Elucidating Design Principles of Type 3 Porous Liquids for Selective Gas Capture
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Nenoff, Tina M. [Sandia National Laboratories (SNL↗
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Cost of Capturing CO 2 from Industrial Sources
The objective of this study is to provide an estimate of the cost to capture carbon dioxide (CO 2 ) from select industrial processes (ammonia, ethylene oxide, ethanol, natural gas processing, coal-to-liquids, gas-to-liquids, refinery hydrogen, cement, iron/steel, and pulp/paper). Each of the ten processes were chosen for analysis due to either the high purity of the CO 2 emission source (99–100 mole percent CO 2 ) or the large quantity of CO 2 potentially available. For each industrial process considered, available plant information, such as existing average plant size, projected new development plant size, or existing plant operations data was used to develop a reference plant for this study.
20 FOSSIL-FUELED POWER PLANTS↗
Porous liquids: an integrated platform for gas storage and catalysis
Porous liquids (PLs) represent a new frontier in materials design, combining the unique features of fluidity in liquids and permanent porosity in solids. By engineering well-defined pores into liquids via designed structure modification techniques, the greatly improved free volume significantly enhances the gas transport and storage capability of PL sorbents. Triggered by the promising applications of PLs in gas separation, PLs are further explored in catalysis particularly to integrate the gas storage and catalytic transformation procedure. This emerging field has demonstrated promising progress to advance catalytic procedures using PLs as catalysts, with performance surpassing that of the pure liquid and porous host counterparts. In this perspective article, the recent discoveries and progress in the field of integrated gas storage and catalysis by leveraging the PL platforms will be summarized, particularly compared with the traditional homogeneous or heterogeneous catalytic procedures. The unique features of PLs endow them with combined merits from liquid and solid catalysts and beyond which will be illustrated first. This will be followed by the unique techniques being utilized to probe the porosity and active sites in PLs and the structural evolution during the catalytic procedures. The catalytic application of PLs will be divided by the reaction categories, including CO 2 -involving transformation, O 2 -involving reaction, H 2 S conversion, hydrogenation reaction, and non-gas involving cascade reactions. In each reaction type, the synthesis approaches and structure engineering techniques of PLs, structure characterization, catalytic performance evaluation, and reaction mechanism exploration will be discussed, highlighting the structure–performance relationship and the advancement benefiting from the unique features of PLs.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Phonon gas model for thermal conductivity of dense, strongly interacting liquids
Developing predictive thermal property models for liquids based on microscopic principles has been elusive. The difficulty is that liquids have gas-like and solid-like attributes that are at odds when considering the frameworks of microscopic models: Models for gases are simple due to randomness and low density, whereas models for crystalline solids rely on symmetry and long-range order for easier calculation. The short-range order in liquids does, however, provide structure to neighboring molecules similar to amorphous solids, and there have been recent advances indicating that collective vibrational modes store heat in liquids. Models combining Debye approximations from solid-state physics and Frenkel’s theory of liquids can accurately predict the heat capacity of liquids. Phonon-like dispersions in liquids have also been widely observed in neutron scattering experiments. These developments motivate us to propose a model where high-frequency vibrational modes, which travel at the speed of sound and have a mean free path on the order of the average intermolecular distance, conduct heat in liquids. We use this liquid phonon gas model to calculate the thermal conductivity of liquids with varying intermolecular interaction energies from strongest to weakest—Coulomb, hydrogen-bonding, Keesom, and London dispersion energy. Generally, the model is more accurate as the intermolecular interaction energy and density of liquids increase. The calculated thermal conductivity of Coulombic-bound molten sodium nitrate and hydrogen-bonded water is within 1.46% and 2.98% of the experimentally measured values, respectively, across their entire temperature ranges. Further modal analysis of the velocity and the mean free path of collective vibrations could establish the liquid phonon gas model as an accurate model for weakly interacting liquids as well.
