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At least 685 records · Page 38
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

The current status of high temperature electrochemistry-based CO 2 transport membranes and reactors for direct CO 2 capture and conversion

The concept of direct CO 2 capture and conversion has attracted significant interest from industries and academia in recent decades due to its potential to address the current grand challenge of global warming/climate change, rapid depletion of fossil fuels and realization of a future carbon neutral ecosystem. The incumbent benchmark technology for CO 2 capture is the post-combustion flue-gas “amine washing”, which is energy intensive and costly for large-scale commercial implementation. The CO 2 conversion technologies, on the other hand, are still at their infancy with many technical challenges to overcome, but primarily being explored in laboratory-scale, low-temperature, solution-based and high-temperature, solid-oxide-based electrochemical cells with renewable electricity perceived as the energy input. In this article, we provide a comprehensive overview on an emergent class of high-temperature electrochemical CO 2 transport membranes that can capture and convert CO 2 into valuable chemicals in single catalytic reactor fashion. The review starts with the chemistry and transport theory of three basic types of membranes purposely designed for different CO 2 feedstocks and downstream conversions. A range of key functional materials used in these membranes and their microstructural/electrochemical properties important to the CO 2 transport are then thoroughly discussed in conjunction with the effects of surface modifications and operating conditions. Several types of combined CO 2 capture and conversion catalytic reactors based on these membranes are also assessed with a focus on their working principles, system configurations and performance demonstrations. Finally, challenges and prospective of these electrochemical CO 2 transport membranes and their associated conversion reactors are candidly discussed for future development.

10 SYNTHETIC FUELS↗
DOE OSTI2020

Ring-opening metathesis polymerization of cobaltocenium derivative to prepare anion exchange membrane with high ionic conductivity

Abstract An efficient method to incorporate a cobaltocenium cation into polymers for anion exchange membranes is described. A cobaltocenium-containing norbornene derivative has been synthesized. It can be homopolymerized, or copolymerized with norbornene, by ring-opening metathesis polymerization (ROMP) with quantitative yields. The composition of the random copolymers can be precisely controlled by adjusting the feed ratio of the monomers. Additionally, the resulting polymers can be cast into thin robust membranes. The morphology of the membranes is characterized by humidity controlled SAXS and TEM, showing disordered interconnected cobaltocenium domains. The high ionic conductivity suggests that such membranes are good candidates for anion exchange membranes.

42 ENGINEERING↗
DOE OSTI2020

Superselective Removal of Lead from Water by Two-Dimensional MoS 2 Nanosheets and Layer-Stacked Membranes

Point-of-use (POU) devices with satisfactory lead (Pb 2+ ) removal performance are urgently needed in response to recent outbreaks of lead contamination in drinking water. This study experimentally demonstrated the excellent lead removal capability of two-dimensional (2D) MoS 2 nanosheets in aqueous form and as part of a layer-stacked membrane. Among all materials ever reported in the literature, MoS 2 nanosheets exhibit the highest adsorption capacity (740 mg/g), and the strongest selectivity/affinity toward Pb 2+ with a distribution coefficient K d that is orders of magnitude higher than that of other lead adsorption materials (5.2 × 10 7 mL/g). Density functional theory (DFT) simulation was performed to complement experimental measurements and to help understand the adsorption mechanisms. The results confirmed that the cation selectivity of MoS 2 follows the order Pb 2+ > Cu 2+ >> Cd 2+ > Zn 2+ , Ni 2+ > Mg 2+ , K + , Ca 2+ . The membrane formed with layer-stacked MoS 2 nanosheets exhibited a high water flux (145 L/m 2 /h/bar), while effectively decreasing Pb 2+ concentration in drinking water from a few mg/L to less than 10 μg/L. The removal capacity of the MoS 2 membrane is a few orders of magnitude higher than that of other literature-reported membrane filters. Therefore, the layer-stacked MoS 2 membrane has great potential for POU removal of lead from drinking water.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Membrane-Confined Iron Oxychloride Nanocatalysts for Highly Efficient Heterogeneous Fenton Water Treatment

