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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Seawater alkalization via an energy-efficient electrochemical process for CO 2 capture

Electrochemical pH-swing strategies offer a promising avenue for cost-effective and energy-efficient carbon dioxide (CO 2 ) capture, surpassing the traditional thermally activated processes and humidity-sensitive techniques. The concept of elevating seawater’s alkalinity for scalable CO 2 capture without introducing additional chemical as reactant is particularly intriguing due to its minimal environmental impact. However, current commercial plants like chlor-alkali process or water electrolysis demand high thermodynamic voltages of 2.2 V and 1.23 V, respectively, for the production of sodium hydroxide (NaOH) from seawater. These high voltages are attributed to the asymmetric electrochemical reactions, where two completely different reactions take place at the anode and cathode. Here, we developed a symmetric electrochemical system for seawater alkalization based on a highly reversible and identical reaction taking place at the anode and cathode. We utilize hydrogen evolution reaction at the cathode, where the generated hydrogen is looped to the anode for hydrogen oxidation reaction. Theoretical calculations indicate an impressively low energy requirement ranging from 0.07 to 0.53 kWh/kg NaOH for established pH differences of 1.7 to 13.4. Experimentally, we achieved the alkalization with an energy consumption of 0.63 kWh/kg NaOH, which is only 38% of the theoretical energy requirements of the chlor-alkali process (1.64 kWh/kg NaOH). Further tests demonstrated the system’s potential of enduring high current densities (~20 mA/cm 2 ) and operating stability over an extended period (>110 h), showing its potential for future applications. Notably, the CO 2 adsorption tests performed with alkalized seawater exhibited remarkably improved CO 2 capture dictated by the production of hydroxide compared to the pristine seawater.

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

Measurement of the Effective Capture Cross Section of 238 Np in the High Flux Isotope Reactor

The cross sections of 237 Np and 238 Np are important for accurate modeling and simulation of 238 Pu in the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL). Uncertainties in these cross sections can impact the ability to predict and optimize the target design and loading for 238 Pu production targets. The effective capture cross section of 237 Np in the location of pneumatic tube 1 in HFIR was measured as a first step in the measurement of the 238 Np capture and fission cross sections. Here, we describe the flux measurements, 237 Np experiments, and data analysis of the 237 Np capture cross section in HFIR.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2014

Detecting non-relativistic cosmic neutrinos by capture on tritium: phenomenology and physics potential

We study the physics potential of the detection of the Cosmic Neutrino Background via neutrino capture on tritium, taking the proposed PTOLEMY experiment as a case study. With the projected energy resolution of Δ ∼ 0.15 eV, the experiment will be sensitive to neutrino masses with degenerate spectrum, m{sub 1} ≅ m{sub 2} ≅ m{sub 3} = m{sub ν} ∼> 0.1 eV. These neutrinos are non-relativistic today; detecting them would be a unique opportunity to probe this unexplored kinematical regime. The signature of neutrino capture is a peak in the electron spectrum that is displaced by 2 m{sub ν} above the beta decay endpoint. The signal would exceed the background from beta decay if the energy resolution is Δ ∼< 0.7 m{sub ν} . Interestingly, the total capture rate depends on the origin of the neutrino mass, being Γ{sup D} ≅ 4 and Γ{sup M} ≅ 8 events per year (for a 100 g tritium target) for unclustered Dirac and Majorana neutrinos, respectively. An enhancement of the rate of up to O(1) is expected due to gravitational clustering, with the unique potential to probe the local overdensity of neutrinos. Turning to more exotic neutrino physics, PTOLEMY could be sensitive to a lepton asymmetry, and reveal the eV-scale sterile neutrino that is favored by short baseline oscillation searches. The experiment would also be sensitive to a neutrino lifetime on the order of the age of the universe and break the degeneracy between neutrino mass and lifetime which affects existing bounds.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

WIMP capture and annihilation in the Earth in effective theories

I calculate the rate of WIMP capture and annihilation in the Earth in the non-relativistic effective theory of dark matter-nucleon interactions. Neglecting operator interference, I consider all Galilean invariant interaction operators that can arise from the exchange of a heavy particle of spin less than or equal to one when WIMPs have spin 0, 1/2 or 1. I compute position and shape of the expected resonances in the mass—capture rate plane and show that Iron is not the most important element in the capture process for many currently ignored interaction operators. I compare these predictions with the recent results of an Earth WIMP analysis of IceCube in the 86-string configuration and set limits on all isoscalar and isovector coupling constants of the effective theory of dark matter-nucleon interactions. For certain interaction operators and for a dark matter particle mass of about 50 GeV, I find that these limits are stronger than those I have previously derived in an analysis of the solar WIMP search performed at IceCube in the 79-string configuration.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2017

