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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Catalyst Ammonia Storage Measurements Using Radio Frequency Sensing1

Motivated by increasingly strict nitrogen oxides (NOx) limits, engine manufacturers have adopted selective catalytic reduction (SCR) technology to reduce engine-out NOx. In the SCR process, NOx react with ammonia (NH3) to form nitrogen and water vapor. The reaction is influenced by several variables, including stored ammonia on the catalyst, exhaust gas composition, and catalyst temperature. Currently, measurements from NOx and/or NH3 sensors upstream and downstream of the SCR are used with predictive models to estimate ammonia storage levels on the catalyst and control urea dosing. This study investigated a radio frequency (RF)-based method to directly monitor the ammonia storage state of the SCR. This approach utilizes the catalyst as a cavity resonator, in which an RF antenna excites electromagnetic waves within the cavity to monitor changes in the catalyst state. Ammonia storage causes changes in the dielectric properties of the catalyst, which directly impacts the RF signal. Changes in the RF signal relative to stored ammonia (NH3) were evaluated over a wide range of frequencies, temperatures, and exhaust conditions. The RF response to NH3 storage, desorption, and oxidation on the SCR was well correlated with changes in the catalyst state. Calibrated RF measurements demonstrate the ability to monitor the adsorption state of the SCR to within 10% of the sensor full scale. The results indicate direct measurement of SCR ammonia storage levels, and resulting catalyst feedback control, via RF sensing to have significant potential for optimizing the SCR system to improve NOx conversion and decrease urea consumption.

Engineering↗
DOE OSTI2017

CATALYST AMMONIA STORAGE MEASUREMENTS USING RADIO FREQUENCY SENSING

Motivated by increasingly strict NO x limits, engine manufactures have adopted selective catalytic reduction (SCR) technology to reduce engine-out NO x below mandated levels. In the SCR process, nitrogen oxides (NO x ) react with ammonia (NH 3 ) to form nitrogen and water vapor. The reaction is influenced by several variables, including stored ammonia on the catalyst, exhaust gas composition, and catalyst temperature. Currently, measurements from NO x and/or NH 3 sensors upstream and downstream of the SCR are used with predictive models to estimate ammonia storage levels on the catalyst and control urea dosing. This study investigated a radio frequency (RF) -based method to directly monitor the ammonia storage state of the SCR catalyst. This approach utilizes the SCR catalyst as a cavity resonator, in which an RF antenna excites electromagnetic waves within the cavity to monitor changes in the catalyst state. Ammonia storage causes changes in the dielectric properties of the catalyst, which directly impacts the RF signal. Changes in the RF signal relative to stored ammonia (NH 3 ) were evaluated over a wide frequency range as well as temperature and exhaust conditions. The RF response to NH 3 storage, desorption, and oxidation on the SCR was observed to be well-correlated with changes in the catalyst state. Calibrated RF measurements demonstrate the ability to monitor the adsorption state of the SCR to within 10 % of the sensor full scale. The results indicate direct measurement of SCR ammonia storage levels, and resulting catalyst feedback control, via RF sensing to have significant potential for optimizing the SCR system to improve NO x conversion and decrease urea consumption.

Aguilar, Jonathan↗
DOE OSTI2020

Molybdenum Carbide Electrocatalysts for Electrochemical Synthesis of Ammonia from Nitrogen: Activity and Stability

Ammonia production has increased from few thousand tons in 1908 to above 200 million tons per year today, revolutionizing the fertilizer industry thanks to the Haber-Bosch (HB) process. However, the HB process is highly energy intensive consuming about 1.4% of fossil energy generated worldwide and releasing 1.87 tons of CO 2 per ton of ammonia produced. This further reduces ammonia’s scope as a carrier fuel for the hydrogen economy. Hence, finding alternative energy efficient ways to synthesize ammonia is important from more than one perspective. Ammonia synthesis from its constituent nitrogen and hydrogen gases is mainly hampered by the nitrogen reduction reaction (NRR) due to the strong N≡N bond (945 kJ mol −1 ). Electrochemical synthesis (ES) routes in this regard offer a milder approach. However, ES of ammonia under different temperatures, utilizing different electrolytes and catalysts has not yet reliably produced ammonia at viable rates and efficiencies. We report an origami-like Mo 2 C cathode catalyst for NRR that achieved a maximum synthesis rate of 2.16 × 10 −11 mol cm −2 s −1 and a faradaic efficiency of 1.8% at 30 °C using Nafion-212 as electrolyte. Origami-like morphology containing numerous kinks appears to improve electrocatalytic activity and show a promising route for fabricating NRR catalysts with higher catalytic activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1993

