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270 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Electrochemical Ammonia Compression

An electrochemical (EC) compressor is a solid-state compression device. For decades, researchers have been studying EC compressors for applications for a variety of energy systems. As the world transitions away from fossil fuel energy sources, EC compression emerges as a promising technique for energy storage, specifically energy stored in the form of pressurized ammonia. Ammonia is also a commonly used refrigerant. The present studies examine the viability of EC compression for ammonia storage and refrigeration. EC ammonia compression increases the concentration of an ammonia-hydrogen mixture via the input of electrical energy and a series of chemical reactions. A polymer electrolyte membrane separates the low-concentration side from the high-concentration side of the device. On the low-pressure (anode) side hydrogen atoms oxidize and react with ammonia molecules, forming positively charge ammonium ions. The ions traverse the membrane electrolytically. The ammonium ions are reduced and revert back to hydrogen and ammonia upon reaching the high-pressure (cathode). An external circuit provides the current needed to sustain the reactions. In this project, we studied the performance of the ammonia EC compressor under a variety of different conditions. We replicated preliminary data and using a small cell with 5 cm2 of active area. We demonstrated the operation of larger cells with 100 cm2 of active area. Further, we used a commercially available hydrogen EC compressor stack to analyze the scaled-up compressor performance. While previous experiments examined only the transient EC compressor performance, we developed test facilities that allowed the compressor to reach steady state. We analyzed the effects of pressure and current on the EC compressor performance. We measured the flow rates of gas leaving the compressors and analyzed the composition using gas chromatography. We tested methods of separating ammonia from the effluent vapor, which contained hydrogen and water vapor. We found that back diffusion adversely affected the performance, especially when we maintained high pressure lifts.

25 ENERGY STORAGE↗
DOE OSTI2024

Formation and transformation of iron oxy-hydroxide precursor clusters to ferrihydrite

Iron (Fe) oxy-hydroxide minerals such as ferrihydrite (Fh) are ubiquitous in Earth-surface environments and important in biogeochemical element cycling. Recent research has suggested that their formation is preceded by the precipitation of ultrasmall (~1 nm) Keggin-like Fe oxy-hydroxide clusters. However, relatively little is understood about the structure of the precursor clusters and the impacts of pH and time on their growth and transformation to more stable phases. Here, we used a new method that involves mixed flow reactors (MFR) to synthesize these Fe oxy-hydroxide precursor clusters at pH 1.0, 1.5, 2.5, and 4.5. In situ and ex situ synchrotron scattering measurements and laboratory small-angle X-ray scattering (SAXS) were used to study the structure and size of Fe oxy-hydroxide clusters and their transformation products, respectively. Results show that with increasing pH, the particle size and structural order of samples increase, forming solids that resemble 2-line Fh at pH 4.5. The experimental data were compared with X-ray pair distribution functions (PDF) calculated for a range of Fe(III) oxyhydroxide clusters, including Fe 13 Keggin isomers computed previously using density functional theory (DFT), which yielded at best only partial agreement at short range (<5 Å). Aging of the clusters synthesized at pH 1.5 and 2.5 results in growth and transformation via Ostwald ripening to mixtures of goethite (Gt) and lepidocrocite (Lp). This process was inhibited by immediately reacting the early-formed clusters with phosphate (PO 4 3– ), suggesting that oxyanion surface complexes can stabilize the initial clusters by preventing growth and crystallization to more stable phases.

58 GEOSCIENCES↗
DOE OSTI2022

Nafion Inhibits Polysulfide Crossover in Hybrid Nonaqueous Redox Flow Batteries

Here, we report on the effectiveness of sodium-exchanged Nafion membranes for inhibiting polysulfide crossover during redox flow battery operation. The solubility of polysulfides allows them to be used as a high-capacity catholyte for nonaqueous redox flow batteries (NARFB). The NARFB cathode capacity is controlled by the total tank catholyte volume and polysulfide concentration and, as such, is independent of polysulfide adsorption sites on carbon fibers or nanotubes as found within traditional Na or Li–S batteries. However, one of the major barriers to the realization of polysulfide NARFBs is associated with developing a robust membrane that has minimal polysulfide crossover under the operating conditions. We found that sodium-exchanged Nafion membrane separators effectively inhibit polysulfide crossover within a Na–sulfur NARFB. These membranes significantly improve both capacity retention (70%) and Coulombic efficiencies (99%) after 50 cycles. Commercial porous membranes showed a large crossover as detected by UV–vis spectroscopy and resulted in low capacity retention (20%) and Coulombic efficiency (74%) after 45 cycles. Electrochemical impedance spectroscopy (EIS) measurements highlighted the trade-off between innate reactivity and ionic conduction of the membranes. The results show that dense, single ion conducting Nafion enables a long cycle life; however, it reacts with Na metal to form a resistive passivation layer and increases the cell resistance. On the contrary, the open pore structure of Celgard allows for higher current charge/discharge, and its chemical nature is compatible with Na; however, it has a high degree of polysulfide crossover.

