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DOE OSTI2025

Surface-Enhanced Raman Detection of the CO 2 Moisture Swing

The development of scalable, energy-efficient carbon dioxide (CO 2 ) capture technologies is critical for achieving net-zero emissions. Moisture swing (MS) sorbents offer a promising alternative to traditional thermal regeneration methods by enabling reversible CO 2 binding through humidity-driven ion hydrolysis. In this study, we investigate the anion speciation dynamics in two classes of MS materials─an anion-exchange resin with a bicarbonate anion and activated carbon impregnated with potassium bicarbonate salt─using both sorption measurements and in situ surface-enhanced Raman spectroscopy (SERS). Ni-coated Ag nanowires were employed as SERS substrates to enhance signal intensity and enable the real-time detection of carbonate (CO 3 2– ), bicarbonate (HCO 3 – ), and hydroxide (OH – ) species under controlled humidity conditions in both air and nitrogen atmospheres. The results reveal humidity-dependent interconversion between anionic species with significant spectral shifts confirming the reversible hydrolysis reactions that drive the MS mechanism. Under humid conditions, we observed the depletion of bicarbonate signals and a concurrent increase in carbonate species, consistent with moisture-induced desorption of CO 2 . With the activated carbon samples, we further observed the formation of hydroxide. These findings not only validate the mechanistic models of humidity-driven anion exchange in MS sorbents but also demonstrate the practical potential of SERS as an operando diagnostic tool for monitoring CO 2 capture media. The ability to resolve and semiquantitatively evaluate the reversible transformation of carbonate, bicarbonate, and hydroxide ions under realistic environmental conditions provides valuable insight for the rational design, performance optimization, and quality control of next-generation sorbent materials for direct air capture applications.

CO2 capture↗

DOE OSTI2023

Techno-economic Analysis of the Cryogenic Flux Capacitor Compared to Other forms of Hydrogen Production and Storage

The Cryogenic Flux Capacitor (CFC) is a cold, dense energy storage core that is being studied in the cryo-compressed, about 300 bar and 80K, region of gaseous hydrogen (GH2) storage and liquid hydrogen (LH2) region near the normal boiling point. The hydrogens storage is improved by physically bonding the molecules within the nanoscale pores of the aerogel composite blanket material. The process of bonding or debonding is governed by principles of physical adsorption (physisorption) and thermodynamics. The large surface area afforded by the nanoporous aerogel (~1,000 m2/g) allows its storage performance to easily exceed capacities of high-pressure GH2 storage for an equivalent volume. With the integrated aerogel, subscale tests have shown that storage is increased by about 49% over a simple tank filled with GH2 at the same operating temperature and pressure. For LH2 conditions, the CFC is shown to operate at equivalent densities. For the techno-economic analysis (TEA), the source of hydrogen is compared between onsite steam methane reforming (SMR) and onsite solar photovoltaic (PV) panels providing power to electrolyzers to produce GH2. The TEA compares pure hydrogen burning in a combined cycle gas turbine (CCGT) to hydrogen fuel cells with an overall net power output of 650 MW. The SMR system uses natural gas as an input and includes a carbon capture and storage (CCS) system. The levelized cost of electricity is developed based on the capital cost and operating cost of the systems. Sensitivities are discussed around the cost of natural gas, ranging from 1.93 USD per MMBTU to 6.75 USD per MMBTU, and carbon dioxide disposal, ranging from 7 USD per tonne to 10 USD per tonne. For comparison to the conventional CCGT baseline, a baseload scenario is adopted with 85% capacity factor. The results of the study show that onsite hydrogen generation from SMR is about 1 to 3 USD per kg over the life of the plant and the PV hydrogen production produces at 4 to 5 USD per kg. The cost of storage for CFC is compared to other systems, including high-pressure GH2 and atmospheric LH2. The system is shown to provide the lowest costs for all these options at the grid scale, due to its higher capacity than high-pressure GH2 and ability to operate at 80K, receiving refrigeration from liquid nitrogen systems reducing capital and operating costs when compared LH2 storage systems. SMR is competitive with CCGT at the gas prices, both of which have lower LCOE than the PV system. When accounting for variability in gas prices, the PV and electrolyzer system is less sensitive to these changes and provides the lowest LCOE across the whole range.