New laboratory measurements on ammonia's inversion spectrum, with implications for planetary atmospheres

Microwave spectral measurements have been performed on pure room-temperature gaseous ammonia at frequencies from 1.75 to 18 GHz (1.7-17 cm), at 50-, 100-, and 300-torr pressures. These measurements are part of a laboratory program to measure the microwave absorption spectrum of ammonia, under conditions applicable to giant planet atmospheres, now in progress at the Jet Propulsion Laboratory. The pure ammonia data reported here agree well with previous data by Bleaney and Loubser (1950) at 100 and 300 torrs, and with predictions of the absorptivity formalism published by Berge and Gulkis. Success with pure ammonia but failure with mixtures of ammonia in hydrogen and helium (Spilker, 1990) indicates that the Berge and Gulkis formalism does not correctly handle foreign-gas effects on ammonia inversion lines. This may require modifying conclusions of radio astronomical and radio occultation studies that used this formalism. Notably, a suggested depletion of ammonia and superabundance of hydrogen sulfide may have been exaggerated as a result of inaccuracies in the Berge and Gulkis formalism.

Spilker, Thomas R.↗
DOE OSTI2023

Efficient turbine engine using integrated ammonia fuel processing

A gas turbine engine includes a core engine that includes a core flow path where air is compressed in a compressor section, communicated to a combustor section, mixed with an ammonia based fuel and ignited to generate a high energy combusted gas flow that is expanded through a turbine section. The turbine section is mechanically coupled to drive the compressor section. An ammonia flow path communicates an ammonia flow to the combustor section. A cracking device is disposed in the ammonia flow path. The cracking device is configured to decompose the ammonia flow into a fuel flow containing hydrogen (H2). At least one heat exchanger is upstream of the cracking device that provides thermal communication between the ammonia flow and a working fluid flow such that the ammonia fluid flow accepts thermal energy from the working fluid flow.

Smith, Lance L.↗
DOE OSTI2023

Sustainable ammonia synthesis from nitrogen wet with sea water by single-step plasma catalysis

Ammonia synthesis at ambient conditions employing intermittent distributed green sources of energy and feedstocks is globally sought to replace the centralized Haber-Bosch (H-B) process operating at high temperature and pressure. We report herein for the first time an effective and sustainable ammonia synthesis pathway from N 2 wet with seawater vapor over spherical SiO 2 and M/SiO 2 (M: Ag, Cu, and Co) catalysts driven by non-thermal plasma (NTP). Experimental results indicate that the presence of a catalyst is required for ammonia production from seawater vapor and N 2 . The Co/SiO 2 catalyst delivered the highest ammonia synthesis rate (r NH 3 ) of 3.7 mmol g cat -1 h -1 and energy yield of 3.2 g NH 3 ∙kW -1 ∙h -1 at a relatively low input power of 2 W. The extraction of H atoms from H 2 O molecules plays an important role in the ammonia synthesis from seawater vapor. Finally, this work unfolds a novel platform for the subsequent optimization of sustainable ammonia production from endless resources such as seawater and N 2 through catalytic non-thermal plasma potentially powered by renewable sources.

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

Co 2 Mo 6 S 8 Catalyzes Nearly Exclusive Electrochemical Nitrate Conversion to Ammonia with Enzyme-like Activity

Electrocatalytic nitrate to ammonia conversion is a key reaction for energy and environmental sustainability. This reaction involves complex multi electron and proton transfer steps, and is impeded by the lack of catalyst for promoting both reactivity and ammonia selectivity. Here, we demonstrate active motifs based on the Chevrel phase Co 2 Mo 6 S 8 exhibit an enzyme-like high turnover frequency of ~95.1 s –1 for nitrate electroreduction to ammonia. We reveal strong synergy of multiple binding sites on this catalyst, such that the ligand effect of Co steers H ad* toward hydrogenation other than hydrogen evolution, the ensemble effect of Co, and the spatial confinement effect that promote the full hydrogenation of NO x to ammonia without N–N coupling. The catalyst exhibits almost exclusive ammonia conversion with a Faradaic efficiency of 97.1% and ammonia yielding rate of 115.5 mmol·g cat –1 ·h –1 in neutral electrolytes. The high activity was also confirmed in electrolytes with dilute nitrate and high chloride concentrations.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Optimizing Renewable Ammonia Production for a Sustainable Fertilizer Supply Chain Transition