25 ENERGY STORAGE↗
DOE OSTI2021

Energy Evaluation of Electron Beam Treatment of Perfluoroalkyl Substances in Water: A Critical Review

Due to their recalcitrant nature and ubiquitous use, per- and polyfluoroalkyl substances (PFAS) will continue to be major water treatment hurdles. Although effective water treatment technologies exist for physical removal of many PFAS from water (e.g., activated carbon and ion-exchange resin), a PFAS-concentrated waste stream is generated as an end product that can potentially reintroduce PFAS back into the environment. Thus, there is an increased interest in developing destructive technologies to decompose and mineralize PFAS directly in water or in these waste streams. High energy electron beam (e-beam) accelerators have been used for water treatment to degrade a wide range of recalcitrant contaminants, including PFAS, since the 1960s. However, large-scale applications of e-beam for water treatment are restricted due to its high energy consumption and inability to treat large flow rates. Considering there are very few available technologies for destructive removal of PFAS, this study provides a critical review on the treatment of PFAS by direct irradiation of contaminated water by e-beam from an energy consumption point of view. To date, very limited studies have been conducted to investigate the success of this technology to treat PFAS. Results from the limited studies were not directly comparable due to the variation in operating conditions and water quality parameters used in the studies. Here, for the first time, we develop and apply the concept of electrical energy per order (EE/O) to assess the performance of e-beam for PFAS treatment. Results show that EE/O is a better performance parameter than the G value of e-beam for interstudy comparisons and to evaluate the effects of water quality and operating parameters on e-beam performance. We additionally developed a kinetic scheme to predict the performance of e-beam to treat PFAS and revealed that the competition between species to react with aqueous electrons is the determinant factor influencing PFAS degradation efficiency. Comparison of EE/O values of e-beam (range: 31–176 kWh m –3 order –1 ) with other destructive technologies (range: 5–9595 kWh m –3 order –1 ) suggest that e-beam, for PFAS treatment, is a promising approach under favorable conditions. Furthermore, this review further elucidates the feasibility and limitations of e-beam technology that could be improved upon to potentially make e-beam viable for large-scale water treatment applications.

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

Protection against Chemical Warfare Agents and Biological Threats Using Metal–Organic Frameworks as Active Layers

The SARS-CoV-2 pandemic outbreak and the unfortunate misuse of toxic chemical warfare agents (CWAs) highlight the importance of developing functional materials to protect against these chemical and pathogen threats. Metal–organic frameworks (MOFs), which comprise a tunable class of crystalline porous materials built from inorganic nodes and organic linkers, have emerged as a class of heterogeneous catalysts capable of rapid detoxification of multiple classes of these harmful chemical or biological hazards. In particular, zirconium-based MOFs (Zr-MOFs) feature Lewis acidic nodes that serve as active sites for a wide range of catalytic reactions, including the hydrolysis of organophosphorus nerve agents within seconds in basic aqueous solutions. In addition, postsynthetic modification of Zr-MOFs enables the release of active species capable of reacting with and deactivating harmful pathogens. Despite this impressive performance, utilizing Zr- MOFs in powder form is not practical for application in masks or protective uniforms. To address this challenge, our team sought to develop MOF/fiber composite systems that could be adapted for use under realistic operating conditions to protect civilians, military personnel, and first responders from harmful pathogens and chemical warfare agents. Over the last several years, our group has designed and fabricated reactive and biocidal MOF/fiber composites that effectively capture and deactivate these toxic species. In this Account, we describe the evolution of these porous and reactive MOF/fiber composites and focus on key design challenges and considerations. First, we devised a scalable method for the integration of Zr-MOFs onto textile substrates using aqueous precursor solutions and without using pretreated textiles, highlighting the potential scalability of this method. Moving beyond standard textiles, we also developed a microbial synthesis strategy to prepare hierarchically porous MOF/bacterial cellulose nanofiber composite sponges that can both capture and detoxify nerve agents when exposed to contaminated gas flows. The mass loading of the MOF in the nanofibrous composite sponge is up to 90%, affording higher work capacities compared to those of textile-fiber-based composites with relatively lower MOF loadings. Next, we demonstrated that heterogeneous polymeric bases are suitable replacements for volatile liquid bases typically used in solution-phase reactions, and we showed that these composite systems are capable of effectively hydrolyzing nerve agents in the solid state by using only water that is present as humidity. Moreover, incorporating a reactive dye precursor into the composite affords a dual function sensing and detoxifying material that changes color from white to orange upon reaction with the byproduct following nerve agent hydrolysis, demonstrating the versatility of this platform for use in decontamination applications. We then created chlorine-loaded MOF/fiber composites that act as biocidal and reactive textiles that are capable of not only detoxifying sulfur-mustard-based chemical warfare agents and simulants but also deactivating both bacteria and the SARS-CoV-2 virus within minutes of exposure. Lastly, we synthesized a mixed-metal Ti/Zr-MOF coating on cotton fibers to afford a photoactive biocidal cloth that shows fast and broad-spectrum biocidal performance against viruses and Gram-positive and Gram-negative bacteria under visible light irradiation. Given the tunable, multifunctional nature of these MOF/fiber composites, we believe that this Account will offer new insights for the rational design and preparation of functional MOF/fiber composites and pave the way toward the development of next-generation reactive and protective textiles.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Preliminary Kinetic Analysis of Non-Equilibrium Plasma- Assisted Methanol Pyrolysis and Oxidation Experiments

