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At least 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Temperature-dependent changes in gas chromatographic separation metrics for trihexyl(tetradecyl)phosphonium-based ionic liquid stationary phases and comparison to conventional polysiloxane stationary phases

Here, to assess whether the trihexyl(tetradecyl)phosphonium chloride ([P 66614 + ][Cl - ]) ionic liquid (IL), employed as a gas chromatographic stationary phase, exhibits temperature-dependent phase transitions or structural heterogeneity, retention thermodynamics for probe molecules of varied chemical structure were investigated by gas chromatography (GC) over the temperature range of 25 to 64 °C using van’t Hoff analysis. All van’t Hoff plots for n-alkanes (C8–C12) and other probe analytes were linear, indicating the absence of detectable phase-transition behavior. The [P 66614 + ][Cl - ] IL was further compared with the [P 66614 + ] bis[(trifluoromethyl)sulfonyl]imide ([P 66614 + ][NTf 2 - ]) IL and commercial polysiloxane stationary phases in terms of temperature-dependent resolution behavior and chromatographic selectivity over the temperature range of 28–52 °C. The resolution factors of analytes in mixtures obtained using gas chromatography–mass spectrometry (GC–MS) and the summation of resolution values decreased smoothly with temperature on both IL stationary phases and on the dimethylphenylcyano-substituted polymeric stationary phase (OV-1701), whereas the poly(50% diphenyl/50% dimethyl siloxane) stationary phase (SPB-50) exhibited irregularities in its temperature-dependent summation of resolution profile, showing a distinct maximum in the temperature range of 34–40 °C. Selectivity values for the IL stationary phases were largely determined by the anion, with the [P 66614 + ][Cl - ] IL providing enhanced separation between polar and aromatic analytes, while the [P 66614 + ][NTf 2 - ] IL favored dispersive and π-π interactions that resulted in a reversal of elution order for some aliphatic–aromatic and alkyne-containing analyte pairs. Capillary columns prepared using different surface activation methods and coated with identical [P 66614 + ][Cl - ] IL stationary phase showed indistinguishable temperature-dependent trends in summation of resolution value and selectivity. An evaluation of analyte-specific selectivity provides insight into the characteristic separation behavior of the stationary phases and enables identification of analyte classes that are more efficiently separated on the [P 66614 + ]-based IL stationary phases compared to conventional stationary phase materials.

Chromatographic selectivity↗
DOE OSTI2019

Simulation methods for liquid–liquid phase separation of disordered proteins

Liquid–liquid phase separation of intrinsically disordered proteins (IDPs) and other biomolecules is a highly complex but robust process used by living systems. Drawing inspiration from biology, phase separating proteins have been successfully utilized for promising applications in fields of materials design and drug delivery. These protein-based materials are advantageous due to the ability to finely tune their stimulus-responsive phase behavior and material properties, and the ability to encode biologically active motifs directly into the sequence. The number of possible protein sequences is virtually endless, which makes sequence-based design a rather daunting task, but also attractive due to the amount of control coming from exploration of this variable space. The use of computational methods in this field of research have come to the aid in several aspects, including interpreting experimental results, identifying important structural features and molecular mechanisms capable of explaining the phase behavior, and ultimately providing predictive frameworks for rational design of protein sequences. We provide an overview of computational studies focused on phase separating biomolecules and the tools that are available to researchers interested in this topic.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Efficient separation and coprecipitation for simplified cathode recycling

Hydrometallurgical recycling of spent lithium-ion batteries is among the most promising recovery approaches. The current hydrometallurgical method for battery recycling faces challenges such as complex separation and precipitation processes, and environmental concerns from the use of caustic inorganic acid and hazardous hydrogen peroxide. Our proposed modified method, namely polyol-metallurgy, uses citric acid in ethylene glycol as dual-function green solution to overcome these obstacles. This bifunctional solution leaches valuable metal ions from cathode materials (e.g., LiCoO 2 ), and then acts as chelating agents to selectively precipitate cobalt through an esterification reaction, without the need for additional precipitation agents. The leaching efficiency of cobalt and lithium reaches 99.55% and 97.65%, respectively, and more than 96% of cobalt could be directly self-precipitated and recovered. Further, the unique characteristics of the dual-function solution also avoids impurities from Al foils and PVDF/carbon black films, enabling the simple separation process. Therefore, the process can be completed in one-pot system with efficient leaching, separation and coprecipitation, making it more efficient and feasible for operation than existing alternatives.

