liquid water increases by a factor of two accompanied by a 30% increase in the salt passage through the membrane. Surprisingly, this leads to a 30% decrease in the overall permeance of water through the membrane. This conundrum is resolved by quantifying the microscopic diffusion coefficient of water inside the PA network with quasi-elastic neutron scattering. In the highest and lowest crosslink density networks, water shows strong signatures of confined diffusion. At short length scales, the water exhibits translational diffusion that is consistent with the jump-diffusion mechanism. This translational diffusion coefficient is approximately five times slower in the lowest crosslinked density network, consistent with the reduced water permeance. This is interpreted as water molecules interacting more strongly with the increased free amine content. Over longer length scales the water diffusion is confined, exhibiting mobility that is independent of length scale. The length scales of confinement from the quasi-elastic neutron scattering experiments at which this transition from confined to translational diffusion occurs is on the order of (5–6) Å, consistent with complementary X-ray scattering, small angle neutron scattering, and positron annihilation lifetime spectroscopy measurements. The confinement appears to come from heterogeneities in the average inter-atomic distances, suggesting that diffusion occurs by water bouncing between chains and occasionally sticking to the polar functional groups. The results obtained here are compared with similar studies of water diffusion through both rigid porous silicates and ion exchange membranes, revealing robust design cues for engineering high-performance RO membranes.

Evaluation of adsorption and mechanical strength of 13X zeolite mixtures with phyllosilicate binders using molecular dynamics simulation and positron annihilation spectroscopy

There is growing interest in developing zeolites with novel internal structures that have optimal adsorptive capacity and high mechanical strength, while offering advantages, such as being light weight. We integrate computational and experimental methods to explore the effect of binder/zeolite types, and weight percentages on the mechanical strength of 13X zeolite and adsorption capacities of N2, H2O, and CO2 for additive manufacturing (AM) applications with the goal of maximizing both adsorption and strength. Zeolite 13X mixtures and phyllosilicate binders (either bentonite or kaolin) are combined using molecular dynamics (MD) simulations to create structures with various binder/zeolite weight percentages. Adsorption capabilities and mechanical strength are assessed using the grand canonical Monte Carlo (GCMC) and ReaxFF modules, respectively. Our modeling shows that an optimized zeolite/binder ratio for N2 adsorption is around 15 wt% for kaolin and roughly 10 wt% for bentonite. The resulting parameters can be applied to facilitate macro-scale computational fluid dynamics (CFD) and finite element method (FEM) simulations of an AM zeolite structure. We also performed Positron Annihilation Lifetime Spectroscopy (PALS) measurements on zeolite samples to explore the effect of changes in the internal volume. The results show an inverse relationship between the free volume and the solid loading. Adding a binder changes the morphology of the zeolite-binder compound and decreases open-volume area significantly.

Evolution of the free volume during water desorption in thermoplastic starch/citric acid films: In situ positron annihilation studies

The effect of citric acid (CA) concentration and water content on the free hole volume of thermoplastic cassava starch films (TPS) was studied. To this aim, continuous in situ positron annihilation lifetime spectroscopy measurements were performed at fixed moisture content and during water desorption. The results show that the increase in CA concentration leads to wider free hole volume distributions with lower mean values. During water desorption, the mean values and width of such distributions systematically decrease with the exposure time, and the evolution of the hole volumes was well-described using the Kohlrausch-Williams-Watts function. The water vapour permeability was significantly higher in films incorporating 5 % (w/w) of CA, in line with the more open network of this material that was revealed in the hole volumes distribution. The Young's modulus of all the developed films increased significantly after partial water desorption, which was attributed to the plasticizer loss reflected in a decrease in the mean hole volume value (between 4 % and 13 %). This work evidences that the control and report of the relative humidity are essential when testing TPS-based films, as their nanostructures are strongly dependent on external conditions.

Flexibility of Mixed Ligand Zeolitic Imidazolate Frameworks (ZIF-7-8) under CO2 Pressure: An Investigation Using Positron Annihilation Lifetime Spectroscopy.