Local renewable ammonia production using electrolytic hydrogen is an emerging approach to alleviate emissions attributed to synthetic nitrogen fertilizer production while also insulating against fluctuations in fertilizer prices and mitigating transportation costs and emissions. However, replacing ammonia currently produced using fossil fuels will not be immediate. To this end, we develop a supply chain transition model, which first optimizes the design and hourly operation of new renewable ammonia facilities to minimize production costs and then optimizes the annual installation timing, production scale, and location of these new renewable facilities along with ammonia transportation to meet county resolution demands. The objective is to augment and eventually replace conventional ammonia market imports in an economically competitive manner. We performed a case study for Minnesota's ammonia supply chain and found that a full transition to in-state renewable production by 2032 is optimal. This is incentivized by the U.S. federal government's clean hydrogen production credits. This transition results in 99 % reduction in carbon intensity along with stable supply costs below $475 per metric tonne. New renewable production facilities are an order of magnitude smaller than existing conventional plants. They use both wind and solar resources and operate dynamically to minimize expensive battery and hydrogen storage capacities.

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

Exsolution of NiCo alloys over Ruddlesden-Popper perovskite for mild electrochemical synthesis of ammonia on protonic ceramic electrochemical cells

Ammonia synthesis from renewable energies on protonic ceramic electrochemical cells (PCECs) shows great potential. The primary challenges in ammonia synthesis on PCECs include sluggish catalytic activity, competition from the hydrogen evolution reaction, and unsatisfactory durability of the cathode, which is the active site of ammonia generation. Here, in this study, we report an elaborate design of the cathode with an intended formula of Pr 4 Ni 1.79 Co 1.2R u 0.01 O 10-δ , where NiCo alloy nanoparticles are exsolved from Ruddlesden-Popper perovskite substrates after the reduction in 5 % H 2 /Ar at 400 °C for 1 h, for electrocatalysis of the nitrogen reduction reaction to ammonia. The host material Pr 4 Ni 1.8 Co 1.2 O 10-δ with embeddable layered structure and stability was deliberately chosen to fix the Ru cation and maximize the catalytic activity of NiCo. Also, density functional theory calculations suggest that Ru doping provides an optimal balance between structural stability and redox activity, facilitating the controlled exsolution of NiCo nanoparticles and enhancing catalytic performance. As a result, the composite electrode with exsolved NiCo alloy and abundant oxygen vacancies on fuel-electrode-supported PCECs achieves a superior electrochemical activity towards ammonia synthesis: a peak ammonia formation rate of 27.84 μg h −1 cm −2 and excellent Faradaic efficiencies of 62.6 % at 350 °C.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Alternative route for electrochemical ammonia synthesis by reduction of nitrate on copper nanosheets

We propose an efficient and clean avenue for ammonia synthesis, via electroreduction of nitrate which could be obtained from industrial wastewater, domestic sewage, sodium nitrate ore, and nitrification of bacteria and electrochemical oxidation of nitrogen, which addresses the water pollution issues and simultaneously upgrades the nitrate to high-value ammonia. At a low overpotential of -0.15 V versus RHE, Cu nanosheets achieved an ammonia formation rate of 390.1 μg mg -1 Cu h -1 and a Faradaic efficiency of 99.7%, attributed to suppression of the HER activity and apparent improvement of the rate of rate-determining step on Cu (111). Such an ammonia formation rate is more than two orders of magnitude higher than electrochemical nitrogen reduction reaction to ammonia. This work not only develops a powerful strategy to the rational design of robust and efficient catalysts by crystal facet engineering, but also provides an alternative route for electrochemical ammonia synthesis by reduction of nitrate.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Ammonia-based chemisorption heat pumps for cold-climate heating applications: A comprehensive review

This paper reviews the state of the art of chemisorption heat pumps that use ammonia as the refrigerant for cold-climate heating applications. In such a system, ammonia vapor is adsorbed by the solid salt through reversible chemisorption reactions, and the thermal effect of the reaction and ammonia phase change is used to extract heat from a cold environment and supply heat to a warm environment. With the high latent heat and low boiling point of ammonia as a low-temperature refrigerant and the high sorption capacity of ammonia-based chemisorption reactions, chemisorption heat pumps have the potential to produce high-efficiency heating, particularly for cold climates. This review first briefly introduces the basics of ammonia-based chemisorption heat pump systems. Then, the latest development of sorbent materials, including ammoniate salts and heat-conductive porous matrix materials, are summarized with the focus on low-temperature heating conditions. The design of system components, as well as cycle configurations, in the literature are summarized. This review concludes with highlights of recent developments on these topics and suggestions of areas for further research.