25 ENERGY STORAGE↗
DOE OSTI2014

Modeling the influence of bubble pressure on grain boundary separation and fission gas release

Grain boundary (GB) separation as a mechanism for fission gas release (FGR), complementary to gas bubble interlinkage, has been experimentally observed in irradiated light water reactor fuel. However there has been limited effort to develop physics-based models incorporating this mechanism for the analysis of FGR. In this work, a computational study is carried out to investigate GB separation in UO2 fuel under the effect of gas bubble pressure and hydrostatic stress. A non-dimensional stress intensity factor formula is obtained through 2D axisymmetric analyses considering lenticular bubbles and Mode-I crack growth. The obtained functional form can be used in higher length-scale models to estimate the contribution of GB separation to FGR.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2012

Microporous Separators for Fe/V Redox Flow Batteries

The Fe/V redox flow battery has demonstrated promising performance that is advantageous over other redox flow battery systems. The less oxidative nature of the Fe(III) species enables use of hydrocarbon - based ion exchange membranes or separators. Daramic(reg. sign) microporous polyethylene separators were tested on Fe/V flow cells using the sulphuric/chloric mixed acid - supporting electrolytes. Among them, Daramic(reg. sign) C exhibited good flow cell cycling performance with satisfactory repeatability over a broad temperature range of 5 - 50 degrees C. Energy efficiency (EE) of C remains above 67% at current densities of 50 - 80 cm{sup -2} in the temperature range from room temperature to 50 degrees C. The capacity decay problem could be circumvented through hydraulic pressure balancing by applying different pump rates to the positive and negative electrolytes. Stable capacity and energy were obtained over 40 cycles at room temperature and 40 degrees C. These results manifest that the extremely low-cost separators ($10/cm2) are applicable in the Fe/V flow battery system at an acceptable sacrifice of energy efficiency. This stands for a remarkable breakthrough in significant reduction of the capital cost of the Fe/V flow battery system, and is promising to promote its market penetration in grid stabilization and renewable integration.

25 ENERGY STORAGE↗
DOE OSTI2012

Magnetically separable {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-Ce-doped TiO{sub 2} core-shell nanocomposites: Fabrication and visible-light-driven photocatalytic activity

Novel visible-light-induced {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-Ce-doped-TiO{sub 2} core-shell nanocomposite photocatalysts capable of magnetic separation have been synthesized by a facile sol-gel and after-annealing process. The as-obtained core-shell nanocomposite is composed of a central {gamma}-Fe{sub 2}O{sub 3} core with a strong response to external fields, an interlayer of SiO{sub 2}, and an outer layer of Ce-doped TiO{sub 2} nanocrystals. UV-vis spectra analysis indicates that Ce doping in the compound results in a red-shift of the absorption edge, thus offering increased visible light absorption. We show that such a {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-Ce-doped-TiO{sub 2} core-shell nanocomposite with appreciated Ce doping amount exhibits much higher visible-light photocatalytic activity than bare TiO{sub 2} and undoped {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-TiO{sub 2} core-shell nanocomposite toward the degradation of rhodamine B (RhB). Moreover, the {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-Ce-doped-TiO{sub 2} core-shell nanocomposite photocatalysts could be easily separated and reused from the treated water under application of an external magnetic field. - Graphical abstract: Novel {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-Ce-doped-TiO{sub 2} core/shell nanocomposite photocatalysts with enhanced photocatalytic activity and fast magnetic separability were prepared. Highlights: Black-Right-Pointing-Pointer Novel {gamma}-Fe{sub 2}O{sub 3}-SiO{sub 2}-Ce-doped TiO{sub 2} core/shell composite photocatalysts were prepared. Black-Right-Pointing-Pointer The resulting core/shell composite show high visible light photocatalytic activity. Black-Right-Pointing-Pointer The nanocomposite photocatalysts can be easily recycled with excellent durability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Magnetically separable mesoporous Fe{sub 3}O{sub 4}/silica catalysts with very low Fe{sub 3}O{sub 4} content