08 HYDROGEN↗

DOE OSTI2024

UZrCN Synthesis via Arc Melting - A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE↗

DOE OSTI2024

UZrCN Formation via Arc Melting – A Novel Synthesis Study

36 MATERIALS SCIENCE↗

DOE OSTI2026

Accelerated Carbon and Water Cycles in the Amazon and Congo Basins Revealed From TRENDY Models and Remote Sensing Products

Tropical forests play a vital role in the global carbon cycle and land–atmosphere interactions. Estimating tropical forest carbon–water dynamics is challenging due to observational and modeling uncertainties. This study leverages the “Trends and drivers of the regional scale terrestrial sources and sinks of carbon dioxide” (TRENDY) project models and satellite observations to assess changes (2003–2021) in vegetation carbon, gross primary production (GPP), evapotranspiration (ET), and net biosphere production (NBP) in the Amazon and Congo. Atmospheric CO 2 , climate variability, and land use and land cover changes constrain these variables between 1700 and 2021 with the overall increasing trends of carbon stock and fluxes. The models overestimate vegetation carbon and GPP, while ET and NBP are consistent with observations. Fire-activated models predict lower values for vegetation carbon and GPP, ET, and NBP, aligning more closely with observations. The higher ET from fire-activated models may result from enhanced soil evaporation due to increased canopy openings. Fire-inactivated models could well estimate the magnitudes of NBP. The high vegetation carbon in nitrogen-enabled models points to simulation uncertainties and imbalance in model numbers regarding the nitrogen cycle. Although the nitrogen cycle enhances water use efficiency in both the Amazon and Congo, the models show a higher sensitivity to the nitrogen cycle in the Congo. This study highlights the challenges in accurately representing tropical biogeochemical cycles and the values of satellite products in model evaluations, underscoring the need for standard modeling protocols that address biogeochemical components (e.g., nutrient cycles) to better resolve process-based representations.

Shi, Mingjie [Pacific Northwest National Laborator↗

DOE OSTI2024

UZrCN Synthesis via Arc Melting

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO 2 ) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO 2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Techno-economic analysis of carbon dioxide capture from low concentration sources using membranes

Rising carbon dioxide (CO 2 ) levels in the atmosphere lead to global warming, causing climate change. As such, carbon capture has become necessary to slow the increase and reduce CO 2 levels in the atmosphere. Point source emissions have a wide range of CO 2 concentrations, but emissions below 3% CO 2 have mostly been ignored because Carbon capture from these sources has been viewed as costly and economically unsustainable. Membrane technologies are considered the most viable solution by virtue of more energy-efficient operation. Our group at Idaho National Laboratory (INL) has developed poly[bis((2-methoxyethoxy)ethoxy)phosphazene] (MEEP)-based carbon dioxide selective membranes with CO 2 /N 2 selectivity greater than 40 and CO 2 permeability greater than 450 Barrer. To understand the economics of carbon capture, a spreadsheet-based techno-economic analysis (TEA) model was developed to consider multiple parameters, including selectivity and permeability of the membranes, performance conditions such as the number of stages, module material, electricity price, membrane price, and capital financing. The cost of carbon capture in US $\$$/metric ton was calculated at various purities and compared with other membrane processes, cryogenic capture, solvent-based capture, and pressure swing adsorption-based capture. It was determined that a MEEP-based three-stage process had a capture cost of US $\$$ 50.1/metric ton for 99.8% purity CO 2 from a 1% CO 2 feed source in nitrogen (N 2 ). In conclusion, the capture cost using the best performing Pebax-based membrane was 464% higher, cryogenic capture was 60%–140% higher, pressure swing adsorption was 55%–165% higher, and chemical absorption was -10%–110% higher than MEEP-based membrane capture, respectively.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