36 MATERIALS SCIENCE↗
Mechanisms and effects of gas intercalation into ionic liquids confined within charged nanoscale volumes
A combined simulation and experimental study into mechanisms and effects of gas intercalation in ionic liquids confined to charged and neutral carbon nanotubes, providing insights for gas sensing and separation technologies.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Enhancement of Carbon Capture Reactor Performance (Final Technical Report)
Significant challenges are still present in post-combustion CO 2 capture and new technologies and advanced components are needed to significantly advance the deployment of CO 2 capture for natural gas combined cycle (NGCC) plants. Critical elements of CO 2 capture that still need to be addressed include how to increase CO 2 mass transfer in the absorber column with liquid to gas ratios of <1.2, while reducing the size of the absorber column to reduce capital costs. Research involving chemical mechanism with design, synthesis, and assembly of materials with targeted functionally were combined with advanced additive manufacturing techniques towards development of enhanced CO 2 capture reactors that can lead to safe, reliable, and low-cost carbon capture technologies. The objective of the project was to develop and test novel carbon capture materials and reactor components that contribute to increased CO 2 mass transfer through increased turbulent gas-liquid interface and improved solvent wetting within the absorber. A technoeconomic analysis (TEA) was completed showing how the proposed technology decreases capital costs by reducing the size of the absorber column and the amount of packing required for high CO 2 capture rates. A technology maturation plan (TMP) was also developed to describe the current technology readiness levels (TRL) and outline additional research and development (R&D) needed to further develop these advanced components for NGCC CO 2 capture plants. The successful completion of this project has shown a pathway to reduce the absorber size and associated construction costs of post-combustion NGCC CO 2 capture systems at 97% capture and promote the utilization of abundant natural gas for production of reliable electricity.
20 FOSSIL-FUELED POWER PLANTS↗
Following O and OH in He/O 2 and He/H 2 O gas mixtures—from the gas phase through the liquid phase to modifications on a biological sample
Abstract Applied cold atmospheric plasma allows for the controlled delivery of reactive oxygen and nitrogen species tailored for specific applications. Through the manipulation of the plasma parameters, feed gases, and careful consideration of the environment surrounding the treatment target, selective chemistries that preferentially influence the target can be produced and delivered. To demonstrate this, the COST reference microscale atmospheric pressure plasma jet is used to study the generation and transport of O and ⋅ OH from the gas phase through the liquid to the biological model target cysteine. Relative and absolute species densities of ⋅ OH and O are measured in the gas phase through laser induced fluorescence (LIF) and two-photon absorption LIF respectively. The transport of these species is followed into the liquid phase by hydrogen peroxide quantification and visualized by a fluorescence assay. Modifications to the model biological sample cysteine exposed to ⋅ OH and H 2 O 2 dominated chemistry (He/H 2 O (0.25%)) and O dominated chemistry (He/O 2 (0.6%)) is measured by FTIR spectroscopy. The origin of these species that modify cysteine is considered through the use of heavy water (H 2 18 O) and mass spectrometry. It is found that the reaction pathways differ significantly for He/O 2 and He/H 2 O. Hydrogen peroxide is formed mainly in the liquid phase in the presence of a substrate for He/O 2 whereas for He/H 2 O it forms in the gas phase. The liquid chemistry resulting from the He/O 2 admixture mainly targets the sulfur moiety of cysteine for oxidation up to irreversible oxidation states, while He/H 2 O treatment leads preferentially to reversible oxidation products. The more O or OH/H 2 O 2 dominated chemistry produced by the two gas admixtures studied offers the possibility to select species for target modification.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Matlab implementation of a novel semi-structured kinetic model for methanotroph-photoautotroph cocultures
This paper presents the MatLab implementation details of a novel semi-structured kinetic model for methanotroph-photoautotroph cocultures. This includes the parameterization of the modeling equations, and the initialization of the simulation based on experimental conditions. More importantly, it provides details on how the differential equations governing mass balances in both gas and liquid phases are integrated together to simulate the system dynamics over time. The semi-structured kinetic model for methanotroph-photoautotroph coculture is validated using a wide range of experimental conditions. The model: Accurate predicts both the coculture growth in liquid phase and the gas composition changes in head space over time; Explicitly models the exchange of in situ produced O 2 and CO 2 within the coculture; Considers the self-shading effect on the growth of photoautotroph.