Two magnetically separable Fe{sub 3}O{sub 4}/SiO{sub 2} (aerogel and MSU-X) composites with very low Fe{sub 3}O{sub 4} content (<1 wt%) have been successfully prepared at room temperature by co-condensation of MPTES-functionalized Fe{sub 3}O{sub 4} nanoparticles (NPs) with a silicon alkoxide. This procedure yields a homogeneous incorporation of the Fe{sub 3}O{sub 4} NPs on silica supports, leading to magnetic composites that can be easily recovered using an external magnetic field, despite their very low Fe{sub 3}O{sub 4} NPs content (ca. 1 wt%). These novel hybrid Fe{sub 3}O{sub 4}/SiO{sub 2} materials have been tested for the oxidation reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) with hydrogen peroxide showing an enhancement of the stability of the NPs in the Fe{sub 3}O{sub 4}/silica aerogel as compared to the Fe{sub 3}O{sub 4} NPs alone, even after five catalytic cycles, no leaching or agglomeration of the Fe{sub 3}O{sub 4}/SiO{sub 2} systems. - Graphical abstract: Novel magnetically separable mesoporous silica-based composites with very low magnetite content. - Highlights: • An innovative way to prepare magnetically separable composites with <1 wt% NPs. • The Fe{sub 3}O{sub 4}/silica composites are readily magnetized/demagnetized. • The Fe{sub 3}O{sub 4}/silica composites can be easily recovered using an external magnetic field. • Excellent catalytic performance and recyclability despite the low Fe{sub 3}O{sub 4} NPs content.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

A novel metal-organic framework for high storage and separation of acetylene at room temperature

A novel 3D microporous metal-organic framework with NbO topology, [Cu{sub 2}(L)(H{sub 2}O){sub 2}]∙(DMF){sub 6}·(H{sub 2}O){sub 2} (ZJU-10, ZJU = Zhejiang University; H{sub 4}L =2′-hydroxy-[1,1′:4′,1″-terphenyl]-3,3″,5,5″-tetracarboxylic acid; DMF =N,N-dimethylformamide), has been synthesized and structurally characterized. With suitable pore sizes and open Cu{sup 2+} sites, ZJU-10a exhibits high BET surface area of 2392 m{sup 2}/g, as well as moderately high C{sub 2}H{sub 2} volumetric uptake capacity of 132 cm{sup 3}/cm{sup 3}. Meanwhile, ZJU-10a is a promising porous material for separation of acetylene from methane and carbon dioxide gas mixtures at room temperature. - Graphical abstract: A new NbO-type microporous metal-organic framework ZJU-10 with suitable pore size and open Cu{sup 2+} sites was synthesized to realize the strong interaction with acetylene molecules, which can separate the acetylene from methane and carbon dioxane gas mixtures at room temperature. Display Omitted - Highlights: • A novel 3D NbO-type microporous metal-organic framework ZJU-10 was solvothermally synthesized and structurally characterized. • ZJU-10a exhibits high BET surface area of 2392 m{sup 2}/g. • ZJU-10a shows a moderately high C{sub 2}H{sub 2} gravimetric (volumetric) uptake capacity of 174 (132) cm{sup 3}/g at 298 K and 1 bar. • ZJU-10a can separate acetylene from methane and carbon dioxide gas mixtures at room temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Enhanced photocatalytic activity of Te-doped Bi{sub 2}MoO{sub 6} under visible light irradiation: Effective separation of photogenerated carriers resulted from inhomogeneous lattice distortion and improved electron capturing ability

Te-doped Bi{sub 2}MoO{sub 6} photocatalyst was hydrothermally synthesized, and nonmetal atoms Te were homogeneously incorporated into Bi{sub 2}MoO{sub 6} lattice with the substitution of Te{sup 4+} to Mo{sup 6+}. With increasing Te-doping concentration in Bi{sub 2}MoO{sub 6}, no detectable band-gap narrowing but more and more severe inhomogeneous lattice distortions were determined. The activity of Bi{sub 2}MoO{sub 6} photocatalyst was evaluated through methylene blue degradation under visible light irradiation (λ>410 nm) and was greatly enhanced by Te-doping. When Te-doped Bi{sub 2}MoO{sub 6} was synthesized at Te/Mo molar ratio of 7.5%, a maximum first-order rate constant of methylene blue degradation was obtained. The inhomogeneous lattice distortion generated an internal dipole moment, and the holes generated with the substitution of Te{sup 4+} to Mo{sup 6+} acted as the capturing centers of photogenerated electrons, thus the effective separation of photogenerated carriers was facilitated to result in a relatively high concentration of holes on the surface of Te-doped Bi{sub 2}MoO{sub 6} to be favorable for the efficient methylene blue degradation. - Graphical abstract: With the substitution of Te{sup 4+} to Mo{sup 6+}, effective separation of photogenerated carriers resulted from inhomogeneous lattice distortion and improved electron capturing ability is achieved to be responsible for enhanced photocatalytic activity of Te-doped Bi{sub 2}MoO{sub 6}. - Highlights: • Nonmetal Te is incorporated into Bi{sub 2}MoO{sub 6} with the substitution of Te{sup 4+} to Mo{sup 6+}. • Revealing inhomogeneous lattice distortion and improved electron capturing ability. • Effective separation of photogenerated carriers in Te-doped Bi{sub 2}MoO{sub 6} is achieved. • The mechanism of methylene blue degradation over Te-doped Bi{sub 2}MoO{sub 6} is proposed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