Thermalization time scales for WIMP capture by the Sun in effective theories

I study the process of dark matter capture by the Sun, under the assumption of a Weakly Interacting Massive Particle (WIMP), in the framework of non-relativistic effective field theory. Hypothetically, WIMPs from the galactic halo can scatter against atomic nuclei in the solar interior, settle to thermal equilibrium with the solar core and annihilate to produce an observable flux of neutrinos. In particular, I examine the thermalization process using Monte-Carlo integration of WIMP trajectories. I consider WIMPs in a mass range of 10–1000 GeV and WIMP-nucleon interaction operators with different dependence on spin and transferred momentum. I find that the density profiles of captured WIMPs are in accordance with a thermal profile described by the Sun's gravitational potential and core temperature. Depending on the operator that governs the interaction, the majority of the thermalization time is spent in either the solar interior or exterior. If normalizing the WIMP-nuclei interaction strength to a specific capture rate, I find that the thermalization time differs at most by 3 orders of magnitude between operators. In most cases of interest, the thermalization time is many orders of magnitude shorter than the age of the solar system.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Self-consistent microscopic calculations for electron captures on nuclei in core-collapse supernovae

Calculations for electron capture rates on nuclei with atomic numbers between 𝑍 = 20 and 𝑍 = 52 are performed in a self-consistent finite-temperature covariant energy density functional theory within the relativistic quasiparticle random-phase approximation. Electron captures on these nuclei contribute most to reducing the electron fraction during the collapse phase of core-collapse supernovae. The rates include contributions from allowed (Gamow-Teller) and first-forbidden (FF) transitions, and it is shown that the latter become dominant at high stellar densities and temperatures. Temperature-dependent effects such as Pauli unblocking and transitions from thermally excited states are also included. The new rates are implemented in a spherically symmetric one-dimensional simulation of the core-collapse phase. The results indicate that the increase in electron capture rates, due to inclusion of FF transitions, leads to reductions of the electron fraction at nuclear saturation density, the peak neutrino luminosity, and enclosed mass at core bounce. The new rates reaffirm that the most relevant nuclei for the deleptonization situate around the 𝑁 = 50 and 82 shell closures, but, compared to previous simulations, nuclei are less proton rich. Here, the new rates developed in this work are available, and will be of benefit to improve the accuracy of multidimensional supernova simulations.

Electron & muon capture↗
DOE OSTI2025

Indirect Measurement of the 23 Na(p, γ) 24 Mg Direct Capture Reaction Rate via ( 3 He,d) Spectroscopy

The cross section of the $^{23}\text{Na}(p,γ)^{24}\text{Mg}$ reaction is dominated by direct capture at low energies relevant for stellar burning. Such cross sections can be constrained using spectroscopic factors($C^2S$) or asymptotic normalization coefficients(ANCs) from transfer reactions. In this work, the $^{23}\text{Na}(^3\text{He},d)^{24}\text{Mg}$ reaction was measured at $E_{lab}=21$ MeV to extract spectroscopic factors for $^{24}\text{Mg}$ states with excitation energies in $E_x=7 - 12$ MeV using the Enge split-pole spectrograph at the Triangle Universities Nuclear Laboratory. A new non-resonant astrophysical S factor and the direct capture reaction rate for the $^{23}\text{Na}(p,γ)$ reaction are calculated and presented based on this measurement. The new rate at $T<0.04$ GK is 43$\%$ smaller than in previous studies. Rigorous treatments of uncertainties are presented using a Bayesian Markov Chain Monte Carlo (MCMC) method. Finally, sources of uncertainties for computing the direct capture cross section are also discussed in detail.

electromagnetic moments↗
DOE OSTI2023

Ab initio calculation of muon capture on 24 Mg

In this work we study ordinary muon capture (OMC) on 24 Mg from a first-principles perspective. Starting from a particular two- and three-nucleon interaction derived from chiral effective field theory, we use the valence-space in-medium similarity renormalization group (VS-IMSRG) framework to construct effective Hamiltonians and muon-capture operators, which nonperturbatively account for many-body physics outside the valence space. Here, the obtained nuclear matrix elements are compared against those from the phenomenological shell model. The impact of including the correlations from the nuclear shell model (NSM) as well as including the induced twobody part is studied in detail. Furthermore, the effects of realistic bound-muon wave function on the operators is studied. Finally, predictions for capture rates to the lowest excited states in 24 Na are given and compared with available data. It is found that the spectroscopic properties of 24 Mg and its OMC daughter 24 Na are fairly well described by both the NSM and VS-IMSRG, and that the effect of the hadronic two-body currents significantly reduces the OMC rates. Both models have some difficulties in matching the measured OMC rates, especially for the 2 + final states. This calls for further studies in other light nuclei with available OMC data.

