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At least 757 records · Page 42

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DOE OSTI2020

Carotenoids promote lateral packing and condensation of lipid membranes

Carotenoids are pigment molecules that protect biomembranes against degradation and may be involved in the formation of functional bacterial membrane microdomains. Little is known on whether different types of carotenoids have different effects on the membrane or if there is any concentration dependence of these effects. Here, we present results from molecular dynamics simulations of phospholipid bilayers containing different amounts of either β-carotene or zeaxanthin. Both β-carotene and zeaxanthin show the ability to laterally condense the membrane lipids and reduce their inter-leaflet interactions. With increasing concentrations, both carotenoids increase the bilayer thickness and rigidity. The results reveal that carotenoids have similar effects to cholesterol on regulating the behavior of fluid-phase membranes, suggesting that they could function as sterol substitutes and confirming their potential role in the formation of functional membrane domains.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Poly(norbornene) anion conductive membranes: homopolymer, block copolymer and random copolymer properties and performance

It has previously been shown that phase-separated block copolymers with non-ion conducting (hydrophobic) blocks and ion conducting (hydrophilic) blocks can form efficient ion conducting channels with high ionic mobility and conductivity. Block copolymers can provide a means for phase segregation and ion channel formation while homopolymers and random copolymers have been shown to have lower ion mobility. In this study, the properties of poly(norbornene) based anion exchange membranes (AEMs) comprising homopolymers, block copolymers, and random copolymers with high ion-exchange capacity (IEC) (3.48–4.55 meq. g -1 ) have been investigated and compared. The polymers were cross-linked with N,N,N',N'-tetramethyl-1,6-hexanediamine before casting the membranes to avoid excessive water swelling due to high water uptake. It was shown that high ionic conductivity can be achieved in both random copolymers and homopolymers even in the absence of microphase-separated structures. For example, the conductivity of a random copolymer was 194 mS cm -1 at 80 °C, which was comparable to the block copolymer, 201 mS cm -1 at 80 °C. The H 2 /O 2 fuel cell performance of random copolymer composite membranes showed a peak power density of 3.05 W cm -2 and peak current density of 7.85 A cm -2 at 80 °C compared to block copolymer membranes (peak power density of 3.21 W cm -2 and peak current density of 8.27 A cm -2 at 80 °C). It is more critical that high water transport be achieved in AEMs than achieving a phase-segregated morphology. Finally, the homopolymer, block copolymer, and random copolymer membranes showed <1.35% degradation after aging in 1 M NaOH at 80 °C for 1000 h.

08 HYDROGEN↗

DOE OSTI2021

Fracture and fatigue of thin crystalline SrTiO 3 membranes

The increasing availability of a variety of two-dimensional materials has generated enormous growth in the field of nanoengineering and nanomechanics. Recent developments in thin film synthesis have enabled the fabrication of freestanding functional oxide membranes that can be readily incorporated in nanomechanical devices. While many oxides are extremely brittle in bulk, recent studies have shown that, in thin membrane form, they can be much more robust to fracture as compared to their bulk counterparts. Here, we investigate the ultimate tensile strength of SrTiO 3 membranes by probing freestanding SrTiO 3 drumheads using an atomic force microscope. We demonstrate that SrTiO 3 membranes can withstand an elastic deformation with an average strain of ~6% in the sub-20 nm thickness regime, which is more than an order of magnitude beyond the bulk limit. Further, we also show that these membranes are highly resilient upon a high cycle fatigue test, surviving up to a billion cycles of force modulation at 85% of their fracture strain, demonstrating their high potential for use in nanomechanical applications.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Multiscale modeling of solute diffusion in triblock copolymer membranes