Efforts to enhance power generation efficiency and reduce emissions have driven interest in novel combustion techniques, including non-equilibrium plasma (NEP) ignitors. NEP ignitors show promise in improving energy conversion efficiency, fuel reforming, emission control, and lean-flammability limits. However, their adoption is hindered by a limited understanding of the interplay between plasma-enhanced combustion and thermal chemistry, particularly for complex fuels under engine-relevant conditions. Developing experimentally validated kinetic mechanisms is therefore critical. Additionally, the increasing interest in renewable biofuels like ethanol and methanol, coupled with the desirable qualities of NEP ignitors, presents a compelling opportunity for study. Therefore, this work acts as an extension of a previous work (Bopaiah et al., 2023) pertaining to the experimental results of NEP-assisted methanol pyrolysis and oxidation. Experiments were performed with a custom-built plasma flow reactor at 0.5 atm and temperatures from 523-1203 K. All reactive mixtures are extremely diluted to minimize exothermicity due to reactivity, allowing isothermal assumptions and the isolation of plasma chemistry from thermal chemistry. A dielectric barrier discharge plasma, at 14 kV and 15 ns full-width half maximum, was applied to the reactive mixture at varying frequencies to maintain the number of pulses with increasing temperature. Steady-state product speciation was performed downstream of the reactor with ex-situ GC/MS diagnostics. The attained experimental results were examined through in-depth analysis performed by means of an in-development plasma-coupled kinetic mechanism. As discussed in the previous work, the plasma significantly accelerates methanol pyrolysis, increasing stable intermediate production, including oxygenated and nitrile species. Plasma-assisted oxidation shows even faster fuel consumption compared to pyrolysis and a 200 K ignition shift compared to thermal oxidation. For plasma-assisted pyrolysis, the model demonstrates that accelerated fuel consumption stems from dissociative quenching of excited N2 states with fuel and H2, generating H radicals that react to rapidly form CH3 and CH2OH radicals. At low temperatures, these radicals recombine to produce oxygenates, while CH3 drives nitrile and hydrocarbon formation at higher temperatures. While the model captures pyrolysis trends well, discrepancies in methane, ethylene, and ethanol predictions are present. Similarly, the model faces challenges in accurately representing plasma-assisted oxidation, predicting a much steeper fuel gradient and ignition 100 K earlier than the experiment. While a similar scheme to pyrolysis is nested in the reaction pathway, the enhancement of the O and H radical fluxes and their initiation of the OH and HO2 radical pools dominate fuel and intermediate oxidation. The overestimation of these processes is shown to be responsible for the divergence of model from experiment. While the modelling predictions of this preliminary mechanism are not perfect, they serve as a valuable starting point. Primarily, they elicited new reaction pathways that are not otherwise possible in thermal chemistry induced reaction kinetics. The results also provide a basis for the future work that should be performed. For example, theoretical and experimental studies on excited nitrogen species and fuel/fuel radical interactions, quantification of the NOx production, and the kinetics behind the slow ignition observed in oxidation should be emphasized.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

UO 2 + 5 vol% ZrB 2 nano composite nuclear fuels with full boron retention and enhanced oxidation resistance