20 ≤ A ≤ 38↗
DOE OSTI2023

Neutron capture-induced nuclear recoils as background for CE$v$⁢NS measurements at reactors

Nuclear reactors represent a promising neutrino source for CE⁢v⁢NS (coherent-elastic neutrino-nucleus scattering) searches. However, reactor sites also come with high ambient neutron flux. Neutron capture-induced nuclear recoils can create a spectrum that strongly overlaps the CEv⁢NS signal for recoils ≲100 eV for nuclear reactor measurements in silicon or germanium detectors. This background can be particularly critical for low-power research reactors providing a moderate neutrino flux. Here, in this work we quantify the impact of this background and show that, for a measurement 10 m from a 1 MW reactor, the effective thermal neutron flux should be kept below ~7 × 10 –4 ⁢n/cm 2 s so that the CE⁢v⁢NS events can be measured at least at a 5⁢σ level with germanium detectors in 100 kg yr exposure time. This flux corresponds to 60% of the sea-level flux but needs to be achieved in a nominally high-flux (reactor) environment. Improved detector resolution can help the measurements, but the thermal flux is the key parameter for the sensitivity of the experiment. For silicon detectors, the constraint is even stronger and thermal neutron fluxes must be near an order of magnitude lower. This constraint highlights the need of an effective thermal neutron mitigation strategy for future low threshold CEv⁢NS searches. In particular, the neutron capture-induced background can be efficiently reduced by active veto systems tagging the deexcitation gamma following the capture.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Resonance Structure of the Charge-Exchange Strength Function and Neutrino-Capture Cross Sections for the Isotopes {sup 71}Ga, {sup 98}Mo, and {sup 127}I

A resonance structure of the charge-exchange strength function S(E) and its effect on the neutrino-capture cross sections for the isotopes {sup 71}Ga, {sup 98}Mo, and {sup 127}I are studied within the self-consistent theory of finite Fermi systems. The calculation of the strength function S(E) takes into account Gamow–Teller, analog, and so-called lower lying pygmy resonances. The neutrino-capture cross sections σ(E) for the above three isotopes are calculated with allowance for the resonance structure of the strength function S(E), and the effect of each resonance on the energy dependence σ(E) is analyzed. It is found that all charge-exchange resonances in the strength function S(E) should be taken into account in calculating the neutrino-capture cross section σ(E) for the isotopes {sup 71}Ga, {sup 98}Mo, and {sup 127}I. The disregard of even highlying resonances leads to a substantial underestimation of the cross section σ(E), and this may affect the interpretation of respective experimental data.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2013

The role of electron-electron interaction in the process of charge-carrier capture in deep quantum wells

The role of electron-electron interaction in the process of electron capture to a deep quantum well is investigated. Using two-level and three-level quantum wells as examples, the basic electron-capture mechanisms, i.e., the interaction with optical phonons and the Coulomb electron-electron interaction, are considered, and the corresponding capture probabilities and electron lifetimes are calculated. The effect of Auger recombination on the charge-carrier distribution in a quantum well is also taken into account. With this taken into consideration, a set of rate equations is solved for a nonsteady-state mode, and the time dependences of the electron concentration at the ground energy level in the quantum well are found. The contributions of each of the recombination processes under consideration are shown.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Promoting CO 2 Release from CO 3 2- -Containing Solvents during Water Electrolysis for Direct Air Capture

The pH swings from water electrolysis are leveraged to condition OH – -based facile CO 2 capture solvents using an electrochemical flow cell for direct air capture (DAC). Besides demonstrating the DAC using a membrane contactor, promoting CO 2 release from a CO 3 2– solution at the anode is specifically studied by adjusting the volumetric flow rate, anode chamber volume, residence time, and K 2 CO 3 concentration. Through case-by-case comparisons coupled with modeled results, increasing current, reducing volumetric flow rate, and/or reducing CO 3 2– concentration are the effective methods to promote CO 2 release from a CO 3 2– -containing solvent, whereas enlarging the anode chamber volume poses a minor effect. Moreover, the discrepancies between the experimental and modeled results may be caused by H + crossover rather than K + transport through the Nafion membrane during water electrolysis based upon the total alkalinity measurements for the K 2 CO 3 solutions gleaned from the anode. Here, it is believed that such results will provide guidance to design and operate an electrochemical flow cell for electrochemistry-assisted DAC and point source CO 2 capture.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2018