Fine tuning of the pore architecture and flexibility of zeolitic imidazolate frameworks (ZIFs) is highly crucial for realizing their applications in molecular gas separation. Mixed ligand frameworks (ZIF-7-8) synthesized by mixing 2-methylimidazole (2meIm) and benzimidazole (bIm) ligands show enhanced gas separation performance, attributable to pore and flexibility tuning. In the present study, positron annihilation lifetime spectroscopy (PALS) measurements under CO2 pressure have been used to experimentally investigate the tuning of the pore architecture and flexibility of mixed ligand frameworks ZIF-7-8 having a ZIF-8 structure and similar morphology with varying bIm content up to 18.2%. The aperture and cavity of frameworks begin to open up with an increasing bIm ligand content followed by a decrease at a higher content. On the contrary, flexibility of the frameworks indexed from PALS measurements carried out under CO2 pressure shows a decreasing trend followed by an increase. The present study shows that mixed ligand frameworks having a larger aperture size are less flexible as a result of inherent open configurations of ligands in the framework lattice. On the other hand, frameworks having a comparatively smaller aperture size show higher flexibility as a result of a possibility of twisting of the ligands under CO2 pressure, resulting in aperture opening. The pore-opening phenomenon as a result of lattice flexibility under CO2 pressure is observed to be fully reversible for ZIF-7-8.

Porosimetry of zeolitic imidazolate frameworks using positron annihilation lifetime spectroscopy

Zeolitic Imidazolate Frameworks (ZIFs) owing to their crystalline morphology have well designed pore architecture. ZIFs show great potential for applications in gas separation, gas storage, catalysis and sensors because of their high surface area, pore volume and well defined pore network. In order to utilize ZIFs for aforementioned applications, investigation of pore architecture (pore size, pore size distribution and interconnectivity) of ZIFs in powder or film form is highly essential. Conventional gas adsorption techniques are found to be incapable for providing complete pore architecture of ZIFs due to ultra-microporosity and pressure dependent framework flexibility. In recent years, positron annihilation lifetime spectroscopy (PALS) has been used to investigate the porosity of few ZIFs. In order to establish the applicability of PALS for pore architecture investigation of ZIFs in general, a systematic study for a number of ZIFs (ZIF-67, ZIF-8, ZIF-7l, ZIF-7n ZIF-62, ZIF-90, ZIF-70.52-8, Zn0.25Co0.75-ZIF-8, and ZIF-8A) have been carried out. These frameworks have been synthesized at room temperature or using solvothermal methods. PALS measurements of these ZIFs confirm the presence of different types of interconnected pores in these frameworks. The estimated pore sizes are compared with the pore sizes determined from other conventional techniques. The present study suggests that PALS is a powerful technique for the investigation of tuning of the pore architecture of all type of ZIFs. The determined pore sizes are the factual average pore size of desolvated bulk ZIF samples free from artifacts. These pore sizes could be correlated with the pore size dependent separation performance of ZIFs.

Barrier Properties of Semicrystalline Polylactide: The Role of the Density of the Amorphous Regions

The work explains the mechanism of the improvement of oxygen barrier performance of cold-crystalized polylactide (PLA) modified with low molecular weight compounds (triethyl citrate, TEC; glycerol, Gly; and polyethylene glycol, PEG). It was found that the incorporation of small amounts of modifier (0.5–1.5 wt %) into the PLA matrix greatly reduces the oxygen transport properties. On the other hand, a further increase in the modifier content in PLA blends led to a deterioration of these properties. Based on the thermal analysis, it was shown that the modifier present in the PLA matrix did not affect the degree of crystallinity. Positron annihilation lifetime spectroscopy (PALS) and density measurements were used to correlate the observed changes in the parameters of oxygen permeability with the molecular packing in the interlamellar amorphous region. Overall, it was found that the nanostructure of the amorphous phase, largely dependent on the content and compatibility of the modifier with the polymer matrix, is of key importance in the barrier properties of PLA/modifier systems.

Influence of Crosslinking Extent on Free Volumes of Silicone Rubber and Water Diffusion after Corona Discharge.

Silicone rubber is widely used as an insulating material. In this article, silicone rubber samples were prepared by varying the content of crosslinker (2,5-bis(tert-butyl-peroxy)-2,5-dimethylhexane, DBPMH), and the free volume holes in the samples were investigated by means of positron annihilation lifetime spectroscopy (PALS) measurement. The surface chemical structure, surface micromorphology and water diffusion of the samples after corona discharge treatment were studied by FTIR, SEM and EIS measurements, respectively. As the crosslinker weight ratio increased from 0.2 wt.% to 1.5 wt.%, the mean free volume hole size first decreased and then remained unchanged. However, the concentration of free volume holes did not vary as the crosslinker weight ratio increased. SEM morphologies show that surface cracks were produced on samples having high crosslinking levels after corona treatment. The water diffusion coefficient of samples after corona treatment increased from 3.13 × 10−10 cm2 s−1 to 17.68 × 10−10 cm2 s−1 in the initial immersion period, as the crosslinker weight ratio increased from 0.2 wt.% to 3.0 wt.%. The results indicated that deterioration of samples with high crosslinking levels were more serious and water repellency more easily lost. The corona resistance ability of low crosslinking level silicone rubber stems from internal low molecular weight molecules.