The boron isotope ( 10 B) can be used as a neutron absorber in UO 2 to control the reactivity of nuclear fuel pellets, however, the boron source can react with oxygen source in UO 2 to form B 2 O 3 that vaporize readily at temperatures above 1200 °C. Unfortunately, the sintering of UO 2 fuel requires hours holding at high temperature (>1700 °C), resulting in an inevitable B loss during sintering and unpredictable B concentration in final product. It is challenging to incorporate boron through a conventional sintering method. In this work, we demonstrated that spark plasma sintering (SPS), a field assisted sintering technology, can effectively densify UO 2 + 5 vol% ZrB 2 composite fuel pellets by rapid consolidation at 1600 °C for a short duration of 5 min under an applied pressure of 40 MPa. Further, thermogravimetric analysis (TGA) measurements confirm that ZrB 2 is fully retained inside the composite fuel pellets. Inside the composite fuel pellets, nano sized ZrB 2 particles are uniformly distributed along the grain boundaries of the UO 2 matrix. The ZrB 2 particle transforms to a glassy B 2 O 3 phase covering the sample surface and grain boundaries of UO 2 matrix after a simple post-sintering annealing at 1000 °C in flowing Argon gas for 4 h. The formed glassy B 2 O 3 slows down the diffusion of oxygen ions and postpones the onset temperature for oxidation of UO 2 from 400 °C to 550 °C. This study demonstrates the capability of SPS, an advanced fuel manufacturing technique, to achieve a full retention of ZrB 2 in UO 2 oxide fuel and increase oxidation resistance through a simple post-sintering annealing. The reported work holds great engineering potential for development of advanced oxide fuel for nuclear application.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Modular high temperature gas reactor core modeling with RELAP5-3D/PHISICS – Optimization schemes for load following

The objective of this study is to develop a 3D/NK model to study the load following operation of a Modular High-Temperature Gas-Cooled Reactor (MHTGR). The selected design is the 350 MW prismatic, graphite moderated, helium cooled thermal reactor based on the MHTGR-350 transient benchmark led by the High-Temperature Gas-Cooled Reactor (HTGR) Methods Core Simulation Group at Idaho National Laboratory (INL) in the framework of the Organization for Economic Cooperation and Development Nuclear Energy Agency (OECD/NEA). This kind of reactor usually reacts very slowly to the perturbation of the core parameters due to the large amount of graphite in the core. This kind of behavior promotes the reactor stability but on the other hand limits the reactor load-following operability. Recently advances in gas reactor designs have made load-following in gas reactors a feasible and achievable goal. Modern nuclear reactors (such as the MHTGR-350) are designed to withstand the structural stresses associated with load-following. Operating the reactor in load-following mode will inevitably reduce the load factor. Although a higher load factor means more revenue and the best usage of the fuel, following the variable energy demand will increase the maximum achievable fraction of generated nuclear power, being no more limited to the base load power generation. In general, if low impact on material aging and the safe operability are demonstrated the plant economics will be minimally affected. In order to ensure that the system can be safely operated in a load-following mode an extensively study has been carried out. Some tests with linear coolant mass flow rate change demonstrated that the reactor behavior is suitable for operation in load following mode. This assumption has been confirmed by a 4 days load following transient test in which the reactor supplied the requested power with a negligible error.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Finite-rate entrainment effects on nitrogen oxide (NO x ) emissions in staged combustors

Axially staged combustors offer the potential for achieving low NO x emissions from gas turbines at the elevated temperatures required to achieve at least 65% combined cycle efficiencies. While there is evidence that premixing between the main burner products and secondary stream reduces NO x , it is important to characterize the specific requirements needed to achieve low emissions at gas turbine conditions. This study examines the sensitivity of NO x to finite-rate, large-scale entrainment of the main and secondary streams under the simplifying assumption of infinitely-fast small-scale mixing. Essentially, this allows us to isolate the effects of limited large-scale entrainment rates by using a homogeneous/uniform condition for the entrained and reacting gases. We use a reduced-order reactor network model to examine a generic staged-combustor whose inputs are physical time scales that embody the finite-rate entrainment characteristics. With simulations conducted over a large parameter space at typical operating conditions (25 atm, 650 K air), the results show that, even when small-scale mixing is infinitely fast and the reaction zone is uniform, entrainment significantly affects NO x emissions due to its influence on the equivalence ratio — and thus the temperature and time — at which the entrained mixture ignites. Fuel-air staging is shown to be vital to NO x reduction in most practical cases where entrainment times exceed roughly 1 ms and the secondary stream finishes entraining before the main burner products. A constrained NO x minimization indicates that using the leanest possible main burner and re-routing as much air as possible to the secondary stage is key to low NO x with finite-rate entrainment; for example, less than 10 ppm NO x can be achieved if the secondary stage contains 20% of the total mass flow.