42 ENGINEERING↗
Molecular beam scattering from flat jets of liquid dodecane and water
Abstract Molecular beam experiments in which gas molecules are scattered from liquids provide detailed, microscopic perspectives on the gas–liquid interface. Extending these methods to volatile liquids while maintaining the ability to measure product energy and angular distributions presents a significant challenge. The incorporation of flat liquid jets into molecular beam scattering experiments in our laboratory has allowed us to demonstrate their utility in uncovering dynamics in this complex chemical environment. Here, we summarize recent work on the evaporation and scattering of Ne, CD 4 , ND 3 , and D 2 O from a dodecane flat liquid jet and present first results on the evaporation and scattering of Ar from a cold salty water jet. In the evaporation experiments, Maxwell–Boltzmann flux distributions with a cos θ angular distribution are observed. Scattering experiments reveal both impulsive scattering (IS) and trapping followed by thermal desorption (TD). Super‐specular scattering is observed for all four species scattered from dodecane and is attributed to anisotropic momentum transfer to the liquid surface. In the IS channel, rotational excitation of the polyatomic scatterers is a significant energy sink, and these species accommodate more readily on the dodecane surface compared to Ne. Our preliminary results on cold salty water jets suggest that Ar atoms undergo some vapor‐phase collisions when evaporating from the liquid surface. Initial scattering experiments characterize the mechanisms of Ar interacting with an aqueous jet, allowing for comparison to dodecane systems. Key Points Molecular beam scattering from flat liquid jets is a powerful technique to elucidate mechanistic detail at the gas–liquid interface. Previous dodecane scattering experiments have uncovered angularly‐resolved thermal desorption fractions and energy transfer at the interface for several small molecule scatterers. Preliminary results on scattering from cold salty water reveal mechanisms of interaction between argon and an aqueous jet.
Yang, Walt↗
Freeze range of a condensing gas propagating in a liquid helium-cooled tube
Understanding air propagation and condensation following a catastrophic vacuum break in particle accelerator beamlines cooled by liquid helium is crucial for maintaining the operational safety of these facilities. Previous experimental investigations on nitrogen gas propagation in both normal liquid helium (He I) and superfluid helium (He II) cooled copper tubes unveiled a nearly exponential deceleration of the gas propagation. A comprehensive theoretical model incorporating gas dynamics, heat transfer, and condensation mechanisms has been developed, which effectively reproduces various key experimental observations. An intriguing phenomenon uncovered in our model simulation is that the gas propagation appears to nearly stop beyond a certain distance from the location where condensation starts. We refer to this distance as the freeze range. In this paper, we present our systematic study of the freeze range at various inlet mass fluxes and tube diameters. We show that the results can be well described by a simple correlation. The underlying physical mechanism that supports this useful correlation is explained. Knowing the freeze range may allow accelerator engineers to develop protocols for controlling frost-layer contamination in the beamline tubes, which is of great practical importance.
43 PARTICLE ACCELERATORS↗
Enabling CO 2 Isothermal Compression Using Liquid Piston and Integrated Gas Cooler
This report outlines the development of a near-isothermal liquid piston compressor. Initially, a proof-of-concept experiment was conducted to validate the feasibility and potential of near-isothermal compression. A first-of-its-kind near-isothermal liquid piston compressor was then successfully built and tested. Additionally, a Matlab-based transient model was developed to capture performance trends accurately. These efforts laid the groundwork for developing a second-generation prototype with enhanced efficiency and design. Subsequent field tests at the Helix Innovation Center in Ohio demonstrated a cooling capacity of 2 kW with a COP of 1.64 at an ambient temperature of 25°C. An improved model was also created to suggest different heat exchanger geometries for better compression efficiency.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
Jet Fuel Production at the Pittsburgh Airport: GTL via Fischer-Tropsch Synthesis
The Pittsburgh International Airport (PIT)—with the Allegheny County Airport Authority (which manages PIT)—has established itself as a leader in resiliency by becoming the first major United States (U.S.) airport to have a self-sustaining microgrid, providing electricity, heating, and cooling for airport operations. The microgrid is powered by natural gas and solar power produced on the airport property and was completed in Summer 2021. This study examines the feasibility of producing jet fuel at the airport to provide a secure supply of aviation fuel, furthering PIT’s ability to weather supply disruptions and operate self-sufficiently. Gas-to-liquids (GTL) is a commercially available technology that converts natural gas to liquid hydrocarbons, including synthetic jet fuel. A GTL facility at PIT could convert natural gas from onsite wells to jet fuel, effectively doubling the onsite fuel stores in the event of a supply disruption. Moreover, GTL provides a pathway to renewable jet fuel production and reduced greenhouse gas (GHG) emissions from the aviation sector, particularly if renewable natural gas (RNG) is used as a feedstock or other renewable energy sources are used for energy inputs. This study has found that it would be technically feasible to construct and operate a GTL facility on PIT’s property. The approximately 6,000-barrel per day (BPD) facility evaluated would produce nearly 70 million (MM) gallons (gal) of synthetic jet fuel per year, which could supplant nearly all (85 percent) current jet fuel consumption at PIT. Given the current blend limitation of 50 percent Fischer-Tropsch fuels by volume, the plant would have excess production capacity available for the United States Air Force (USAF) Pittsburgh Air Reserve Station and the USAF 171st Air Refueling Wing co-located at the airport.
