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DOE OSTI2021

Sequentially prepared Mo-V-Based SCR catalyst for simultaneous Hg 0 oxidation and NO reduction

Molybdenum (Mo)-vanadium (V)-based selective catalytic reduction (SCR) catalyst synthesized by the sequential impregnation of Mo and W followed by V was investigated for simultaneous elemental mercury (Hg 0 ) oxidation and nitrogen oxide (NO) reduction in an existing SCR unit with respect to different TiO 2 phases, calcination temperatures, flue gas constituents, gas velocities, and reaction temperatures. Anatase phase TiO 2 and the calcination temperatures of 400 and 500 degrees C resulted in similar to 69% Hg 0 oxidation at 10 ppmv HCl and 350 degrees C. The high calcination temperature of 700 degrees C resulted in TiO 2 phase transformation from anatase to rutile and agglomeration. The modified SCR catalyst prepared with the impregnation sequence of Mo and W followed by V using anatase TiO 2 and calcination temperature 500 degrees C showed similar to 99% Hg 0 oxidation and 87% NO reduction conversions at an NH 3 /NO molar ratio of 0.9 under 350 degrees C and 5,000 hr -1 space velocity in typical sub-bituminous and lignite coal simulated flue gases. Finally, the effects of these parameters and conditions were further investigated using various characterization techniques including BET, TEM, XRD, NH 3 TPD and XAFS.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Large enhancement of ferroelectric properties of perovskite oxides via nitrogen incorporation

Perovskite oxides have a wide variety of physical properties that make them promising candidates for versatile technological applications including nonvolatile memory and logic devices. Chemical tuning of those properties has been achieved, to the greatest extent, by cation-site substitution, while anion substitution is much less explored due to the difficulty in synthesizing high-quality, mixed-anion compounds. Here, nitrogen-incorporated BaTiO3 thin films have been synthesized by reactive pulsed-laser deposition in a nitrogen growth atmosphere. The enhanced hybridization between titanium and nitrogen induces a large ferroelectric polarization of 70 μC/cm2 and high Curie temperature of ~1213 K, which are ~2.8 times larger and ~810 K higher than in bulk BaTiO3, respectively. These results suggest great potential for anion-substituted perovskite oxides in producing emergent functionalities and device applications.

Wang, Tao↗

NASA NTRS2011

Two Catalysts for Selective Oxidation of Contaminant Gases

Two catalysts for the selective oxidation of trace amounts of contaminant gases in air have been developed for use aboard the International Space Station. These catalysts might also be useful for reducing concentrations of fumes in terrestrial industrial facilities especially facilities that use halocarbons as solvents, refrigerant liquids, and foaming agents, as well as facilities that generate or utilize ammonia. The first catalyst is of the supported-precious-metal type. This catalyst is highly active for the oxidation of halocarbons, hydrocarbons, and oxygenates at low concentrations in air. This catalyst is more active for the oxidation of hydrocarbons and halocarbons than are competing catalysts developed in recent years. This catalyst completely converts these airborne contaminant gases to carbon dioxide, water, and mineral acids that can be easily removed from the air, and does not make any chlorine gas in the process. The catalyst is thermally stable and is not poisoned by chlorine or fluorine atoms produced on its surface during the destruction of a halocarbon. In addition, the catalyst can selectively oxidize ammonia to nitrogen at a temperature between 200 and 260 C, without making nitrogen oxides, which are toxic. The temperature of 260 C is higher than the operational temperature of any other precious-metal catalyst that can selectively oxidize ammonia. The purpose of the platinum in this catalyst is to oxidize hydrocarbons and to ensure that the oxidation of halocarbons goes to completion. However, the platinum exhibits little or no activity for initiating the destruction of halocarbons. Instead, the attack on the halocarbons is initiated by the support. The support also provides a high surface area for exposure of the platinum. Moreover, the support resists deactivation or destruction by halogens released during the destruction of halocarbons. The second catalyst is of the supported- metal-oxide type. This catalyst can selectively oxidize ammonia to nitrogen at temperatures up to 400 C, without producing nitrogen oxides. This catalyst converts ammonia completely to nitrogen, even when the concentration of ammonia is very low. No other catalyst is known to oxidize ammonia selectively at such a high temperature and low concentration. Both the metal oxide and the support contribute to the activity and selectivity of this catalyst.