A novel magnetically separable TiO{sub 2}/CoFe{sub 2}O{sub 4} nanofiber with high photocatalytic activity under UV-vis light

Graphical abstract: A novel magnetically separable composite photocatalyst TiO{sub 2}/CoFe{sub 2}O{sub 4} nanofiber was prepared by sol-gel method and electrospinning technique, which can be reclaimed with a magnet, and the decolorizing efficiency of MB solution reached 95.87%. Highlights: Black-Right-Pointing-Pointer The composite TiO{sub 2}/CoFe{sub 2}O{sub 4} nanofibers with diameter of 110 {+-} 28 nm have been successfully synthesized by the combination of sol-gel method and electrospinning technique. Black-Right-Pointing-Pointer The presence of Co{sup 2+} or/and Fe{sup 3+} ions may occupy some of the lattice sites of TiO{sub 2} to form an iron-titanium solid solution and narrow the band gap, which broadens the response region of visible light. Black-Right-Pointing-Pointer The resultant nanofibers not only have high decomposition efficiency with methylene blue (MB) under the UV irradiation, which is close to that of Degussa P25, but also can be separated with a magnet and avoid the secondary pollution of the treated water. -- Abstract: A novel magnetically separable heterogeneous photocatalyst TiO{sub 2}/CoFe{sub 2}O{sub 4} nanofiber was prepared by sol-gel method and electrospinning technology, followed by heat treatment at 550 Degree-Sign C for 2 h. The phase structure, morphology and magnetic property of the composite nanofibers were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscope and vibrating sample magnetometer analysis. The photocatalytic studies of TiO{sub 2}/CoFe{sub 2}O{sub 4} fibers suggested that the presence of CoFe{sub 2}O{sub 4} not only enhanced the absorbance of UV light, but also broadened the response region to visible light. The decolorizing efficiency of methylene blue (MB) solution reaches 95.87% over TiO{sub 2}/CoFe{sub 2}O{sub 4} nanofibers under 300 W Hg lamp after 5 h, which is close to that of Degussa P25. Furthermore, these fibers can be collected with a magnet for reuse and effectively avoid the secondary pollution of the treated water.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Improvement of charge separation in TiO{sub 2} by its modification with different tungsten compounds

Highlights: • Ammonium m-tungstate doped to TiO{sub 2} highly improved charge separation in TiO{sub 2}. • Negative electrokinetic potential of TiO{sub 2} facilitates holes migration to its surface. • Fast migration of holes to TiO{sub 2} surfaces increased yield of OH radicals formation. • Adsorption of dyes on photocatalyst increased its decomposition under visible light. - Abstract: Three different tungsten precursors were used for TiO{sub 2} modification: H{sub 2}WO{sub 4}, WO{sub 2}, and ammonium m-tungstate. It was proved that modification of TiO{sub 2} with tungsten compounds enhanced its photocatalytic activity through the improvement of charge separation. This effect was obtained by coating of TiO{sub 2} particles with tungsten compound, which changed their surficial electrokinetical potential from positive onto negative. The most efficient tungsten compound, which caused enhanced separation of free carriers was ammonium m-tungstate (AMT). Two dyes with different ionic potential were used for the photocatalytic decomposition. It appeared that cationic dye—Methylene Blue was highly adsorbed on the negatively charged surface of TiO{sub 2} modified by AMT and decomposed, however this photocatalyst was quickly deactivated whereas anionic dye—acid red was better adsorbed on the less acidic surface of TiO{sub 2} and was rapidly decomposed with almost the same rate in the five following cycles.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Facile preparation of zinc oxide nanorods surrounded by graphene quantum dots both synthesized via separate pyrolysis procedures for photocatalyst application