Heterogeneous advanced oxidation processes (AOPs) allow for the destruction of aqueous organic pollutants via oxidation by hydroxyl radicals ( • OH). However, practical treatment scenarios suffer from the low availability of short-lived • OH in aqueous bulk, due to both mass transfer limitations and quenching by water constituents, such as natural organic matter (NOM). In this work, we overcome these challenges by loading iron oxychloride catalysts within the pores of a ceramic ultrafiltration membrane, resulting in an internal heterogeneous Fenton reaction that can degrade organics in complex water matrices with pH up to 6.2. With • OH confined inside the nanopores (~ 20 nm), this membrane reactor completely removed various organic pollutants with water fluxes of up to 100 L m –2 h –1 (equivalent to a retention time of 10 s). This membrane, with a pore size that excludes NOM (>300 kDa), selectively exposed smaller organics to •OH within the pores under confinement and showed excellent resiliency to representative water matrices (simulated surface water and sand filtration effluent samples). Moreover, the membrane exhibited sustained AOPs (>24 h) and could be regenerated for multiple cycles. Our results suggest the feasibility of exploiting ultrafiltration membrane-based AOP platforms for organic pollutant degradation in complex water scenarios.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Stimulated Raman Scattering Microscopy: Real-Time In-Situ Physical and Chemical Characterization of Reverse Osmosis Desalination Membrane Scaling

We introduce a stimulated Raman scattering (SRS) methodology designed for rapid, real-time, and in situ monitoring of RO membrane scaling adapted for bench-scale desalination flow cells. The methodology can provide new insights into membrane scaling dynamics by offering time-resolved reflection imaging of inorganic crystal growth, coupled with chemical identification from Raman spectral data. These capabilities allow for direct local measurement of the membrane surface area covered by different scalants as well as an approximation of the scalant volume using three-dimensional, integrated Raman intensity. The 2D and 3D SRS results obtained from CaSO 4 scaling experiments are compared to and are in reasonable agreement with those provided by confocal microscopy. The real-time physical and chemical characterization capabilities presented here could be extended to study combinations of inorganic, organic, and biological fouling. Overall, the SRS methodology represents an advancement in real-time sensing of membrane fouling that offers the potential for improved operation, lower cost, and more resilient RO membrane systems for sustainable water management.

42 ENGINEERING↗
DOE OSTI2024

Effects of Normal and Lateral Electric Fields on Membrane Mechanical Properties

As a core component of biological and synthetic membranes, lipid bilayers are key to compartmentalizing chemical processes. Bilayer morphology and mechanical properties are heavily influenced by electric fields such as those caused by biological ion concentration gradients. We present atomistic simulations exploring the effects of electric fields applied normally and laterally to lipid bilayers. We find that normal fields decrease membrane tension, while lateral fields increase it. Free energy perturbation calculations indicate the importance of dipole-dipole interactions to these tension changes, especially for lateral fields. We additionally show that membrane area compressibilities can be related to their cohesive energies, allowing us to estimate changes in membrane bending rigidity under applied fields. We find that normal fields decrease bending rigidity, while lateral fields increase it. Furthermore, these results point to the use of directed electric fields to locally control membrane stiffness, thereby modulating associated cellular processes.

Chemistry↗
DOE OSTI2020

The Effect of Cholesterol on Membrane Binding and Self-Assembly of Collagen Fibrils

Collagen is a skeleton of native extracellular matrix (ECM) that is known to provide mechanical and structural stability. In an attempt to develop a new connective cellular model with the surrounding ECM without further experimental complications, such as the reconstitution of ECM receptors, we designed the experiments and discovered that the fibrillogenesis of membrane-bound collagen is not spontaneous as it is in the form of free collagen in bulk solution. Furthermore, the confocal microscopic results suggest that cholesterol is a crucial component that facilitates the fibril formation on the membrane surface. In situ X-ray and neutron reflectivity on Langmuir monolayer and solid-supported lipid bilayer models, respectively, reveal two features of cholesterol effects on the collagen fibril formation. Mainly, cholesterol increases the lateral lipid headgroup separation on the membrane surface, which promotes the association degree of collagen monomers. It also enhances the elastic modulus of the membrane to impede membrane filtration by the collagen assemblies.

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

Exponential Water Uptake in Ionomer Membranes Results from Polymer Plasticization

Water content is the most influential factor in the performance of ion-exchange membranes (IEMs), controlling their mechanical rigidity, ionic conductivity, and degradation rates. Membranes absorb water exponentially at high water activity (a w ), making that region of the sorption isotherm the most influential on membrane properties. Plasticization of the polymer by water has been proposed to cause this exponential uptake at high a w . However, an integrated microscopic picture of the structure, thermodynamic, and mechanical properties of IEMs as a function of a w has remained elusive. In this work, we use large-scale molecular simulations validated with experimental measurements to compute the sorption isotherms, Young’s modulus, polymer dynamics, and structure of IEMs. The simulations unveil that the exponential increase in water uptake (WU) coincides in all cases with the glass to rubber transition of the membrane, as measured through its Young’s modulus and segmental polymer dynamics. Functionalization of the polymer with alkyl groups further contributes to its plasticization, increasing the WU at a given a w and ion-exchange capacity (IEC). The alkyl chains act synergistically with water to plasticize the polymer matrix and allow water penetration in the membrane. The simulations reveal that the width of the water channels depends on the ratio λ of water to ions in the polymer but is independent of its IEC. We conclude that differences in the polymer matrix–not the water channels–are responsible for the distinct uptake response of IEMs to the thermodynamic driving force of water activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