Wright, John D.↗

DOE OSTI2021

Ultra-clean condensing gas furnace enabled with acidic gas reduction

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Clean Condensing Gas Furnace

Natural gas furnaces are the most common space heating equipment in the U.S. residential and commercial building markets. However, current residential natural gas condensing furnaces generate substantial acidic condensate as well as significant emissions of sulfur oxides (SOx), nitrogen oxides (NOx), carbon monoxide (CO), hydrocarbons (HC), and methane (CH 4 ) contributing to environmental degradation of air, water, and soil. This report describes a novel solution to reduce the environmental impact of natural gas condensing furnaces based on the technology of a monolithic acidic gas reduction (AGR) catalyst for SOx trapping, NOx redox to nitrogen, and oxidation of formic acid, CO, HC, and CH 4 . The AGR technology offers the following benefits: (1) a neutral furnace condensate with a pH of ~7, allowing its safe release into the sewer system thus eliminating a second drainage system; (2) trapping and removing nearly all SOx emissions; (3) NOx emissions nearly at nearly 1-2 ng/J, more than 95% lower than new emissions standards in California; (4) the use of a low-cost heat exchanger as a condensing heat exchanger (HX) since the condensate is not acidic, avoiding the need for expensive stainless steel alloys; and (5) unburnt fuel energy recovery to boost efficiency.The AGR component and AGR-enabled furnace performance were broadly tested to determine their effects on long-term reliability and durability, as well as SOx storage and regeneration activity. The AGR regeneration does not impair the performance in achieving neutral condensate and ultra-low NOx emissions, and the AGR catalyst subjected to regeneration activities continued to function well and achieved slightly better annual fuel utilization efficiency (AFUE). The 400-hour reliability and durability test of the retrofitted condensing furnace with the AGR component shows that the furnace unit still achieves a neutral furnace condensate with a pH of ~7 and enables 0~3 ng/J of NOx emissions. However, the 400-hour operation slightly degraded the AFUE because of soot particle accumulation caused by frequent incomplete combustion owing to inappropriate condensate drainage during testing. Thus, proper condensate drainage is critical for AGR-enabled furnaces. Furthermore, neutron computed tomography was employed to survey the aged AGR component and demonstrate high-resolution 2D and 3D representations for the nondestructive diagnosis of the AGR component. The tomography showed that the AGR component did not deform or suffer broken AGR channels. A new AGR catalyst with low precious metal loading was preliminarily explored to identify a pathway of optimizing AGR material loading and maximizing acidic gas reduction at low cost. The new AGR component can reduce precious metal loading by 38% and still achieve neutral condensate and ultralow NOx emissions. The furnace with the AGR component of low Pt/Rh loading enables a maximum AFUE of 97%, which is meaningfully higher than the original furnace. Long-duration testing for the furnace enabled with the low precious metal loading AGR component will be vital in future research. Although the current work demonstrates a proof of concept for the AGR-enabled furnace, the AGR assembly needs to be optimized and integrated into the design of new OEM furnace products. Furthermore, the AGR technology can be applied not only for residential gas furnaces, but also for commercial rooftop units, gas heat pumps, gas-fired water heaters, combustion boilers, and other systems.

03 NATURAL GAS↗

NASA NTRS1953

ROCKET ENGINE STARTING WITH MIXED OXIDES OF NITROGEN AND LIQUID AMMONIA BY FLOW-LINE ADDITIVES

Rocket engine starting with mixed oxides of nitrogen and liquid ammonia by flow-line additives

ROCKET ENGINE↗

NASA NTRS1981

Effect of fuel nitrogen and hydrogen content on emissions in hydrocarbon combustion

How the emissions of nitrogen oxides and carbon monoxide are affected by: (1) the decreased hydrogen content and (2) the increased organic nitrogen content of coal derived fuels is investigated. Previous CRT experimental work in a two stage flame tube has shown the effectiveness of rich lean two stage combustion in reducing fuel nitrogen conversion to nitrogen oxides. Previous theoretical work gave preliminary indications that emissions trends from the flame tube experiment could be predicted by a two stage, well stirred reactor combustor model using a detailed chemical mechanism for propane oxidation and nitrogen oxide formation. Additional computations are reported and comparisons with experimental results for two additional fuels and a wide range of operating conditions are given. Fuels used in the modeling are pure propane, a propane toluene mixture and pure toluene. These give hydrogen contents 18, 11 and 9 percent by weight, respectively. Fuel bound nitrogen contents of 0.5 and 1.0 percent were used. Results are presented for oxides of nitrogen and also carbon monoxide concentrations as a function of primary equivalence ratio, hydrogen content and fuel bound nitrogen content.