03 NATURAL GAS↗
Understanding Selectivity Control in the Electrocatalytic Reduction of CO2 to Liquid Products in Gas-Fed Electrolyzers
The room-temperature electrochemical reduction of carbon dioxide to liquid products is a soaring carbon utilization technology with an energy and environmental impact, offering a pathway to convert renewable energy into valuable C1 (e.g., formic acid) and C2+ products (e.g., ethanol and n-propanol)1. Gas-fed flow electrolyzers, in which a gas diffusion layer is used to transport gaseous CO2 into the electrode, have emerged as promising electrocatalytic reactors for large-scale applications, reaching competitive production costs for carbon monoxide (CO) and formic acid (HCOOH). Despite their increased use in recent years, several factors governing their performance have yet to be understood.
Berch, John El↗
Relative permeabilities for two-phase flow through wellbore cement fractures
Multiple fluids are likely to exist in fractures and flow paths associated with leaky wellbores, including liquids (e.g., crude oil) and gases (e.g., gas exsolved from liquid). These fluids occupy and move through different portions of the pore spaces within the fractures depending on many factors, including fluid properties, fracture size, and the amount of the different fluids. Upward leakage of any phase, through the fracture, can contaminate water-bearing formations, create hazardous surface conditions, and compromise the functionality of the wellbore. Early signs of wellbore leaks may be expressed by anomalous pressure behavior at surface monitoring points on cavern storage wells. These pressure anomalies are difficult to interpret, necessitating knowledge of the factors that affect the multiphase flow in fractures and porous media. These parameters are critical to modeling multiphase flow in fractures. This insight can guide further diagnosis and maximize leak remediation. Here, our study focuses on the relationship of the liquid–gas relative permeabilities for representative variable-aperture wellbore cement fracture. To obtain the relative permeability of each phase, two-phase flow tests were conducted where both fluids were flowing simultaneously through a fractured wellbore cement specimen under a range of factors, namely (1) aperture size, (2) capillary numbers, and (3) viscosity ratio. The flow experiments were conducted under a range of confining stresses and flow velocities, using nitrogen gas and silicone oils (of different viscosities) in a specially designed pressure vessel. The sum of gas and oil relative permeabilities were found to be less than one under all conditions, which indicates that the presence of one phase affects the permeability of the other phase, and vice versa. Since the gas phase flow conditions include a significant inertial flow component in addition to viscous flow, the inertial flow coefficients at different saturation states are presented. The factors affecting the relationship between the relative permeabilities are discussed in detail. A new mathematical model for estimating the relative permeability of wellbore cement fracture is presented and experimentally validated.
58 GEOSCIENCES↗
Leakoff assessment of nanoparticle-stabilized CO 2 foams for fracturing applications
The leakoff of multiphase systems through porous media is a complicated process. In this study, we have designed an experimental setup that is used to assess the leakoff of the liquid and gas phase under pressurized conditions. The novelty of this study is that while most previous studies utilized fluid/gas in the aqueous phase, nanoparticles are introduced in this study, which formed a solid/fluid/gas multiphase system to boost foam performance and reduce leakoff. In the parametric experimental analysis, the effects of foam quality, core permeability, surfactant concentration, and polymer concentration on the dynamic and static leakoff rates of liquid and gas are evaluated. It was found that core permeability affects the leakoff of foam the most with a leakoff coefficient of up to 1.37015 $ft/\sqrt{min}$ for gas and up to 0.1056 $ft/\sqrt{min}$ for liquid under the experiment settings herein. The leakoff rate of gas is generally several magnitudes higher than that of the liquid. When CO 2 gas is present in the foam, the leakoff coefficient falls in the range between 0 and 1.37015 $ft/\sqrt{min}$ for gas, and between 0.0005 and 0.1056 $ft/\sqrt{min}$ for liquid. Finally, the methodology and results of this study shed light on the mechanistic understanding of the leakoff properties of multiphase systems and could be used to assist the design of foam fracturing for reservoir stimulation.