Highlights: • ZnO NRs and GQDs were made separately via a simple and one-stage pyrolysis method. • Because of the employed compositing method, GQDs compactly surrounded the ZnO NRs. • Bandgap of ZnO NRs decreased from 3.2 to 2.8 eV after they were surrounded by GQDs. • Despite being inefficient alone, GQDs largely enhanced ZnO photocatalytic activity. • The mechanism was mainly attributed to the decrease in recombination rate of ZnO. - Abstract: A facile pyrolysis method was employed for separate synthesis of zinc oxide nanorods (ZnO NRs) and graphene quantum dots (GQDs) and the structures were composited. The structures were characterized by field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray diffractometry (XRD), and Fourier transform infrared (FTIR) spectroscopy. The structures were optically characterized by UV–vis and photoluminescence (PL) spectrometry techniques, showing that the absorption of ZnO NRs increases in the visible region after being surrounded by GQDs. Optical bandgaps of ZnO NRs and ZnO NRs/GQDs composite were estimated as 3.2 and 2.8 eV, respectively. Based on PL analysis, it was deduced that the generated electron-hole recombination rate of ZnO NRs decreases after being surrounded by GQDs. Finally, it was shown that our GQDs, despite being relatively inefficient separately, significantly enhance the photocatalytic activity of ZnO on methylene blue mainly through decreasing the e-h recombination rate of ZnO NRs.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2018

Bi2WO6/ZnFe2O4 heterostructures nanofibers: Enhanced visible-light photocatalytic activity and magnetically separable property

Highlights: • Bi{sub 2}WO{sub 6} nanosheets were grown on ZnFe{sub 2}O{sub 4} nanofibers by a hydrothermal method. • The Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures nanofibers showed high photodegredation of RhB under visible-light. • The Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures nanofibers possessed magnetically separable property. - Abstract: Bi{sub 2}WO{sub 6} nanosheets were uniformly grown on electrospun ZnFe{sub 2}O{sub 4} nanofibers via a solvothermal technique. The loading amounts of Bi{sub 2}WO{sub 6} in the Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures nanofibers could be controlled by adjusting the precursor concentration in solvothermal process. Under visible-light irradiation, the degradation rate constant (rhodamine B) of the Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures was 11.6 times than that of pure ZnFe{sub 2}O{sub 4} nanofibers and 5.8 times than that of pure Bi{sub 2}WO{sub 6} nanosheets, mainly owing to the effective separation of the photogenerated electron-hole pairs in the Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures. Notably, the Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures nanofibers could be easily separated from the solution under an external magnetic field by employing the ferromagnetic behaviors of ZnFe{sub 2}O{sub 4}. After several cycles, the photocatalytic activity of the Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures nanofibers did not decrease significantly suggesting that the Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures possess stable characteristics. This kind of Bi{sub 2}WO{sub 6}/ZnFe{sub 2}O{sub 4} heterostructures nanofibers with high visible-light photocatalytic activity, excellent stability and excellent recyclability could be significance in environmental application.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Kinetics and mechanism of light-induced phase separation in a mixed-halide perovskite

Halide ion phase separation is a barrier to the application of mixed-halide perovskites, whereby the presence of large populations of photo-generated or injected carriers causes undesirable changes in the local band gap. Here, we investigate the mechanism of phase separation in CsPbI x Br 3-x perovskite single crystals driven by light. The phase separation process and its dynamics are visualized at the nanometer scale at cryogenic temperatures using in-situ scanning transmission electron microscopy and cathodoluminescence. Combined with phase field modeling that accounts for the coupling between electronic and chemical driving forces, our observations point to a spinodal decomposition mechanism in which both the amplitude of composition fluctuation and the characteristic length scale grow non-linearly with time. Our findings provide microscopic insights that can assist in further engineering mixed-halide perovskites either for stability or for intentional programming of the local halide ion composition, opening pathways to a wide range of applications.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Ultem((R))/ZIF-8 mixed matrix hollow fiber membranes for CO2/N-2 separations

Organic-inorganic hybrid (mixed matrix) membranes can potentially extend the separation performance of traditional polymeric materials while maintaining processing convenience. Although many dense films studies have been reported, there have been few reported cases of these materials being successfully extended to asymmetric hollow fibers. In this work we report the first successful production of mixed matrix asymmetric hollow fiber membranes containing metal-organic-framework (MOF) ZIF-8 fillers. Specifically, we have incorporated ZIF-8 into a polyetherimide (Ultem((R)) 1000) matrix and produced dual-layer asymmetric hollow fiber membranes via the dry jet-wet quench method. The outer separating layer of these composite fibers contains 13 wt% (17 vol%) of ZIF-8 filler. These membranes have been tested over a range of temperatures and pressures for a variety of gas pairs. An increase in separation performance for the CO2/N-2 gas pairs was observed for both pure gas and mixed gas feeds. (C) 2012 Elsevier B.V. All rights reserved.