Bittker, D. A.↗

NASA NTRS1971

Application of a Chemiluminescence Detector for the Measurement of Total Oxides of Nitrogen and Ammonia in the Atmosphere

By means of the thermal conversion of nitrogen dioxide to the nitric oxide, the chemiluminescent nitric oxide monitor, based on the nitric oxide plus ozone reaction, may be used for monitoring nitrogen dioxide plus nitric oxide (NO(x)). Under conditions previously described, ammonia is also converted to nitric oxide and therefore interferes. A metal surface, gold wool or stainless steel, operated at two different temperatures has been used to convert only nitrogen dioxide or nitrogen dioxide plus ammonia. Quantitative conversion of nitrogen dioxide to nitric oxide has been obtained at temperatures as low as 200 C. Conversion of ammonia is effected at temperatures of 300 C or higher. By the addition of a converter the basic nitric oxide monitor may be used for measuring NO(x) or NO(x) plus ammonia. As an alternate mode, for a fixed high temperature, a specific scrubber is described for removing NH3 without affecting NO2 concentrations.

Hodgeson, J. A.↗

NASA NTRSDate not supplied

Biomass burning declines lead to large net reductions in NO2 concentrations over north equatorial Africa in spite of growing fossil fuel emissions

Socio-economic development in low and middle-income countries has been accompanied by increased emissions of air pollutants such as nitrogen oxides (NOx: nitrogen dioxide (NO2) + nitric oxide (NO)), which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, biomass burning—another important NOx source—has declined in Africa’s northern biomass burning region, attributed to changes in climate and anthropogenic fire management associated with agricultural development. Here we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to over 350 million people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the biomass burning season of November through February. Reductions in burned area explained the majority of these change in NO2 VCDs, but there were also weaker relationships between changes in NO2 VCDs and fossil fuel emissions over parts of West Africa, which were stronger during rainy season. Over Africa’s biomass burning regions, NO2 VCDs tended to decrease with increasing population density up to a threshold of approximately 180 people per km2, suggesting that anthropogenic activity causes a net reduction in NO2 emissions across roughly 90% of the continent’s biomass burning regions. In contrast to the widely-held perception that socio-economic development worsens air quality in low and middle-income nations, our results suggest that countries in Africa’s northern biomass burning region are following a different pathway, resulting in regional air quality benefits. However, these benefits may be lost with increasing fossil fuel use.

Biomass burning↗

NASA NTRS2021

Reductions in NO2 Burden Over North Equatorial Africa from Decline in Biomass Burning in Spite of Growing Fossil Fuel Use, 2005 to 2017

Socioeconomic development in low- and middle-income countries has been accompanied by increased emissions of air pollutants, such as nitrogen oxides [NOx: nitrogen dioxide (NO2) + nitric oxide (NO)], which affect human health. In sub-Saharan Africa, fossil fuel combustion has nearly doubled since 2000. At the same time, landscape biomass burning—another important NOx source—has declined in north equatorial Africa, attributed to changes in climate and anthropogenic fire management. Here, we use satellite observations of tropospheric NO2 vertical column densities (VCDs) and burned area to identify NO2 trends and drivers over Africa. Across the northern ecosystems where biomass burning occurs—home to hundreds of millions of people—mean annual tropospheric NO2 VCDs decreased by 4.5% from 2005 through 2017 during the dry season of November through February. Reductions in burned area explained the majority of variation in NO2 VCDs, though changes in fossil fuel emissions also explained some variation. Over Africa’s biomass burning regions, raising mean GDP density (USD·km−2) above its lowest levels is associated with lower NO2 VCDs during the dry season, suggesting that economic development mitigates net NO2 emissions during these highly polluted months. In contrast to the traditional notion that socioeconomic development increases air pollutant concentrations in low- and middle-income nations, our results suggest that countries in Africa’s northern biomass-burning region are following a different pathway during the fire season, resulting in potential air quality benefits. However, these benefits may be lost with increasing fossil fuel use and are absent during the rainy season.

air pollution↗

NASA NTRS2021

Continental and Ecoregion-Specific Drivers of Atmospheric NO2 and NH3 Seasonality Over Africa Revealed by Satellite Observations