ACS Spotlight: Bipolar Membranes for Electrochemical Energy Conversion, Chemical Manufacturing, and Separations

Sustainable energy conversion, chemical manufacturing, and separations are central to addressing the world’s energy and environmental challenges. Electrochemical platforms stand as a cornerstone in addressing these challenges because they are low exergy and can be powered on renewable electrons. In electrochemical systems, bipolar membranes (BPMs) are emerging as a unique class of ion exchange membranes poised to revolutionize various electrochemical processes via pH control of anode and cathode chambers and in situ pH adjustment. In this Spotlight Review, we provide a comprehensive review of electrochemical platforms utilizing BPMs for energy conversion (water electrolyzers for hydrogen production, fuel cells, and flow batteries), chemical manufacturing (electrolyzers that convert carbon dioxide into value-added chemicals and nitrate into ammonia), and separations. The motivation for using BPMs, as well as their performance and durability, in electrochemical platforms are disseminated. We also discuss current challenges that impede BPM electrochemical systems from competing with state-of-the-art electrochemical systems using monopolar ion-exchange membranes (e.g., anion/hydroxide exchange membranes and cation/proton exchange membranes). Here, the review also covers molecular modeling and continuum modeling efforts to understand the basic mechanisms that govern BPM performance.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Pyrazine-Fused Porous Graphitic Framework-Based Mixed Matrix Membranes for Enhanced Gas Separations

Membrane-based separations can mitigate the capital- and energy-intensive challenges associated with traditional thermally driven processes. To further push the boundary of gas separations, mixed matrix membranes (MMMs) have been extensively exploited; however, identifying an optimal nanofiller to boost the separation performance of MMMs beyond Robeson permeability-selectivity upper bounds remains an ongoing challenge. In this study, a new class of MMMs based on pyrazine-fused crystalline porous graphitic frameworks (PGFs) is reported. At a loading of 6 wt % PGFs, the MMMs surpass the current H 2 /CH 4 Robeson upper bound, ideally suited for applications such as H 2 regeneration. In addition, the fabricated MMMs exhibit appealing CO 2 separation performance, closely approaching the current Robeson upper bounds for CO 2 separation. Compared with the pristine polymeric membranes, the PGF-based MMMs display a record-high enhancement of gas permeability over 120% while maintaining intrinsic gas selectivities. Highlighting the crucial role of the crystallinity of nanofillers, this study demonstrates a facile and effective approach in formulating high-performance MMMs, complementing state-of-the-art membrane formation processes. The design principles open the door to energy-efficient separations of gas mixtures with enhanced productivity compatible with the current membrane manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Coordinated Cation Transport in Ti 3 C 2 T x MXene Membranes

Membrane nanofiltration is an attractive strategy for the selective recovery of high-demand metals from wastewater and brine. Effective sieving of ions in aqueous environments will require precise control over membranes’ nanochannel size and chemistry. Ti 3 C 2 T x MXene is an environmentally stable 2D material that can be processed into laminar membranes containing nanoscale interlayer spaces. The MXene interlayer environment depends on the ion species and amount of water intercalated between MXene sheets, and it is the major factor governing permeation and selectivity through MXene membranes. Coordinated ion–ion and ion-interlayer dynamics in the presence of complex mixtures can impact ion permeability and selectivity. Herein, we observe strong competitive effects between different cations (Li + , Na + , and Ca 2+ ) in binary mixtures, resulting in reduced selectivity when compared with single-salt permeability ratios. X-ray diffraction, molecular dynamics, and density functional theory simulations support the conclusion that cations with stronger attraction to MXene flakes can preferentially occupy the MXene nanochannels and hinder other ions via charge or size exclusion. In conclusion, elucidation of ion transport behavior in MXene under complex conditions will allow for more rational design of efficient ion-sieving membranes.