03 NATURAL GAS↗
DOE OSTI2026

Distributed Mafic Rock Resources for Carbon Mineralization in Arizona

Ex-situ carbon mineralization is a process by which CO2 is reacted with alkaline silicate minerals and rocks to produce stable carbonate materials, which can be used for other industrial processes. Arizona, U.S.A., hosts abundant surficial mafic rocks in three young volcanic fields, Geronimo-San Bernardino, San Francisco, and Springerville, and other distributed locations throughout the state. We created a Mafic Rock Resource Inventory (MRRI) that categorizes geochemical, physical, and textural characteristics of a diverse suite of surficial mafic rock samples and provide a benchmark reaction dataset parameterizing the temperature, pressure, and pH conditions best suited ex-situ mineralization in different rock types. MRRI data is publicly available online via a map-viewer. We establish two reaction condition sets, varied in temperature, pressure, and pH, where crystal-rich and glassy rocks reach maximum reaction extent and different carbonate phases are formed. Systematic ex-situ mineralization experiments on 21 diverse rock types show trends in geochemical, mineralogical, and reactivity behavior and establish maximum effective capture capacity. From this, scoria cones in three Arizona volcanic fields have a ~62 Gt effective CO₂ storage capacity with one of the fields having a ~42 Gt storage capacity in lava flows. Reactivity results have applications to alkaline mafic rock resources exposed globally, including producing additional effective storage capacity estimates and scaled commercialization of mafic rock ex-situ mineralization, should reaction extents be improved through advances in mineralization techniques. MRRI data were used to create a Direct Air Capture to Mineralization (DACM) systems model, technoeconomic analysis, and life-cycle assessment. These documents are presented as three appendices.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

Development of metallic nuclear material purification process via simultaneous chlorination and volatilization

Here, a purification process involving simultaneous chlorination and volatilization is reported using aluminum, iron, gallium, and uranium separation from cerium metal as the demonstration system. Anhydrous Cl 2 gas was reacted with the metal after it had been converted to small particles of hydride at temperatures ranging from 523 to 973 K. Each of the impurities should form chlorides with relatively high saturated vapor pressures. The objective of the process was to volatilize these chlorides after first achieving near-complete conversion of the metals to hydride and then chlorides. Complete conversion of hydrides to chlorides could not be achieved using relatively low-grade (99.5%) Cl 2 . High decontamination factors for all of the metal impurities required near complete conversion to chloride. It was concluded that oxygen contamination of the feed gas stream likely limits the conversion to chlorides by forming oxides instead, which then limits the volatilization of contaminants. Uranium was particularly challenging to remove in experiments suspected of having high oxygen contamination in the feed gas stream. After switching to ultra-high purity (99.999%) Cl 2 , complete conversion to chlorides within the measurement error was possible for the entire temperature range studied. Decontamination factors for aluminum, iron, gallium, and uranium were found to have average values of 1.9, 9.8, 14, and 5, respectively, at 973 K. While the process was most extensively studied using a once-through gas flow, recycling unreacted Cl 2 gas succeeded at minimizing waste while still maintaining complete conversion and similar decontamination factors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Subtask 2.6 – Optimization of Aerosol Mitigation Technology for Postcombustion CO 2 Capture