Versatile soil gas concentration and isotope monitoring: optimization and integration of novel soil gas probes with online trace gas detection

Abstract. Gas concentrations and isotopic signatures can unveil microbial metabolisms and their responses to environmental changes in soil. Currently, few methods measure in situ soil trace gases such as the products of nitrogen and carbon cycling or volatile organic compounds (VOCs) that constrain microbial biochemical processes like nitrification, methanogenesis, respiration, and microbial communication. Versatile trace gas sampling systems that integrate soil probes with sensitive trace gas analyzers could fill this gap with in situ soil gas measurements that resolve spatial (centimeters) and temporal (minutes) patterns. We developed a system that integrates new porous and hydrophobic sintered polytetrafluoroethylene (sPTFE) diffusive soil gas probes that non-disruptively collect soil gas samples with a transfer system to direct gas from multiple probes to one or more central gas analyzer(s) such as laser and mass spectrometers. Here, we demonstrate the feasibility and versatility of this automated multiprobe system for soil gas measurements of isotopic ratios of nitrous oxide (δ18O, δ15N, and the 15N site preference of N2O), methane, carbon dioxide (δ13C), and VOCs. First, we used an inert silica matrix to challenge probe measurements under controlled gas conditions. By changing and controlling system flow parameters, including the probe flow rate, we optimized recovery of representative soil gas samples while reducing sampling artifacts on subsurface concentrations. Second, we used this system to provide a real-time window into the impact of environmental manipulation of irrigation and soil redox conditions on in situ N2O and VOC concentrations. Moreover, to reveal the dynamics in the stable isotope ratios of N2O (i.e., 14N14N16O, 14N15N16O, 15N14N16O, and 14N14N18O), we developed a new high-precision laser spectrometer with a reduced sample volume demand. Our integrated system – a tunable infrared laser direct absorption spectrometry (TILDAS) in parallel with Vocus proton transfer reaction mass spectrometry (PTR-MS), in line with sPTFE soil gas probes – successfully quantified isotopic signatures for N2O, CO2, and VOCs in real time as responses to changes in the dry–wetting cycle and redox conditions. Broadening the collection of trace gases that can be monitored in the subsurface is critical for monitoring biogeochemical cycles, ecosystem health, and management practices at scales relevant to the soil system.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Life Cycle Assessment of Innovative Carbon Dioxide Selective Membranes from Low Carbon Emission Sources: A Comparative Study

Carbon capture has been an important topic of the twenty-first century because of the elevating carbon dioxide (CO2) levels in the atmosphere. CO2 in the atmosphere is above 420 parts per million (ppm) as of 2022, 70 ppm higher than 50 years ago. Carbon capture research and development has mostly been centered around higher concentration flue gas streams. For example, flue gas streams from steel and cement industries have been largely ignored due to lower associated CO2 concentrations and higher capture and processing costs. Capture technologies such as solvent-based, adsorption-based, cryogenic distillation, and pressure-swing adsorption are under research, but many suffer from higher costs and life cycle impacts. Membrane-based capture processes are considered cost-effective and environmentally friendly alternatives. Over the past three decades, our research group at Idaho National Laboratory has led the development of several polyphosphazene polymer chemistries and has demonstrated their selectivity for CO2 over nitrogen (N2). Poly[bis((2-methoxyethoxy)ethoxy)phosphazene] (MEEP) has shown the highest selectivity. A comprehensive life cycle assessment (LCA) was performed to determine the life cycle feasibility of the MEEP polymer material compared to other CO2-selective membranes and separation processes. The MEEP-based membrane processes emit at least 42% less equivalent CO2 than Pebax-based membrane processes. Similarly, MEEP-based membrane processes produce 34–72% less CO2 than conventional separation processes. In all studied categories, MEEP-based membranes report lower emissions than Pebax-based membranes and conventional separation processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Effect of ammonia addition on suppressing soot formation in methane co-flow diffusion flames