2D Materials↗
DOE OSTI2022

Two-Step Thermoresponsive Ultrafiltration Membranes from Polymerization of Lyotropic Liquid Crystals

Here, in this study, we present the fabrication of a two-step thermoresponsive ultrafiltration (UF) membrane through polymerization of a lyotropic liquid crystal (LLC). A mixture of commercially available Pluronic F 127 block copolymer, water (containing ammonium persulfate as the initiator), and polymerizable oil (n-butyl acrylate/ethylene glycol dimethacrylate) is used to create an LLC with a lamellar structure, as characterized by cross-polarized light microscopy and atomic force microscopy. Differential scanning calorimetry is employed to evaluate the thermoresponsive behavior of the polymerized LLC (polyLLC). Two-step thermoresponsiveness (~35 and ~50 °C) of the polyLLC is observed due to the lower critical solution temperature (LCST) of F 127 and melting of the crystalline structure of the polyethylene oxide (PEO) chains of the F 127 surfactant. In the next step, the obtained mesophase is cast on a nonwoven polyester support sheet followed by thermal polymerization. The hydration capacity, water flux, water flux recovery after fouling, and molecular weight cutoff (MWCO) of the obtained membrane are evaluated at different temperatures to examine its thermoresponsiveness. The experimental results reveal that the UF membrane has a reversible thermoresponsive behavior at the LCST and PEO melting of polyLLC. Additionally, the cleaning efficiency of the fouled membrane can be enhanced by using its thermoresponsive behavior, resulting in an extended lifetime of the product. Furthermore, the MWCO of the membrane can be altered with temperature due to the pore size change with temperature stimulus.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Coupled Interfacial Kinetics and Transport Resistances Govern High-Current Behavior in Bipolar Membranes

Bipolar membranes (BPMs) enable electrochemical systems that operate across large pH gradients; however, high-current operation is often limited by voltage losses whose origins remain difficult to resolve in membrane−electrode assemblies. Here, we combine electrochemical impedance spectroscopy with distribution of relaxation times (EIS–DRT) analysis and operando synchrotron X-ray diffraction to examine interfacial polarization, membrane hydration, and transport in commercial and synthesized BPMs. EIS–DRT isolates the BPM-associated interfacial contribution and shows that the commercial BPM exhibits larger water-dissociation-associated overpotentials than the synthesized BPM. Operando hydration mapping shows that both membranes retain water at the bipolar junction during high-current operation, while anode-adjacent hydration gradients are more pronounced in the commercial membrane. These results indicate that high-current voltage losses are not governed by junction water starvation alone but by coupled interfacial polarization and transport resistances.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electrocoagulation Combined with Ultrafiltration Membranes as Pretreatment for RO Desalination of Synthetic Cooling Tower Blowdown Water

Electrocoagulation (EC), an electrochemical water treatment process, is commonly used to remove particulate and colloidal matter from water. Here, in this study, we demonstrate that EC, when coupled with membrane filtration, is also capable of removing dissolved species, such as Ca + , Mg 2+ , and SiO x . The removal of such species is important for downstream membrane-based desalination treatment of the water that can suffer from reduced performance due to membrane scaling. Here, we describe how EC can be combined with a low-pressure membrane (LPM) system to offer efficient (and potentially universal) pretreatment for downstream membrane desalination. Synthetic water, simulating cooling tower blowdown (CTBD) with elevated concentrations of hardness and silicates (Ca: 418 ppm, Mg: 63 ppm, SiO 2 : 50 ppm) is treated using EC coupled to ultrafiltration (UF) to remove Mg up to 30 ± 1%, Ca up to 29 ± 1%, and silica up to 99 ± 1%. We evaluated the effectiveness of the EC-UF pretreatment system in reducing downstream RO scaling using thermodynamic modeling to predict the saturation index (SI) at the RO membrane/water interface. An SI value below zero (SI < 0) indicates under-saturated conditions (with respect to a particular mineral) where mineral scaling does not take place, which correlates with improved water recovery. Our findings suggest that the EC-UF pretreatment system was able to increase water recovery by up to 30%, compared to 0% recovery without pretreatment, under optimal conditions (feed solution pH of 7 and an EC charge loading of 1800 C/L). Finally, we conducted an economic analysis showing that implementing an EC-UF system for CTBD water could yield a cost benefit of up to $\$$14.13 per m 3 compared to direct brine disposal.