42 ENGINEERING↗
DOE OSTI2015

Crystal structure and characterization of a novel L-serine ammonia-lyase from Rhizomucor miehei

L-serine ammonia-lyase, as a member of the β-family of pyridoxal-5′-phosphate (PLP) dependent enzymes, catalyzes the conversion of L-serine (L-threonine) to pyruvate (α-ketobutyrate) and ammonia. The crystal structure of L-serine ammonia-lyase from Rhizomucor miehei (RmSDH) was solved at 1.76 Å resolution by X-ray diffraction method. The overall structure of RmSDH had the characteristic β-family PLP dependent enzyme fold. It consisted of two distinct domains, both of which show the typical open twisted α/β structure. A PLP cofactor was located in the crevice between the two domains, which was attached to Lys52 by a Schiff-base linkage. Unique residue substitutions (Gly78, Pro79, Ser146, Ser147 and Thr312) were discovered at the catalytic site of RmSDH by comparison of structures of RmSDH and other reported eukaryotic L-serine ammonia-lyases. Optimal pH and temperature of the purified RmSDH were 7.5 and 40 °C, respectively. It was stable in the pH range of 7.0–9.0 and at temperatures below 40 °C. This is the first crystal structure of a fungal L-serine ammonia-lyase. It will be useful to study the catalytic mechanism of β-elimination enzymes and will provide a basis for further enzyme engineering. - Highlights: • The crystal structure of a fungal L-serine ammonia-lyase (RmSDH) was solved. • Five unique residue substitutions are found at the catalytic site of RmSDH. • RmSDH was expressed in Pichia. pastoris and biochemically characterized. • RmSDH has potential application in splitting D/L-serine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Gas sensor based on three dimensional Bi2S3 nanowires network for ammonia detection at room temperature

Highlights: • Three dimensional Bi{sub 2}S{sub 3} nanowires networks. • High response to NH{sub 3} gas. • Good selectivity. • Wide linear range. • Work at room temperature. - Abstract: A film containing three dimensional Bi{sub 2}S{sub 3} nanowires network was obtained using Bi(NO{sub 3}){sub 3} and thioacetamide as starting materials through three steps, namely the chemical synthesis of Bi{sub 2}S{sub 3}, preparation of its sol under ultrasonic condition and crystal self-assembly at 25 °C. The nanowires had diameters of 20–100 nm. The formation mechanism of the 3D nanowires network is the anisotropic growth of Bi{sub 2}S{sub 3}. The sensor based on 3D Bi{sub 2}S{sub 3} nanowires network with an excellent response to ammonia at 30 °C. The response mechanism of the sensor for ammonia is a weak coordination adsorption of ammonia molecule on the Bi{sub 2}S{sub 3} nanowires and the electron is partially transferred from ammonia molecule to bismuth (III) ion. The maximum response of the sensor to ammonia was up to 82.3 and had a good linear range from 30 to 350 ppm concentration, indicating its potential applications in the determination and leak alarm of ammonia.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

High-throughput screening to predict highly active dual-atom catalysts for electrocatalytic reduction of nitrate to ammonia

Ammonia is an essential chemical owing to its importance in fertilizer production and other industrial applications. Electrocatalytic nitrate reduction to ammonia (NO 3 RR) holds great promise for low-temperature ammonia production while simultaneously addressing nitrate-based environmental concerns. To provide the mechanistic understanding needed to design an effective electrocatalyst, we systematically investigated the catalytic performance of metal-based dual-atom catalysts (DACs) anchored on two-dimensional (2D) expanded phthalocyanine (Pc) for NO 3 RR. We found that NO 3 RR can efficiently produce ammonia on Cr 2 -Pc, V 2 -Pc, Ti 2 -Pc, and Mn 2 -Pc surfaces with low limiting potentials of – 0.02, – 0.25, – 0.34, and – 0.41 V RHE , respectively. Moreover, using the free energy difference of *NO 3 - and *H as a descriptor, we found that the hydrogen evolution reaction is significantly suppressed on the DAC surface due to an ensemble effect in which the two metal atoms cooperate to selectively form ammonia. We performed high-throughput screening to develop an efficient metal-based DAC for NO 3 - reduction, followed by a mechanistic study to elucidate the NO3RR pathway on the DAC. Finally, this work provides design information for advancing sustainable ammonia synthesis under ambient conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Ammonia gas sensors: A comprehensive review

We report that in recent years, sensitive, selective and accurate sensing techniques for ammonia gas detection have been highly demanded since ammonia is both a commonly utilized gas in various industrial sectors and a highly toxic and corrosive agent that can threat human health and environment. This review article discusses the widely used gas sensing techniques in ammonia detection. The fundamental working principles of the ammonia detection techniques relying on electronics, electrochemistry, tunable diode laser spectroscopy, surface acoustic wave, and field effect transistors are briefly described first, in conjunction with various sensing materials. Furthermore, recent progress in the development of advanced ammonia gas sensors was comprehensively reviewed and summarized. Finally, the outlook for future development of high-performance ammonia sensors was presented.