Surfactant functionalised cobalt silica membranes – Gas permeation and thin film positron annihilation lifetime spectroscopy characterisation

This work investigates the use of positron annihilation lifetime spectroscopy (PALS) for the in-situ structural characterisation of silica derived thin film membranes. By using a quantified maximum entropy method, PALS allowed for the measurement of a pore size distribution depth profile. PALS measurements were carried out on a series of silica derived membranes where alumina supports were coated with four layers of cationic HTBA surfactant cobalt silica sols wherein the surfactant/cobalt molar ratio loading varied from 0 to 3. PALS results showed that the coated layers adjacent to the porous alumina substrate were characterised by micropores and broad mesopores, a clear indication that the porosity of the substrate affected the pore size at the substrate and thin film interface. The last coated layer resulted in a high concentration of ultra-micropores (dp < 6 Å). This was attributed to the surface smoothness conferred by three previous coated layers. Higher surfactant loadings resulted in an increase in gas permeation and reduction of He/CO2 permselectivity from 91.5 to 3.8. A strong correlation with R2 up to 0.999 was found between the ultra-micropores in the top layer and gas permselectivity, a clear indication that gas separation is controlled by small pore sizes. In this work, PALS showed to be a powerful tool for the characterisation of the structural features of thin films.

ELECTRON IRRADIATED EFFECT IN POLYURETHANES STUDIED BY POSITRON ANNIHILATION LIFETIME SPECTROSCOPY

The intensity variation of positronium as a result of electron irradiation has been studied on polyurethanes (PU) using positron annihilation lifetime spectroscopy (PALS). The PALS measurement was carried out at room temperature with a conventional fast-fast coincidence system. The lifetime spectra were analyzed into four components using melt program to extract the positron parameters such as lifetime and intensity. Due to irradiation a decrease of intensity about 2.7% was observed up to 10kGy. Free volume radius has been calculated for electron irradiated PU. PALS measurement has also been performed to study the effect of temperature variation in the range 30K to 310K. Analysis by melt program on the spectra shows that the fourth lifetime component increases significantly above glass transition temperature.

Interface effect of Fe and Fe2O3 on the distributions of ion induced defects

The stability of structural materials in extreme nuclear reactor environments—with high temperature, high radiation, and corrosive media—directly affects the lifespan of the reactor. In such extreme environments, an oxide layer on the metal surface acts as a passive layer protecting the metal underneath from corrosion. To predict the irradiation effect on the metal layer in these metal/oxide bilayers, nondestructive depth-resolved positron annihilation lifetime spectroscopy (PALS) and complementary transmission electron microscopy (TEM) were used to investigate small-scale defects created by ion irradiation in an epitaxially grown (100) Fe film capped with a 50 nm Fe2O3 oxide layer. In this study, the evolution of induced vacancies was monitored, from individual vacancy formation at low doses—10−5 dpa—to larger vacancy cluster formation at increasing doses, showing the sensitivity of positron annihilation spectroscopy technique. Furthermore, PALS measurements reveal how the presence of a metal–oxide interface modifies the distribution of point defects induced by irradiation. TEM measurements show that irradiation induced dislocations at the interface is the mechanism behind the redistribution of point defects causing their accumulation close to the interface. This work demonstrates that the passive oxide layers formed during corrosion impact the distribution and accumulation of radiation induced defects in the metal underneath and emphasizes that the synergistic impact of radiation and corrosion will differ from their individual impacts.

Influence of nanosized defects on photoluminescence efficiency of Er3+ ions co-doped with Au2 O3 in a lead boroselenate glass ceramic system: a novel approach using positron annihilation lifetime spectroscopy.