We develop a multiscale simulation model for diffusion of solutes through porous triblock copolymer membranes. The approach combines two techniques: self-consistent field theory (SCFT) to predict the structure of the self-assembled, solvated membrane and on-lattice kinetic Monte Carlo (kMC) simulations to model diffusion of solutes. Solvation is simulated in SCFT by constraining the glassy membrane matrix while relaxing the brush-like membrane pore coating against the solvent. The kMC simulations capture the resulting solute spatial distribution and concentration-dependent local diffusivity in the polymer-coated pores; we parameterize the latter using particle-based simulations. We apply our approach to simulate solute diffusion through nonequilibrium morphologies of a model triblock copolymer, and we correlate diffusivity with structural descriptors of the morphologies. We also compare the model’s predictions to alternative approaches based on simple lattice random walks and find our multiscale model to be more robust and systematic to parameterize. Furthermore, our multiscale modeling approach is general and can be readily extended in the future to other chemistries, morphologies, and models for the local solute diffusivity and interactions with the membrane.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Preparation of a membrane-sealed cell for studying catalyst nanoparticles in flowing gas with high vacuum x-ray photoelectron spectrometer

Here a sealing-style x-ray photoelectron spectroscopy study of the surface of a 1.0 wt. %Ni/TiO2 nanoparticle catalyst in a flowing mixture of CO and O2 at 1 bar was performed with a graphene membrane-sealed Si3N4 window-based miniature cell. We report the details on how a commercial Si3N4 window is modified before assembling a graphene membrane, how single-layer graphene membranes are transferred from their metal supports to the modified Si3N4 window, how a modified Si3N4 window covered with a double-layer graphene membrane is assembled onto a blank cell cap, how a nanoparticle catalyst is introduced to the cell cap and then the cell cap is installed onto a cell body to form a complete reaction cell, and how a complete cell is interfaced with a high vacuum chamber of an XPS system before an XPS study of 1.0 wt. %Ni/TiO2 catalyst surface in a flowing mixture for 0.2 bar CO and 0.8 bar O2 is performed. How the characterization of a catalyst using this type of graphene membrane-sealed Si3N4 window-based miniature cell is relevant to the finding of the actual surface chemistry of a catalyst during catalysis is discussed.

Instruments & Instrumentation↗

DOE OSTI2024

Structures of methane and ammonia monooxygenases in native membranes

Methane- and ammonia-oxidizing bacteria play key roles in the global carbon and nitrogen cycles, respectively. These bacteria use homologous copper membrane monooxygenases to accomplish the defining chemical transformations of their metabolisms: the oxidations of methane to methanol by particulate methane monooxygenase (pMMO) and ammonia to hydroxylamine by ammonia monooxygenase (AMO), enzymes of prime interest for applications in mitigating climate change. However, investigations of these enzymes have been hindered by the need for disruptive detergent solubilization prior to structure determination, confounding studies of pMMO and precluding studies of AMO. Here, we overcome these challenges by using cryoEM to visualize pMMO and AMO directly in their native membrane arrays at 2.4 to 2.8 Å resolution. These structures reveal details of the copper centers, numerous bound lipids, and previously unobserved components, including identifiable and distinct supernumerary helices interacting with pMMO and AMO, suggesting a widespread role for these helices in copper membrane monooxygenases. Comparisons between these structures, their metallocofactors, and their unexpected protein–protein interactions highlight features that may govern activity or the formation of higher-order arrays in native membranes. The ability to obtain molecular insights within the native membrane will enable further understanding of these environmentally important enzymes.

Science & Technology - Other Topics↗

DOE OSTI2023

Water transport in reverse osmosis membranes is governed by pore flow, not a solution-diffusion mechanism

We performed nonequilibrium molecular dynamics (NEMD) simulations and solvent permeation experiments to unravel the mechanism of water transport in reverse osmosis (RO) membranes. The NEMD simulations reveal that water transport is driven by a pressure gradient within the membranes, not by a water concentration gradient, in marked contrast to the classic solution-diffusion model. We further show that water molecules travel as clusters through a network of pores that are transiently connected. Permeation experiments with water and organic solvents using polyamide and cellulose triacetate RO membranes showed that solvent permeance depends on the membrane pore size, kinetic diameter of solvent molecules, and solvent viscosity. This observation is not consistent with the solution-diffusion model, where permeance depends on the solvent solubility. Motivated by these observations, we demonstrate that the solution-friction model, in which transport is driven by a pressure gradient, can describe water and solvent transport in RO membranes.