Growing concerns over the impact of CO 2 emissions from combustion sources on global climate change have prompted numerous research and development projects aimed at developing cost-effective technologies for CO 2 capture. One family of technologies being demonstrated at pilot and full scale globally is postcombustion CO 2 capture (PCCC) systems that employ amine-based solvents. The captured CO 2 can be compressed and permanently stored underground or used for enhanced oil recovery (EOR). The proximity of North Dakota’s lignite-fired fleet of power plants to potential CO 2 storage options creates a unique atmosphere for PCCC within the state. However, the aerosols present in lignite flue gas present a challenge for large-scale PCCC at North Dakota power plants. Aerosols can negatively impact the long-term performance of amine-based solvents for CO 2 capture. Amine-based solvents are volatile, and aerosols provide nucleation sites where amine vapors can condense. Because aerosols cannot be easily captured at the column outlet using conventional technologies, the amine-laden aerosols escape the system and lead to accelerated solvent losses. Moreover, aerosol components can chemically react with amines to form degradation products that can permanently deactivate the amine, cause fouling, and lead to hazardous emissions. Many of the elements that have been shown to catalyze solvent degradation are present in lignite coals and can exacerbate solvent replacement economics. Understanding this issue is critical to the implementation of solvent-based CO 2 capture systems as applied to lignite-fired generation systems. The Energy & Environmental Research Center (EERC) designed and carried out this project to optimize aerosol mitigation technology for PCCC at a lignite-fired power plant. To meet the goal of this project, the following objectives were identified: Determine the effectiveness of a wet electrostatic precipitator (WESP) on collection of aerosols at a low-rank coal-fired power station. Determine the impact of aerosols on the efficiency and degradation products of amine-based carbon capture systems fired with low-rank fuels. Work was conducted at Minnkota Power Cooperative’s (MPC’s) Milton R. Young (MRY) Station Unit 2 using a slipstream of flue gas from the outlet of the plant’s flue gas desulfurization (FGD) unit. To gather initial data for sizing and specifying a WESP for this system, a temporary pilot-scale WESP was rented and installed on-site. Several different conditions were tested to examine the impact of flow rate, voltage, and current on WESP performance. The WESP was effective at removing large particulate (>200 nm) but caused an increase in fine particulate (<75 nm). Fine particulate material at the inlet and outlet of the WESP was collected, analyzed, and showed that crystalline sulfates carried over from the plant’s FGD unit were being converted to fine aerosols and SO 2 was being converted to SO 3 through the WESP. Additionally, the high moisture content of the flue gas stream at this sample location also contributed to an overall increase in aerosol mass under some of the test conditions. Using the results from the rented WESP, the project team installed a smaller-scale WESP upstream of the EERC’s slipstream CO 2 capture system. Flue gas was routed through a pilot-scale FGD unit to remove SO 2 to very low levels (~1 ppm) and then through a direct contact cooler (DCC) to further cool the gas and to remove moisture. The gas exiting the DCC was then routed through the new WESP before passing to the CO 2 absorber columns. Fluor’s amine-based solvent was used to scrub CO 2 from the slipstream through a set of two absorber columns. The rich solvent was regenerated in a stripper column by heating to drive off captured CO 2 . The system operated using a catch-and-release method where the CO 2 was separated to provide data on the process, but the captured CO 2 was released back into the host site stack. Aerosols and sulfur species were measured at multiple locations throughout the pilot-scale system. The inlet FGD and DCC removed much of the particulate matter and gaseous sulfur upstream of the WESP. With this configuration, the WESP achieved >95% particulate capture. The new WESP did not show any of the increases in SO 3 or other aerosol species that had been consistently observed with the larger-scale WESP installed immediately downstream of the plant’s full-scale FGD unit. Particulate samples captured and analyzed from the WESP inlet did not show any presence of crystalline sulfate materials, indicating that the pilot-scale FGD and DCC were efficient at reducing carryover from the plant’s full-scale FGD unit. A set of parametric tests were conducted on the new WESP to assess the impacts of flow rate, voltage, number of online WESP fields, and gas-phase sulfur content on aerosol and sulfur transformations. The results showed that the WESP performed similarly well at all sets of conditions. Sulfur and particulate matter exiting the WESP were further reduced through the absorber column as the amine-based solvent captured some of the residual contaminants. Solvent analysis showed that these species were slowly concentrating in the solvent over the duration of the test. When the WESP was taken offline and the sulfur slip through the FGD allowed to rise, the sulfate content in the solvent rose sharply, showing that the extra FGD and WESP were effective at reducing sulfate and cation uptake. This would be expected to extend amine-based solvent life by slowing the formation of heat-stable salts and other degradation products. This subtask was cofunded through the EERC–U.S. Department of Energy Joint Program on Research and Development for Fossil Energy-Related Resources Cooperative Agreement No. DE-FE0024233. Nonfederal funding was provided by the North Dakota Industrial Commission and MPC.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2021

Computational Fluid Dynamics Modeling to Simulate a Combined Reforming Process for Syngas and Hydrogen Production