Effective Elastic and Neutron Capture Cross Section Calculations Corresponding to Simulated Fluid Properties from CO2 Push-Pull Simulations

The submission contains a .xls files consisting of 10 excel sheets, which contain combined list of pressure, saturation, salinity, temperature profiles from the simulation of CO2 push-pull using Brady reservoir model and the corresponding effective compressional and shear velocity, bulk density, and fluid and time-lapse neutron capture cross section profiles of rock at times 0 day (baseline) through 14 days. First 9 sheets (each named after the corresponding CO2 push-pull simulation time) contains simulated pressure, saturation, temperature, salinity profiles and the corresponding effective elastic and neutron capture cross section profiles of rock matrix at the time of CO2 injection. Each sheet contains two sets of effective compressional velocity profiles of the rock, one based on Gassmann and the other based on Patchy saturation model. Effective neutron capture cross section calculations are done using a proprietary neutron cross-section simulator (SNUPAR) whereas for the thermodynamic properties of CO2 and bulk density of rock matrix filled with fluid, a standalone fluid substitution tool by Schlumberger is used. Last sheet in the file contains the bulk modulus of solid rock, which is inverted from the rock properties (porosity, sound speed etc) based on Gassmann model. Bulk modulus of solid rock in turn is used in the fluid substitution.

15 GEOTHERMAL ENERGY↗
DOE OSTI2019

Recent developments on polymeric membranes for CO 2 capture from flue gas

Polymeric membranes have been widely considered as one of the next-generation technologies for CO 2 capture from fossil fuel-derived flue gases. This separation modality requires novel polymeric materials that possess efficient CO 2 /N 2 separation properties, as well as chemical and mechanical stability for a multiyear membrane lifetime. In this paper, recent developments in polymeric membranes tailored for post-combustion carbon capture are reviewed. The selected polymeric materials encompass ether oxygen-rich polymers, polynorbornenes, ionic liquid membranes, and facilitated transport membranes. In each of the selected materials, noteworthy research efforts for material design and membrane formation are highlighted. The performances of the selected materials are compared in the CO 2 /N 2 selectivity-CO 2 permeance plot. As the only class of materials reviewed herein that have demonstrated the fabrication of thin-film composite membranes in scale, facilitated transport membranes have shown both high selectivity and permeance at relevant conditions for post-combustion carbon capture. Finally, comprehensive field tests are needed to resolve the technical gap between the material development and the commercial application.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2022

Latent Space Simulation for Carbon Capture Design Optimization

The CO2 capture efficiency in solvent-based carbon capture systems (CCSs) critically depends on the gas-solvent interfacial area (IA), making maximization of IA a foundational challenge in CCS design. While the IA associated with a particular CCS design can be estimated via a computational fluid dynamics (CFD) simulation, using CFD to derive the IAs associated with numerous CCS designs is prohibitively costly. However, previous works such as Deep Fluids (Kim et al., 2019) show that large simulation speed-ups and low error are achievable by replacing CFD simulators with neural-network (NN) surrogates that mimic the CFD simulation process. This raises the possibility for a fast, accurate replacement for a CFD simulator, and thus computationally feasible IA-based CCS-design optimization. As such, here, we explore whether an existing NN-surrogate approach (and variants we develop) can successfully be applied to our complex carbon-capture CFD simulations, with the ultimate goal of obtaining a fast and accurate simulator for our CCS-design application. Our experiments build on the Deep Fluids approach and find that resulting surrogates can produce large speed ups (4000x) while maintaining IA relative errors as low as 4% on unseen CCS configurations (interpolating between configurations seen during training). Thus, despite less faithfulness to the underlying physics of the problem, NN surrogates may be a promising tool for our CCS design optimization problem. Notably, though, the Deep Fluids approach has limitations for our application (such as model non-transferability to CCS-packing changes), which we discuss. We conclude with potential directions for future work that may, like innovations we introduced here (e.g., transformer-based dynamics prediction), improve performance on our complicated dataset of CCS CFD simulations.