42 ENGINEERING↗

DOE OSTI2025

Hyperselective carbon membranes for precise high-temperature H 2 and CO 2 separation

More than 90% of the world’s hydrogen (H 2 ) is produced from fossil fuel sources, which requires energy-intensive separation and purification to produce high-purity H 2 fuel and to capture the carbon dioxide (CO 2 ) by-product. While membranes can decarbonize H 2 /CO 2 separation, their moderate H 2 /CO 2 selectivity requires secondary H 2 purification by pressure swing adsorption. Here, we report hyperselective carbon molecular sieve hollow fiber membranes showing H 2 /CO 2 selectivity exceeding 7000 under mixture permeation at 150°C, which is almost 30 times higher than the most selective nonmetallic membrane reported in the literature. The membrane is able to maintain an ultrahigh H 2 /CO 2 selectivity over 1400 under mixture permeation at 400°C. Pore structure characterization suggests that highly refined ultramicropores are responsible for effectively discriminating the closely sized H 2 and CO 2 molecules in the hyperselective carbon molecular sieve membrane. Modeling shows that the unprecedented H 2 /CO 2 selectivity will potentially allow one-step enrichment of fuel-grade H 2 from shifted syngas for decarbonized H 2 production.

Science & Technology - Other Topics↗

DOE OSTI2023

Electrochemical Measurement of Water Transport Numbers in Anion-Exchange Membranes

Anion-exchange membranes (AEMs) are a possible replacement for perfluorosulfonic-acid membranes in energy-conversion devices, primarily due to the hydroxide mobile ion allowing the devices to operate in alkaline conditions with less expensive electrocatalysts. However, the transport properties of AEMs remain understudied, especially electro-osmosis. In this work, an electrochemical technique, where the open-circuit voltage is measured between two ends of a membrane maintained at different relative humidities, is used to determine the water transport number of various ionomers, including Versogen and Sustainion AEMs and Nafion cation-exchange membrane (CEM), as a function of water content and temperature. In addition, the CEMs and AEMs are examined in differing single-ion forms, specifically proton and sodium (CEM) and hydroxide and carbonate (AEM). Carbonate-form AEMs have the highest transport number (∼11), followed by sodium-form CEMs (∼8), hydroxide-form AEMs (∼6), and proton-form CEMs (∼3). Finally, a multicomponent transport model based on the Stefan-Maxwell-Onsager framework of binary interactions is used to develop a link between water transport number and water-transport properties, extracting a range for the unmeasured membrane water permeability of Versogen as a function of water content.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2026

How Selective Transport Layer Improves Efficiency and Durability of Proton Exchange Membrane Fuel Cells

In any electrochemical device, the separator or membrane allows specific ions to transport but blocks electrons and other chemical species, enabling the electrochemical energy to be harvested. However, small amounts of undesired species are known to permeate through the membrane, reducing overall system efficiency and lifetime. An emerging concept called the “Selective Transport Layer” preferentially allows only protons to pass through but reduces the permeance of other species by a meaningful degree. Here, in this study, we demonstrate that a 60 nm thick graphene oxide composite layer can be very effective in reducing gas and ion permeation, even for a gas as small as H 2 , while not noticeably increasing proton transport resistance. In electrode and membrane accelerated stability tests, we show that both electrode and membrane durability are improved by a factor of two. Microscopy and mathematic simulations confirm that the graphene oxide composite is effective in blocking transport of dissolved Pt 2+ . The improved durability and reduced H 2 fuel crossover are expected to substantially reduce initial and operating costs of the fuel cell system. How this technology may affect other membrane-based electrochemical devices is also discussed.