Dai, Y↗
DOE OSTI2019

Addition-type alkoxysilyl-substituted polynorbornenes for post-combustion carbon dioxide separations

The separation of CO 2 from N 2 using polymeric membranes has proven a particularly challenging task. One promising class of polymers for this application is alkoxysilyl-substituted vinyl-added polynorbornenes (VAPNBs), which are high T g materials that often exhibit notable CO 2 /N 2 separation performance. This performance is believed to arise from their anomalous behavior in which they display high levels of solubility selectivity, a trait more commonly encountered in rubbery polymers than high T g glassy materials. While this trait has been documented in literature, no systematic investigations have been reported that probe the relationship between alkoxysilyl-substituted VAPNB structure and their resultant gas separation behavior. Here, we describe the synthesis and evaluation of three sets of alkoxysilyl-substituted VAPNBs that are designed to probe distinct facets of their structure-transport relationship. This includes investigations into the effect that alkoxysilyl branching, chain length, and carbon linker length have on CO 2 /N 2 permeability, solubility, and diffusivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Polystyrene sulfonate (PSS) stabilized polyethylenimine (PEI) membranes fabricated by spray coating for highly effective CO 2 /N 2 separation

Greenhouse effect, largely caused by CO 2 emission, has become a major concern for global climate change. Post-combustion CO 2 capture is one of the critical strategies to mitigate this issue. Membrane technology for carbon capture has drawn significant attention because of the cost and energy efficiency and scalability. Many membranes for CO 2 capture are limited by the trade-off between CO 2 permeability and CO 2 /N 2 selectivity and the long-term stability under practical operating conditions. Facilitated transport membranes with efficient CO 2 carriers have demonstrated potential to surpass the permeability-selectivity trade-off, but these carriers are often lost under operational conditions. In this work, we designed and fabricated a polystyrene sulfonate (PSS) stabilized polyethylenimine (PEI) membrane by a facile and scalable spray-coating method. The deposited defect-free selective layer, in which the amine carriers in PEI can be stabilized electrostatically by PSS, exhibited superior CO 2 separation performance with good long-term stability under practical operating conditions. The separation performance was optimized by spray-coating cycles, CNT network loading, and PSS loading. Our membrane showed CO 2 permeance ranging from 820 to 1,770 GPU and CO 2 /N 2 selectivity varying from 395 to 460 under vacuum operation mode in the temperature range between 80 and 90 °C. Furthermore, the membrane was successfully scaled up to 200 cm 2 with good uniformity. These results might suggest a novel membrane structure and a scalable approach for fabrication of highly efficient CO 2 separation membranes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Ultrathin-film composite (uTFC) membranes based on amorphous perfluoropolymers for liquid separations

Thin-film composite membranes based on ~100nm cross-linked polyamides (PAs) are state-of-the-art membranes for liquid separations such as desalination. However, the PA layer shows poor antifouling properties and instability in chlorine solutions. Herein, we show for the first time that glassy amorphous perfluoropolymers (PFPs, such as Teflon AF and Hyflon AD) can be fabricated into ultrathin film composite (uTFC) membranes with a selective layer of <20nm for desalination. Increasing the polymer concentration in the coating solutions from 0.05 mass% to 0.3 mass% increases the selective layer thickness from 9 to 25nm. When Teflon AF2400 was fabricated into 16-nm selective layers on various porous supports, the water permeance decreases from 0.37 LMH/bar for PES10k to 0.07 LMH/bar for PES1k, and the Na 2 SO 4 rejection increases from 86.6% to 95.2%. While the water permeance is lower than the commercial PA-based NF membranes, the rejection in these PFP-based membranes is comparable. Furthr, the effect of the porous support on the water permeance can be ascribed to the geometric restriction and satisfactorily described using an empirical model. Interestingly, the membranes also exhibit good Na + /Li + separation performance and stable performance for organic solvent nanofiltration, showcasing the versatility of the PFP-based uTFC membranes for various liquid separations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