Due to issues surrounding carbon dioxide emissions from carbon-containing fuels, there is growing interest in ammonia (NH 3 ) as an alternative combustion fuel. One attractive method of burning NH 3 is to co-fire it with hydrocarbons, such as natural gas, and in this case soot formation is possible. To begin understanding the influence of NH 3 on soot formation when co-fired with hydrocarbons, soot volume fractions and mole fractions of gas-phase species were computationally and experimentally interrogated for CH 4 flames with up to 40% NH 3 by volumetric fuel fraction. Mole fractions of gas-phase species, including C 2 H 2 and C 6 H 6 , were measured with on-line electron impact mass spectrometry, and soot volume fractions were obtained via color-ratio pyrometry. The simulations employed a detailed chemical mechanism developed for capturing nitrogen interactions with hydrocarbons during combustion. The results are compared to findings in N 2 -CH 4 flames, in order to separate thermal and dilution effects from the chemical influence of NH 3 on soot formation. Experimentally, C 2 H 2 concentrations were found to decrease slightly for the NH 3 -CH 4 flames relative to N 2 -CH 4 flames, and a stronger suppression of C 6 H 6 was found for NH 3 relative to N 2 additions. The measured results show a strong suppression of soot with the addition of NH 3 , with soot concentrations reduced by over a factor of 10 with addition of up to 20% or more NH 3 by mole fraction. The model satisfactorily captured relative differences in maximum centerline C 2 H 2 , C 6 H 6 , and soot concentrations with addition of N 2 , but was unable to match measured differences in NH 3 -CH 4 flames. Furthermore, these results highlight the need for an improved understanding of fuel-nitrogen interactions with higher hydrocarbons to enable accurate models for predicting particulate emissions from NH 3 /hydrocarbon combustion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Metabolic Profiling Reveals Biochemical Pathways Responsible for Eelgrass Response to Elevated CO2 and Temperature

Abstract As CO 2 levels in Earth’s atmosphere and oceans steadily rise, varying organismal responses may produce ecological losers and winners. Increased ocean CO 2 can enhance seagrass productivity and thermal tolerance, providing some compensation for climate warming. However, the metabolic shifts driving the positive response to elevated CO 2 by these important ecosystem engineers remain unknown. We analyzed whole-plant performance and metabolic profiles of two geographically distinct eelgrass ( Zostera marina L.) populations in response to CO 2 enrichment. In addition to enhancing overall plant size, growth and survival, CO 2 enrichment increased the abundance of Calvin Cycle and nitrogen assimilation metabolites while suppressing the abundance of stress-related metabolites. Overall metabolome differences between populations suggest that some eelgrass phenotypes may be better suited than others to cope with an increasingly hot and sour sea. Our results suggest that seagrass populations will respond variably, but overall positively, to increasing CO 2 concentrations, generating negative feedbacks to climate change.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Root responses to elevated CO 2 , warming and irrigation in a semi-arid grassland: Integrating biomass, length and life span in a 5-year field experiment