Ngo, Phuong Quynh [General Motors, Pontiac, MI (Un↗

DOE OSTI2024

Development of Mixed Matrix Membranes by Using NH 2 ‐Functionalized UiO‐66 and [APTMS][AC] Ionic Liquid for the Separation of CO 2

The ever‐escalating CO 2 concentration in the atmosphere calls for accelerated development and deployment of carbon capture processes to reduce emissions. Mixed matrix membranes (MMMs), which are fabricated by incorporating the beneficial properties of highly selective inorganic fillers into a polymer matrix, have exhibited significant progress and the ability to enhance the performance of a membrane for gas separation. In this research, an amine‐based ionic liquid (IL) [APTMS][AC] was prepared, which has greater CO 2 affinity and greater solubility due to its amine moiety. The metal–organic framework (MOF) UiO‐66 with a multidimensional crystalline structure was used as a filler due to its appropriate porosity and tunable properties, and it was functionalized with NH 2 . MOFs were further modified with an IL to prepare UiO‐66@IL and UiO‐66‐NH 2 @IL, and MMMs incorporating each MOF were fabricated with the polymer Pebax‐1657. All the prepared membranes and MOFs were characterized to predict their separation efficiency. Several characterization techniques, namely, FTIR spectroscopy, XRD, and SEM, were used to successfully synthesize UiO‐66@IL and UiO‐66‐NH 2 @IL composites and confirmed proper dispersion and excellent polymer‒filler compatibility at filler loadings ranging from 0 to 30 wt.%. The separation performances were investigated, and the results showed that the incorporation of RTIL with the highly crystalline structure and large surface area of UiO‐66 enhanced the separation efficiency of the membrane. The permeability of CO 2 for all fabricated membranes continuously increased with increasing filler concentration, wherein the permeability was comparatively high for the UiO‐66‐NH 2 MMMs. The CO 2 /CH 4 selectivity improved by 35%, 54%, and 60%, respectively, for UiO‐66@IL, UiO‐66‐NH 2 , and UiO‐66‐NH 2 @IL MMMs compared to simple UiO‐66 for CO 2 /CH 4 and by 28%, 36%, and 63%, respectively, for CO 2 /N 2 , with an increase in filler loading in the MMMs.

Khalid, Hafiza Mamoona (ORCID:0009000135165855)↗

DOE OSTI2022

Innovative Proton Conductive Membranes Based on Two-Dimensional Materials

The team of Oak Ridge National Laboratory, New Mexico State University, and General Graphene Corporation staff will develop and commercialize paradigm-shifting low-cost, high-performing, proton-conductive membranes made from abundant and durable 2D materials. Proposed membranes are expected to be an order of magnitude better in performance and cost compared with the current state-of-the-art formulation, Nafion, and thus are expected to eliminate huge roadblocks in proliferation of fuel cells and flow batteries. The major goal for this work is to develop a fundamentally new learning curve for novel proton exchange membranes needed for various applications. The new technology will overcome the shortcomings of the current state-of-the-art membranes that are based upon Nafion polymer by offering higher proton conductivities, the ability to operate at much lower external humidity levels and higher temperatures (>120°C), and negligible fuel and oxidant crossover through the membrane.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Multiplication of freestanding III-V semiconductor membranes from a single wafer by alternating growth with amorphous graphene interlayer

Freestanding single-crystalline III-V compound semiconductors are important building blocks for functional devices due to their high electron mobilities, a wide range of bandgaps, and excellent optoelectronic properties. Despite efforts to produce such membranes by detaching epitaxial layers from donor wafers, current methods suffer from either slow processes or poor material quality. Here, we demonstrate a technique to grow and harvest multiple epitaxial membranes with extremely high throughput at the wafer scale. For this, a process to directly grow amorphous graphene on III-V substrates in metal-organic chemical vapor deposition reactors is developed, which enables an advanced remote epitaxy scheme comprised of multiple alternating layers of amorphous graphene and III-V epitaxial layers that can be formed by a single epitaxy run. Each epilayer in the multi-stack structure is then harvested by layer-by-layer peeling, producing multiple freestanding membranes with unprecedented throughput from a single wafer. Because amorphous graphene provides a weak van der Waals interface that allows peeling at the interface without damaging the epilayer or the substrate, wafers can be reused for subsequent membrane production. Therefore, this work represents a meaningful step toward high-throughput and low-cost production of single-crystal membranes that can be heterointegrated.