This study consists of the results of an investigation into the influence of the free-volume space (fv ) defects on luminescence efficiency (LE) of erbium ions in Au2 O3 -doped PbO-B2 O3 -SeO2 (PBS) glass ceramics. Glass ceramics containing fixed concentrations of Er3+ ions and varied concentrations of Au2 O3 were synthesized. X-ray diffraction studies indicated that the samples contained Au2 (SeO3 )3 crystalline phase and nano gold metallic particles. The concentration of defects entrenched in the glass ceramics estimated in terms of Au2 O3 content using positron annihilation lifetime spectroscopy measurement indicated the highest content in the glass ceramic containing 0.075 mol% of Au2 O3 . Optical absorption and the photoluminescence (PL) spectra of the glass ceramics were studied in the visible region. The observed increase of PL efficiency was attributed to the enhanced concentration of free-volume imperfections in the samples. A perfect correlation could be achieved between the free-volume fraction and the PL efficiency of erbium ions in these glass ceramics.

The Properties of Poly(ester amide)s Based on Dimethyl 2,5-Furanedicarboxylate as a Function of Methylene Sequence Length in Polymer Backbone.

A series of poly(ester amide)s based on dimethyl furan 2,5-dicarboxylate (DMFDC), 1,3-propanediol (PDO), 1,6-hexylene glycol (HDO), and 1,3-diaminopropane (DAP) were synthesized via two-step melt polycondensation. The phase transition temperatures and structure of the polymers were studied by differential scanning calorimetry (DSC). The positron annihilation lifetime spectroscopy (PALS) measurement was carried out to investigate the free volume. In addition, the mechanical properties of two series of poly(ester amide)s were analyzed. The increase in the number of methylene groups in the polymer backbone resulted in a decrease in the values of the transition temperatures. Depending on the number of methylene groups and the content of the poly(propylene furanamide) (PPAF), both semi-crystalline and amorphous copolymers were obtained. The free volume value increased with a greater number of methylene groups in the polymer backbone. Moreover, with a lower number of methylene groups, the value of the Young modulus and stress at break increased.

The porosity of carbohydrate-based spray-dried microparticles containing limonene stabilized by pea protein: Correlation between porosity and oxidative stability

In this study, the effects of different concentrations of pea protein concentrate (PPC) in the physical properties, porosity features, and oxidative stability of maltodextrin-based spray-dried microparticles containing orange essential oil (OEO, rich in limonene) were evaluated. The use of PPC resulted in spray-dried microparticles with encapsulation efficiencies of about 99 wt%, without visible pores, and relatively high glass transition temperature (66,4 °C) at Aw ∼ 0.3. The nitrogen adsorption and positron annihilation lifetime spectroscopy measurements showed that the increase of PPC concentration from 2.4 to 4.8 wt% (g of PPC/100 g of emulsion) did not affect the porosity features of the microparticles. These results were confirmed by the profiles of OEO retention and limonene oxide production, which were similar for both samples throughout four weeks of storage. Based on these results, we verified that the lower amount of PPC we tested can effectively protect the OEO during storage, showing that a relatively cheaper orange flavor powder can be produced using less protein.

Mechanically Strong, Thermally Stable Gas Barrier Polyimide Membranes Derived from Carbon Nanotube-Based Nanofluids.

Gas barrier membranes with impressive moisture permeability are highly demanded in air or nature gas dehumidification. We report a novel approach using polyetheramine oligomers covalently grafted on the carbon nanotubes (CNTs) to engineer liquid-like CNT nanofluids (CNT NFs), which are incorporated into a polyimide matrix to enhance the gas barrier and moisture permeation properties. Benefiting from the featured liquid-like characteristic of CNT NFs, a strong interfacial compatibility between CNTs and the polyimide matrix is achieved, and thus, the resulting membranes exhibit high heat resistance and desirable mechanical strength as well as remarkable fracture toughness, beneficially to withstanding creep, impact, and stress fatigue in separation applications. Positron annihilation lifetime spectroscopy measurements indicate a significant decrease in fractional free volume within the resulting membranes, leading to greatly enhanced gas barrier properties while almost showing full retention of moisture permeability compared to that of the pristine membrane. For membranes with 10 wt % CNT NFs, the gas transmission rates, respectively, decrease 99.9% for CH4, 94.4% for CO2, 99.2% for N2, and 97.9% for O2 compared with that of the pristine membrane. Most importantly, with the increasing amount of CNT NFs, the hybrid membranes demonstrate a simultaneous increase of barrier performance and permselectivity for H2O/CH4, H2O/N2, H2O/CO2, and H2O/O2. All these results make these membranes potential candidates for high-pressure natural gas or hyperthermal air dehydration.