Plant roots mediate the impacts of environmental change on ecosystems, yet knowledge of root responses to environmental change is limited because few experiments evaluate multiple environmental factors and their interactions. Inferences about root functions are also limited because root length dynamics are rarely measured. Using a 5-year experiment in a mixed-grass prairie, we report the responses of root biomass, length and life span to elevated carbon dioxide (CO 2 ), warming, elevated CO 2 and warming combined, and irrigation. Root biomass was quantified using soil cores and root length dynamics were assessed using minirhizotrons. By comparing root dynamics with published results for soil resources and above-ground productivity, we provide mechanistic insights into how climate change might impact grassland ecosystems. In the upper soil layer, 0–15 cm depth, both irrigation and elevated CO 2 alone increased total root length by twofold, but irrigation decreased root biomass and elevated CO 2 had only small positive effects on root biomass. The large positive effects of irrigation and elevated CO 2 alone on total root length were due to increases in both root length production and root life span. The increased total root length and life span under irrigation and elevated CO 2 coincided with apparent shifts from water limitation of plant growth to nitrogen limitation. Warming alone had minimal effects on root biomass, length and life span in this shallow soil layer. Warming and elevated CO 2 combined increased root biomass and total root length by c. 25%, but total root length in this treatment was lower than expected if the effects of CO 2 and warming alone were additive. Treatment effects on total root length and root life span varied with soil depth and root diameter. Synthesis. Sub-additive effects of CO 2 and warming suggest studies of elevated CO 2 alone might overestimate the future capacity of grassland root systems to acquire resources. In this mixed-grass prairie, elevated CO 2 with warming stimulated total root length and root life span in deeper soils, likely enhancing plant access to more stable pools of growth-limiting resources, including water and phosphorus. Therefore, these root responses help explain previous observations of higher, and more stable, above-ground productivity in these projected climate conditions.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Combining organic amendments with enhanced rock weathering shifts soil carbon storage in croplands

Enhanced rock weathering (ERW) involves applying crushed silicate minerals to cropland soils to remove carbon dioxide and stabilize the global climate. If practiced widely, ERW has the potential to mitigate climate change and improve soil health and crop productivity. However, most ERW studies emphasize inorganic carbon (IC) chemistry, using model-based estimates and short-term mesocosms. Limited field data exist on how ERW interacts with organic amendments to affect organic carbon (C) cycling in soils. In a three-year field study in conventionally managed, irrigated maize fields, we monitored how key soil variables responded to crushed rock-alone, and in combination with compost and/or biochar. We measured weathering indicators (pH, major cations, and IC contents) and organic fractions, including particulate organic matter (POM), mineral-associated organic matter (MAOM), microbial biomass C, and water-extractable organic C. Rock-alone treatments increased weathering proxies (pH and IC) and showed an increasing trend in POM and MAOM, relative to control. In contrast, combining crushed rock with organic amendments resulted in lower soil organic C and nitrogen (N) concentrations (in both POM and MAOM) compared to organic amendments alone, though IC increased in the rock+compost treatment. Combining rock with both compost and biochar (compost/biochar) significantly lowered MAOM-N compared to compost/biochar alone. Overall, co-applying rock with organic inputs may promote weathering and C accrual but slow the accrual rate of organic C and N relative to organic amendments alone. Quantifying these trade-offs over multiple years and scales is critical to integrating ERW with existing soil health practices and climate mitigation strategies.

Biological and medical sciences↗

DOE OSTI2020

The Effects of Synthesis Conditions on the Carbon Capture Capacity of Polyethylenimine Impregnated Protonated Titanate Nanotubes

Capture and storage of carbon dioxide emitted from power plants, which burn fossil fuels, is one of the best ways to mitigate climate change. Polyethylenimine (PEI) impregnated protonated titanate nanotubes (PEI-PTNTs) are efficient amine-modified solid adsorbents for post combustion carbon capture. This study is to investigate the effects of synthesis conditions of titanate nanotubes on the carbon capture capacity of PEI-PTNTs. PTNTs are synthesized using hydrothermal treatment of TiO 2 anatase powder at different temperatures and in different days, followed by washing with dilute HCl solution and deionized water. PEI-PTNTs are prepared by loading PEI (M.W. = 10,000) onto PTNTs at a weight ratio of 1:1 using a wet impregnation process. PTNTs and PEI-PTNTs are characterized using transmission electron microscopy, porosity and surface area analysis, powder X-ray diffraction, and Fourier transform infrared spectroscopy. CO 2 adsorption is conducted at 75 °C using simulated flue gas, and CO 2 desorption is performed at 110 °C by purging the adsorbent with dry nitrogen gas. CO 2 adsorption experiments demonstrate that the PEI-PTNTs synthesized at 130 °C within 3 or 5 days, have the highest CO 2 capture capacity. These optimized PEI-PTNTs have a significant potential to capture CO 2 from power plants.