An Oxygen Transport Membrane (OTM) combined reforming technology for producing syngas and hydrogen integrates the advantages of multiple processes—steam methane reforming (SMR), autothermal reforming (ATR), an air separation unit (ASU)—into a single integrated technology. The OTM consists of a primary reforming tube, in which desulfurized natural gas is partially reformed by steam at high pressure in the presence of a metal catalyst. This process is followed in series by a ceramic OTM with a secondary reformer, in which residual methane reforms and O 2 - ions react with a portion of the CO and H 2 fuel to provide the heat to support both primary and secondary reforming. Although the OTM combined reformer technology for syngas and H 2 production has been substantially developed in the last decade, several challenges that affect the overall production efficiency and reliability are yet to be fully understood, addressed, and resolved. Therefore, developing Computational Fluid Dynamics (CFD) models that incorporate fluid dynamics, mass transport, kinetics, heat transport, and structural mechanics is critical to understanding and minimizing the probability of tube failures during the startup and operation. In this report, an exhaustive literature review was performed to survey the current state of technology for producing syngas and H 2 using either conventional or renewable energy sources. The feedstocks reviewed include natural gas and coal for the conventional technologies, whereas biomass, solar, wind, and nuclear energy for the renewable technologies. The existing industry-grade COMSOL multiphysics models of OTM were upgraded for the latest software release. In addition, they were improved to help achieve grid and solver independence and were successfully ported on the ORNL high-performance computing clusters to speed up their run times. A 42% reduction in the simulation run time was achieved. A new higher-fidelity CFD model of an OTM tube was developed in the StarCCM+ simulation platform. This new model was designed to simulate various physics using first principles, e.g., turbulent flow, heat transfer, and chemical reactions while avoiding unnecessary simplifications. The resulting predictions were qualitatively assessed and provided useful insights into the multiphysics complexity of an OTM tube.

08 HYDROGEN↗
DOE OSTI2023

A Novel Dew Point Meter: Application to the Measurement of the Sulfuric Acid Dew Point for Combustion Flue Gas

Accurate knowledge of acid dew point is essential for industrial and applied combustion. Sulfur in the fuel or raw materials is converted to sulfur dioxide (SO2) during combustion, and a portion of the SO2 is oxidized to sulfur trioxide (SO3). The SO3 will react to form H2SO4 vapor when in the presence of water vapor. Even with just trace levels of H2SO4 vapor in the gas phase (1-10 ppm), the dew point can reach 100°C and higher. To avoid acid condensation and the resulting corrosion on heat recovery equipment, plant engineers must ensure that surface temperatures are above the acid dew point, but this decreases the efficiency of the thermal energy recovery. Thus, there is a trade-off between minimizing equipment corrosion and maximizing thermal energy recovery efficiency, and the acid dew point is a key parameter for this optimization. In this work, we analyze and discuss the theory of the sulfuric acid condensation process and develop a novel dew point meter based on this analysis. The meter consists of a novel optical instrument that is designed to monitor the slightest appearance of condensation on a hydrophobic window surface, and the surface temperature of the window is slowly decreased until condensation is first observed, yielding an accurate measurement of the dew point. The basis of the instrument is that a collimated beam from a diode laser generates scattered light when encountering surface condensate, and a sophisticated array detector is used to sensitively monitor the light scattering. The measurement procedures are established to rapidly find the acid dew point, while minimizing error. Further, we propose a calibration system based on a liquid bubbler, which can generate a stable gas flow with known sulfuric acid dew point, to test the dew point meter. Test results show that the dew point meter can accurately measure the acid dew point over a wide range.

Cheng, Mao↗
DOE OSTI2024

A Novel Dew Point Meter: Application to the Measurement of the Sulfuric Acid Dew Point for Combustion Flue Gas

Accurate knowledge of acid dew point is essential for industrial and applied combustion applications. Sulfur in the fuel or raw materials is converted to sulfur dioxide (SO2) during combustion, and a portion of the SO2 is oxidized to sulfur trioxide (SO3). The SO3 will react to form H2SO4 vapor when in the presence of water vapor. Even with just trace levels of H2SO4 vapor in the gas phase (1-10 ppm), the dew point can reach 100°C and higher. To avoid acid condensation and the resulting corrosion on heat recovery equipment, plant engineers must ensure that surface temperatures are above the acid dew point, but this decreases the efficiency of thermal energy recovery. Thus, there is a trade-off between minimizing equipment corrosion and maximizing thermal energy recovery, and the acid dew point is a key parameter for this optimization. Commercially available acid dew point meters use electric conductivity sensors. These sensors are known to greatly underestimate the dew point due to their low sensitivity. In addition, no validation testing has been reported for these units and they are often expensive. In this work, we analyze the theory of the sulfuric acid condensation and develop a novel dew point meter based on this analysis. The meter consists of a novel optical instrument that is designed to monitor the slightest appearance of condensation on a hydrophobic window surface as the surface temperature of the window is slowly decreased. In this way, an accurate measurement of the dew point is obtained under a wide range of concentrations. The basis of the instrument is that a collimated beam from a diode laser will generate forward scattered light when the beam encounters surface condensate, and a sophisticated array detector is used to sensitively monitor the onset of light scattering. The measurement procedures are established to rapidly find the acid dew point, while minimizing error. Further, to calibrate the dew point meter we developed a calibration system based on a liquid bubbler that can generate a stable gas flow with a known sulfuric acid dew point. Test results show that the dew point meter can accurately measure acid dew point over a wide range. For H2SO4 vapor concentrations as low as 6 ppm the acid dew point is measured with an error of only ~1°C. To demonstrate the versatility of this instrument, the dew point meter was adapted for use with a high-pressure flow cell to allow for measurements of the dew point of flue gas from pressurized oxy-fuel combustion in a 100 kWth pressurized reactor.