cooling tower blowdown↗
DOE OSTI2022

Tunable Ion Transport with Freestanding Vermiculite Membranes

Membranes integrating two-dimensional (2D) materials have emerged as a category with unusual ion transport and potentially useful separation applications in both aqueous and nonaqueous systems. The interlayer galleries in these membranes drive separation and selectivity, with specific transport properties determined by the chemical and structural modifications within the inherently different interlayers. Here, in this work, we report an approach to tuning interlayer spacing with a single source material–exfoliated and restacked vermiculite with alkanediamine cross-linkers–to both control the gallery height and enhance the membrane stability. The as-prepared cross-linked 2D vermiculite membranes exhibit ion diffusivities tuned by the length of the selected diamine molecule. The 2D nanochannels in these stabilized vermiculite membranes enable a systematic study of confined ionic transport.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

The Effects of Morphology and Hydration on Anion Transport in Self-Assembled Nanoporous Membranes

Ordered nanoporous polymer membranes offer opportunities for systematically probing the mechanisms of ion transport under confinement and for realizing useful materials for electrochemical devices. Here, we examine the impact of morphology and ion hydration on the transport of hydroxide and bromide anions in nanostructured polymer membranes with 1 nm scale pores. We use aqueous lyotropic self-assembly of an amphiphilic monomer, with a polymerizable surfactant to create direct hexagonal (H I ) and gyroid mesophases. UV-induced cross-linking leads to the formation of nanoporous polymers with water continuous channels. The membranes are mechanically robust and chemically durable, resisting degradation during extended exposure to 1 M NaOH solutions. We use a combination of electrochemical impedance spectroscopy, pulsed-field gradient NMR spectroscopy, and molecular simulations to elucidate anion and water transport. The as-prepared hexagonal systems display higher conductivity and lower activation energies for both anions relative to the gyroid system. When compared at equivalent hydration, however, gyroid and hexagonal membranes show similar activation energies, with nearly identical conductivities at ambient temperatures. Both ionic conductivity and water diffusivity increase with increasing hydration. Here, the water uptake as a function of relative humidity for the hexagonal and gyroid mesophases ultimately dictates the water diffusion and magnitude of the ionic conductivity, with the hexagonal system showing overall higher capacity for hydration and thus faster ion transport. The durability of these materials under aggressive alkaline conditions and their relatively high hydroxide ion conductivity suggest that these nanostructured polymers could be of interest as membranes for alkaline fuel cells.

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

Brominated lipid probes expose structural asymmetries in constricted membranes

Lipids in biological membranes are thought to be functionally organized, but few experimental tools can probe nanoscale membrane structure. Using brominated lipids as contrast probes for cryo-EM and a model ESCRT-III membrane-remodeling system composed of human CHMP1B and IST1, we observed leaflet-level and protein-localized structural lipid patterns within highly constricted and thinned membrane nanotubes. These nanotubes differed markedly from protein-free, flat bilayers in leaflet thickness, lipid diffusion rates and lipid compositional and conformational asymmetries. Simulations and cryo-EM imaging of brominated stearoyl-docosahexanenoyl-phosphocholine showed how a pair of phenylalanine residues scored the outer leaflet with a helical hydrophobic defect where polyunsaturated docosahexaenoyl tails accumulated at the bilayer surface. Combining cryo-EM of halogenated lipids with molecular dynamics thus enables new characterizations of the composition and structure of membranes on molecular length scales.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Functional lipid pairs as building blocks of phase-separated membranes

Biological membranes exhibit a great deal of compositional and phase heterogeneity due to hundreds of chemically distinct components. As a result, phase separation processes in cell membranes are extremely difficult to study, especially at the molecular level. It is currently believed that the lateral membrane heterogeneity and the formation of domains, or rafts, are driven by lipid–lipid and lipid–protein interactions. Nevertheless, the underlying mechanisms regulating membrane heterogeneity remain poorly understood. In the present work, we combine inelastic X-ray scattering with molecular dynamics simulations to provide direct evidence for the existence of strongly coupled transient lipid pairs. These lipid pairs manifest themselves experimentally through optical vibrational (a.k.a. phononic) modes observed in binary (1,2-dipalmitoyl- sn -glycero-3-phosphocholine [DPPC]–cholesterol) and ternary (DPPC–1,2-dioleoyl- sn -glycero-3-phosphocholine/1-palmitoyl-2-oleoyl-glycero-3-phosphocholine [DOPC/POPC]–cholesterol) systems. The existence of a phononic gap in these vibrational modes is a direct result of the finite size of patches formed by these lipid pairs. The observation of lipid pairs provides a spatial (subnanometer) and temporal (subnanosecond) window into the lipid–lipid interactions in complex mixtures of saturated/unsaturated lipids and cholesterol. Our findings represent a step toward understanding the lateral organization and dynamics of membrane domains using a well-validated probe with a high spatial and temporal resolution.

60 APPLIED LIFE SCIENCES↗