Ammonia (NH3) and nitrogen oxides (NOx: nitrogen dioxide (NO2) + nitric oxide (NO)) play important roles in atmospheric chemistry. Throughout most of Africa, emissions of these gases are predominantly from soils and biomass burning. Here we use observations of tropospheric NO2 vertical column densities (VCDs) from the Ozone Monitoring Instrument (OMI) from 2005 through 2017 and atmospheric NH3 VCDs from the Infrared Atmospheric Sounding Interferometer (IASI) from 2008 through 2017 to evaluate seasonal variation of NO2 and NH3 VCDs across Africa and in seven African ecoregions. In regions where mean annual precipitation (MAP) is under 500 mm/yr we find that NO2 and NH3 VCDs are positively related to monthly precipitation, and where MAP is between 500 and 1750 mm yr-1 or higher, NO2 VCDs are negatively related to monthly precipitation. In dry ecoregions, temperature and precipitation were important predictors of NH3 and NO2 VCDs, likely related to variation in soil emissions. In mesic ecoregions, monthly NO2 VCDs were strongly related to burned area, suggesting that biomass burning drives seasonality. NH3 VCDs in mesic ecoregions were positively related to both monthly temperature and monthly CO VCDs, suggesting that a mixture of soil and biomass burning emissions influenced NH3 seasonality. In northern mesic ecoregions monthly temperature explained most of the variance in monthly NH3 VCDs, suggesting that soil sources, including animal excreta, determined NH3 seasonality. In southern mesic ecoregions, monthly CO VCDs explained more variation in NH3 VCDs than temperature, suggesting that biomass burning may have greater influence over NH3 seasonality.

Jonathan E. Hickman↗

NASA NTRS1973

Atmospheric oxidants

The ingredients which cause the air pollution are a mixture of oxides of organic matter (mostly nitrogen oxides and hydrocarbons) and ozone. Ozone, although considered one of the rare atmospheric gases, needs consideration in spacecraft design because of its chemical reaction (oxidation) with organic materials, especially rubber, which becomes hard and brittle under tension in a few minutes time. At the earth surface, a maximum of 60 parts per hundred million of oxidants composed of nitrogen oxides, hydrocarbons, sulphur dioxide, sulphur trioxides, peroxides, and ozone can be expected for 72 hours when smog occurs. A table representing distribution of ozone concentration with atmospheric altitude is included.

Daniels, G. E.↗

NASA NTRS2005

Study Uncovers Dirty Little Secret: Soil Emissions are Much-Bigger-than-Expected Component of Air Pollution

Nitrogen oxides produced by huge fires and fossil fuel combustion are a major component of air pollution. They are the primary ingredients in ground-level ozone, a pollutant harmful to human health and vegetation. But new research led by a University of Washington atmospheric scientist shows that, in some regions, nitrogen oxides emitted by the soil are much greater than expected and could play a substantially larger role in seasonal air pollution than previously believed. Nitrogen oxide emissions total more than 40 million metric tons worldwide each year, with 64 percent coming from fossil fuel combustion, 14 percent from burning and a surprising 22 percent from soil, said Lyatt Jaegle, a UW assistant professor of atmospheric sciences. The new research shows that the component from soil is about 70 percent greater than scientists expected. Instead of relying on scattered ground-based measurements of burning and combustion and then extrapolating a global total for nitrogen oxide emissions, the new work used actual observations recorded in 2000 by the Global Ozone Monitoring Experiment aboard the European Space Agency's European Remote Sensing 2 satellite. Nitrogen oxide emissions from fossil fuel combustion are most closely linked to major population centers and show up in the satellite's ozone-monitoring measurements of nitrogen dioxide, part of the nitrogen oxides family.

Stricherz, Vince↗

NASA NTRS1969

Removal of acid gases and oxides of nitrogen from space cabin atmospheres

Removal of acid gases and oxides of nitrogen from spacecraft cabin atmospheres at ambient temperatures

Bethea, R. M.↗

NASA NTRS1980

Ground cloud air quality effects

The effects of the ground cloud associated with launching of a large rocket on air quality are discussed. The ground cloud consists of the exhaust emitted by the rocket during the first 15 to 25 seconds following ignition and liftoff, together with a large quantity of entrained air, cooling water, dust and other debris. Immediately after formation, the ground cloud rises in the air due to the buoyant effect of its high thermal energy content. Eventually, at an altitude typically between 0.7 and 3 km, the cloud stabilizes and is carried along by the prevailing wind at that altitude. For the use of heavy lift launch vehicles small quantities of nitrogen oxides, primarily nitric oxide and nitrogen dioxide, are expected to be produced from a molecular nitrogen impurity in the fuel or liquid oxygen, or from entrainment and heating of ambient air in the hot rocket exhaust. In addition, possible impurities such as sulfur in the fuel would give rise to a corresponding amount of oxidation products such as sulfur dioxide.