03 NATURAL GAS↗
Effect of Computational Schemes on Coupled Flow and Geo-Mechanical Modeling of CO 2 Leakage through a Compromised Well
Carbon capture, utilization, and storage (CCUS) describes a set of technically viable processes to separate carbon dioxide (CO 2 ) from industrial byproduct streams and inject it into deep geologic formations for long-term storage. Legacy wells located within the spatial domain of new injection and production activities represent potential pathways for fluids (i.e., CO 2 and aqueous phase) to leak through compromised components (e.g., through fractures or micro-annulus pathways). The finite element (FE) method is a well-established numerical approach to simulate the coupling between multi-phase fluid flow and solid phase deformation interactions that occur in a compromised well system. We assumed the spatial domain consists of a three-phases system: a solid, liquid, and gas phase. For flow in the two fluids phases, we considered two sets of primary variables: the first considering capillary pressure and gas pressure (PP) scheme, and the second considering liquid pressure and gas saturation (PS) scheme. Fluid phases were coupled with the solid phase using the full coupling (i.e., monolithic coupling) and iterative coupling (i.e., sequential coupling) approaches. The challenge of achieving numerical stability in the coupled formulation in heterogeneous media was addressed using the mass lumping and the upwinding techniques. Numerical results were compared with three benchmark problems to assess the performance of coupled FE solutions: 1D Terzaghi’s consolidation, Liakopoulos experiments, and the Kueper and Frind experiments. We found good agreement between our results and the three benchmark problems. For the Kueper and Frind test, the PP scheme successfully captured the observed experimental response of the non-aqueous phase infiltration, in contrast to the PS scheme. These exercises demonstrate the importance of fluid phase primary variable selection for heterogeneous porous media. We then applied the developed model to the hypothetical case of leakage along a compromised well representing a heterogeneous media. Considering the mass lumping and the upwinding techniques, both the monotonic and the sequential coupling provided identical results, but mass lumping was needed to avoid numerical instabilities in the sequential coupling. Additionally, in the monolithic coupling, the magnitude of primary variables in the coupled solution without mass lumping and the upwinding is higher, which is essential for the risk-based analyses.
deformation flow↗
Two-component dynamics and the liquid-like to gas-like crossover in supercritical water
Molecular-scale dynamics in sub- to super-critical water is studied with inelastic X-ray scattering and molecular dynamics simulations. The obtained longitudinal current correlation spectra can be decomposed into two main components: a low-frequency (LF), gas-like component and a high-frequency (HF) component arising from the O--O stretching mode between hydrogen-bonded molecules, reminiscent of the longitudinal acoustic mode in ambient water. With increasing temperature, the hydrogen-bond network diminishes and the spectral weight shifts from HF to LF, leading to a transition from liquid-like to gas-like dynamics with rapid changes around the Widom line.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Charges on a suspended silicon nitride membrane under a high-energy electron beam
Thin silicon nitride (SiN x ) membranes are widely used in gas and liquid phase transmission electron microscopy (TEM) and as phase plates to enhance imaging contrast. SiN x contains trap sites for both positive and negative charges, which can be manipulated by high-energy electron irradiation, external potential biasing, or light exposure. Charge accumulation on the membrane can significantly affect in situ TEM processes, including chemical and electrochemical reactions, nanoparticle dynamics, and catalytic activity, or introduce unwanted phase shifts when used as a phase plate. Here, in this study, charge accumulation on suspended SiN x membranes was investigated using off-axis electron holography combined with model-free charge analysis, supported by custom finite element analysis (FEA) simulations. An average residual positive charge density of approximately 2.8 × 10 −4 C m −2 was measured. Localized and stable regions of both positive and negative charges were identified on the membrane. The global positive and localized positive/negative charges give rise to strong electric fields and electroosmotic slip velocities at the membrane surface, which are sufficient to induce non-Brownian particle behavior and directional fluid flow, offering a physical explanation for previously observed anomalies in particle dynamics, nucleation, and growth during gas and liquid phase TEM experiments. These results provide a benchmark for understanding charge behavior at SiNx interfaces in gas and liquid phase TEM. Furthermore, the FEA simulations establish a framework for future investigations into charge distribution, electrostatic potentials, and electrical double layers at solid–liquid interfaces, particularly in complex geometries and chemically dynamic environments.
Suspended silicon↗