Materials Science↗

DOE OSTI2021

Hyperstoichiometric Uranium Dioxides: Rapid Synthesis and Irradiation-Induced Structural Changes

Uranium dioxide (UO 2 ), the primary fuel for commercial nuclear reactors, incorporates excess oxygen forming a series of hyperstoichiometric oxides. Thin layers of these oxides, such as UO 2.12 , form readily on the fuel surface and influence its properties, performance, and potentially geologic disposal. This work reports a rapid and straightforward combustion process in uranyl nitrate–glycine–water solutions to prepare UO 2.12 nanomaterials and thin films. We also report on the investigation of the structural changes induced in the material by irradiation. Despite the simple processing aspects, the combustion synthesis of UO 2.12 has a sophisticated chemical mechanism involving several exothermic steps. Raman spectroscopy and single-crystal X-ray diffraction (XRD) measurements reveal the formation of a complex compound containing the uranyl moiety, glycine, H 2 O, and NO 3 – groups in reactive solutions and dried combustion precursors. Combustion diagnostic methods, gas-phase mass spectroscopy, differential scanning calorimetry (DSC), and extracted activation energies from DSC measurements show that the rate-limiting step of the process is the reaction of ammonia with nitrogen oxides formed from the decomposition of glycine and uranyl nitrate, respectively. However, the exothermic decomposition of the complex compound determines the maximum temperature of the process. In situ transmission electron microscopy (TEM) imaging and electron diffraction measurements show that the decomposition of the complex compound directly produces UO 2 . The incorporation of oxygen at the cooling stage of the combustion process is responsible for the formation of UO 2.12 . Spin coating of the solutions and brief annealing at 670 K allow the deposition of uniform films of UO 2.12 with thicknesses up to 300 nm on an aluminum substrate. Irradiation of films with Ar 2+ ions (1.7 MeV energy, a fluence of up to 1 × 10 17 ions/cm 2 ) shows unusual defect-simulated grain growth and enhanced chemical mixing of UO 2.12 with the substrate due to the high uranium ion diffusion in films. As a result, the method described in this work allows the preparation of actinide oxide targets for fundamental nuclear science research and studies associated with stockpile stewardship.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2024

Sol-gel derived silicate-phosphate glass SiO 2 –P 2 O 5 –CaO–TiO 2 : The effect of titanium isopropoxide on porosity and thermomechanical stability

Despite of several decades lasting extensive research of bioactive and bioresorbable glasses the systematic parametrization and determination of the key factors affecting porosity and thermomechanical characteristics still remains challenging. Here, we present silica-phosphate glasses, with the composition 70SiO 2 - 20P 2 O 5 - (10-x)CaO-xTiO 2 (mol%; x = 0, 2.5, 5, and 7.5), prepared by sol -gel method and reinforced by titanium dioxide via titanium isopropoxide (TTIP) incorporation which demonstrated tunable variation of porosity from micro-to macro -region and superb mechanical integrity during the calcination process. The presence of 7.5 mol% TiO 2 promotes dimensional stability up to 1000°C as investigated by thermomechanical analysis. The XRD showed the dominant presence of silicon phosphate [Si(P 2 O 7 )], titanium phosphate [Ti(P 2 O 7 )] and calcium phosphates [β-Ca(P 2 O 6 ) and γ- Ca 2 (P 2 O 7 )]. The effect of TiO 2 doping on the multiscale morphology and porosity was investigated by means of SEM, MIP, μCT, N 2 adsorption and USAXS/SAXS. Increasing TiO 2 content leads to the formation of open porosity up to 70vol% and drives the formation of a refined interconnected macroporosity of 2-30 μm. In contrast, mesoporosity with a dominance of 3-6nm pores decreases in all samples with increasing TiO 2 content. USAXS/SAXS revealed an increase in primary particle size with increasing TiO 2 content which is in good agreement with the nitrogen physisorption analysis showing that microporosity decreases with increasing TiO2 content.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Insights into Controls of Mineralogy and Pore Structure on the Density of Methane Adsorption Phase in Shales under Supercritical Conditions