Brubaker, K. L.↗

NASA NTRS1979

Low NO(x) heavy fuel combustor program

The 'low nitrogen oxides heavy fuel combustor' program is described. Main program objectives are to generate and demonstrate the technology required to develop durable gas turbine combustors for utility and industrial applications, which are capable of sustained, environmentally acceptable operation with minimally processed petroleum residual fuels. The program will focus on 'dry' reductions of oxides of nitrogen, improved combustor durability, and satisfactory combustion of minimally processed petroleum residual fuels. Other technology advancements sought include: fuel flexibility for operation with petroleum distillates, blends of petroleum distillates and residual fuels, and synfuels (fuel oils derived from coal or shale); acceptable exhaust emissions of carbon monoxide, unburned hydrocarbons, sulfur oxides and smoke; and retrofit capability to existing engines.

Lister, E.↗

DOE OSTI2021

Dioxygen Activation Kinetics over Distinct Cu Site Types in Cu-Chabazite Zeolites

Cu-exchanged zeolites activate dioxygen to form active sites for partial methane oxidation (PMO), nitrogen oxide decomposition, and carbon monoxide oxidation. Apparent rates of O 2 activation depend both on the intrinsic kinetics of distinct Cu site types and the distributions of such sites within a given zeolite, which depend on the density and arrangement of the framework Al atoms. In this work, we use hydrothermal synthesis methods to control the arrangement of framework Al sites in chabazite (CHA) zeolites and, in turn, the distinct Cu site types formed. Time-resolved in situ Raman spectroscopy reveals the kinetics of O 2 adsorption and activation within these well-defined Cu-CHA materials and the concomitant structural evolution of copper–oxygen (Cu x O y ) complexes, which are interpreted alongside Cu(I) oxidation kinetics extracted from in situ X-ray absorption spectroscopy (XAS). Raman spectra of several plausible Cu x O y species simulated using density functional theory suggest that experimental spectra (λ ex = 532 nm) capture the formation of mono(μ-oxo)dicopper species (ZCuOCuZ). Transient experiments show that the timescales required to form Cu x O y structures that no longer change in Raman spectra correspond to the durations of oxidative treatments that maximize CH 3 OH yields in stoichiometric PMO cycles (approximately 2 h). Yet, these periods extend well beyond the timescales for the complete conversion of the initial Cu(I) intermediates to their Cu(II) states (<0.3 h, reflected in X-ray absorption near edge spectroscopy spectra), which demonstrates that Cu x O y complexes continue to evolve structurally following rapid Cu(I) oxidation. The dependence of ZCuOCuZ formation rates on O 2 pressure, H 2 O pressure, and temperature is consistent with a mechanism in which ZCuOH reduces to form ZCu + sites that bind molecular oxygen and form ZCu-O 2 intermediates. Subsequent reaction with proximate ZCu + forms bridging peroxo dicopper complexes that cleave O–O bonds to form ZCuOCuZ in steps facilitated by water. These data and interpretations provide evidence for the chemical processes that link rapid and kinetically irrelevant Cu oxidation steps (frequently probed by XAS and UV–vis spectroscopy) to the relatively slow genesis of reactive Cu complexes that form CH 3 OH during PMO. In doing so, we reveal previously unrecognized complexities in the processes by which Cu ions in zeolites activate O 2 to form active Cu x O y complexes, which underscore the insight afforded by judicious combinations of experimental and theoretical techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Minimum conditions for accurate modeling of urea production via co-electrolysis

Co-electrolysis of carbon oxides and nitrogen oxides promise to simultaneously help restore the balance of the C and N cycles while producing valuable chemicals such as urea. However, co-electrolysis processes are still largely inefficient and numerous knowledge voids persist. Here, we provide a solid thermodynamic basis for modelling urea production via co-electrolysis. First, we determine the energetics of aqueous urea produced under electrochemical conditions based on experimental data, which enables an accurate assessment of equilibrium potentials and overpotentials. Next, we use density functional theory (DFT) calculations to model various co-electrolysis reactions producing urea. The calculated reaction free energies deviate significantly from experimental values for well-known GGA, meta-GGA and hybrid functionals. These deviations stem from errors in the DFT-calculated energies of molecular reactants and products. In particular, the error for urea is approximately -0.25 ± 0.10 eV. Finally, we show that all these errors introduce large inconsistencies in the calculated free-energy diagrams of urea production via co-electrolysis, such that gas-phase corrections are strongly advised.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