47 OTHER INSTRUMENTATION↗
DOE OSTI2017

Biochar to reduce ammonia emissions in gaseous and liquid phase during composting of poultry manure with wheat straw

Highlights: • Biochar can function as an amendment for low C/N and low porosity raw materials. • Biochar reduced the gaseous emissions of ammonia during poultry manure composting. • Significant ammonia emissions [NH{sub 4}{sup +}] in the condensate were registered. • Biochar has a potential impact on N retention during composting of high N materials. •easuring [NH{sub 4}{sup +}] in condensate allows closing up the N balance during composting. - Abstract: Composting of poultry manure which is high in N and dense in structure can cause several problems including significant N losses in the form of NH{sub 3} through volatilization. Biochar due to its recalcitrance and sorption properties can be used in composting as a bulking agent and/or amendment. The addition of a bulking agent to high moisture raw materials can assure optimal moisture content and enough air-filled porosity but not necessarily the C/N ratio. Therefore, amendment of low C/N composting mixtures with biochar at low rates can have a positive effect on composting dynamics. This work aimed at evaluating the effect of selected doses of wood derived biochar amendment (0%, 5% and 10%, wet weight) to poultry manure (P) mixed with wheat straw (S) (in the ratio of 1:0.4 on wet weight) on the total ammonia emissions (including gaseous emissions of ammonia and liquid emissions of ammonium in the collected condensate and leachate) during composting. The process was performed in 165 L laboratory scale composting reactors for 42 days. The addition of 5% and 10% of biochar reduced gaseous ammonia emission by 30% and 44%, respectively. According to the obtained results, the measure of emission through the condensate would be necessary to assess the impact of the total ammonia emission during the composting process.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2017

An environmental friendly animal waste disposal process with ammonia recovery and energy production: Experimental study and economic analysis

Highlights: • An environmental friendly animal manure waste treatment scheme was proposed. • Ammonia was removed and recovered from manure waste in the form of struvite. • Horse manure waste gasification was successfully conducted in a 10 kW gasifier. • Gasifier produces comparable or higher heating value of syngas as other feedstocks. • The proposed scheme is financially superior to pure gasification and incineration. - Abstract: Animal manure waste is considered as an environmental challenge especially in farming areas mainly because of gaseous emission and water pollution. Among all the pollutants emitted from manure waste, ammonia is of greatest concern as it could contribute to formation of aerosols in the air and could hardly be controlled by traditional disposal methods like landfill or composting. On the other hand, manure waste is also a renewable source for energy production. In this work, an environmental friendly animal waste disposal process with combined ammonia recovery and energy production was proposed and investigated both experimentally and economically. Lab-scale feasibility study results showed that 70% of ammonia in the manure waste could be converted to struvite as fertilizer, while solid manure waste was successfully gasified in a 10 kW downdraft fixed-bed gasifier producing syngas with the higher heating value of 4.9 MJ/(N m{sup 3}). Based on experimental results, economic study for the system was carried out using a cost-benefit analysis to investigate the financial feasibility based on a Singapore case study. In addition, for comparison, schemes of gasification without ammonia removal and incineration were also studied for manure waste disposal. The results showed that the proposed gasification-based manure waste treatment process integrated with ammonia recovery was most financially viable.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Rapid, efficient reduction of iron oxide with ammonia

Reducing iron oxide to iron metal with fossil fuels produces circa 4% of annual anthropogenic CO 2 , ca. 2 Gt/a, as direct chemical emissions from the process. Using ammonia instead of coke—releasing only water and nitrogen as byproducts—could be a widely deployable method of decarbonizing industrial ironmaking, because ammonia carries hydrogen and can be transported easily worldwide. However, initial reports suggest that the reaction of ammonia with iron oxide is slow and inefficient, completed only in hours and using only a few percent of the ammonia supplied. Drawing on thermodynamic and kinetic analysis of the reaction, we explored high-temperature, high-flow reaction conditions designed to increase the reaction rate and the ammonia utilization. We report the reduction of iron oxide in 1 min while using 64% of the ammonia supplied. We show that these insights translate to the gram scale and the reduction of pelletized ore, a common form used industrially.

36 MATERIALS SCIENCE↗