AI Surrogate Simulation, Carbon Capture, design op↗
DOE OSTI2017

Novel Silica Nanostructured Platforms with Engineered Surface Functionality and Spherical Morphology for Low-Cost High-Efficiency Carbon Capture

Carbon capture is an integral part of the CO 2 mitigation efforts, and encompasses, among other measures, the demonstration of effective and inexpensive CO 2 capture technologies. The project demonstrated a novel platform—the amine-functionalized stellate mesoporous silica nanosphere (MSN)—for effective CO 2 absorption. The reported CO 2 absorption data are superior to the performance of other reported silica matrices utilized for carbon capture, featuring an amount of over 4 milimoles CO 2 /g sorbent at low temperatures (in the range of 30-45 ºC), selected for simulating the temperature of actual flue gas. The reported platform is highly resilient, showing recyclability and 85 % mass conservation of sorbent upon nine tested cycles. Importantly, the stellate MSNs show high CO 2 selectivity at room temperature, indicating that the presence of nitrogen in flue gas will not impair the CO 2 absorption performance. The results could lead to a simple and inexpensive new technology for CO 2 mitigation which could be implemented as measure of CO 2 mitigation in current fossil-fuel burning plants in the form of solid sorbent.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2018

Demonstration of Carbon Capture and Sequestration of Steam Methane Reforming Process Gas Used for Large-Scale Hydrogen Production

The large-scale, on-purpose production of hydrogen in the United States (i.e., ~4600 million standard cubic feet per day) represents one of the most significant industrial sources of CO 2 emissions within the chemical industry. Most of the hydrogen is produced by the steam methane reforming (SMR) process, through which methane and water are converted to H 2 and CO 2 , and virtually all of the co-produced CO 2 is emitted to the atmosphere. However, the process streams in the SMR plants contain CO 2 at concentrations that are amenable to utilization of conventional adsorption and emerging CO 2 capture technologies. If implemented commercially, these technologies could represent an early and sizeable impact in reducing industrial CO 2 emissions. Therefore, Air Products, working closely with the Department of Energy, has conducted a carbon capture and sequestration (CCS) project to demonstrate a first-of-a-kind retrofit system to capture CO 2 from large-scale industrial SMR plants. Working with the support of Denbury Onshore, LLC (“Denbury Onshore”) and its affiliate, Denbury Green Pipeline-Texas, LLC (“Denbury Green Pipeline”), Air Products designed, constructed and continues to operate a state-of-the-art system located at the Valero Port Arthur Refinery in Port Arthur, TX. This system concentrates the CO 2 from two SMR waste streams and delivers it into the Green Pipeline-Texas for transport to and use in the West Hastings Unit enhanced oil recovery (EOR) project. The CO 2 removal units were designed by Air Products and utilize vacuum swing adsorption (VSA) units that were retrofitted into each of the SMR trains upstream of existing pressure swing adsorption (PSA) units. This project is unique because the site has two large-scale, highly integrated SMRs located in proximity to one another. The CO 2 from this project is concentrated from 15% in the SMR waste stream to at least 98%, then flowed into the Green Pipeline-Texas along the eastern Gulf Coast. The Green Pipeline collects CO 2 from a variety of sources that is utilized for tertiary oil recovery in Texas. This project alone can prevent over 1 million tons per year of CO 2 from being emitted into the atmosphere, and thus play a major role in significantly reducing greenhouse gas emissions.

08 HYDROGEN↗
DOE OSTI2019

Evaluation of amine-incorporated porous polymer networks (aPPNs) as sorbents for post­combustion CO 2 capture

This is the final report for the TAMU project “Evaluation of amine-incorporated porous polymer networks (aPPNs) as sorbents for post­combustion CO 2 capture.” During this project, a team consisting of the Zhou group at Texas A&M University and framergy Inc. were tasked with developing a porous polymer network (PPN) based sorbent system for CO 2 capture applications. The three year project was divided up into 3 individual budget periods. During budget period 1 the team develop multiple novel PPN based sorbents and began initial CO 2 capture experiments. During the course of this research the team determined that two sorbents were the standout targets, PPN-150-DETA and PPN-151-DETA. During budget period 2 the team further developed these two materials, gathering data to determine their performance under both wet and dry conditions, determine their CO 2 adsorption capacities, heats of adsorption, regenerative energy demands, and mechanical attrition. In addition, budget period 2 saw the development of 50 g and 250 g batches of both sorbents, while still maintaining >0.10 g/g uptake capacity under wet gas conditions. Following budget period 2 testing, the team opted to continue on with PPN-151-DETA due to its superior CO 2 cycling capabilities, with a consistent uptake capacity observed over 30 cycles at the lab scale. During budget period 3 the team further developed the material at scale, producing a 1 kg batch of material. Following this, the team performed multiple long-term cycling tests in the presence and absence of SO 2 using a 100 mL column. During this testing the team observed that the material loses significant uptake capacity due to SO 2 , as well as shows some level of DETA loss, which resulted in instrument breakdown and a request for a no-cost extension. The team was able to finalize the experiment with a test using a 1.5 L column in the absence of SO 2 , with the final cycle uptakes being around 0.035 g/g due to the need to harshly activate the material to prevent DETA desorption.

20 FOSSIL-FUELED POWER PLANTS↗