Cheng, Mao↗
DOE OSTI2020

O · , H · , and · OH radical etching probability of polystyrene obtained for a radio frequency driven atmospheric pressure plasma jet

Atmospheric pressure plasma jets have great potential for the surface modification of polymers. In this work, the authors report on polystyrene etching by a radio frequency driven atmospheric pressure plasma jet with a focus on the role of H · , O · , and · OH radicals in this process. The absolute flux of H · , O · , and · OH radicals reaching the surface of the polymer was determined by a COMSOL MULTIPHYSICS reacting fluid dynamics model incorporating detailed transport phenomena in the boundary layer near the substrate. The simulated results of H · and · OH densities in the jet effluent were experimentally verified by two-photon absorption laser induced fluorescence and laser induced fluorescence, respectively. The carbon atom removal flux from the polystyrene surface was taken from previously reported measurements using the same plasma source. The authors show that the boundary layer effects in the interfacial region above the substrate can have a significant impact on the calculated etching probabilities. The reaction probability (β) has a significant uncertainty although a variation of 2 orders of magnitude in β leads to uncertainties of approximately 1 order of magnitude variation in the determined etching probability. The etching probability of polystyrene by · OH radicals was confirmed to be at least an order of magnitude larger than the polystyrene etching probability by O · radicals. The authors also confirmed the weak polystyrene etching probability by H · radicals. The model suggests that the presence of a 30 ppm O 2 impurity can lead to the production of · OH radicals in the far effluent of the Ar + 1% H 2 plasma jet close to the substrate at sufficient densities to enable effective etching.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Detonation Waves in High Explosives

A material at high temperature can react or decompose. For an energetic material, the reaction is exothermic and releases chemical energy that would further increase the temperature. Under some circumstances, when a reaction is triggered, such a reaction can propagate and the material rapidly releases a large amount of energy giving rise to an explosion. Examples of such materials are aerosols, suspensions of solid particles or liquid droplets in a gas; such as coal dust, grain dust and fuel-air explosions. Frequently, explosions are due to accidents. A spectacularly destructive example is the recent explosion of a large quantity of ammonium nitrate (thousands of tons) in Beirut, Lebanon (August 2020); see for example Beirut explosion. Ammonium nitrate is used as a fertilizer. It and the aerosols are not considered to be explosives due to the limited conditions for which an explosion can occur. An aerosol gets the oxidizer from the surrounding air. Burning requires diffusion of the oxidizer to the particle surface where the reaction occurs. A large density of small particles is required for a fast enough reaction to support an explosion. In contrast, an explosive is an energetic material with both fuel and oxidizer mixed on a molecular scale (either premixed gases or within molecules of a solid). This allows fast enough reactions over a wide range of conditions to support a self-propagating reactive wave known as a detonation wave. A detonation wave can be controlled and an explosive used for useful purposes such as in mining, construction, demolition, explosive welding, argon flash lamp, pulsed power using a magnetic flux generator [see also Goforth et al., 2015], jet cutter with shaped charge, explosive art, and generating conditions to study the response of materials at high strain rates and high pressures [see for example, Marsh, 1980]. Explosives are also used in conventional munitions and nuclear weapons. The focus of this book is on the theory and phenomenology of solid high explosives (HEs); in particular, plastic-bonded explosives (PBXs). Some aspects of detonation wave theory are needed to interpret explosive data. Hence, the theory is presented before the detonation wave phenomenology. A familiarity with fluid flow, specifically the notion of shock waves and the shock loci are assumed. In the remainder of this chapter we give a brief overview on the basic properties of detonation waves and PBXs.

36 MATERIALS SCIENCE↗