Han, Ne Myo↗

DOE OSTI2021

Enabling Efficient Water Splitting with Advanced Materials Designed for High pH Membrane Interface

This project was focused on developing the durable, high-performance materials and interfaces for advanced water splitting, enabling a clear pathway for achieving <$2/Kg H2 (on scale) with efficiency of 43 kWh/kg H 2 via anion exchange membrane (AEM)-based electrolysis. We aimed to advance these final goals via an improved fundamental understanding of both hydrogen and oxygen evolution reactions (HER/OER) leading to novel platinum group metal (PGM)-free catalyst materials in conjunction with critical improvements in membrane and ionomers and gas evolution electrodes with corresponding characterization and testing. Northeastern University (NU) lead this effort focusing on catalyst development and characterization (both in situ and ex situ) while project partners lead improvements in ionomer and membrane materials and will aid in the development of specialized electrode and membrane electrode assemblies. In addition, close collaboration occured with the HydroGEN Energy Materials Network (EMN) National Laboratory consortium including efforts related to use of advanced ionomers, durability protocols and validation of electrolyzer materials (e.g. NREL), multiscale modeling and computation (e.g. LBNL), and molecular dynamics (MD) simulations of the membrane catalyst interface (e.g. SNL). The interactions with HydroGEN included exchange of data and materials as needed to facilitate project success.

08 HYDROGEN↗

DOE OSTI2024

Field Validation of a Pilot-scale Black Liquor Membrane for Water Removal at Ahlstrom-Munksjö Paper Mill in Mosinee, WI

Project Background: The Industrial Technology Validation (ITV) program aims to identify and demonstrate the performance of new, emerging, and underutilized technologies in the industrial sector to help inform decisions towards accelerating commercialization and deployment. Pulp and paper is considered one of the most energy-intensive industries in the manufacturing sector. There are several methodologies for converting wood into pulp in the paper-making industry. The kraft process is a chemical method for producing wood pulp. The kraft process generates black liquor as a byproduct of pulp production. Traditionally, water is evaporated from the liquor by a set of multi-effect evaporators (MEEs), which concentrate weak black liquor (WBL) into strong black liquor (SBL) to support efficient combustion in a recovery boiler. Concentrating black liquor is an energy-intensive step in recovering pulping chemicals and generating high-pressure steam from dissolved wood solids. About 7% of pulp and paper energy usage, or nearly 164 trillion Btu, is used to remove water from black liquor in U.S. kraft pulp mills per year. The U.S. DOE’s IEDO is interested in the black liquor membrane technology evaluated in this report because it offers the potential for a more energy-efficient and less carbon-intensive kraft pulping process across 99 kraft pulp mills in 24 states (Agenda 2020 Technology Alliance 2016). This ITV project validates an innovative black liquor membrane technology for kraft pulp mills to understand its impact and benefits. Via Separations is a technology vendor that developed a graphene oxide membrane system to remove water from WBL before entering the evaporator set. High-pressure positive displacement (HPR) pumps move the black liquor through membranes that separate water and create a more concentrated black liquor. The vendor claims their pre-commercial technology reduces evaporator steam consumption by dewatering WBL before entering the evaporators. They also claim their technology has non-energy benefits such as enhanced soap collection and improved pulp throughput. This evaluation focuses on validating the energy and carbon dioxide (CO 2 e) emissions benefits associated with the membrane system.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2023

Investigation of the Effect of Atmospheric Plasma Treatment in Nanofiber and Nanocomposite Membranes for Piezoelectric Applications