With gradually increasing enhancing population and industrialization, exploitation of shale gas is enhancing in the world to satisfy the growing demand for energy worldwide. To exploit shale gas efficiently, accurate assessment of shale gas in place (GIP) is necessary for determining production strategies. Unlike free and dissolved gas, adsorbed gas contributes to the shale GIP up to 85% due to the well-developed surface area and micropores. Measured excess adsorption of methane (up to over 95% of subsurface shale gas) is often corrected to absolute adsorption to obtain the actual amount of adsorption under supercritical (or geological) conditions. During the correction, adsorption phase density (APD) is critical. However, the APD of subsurface shale gas and the effects of shale properties (e.g., mineralogy and pore structure) on APD remain poorly understood. A series of high-pressure methane adsorption isotherms (HPMAI) on Caney Shales were collected and analyzed in conjunction with other United States and Chinese shales from the literature at 35–125 °C and up to 15 MPa. Here, a three-layer Ono–Kondo (OK3) model is utilized to derive the temperature- and pressure-dependent APD coupling low-pressure nitrogen adsorption isotherms (LPNAI) and HPMAI. X-ray diffraction and organic geochemistry are combined to reveal the mineralogy. Brunauer–Emmett–Teller, Barrett–Joyner–Halenda, and Horvath–Kawazoe analyses via LPNAI are used to investigate the pore structures. Results show that APD increases with organic matter (OM) proxied by total organic carbon and decreases with clay minerals and the sum of quartz and feldspar. OM dramatically contributes to the APD as multiple-layer adsorption exists, and the APD for OM could be 1.4–8.5 times that for clay minerals. Other inorganic minerals contribute less to APD. The properties and constitution of the surface area instead of the volume fraction contribute to the APD in shales. APD does not show an obvious correlation with micropore volume, likely related to the ratio of micropore volume to the total pore volume. Here, we provide a significant and comprehensive study of petrological factors that impact the APD of subsurface shale gas, which will improve the estimation of supercritical adsorption and shale GIP under reservoir conditions. Also, the findings in this work can provide applications for subsurface carbon dioxide adsorption and storage.

58 GEOSCIENCES↗

DOE OSTI2026

Ammonia in northeast Colorado is increasing, rising most quickly in regions close to confined animal feeding operations

The Colorado Front Range urban corridor and nearby agricultural operations are important source regions of atmospheric ammonia (NH 3 ). Upslope flows periodically transport these emissions into Rocky Mountain National Park (RMNP), located 50 km west of the urban corridor, where wet and dry deposition of excess reactive nitrogen (N) impacts ecosystems. Here, we use a combination of in situ passive NH 3 measurements and NH 3 vertical column density retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) to assess variability and changes in NH 3 across three land use categories in the northeast Colorado source region (agricultural, urban, and remote) during the period 2013-2023. A strong seasonal cycle is present across the region with increased NH 3 during summer months. Elevated NH 3 is spatially correlated with the number of permitted animal units in confined animal feeding operations (CAFOs) within 12 km. Ground-level NH 3 concentrations are strongly positively correlated with monthly gridded IASI satellite column densities. Satellite retrievals reveal an increasing trend in NH 3 column amounts of ∼3% per year in agricultural and ∼2% per year in urban sub-regions. The magnitude of the trend observed in NH 3 columns averaged over the agricultural sub-region is > 3 times larger than observed near and over Denver. The largest increases in NH 3 are closely aligned with the distribution of CAFOs. Reductions in particle sulfate associated with declining sulfur dioxide (SO 2 ) emissions could account for only ∼0.1% per year increase in gaseous NH 3 . Wildfire smoke across the region has increased but appears unlikely to explain the majority of the observed NH 3 increase.

54 ENVIRONMENTAL SCIENCES↗