In this work, we report the effect of steady-state atmospheric plasma (Corona discharge) in nanofibers and nanocomposite membranes for piezoelectric applications. The investigation was performed in PVDF (Poly vinylidene fluoride) nanofibers, CNT (Carbon Nanotubes)-reinforced PVDF nanocomposites, and PAN (Poly acrylonitrile) nanofiber membranes. Steady-state plasma was generated with a high voltage power source with 1 mA discharge current output and 6 kV discharge voltage, and the gap between tip and the material was maintained to be 1 cm. For the fabrication of nanofibers and nanocomposite membranes, an electrospinning method was used. The electrospinning parameters, such as flow rate and voltage, were optimally tuned for obtaining uniform nanofibers and nanomembranes. Along with the plasma treatment, heat treatment above the glass transition temperature was also conducted on the nanofiber membranes. Using a Scanning Electron Microscope (SEM), the morphology of the nanofibers was observed. X-ray Diffraction (XRD) demonstrated the polycrystallinity of the nanofibers. Fourier Transform Infrared Spectroscopy (FTIR) analysis of the PVDF nanofibers shows a peak at 796 cm−1 representing α-phase (C-H rocking) in the control sample which is absent in the treated samples. Raman spectroscopy of PVDF nanofibers identifies a Raman shift from 873 cm−1 to 877 cm−1 (denoting β-phase) for plasma-treated samples only. Electron Paramagnetic Resonance (EPR) concludes that the intensity of the free radicals increases from 1.37 to 1.46 (a.u.) after plasma treatment. Then, sensors were fabricated from the PVDF nanofibers, MWCNT-reinforced PVDF nanofibers, and PAN nanofibers to characterize their piezoelectric properties. The impact test results showed that the atmospheric plasma and heat-treated samples had 86%, 277%, and 92% increases of the d33 value (piezoelectric coefficient) in the case of PVDF nanofibers, MWCNT-reinforced nanofibers, and PAN nanofibers, respectively. It was also observed that the capacitance of the nanofiber membranes has increased due to the plasma treatment.

Biochemistry & Molecular Biology↗

DOE OSTI2023

Developing Enzyme Immobilization with Fibrous Membranes: Longevity and Characterization Considerations

Fibrous membranes offer broad opportunities to deploy immobilized enzymes in new reactor and application designs, including multiphase continuous flow-through reactions. Enzyme immobilization is a technology strategy that simplifies the separation of otherwise soluble catalytic proteins from liquid reaction media and imparts stabilization and performance enhancement. Flexible immobilization matrices made from fibers have versatile physical attributes, such as high surface area, light weight, and controllable porosity, which give them membrane-like characteristics, while simultaneously providing good mechanical properties for creating functional filters, sensors, scaffolds, and other interface-active biocatalytic materials. This review examines immobilization strategies for enzymes on fibrous membrane-like polymeric supports involving all three fundamental mechanisms of post-immobilization, incorporation, and coating. Post-immobilization offers an infinite selection of matrix materials, but may encounter loading and durability issues, while incorporation offers longevity but has more limited material options and may present mass transfer obstacles. Coating techniques on fibrous materials at different geometric scales are a growing trend in making membranes that integrate biocatalytic functionality with versatile physical supports. Biocatalytic performance parameters and characterization techniques for immobilized enzymes are described, including several emerging techniques of special relevance for fibrous immobilized enzymes. Diverse application examples from the literature, focusing on fibrous matrices, are summarized, and biocatalyst longevity is emphasized as a critical performance parameter that needs increased attention to advance concepts from lab scale to broader utilization. This consolidation of fabrication, performance measurement, and characterization techniques, with guiding examples highlighted, is intended to inspire future innovations in enzyme immobilization with fibrous membranes and expand their uses in novel reactors and processes.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Composite Membrane for Sodium Polysulfide Hybrid Redox Flow Batteries

Non-aqueous redox flow batteries (NARFBs) using earth-abundant materials, such as sodium and sulfur, are promising long-duration energy storage technologies. NARFBs utilize organic solvents, which enable higher operating voltages and potentially higher energy densities compared with their aqueous counterparts. Despite exciting progress throughout the past decade, the lack of low-cost membranes with adequate ionic conductivity and selectivity remains as one of the major bottlenecks of NARFBs. Here, we developed a composite membrane composed of a thin (<25 µm) Na+-Nafion coating on a porous polypropylene scaffold. The composite membrane significantly improves the electrochemical stability of Na + -Nafion against sodium metal, exhibiting stable Na symmetric cell performance for over 2300 h, while Na + -Nafion shorted by 445 h. Additionally, the composite membrane demonstrates a higher room temperature storage modulus than the porous polypropylene scaffold and Na + -Nafion separately while maintaining high Na + conductivity (0.24 mS/cm at 20 °C). Our method shows that a composite membrane utilizing Na + -Nafion is a promising approach for sodium-based hybrid redox flow batteries.

25 ENERGY STORAGE↗