Sensitivity of Modeled Soil NOx Emissions to Soil Moisture
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Daniel E. Huber↗
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Experimental Measurements and CFD Predictions of NOx Emissions from a Water-Cooled Rotating Detonation Engine
Paper presented at Turbo Expo 2023, Boston, Massachusetts, June 26-30, 2023.
Strakey, Peter↗
CFD Modeling of NOx Formation in a Rotating Detonation Engine
This paper focuses on the development and validation of a combustion model for Computational Fluid Dynamics (CFD) modeling of a Rotating Detonation Engines (RDE).
Strakey, Peter↗
Investigation of Ammonia Carrier Materials for Next Generation Ammonia Dosing System - CRADA 334 (Abstract)
Lean-burn gasoline and diesel engines can offer substantially higher fuel efficiency, good driving performance, and reduced carbon dioxide emission compared to stoichiometric gasoline engines. Various catalyst technologies have been developed to remove the pollutants from these engines. For example, a three-way catalyst (TWC) is used to remove hydrocarbons (HC), carbon monoxide (CO), and nitrogen oxides (NOx) from gasoline engines during the stoichiometric conditions. During the lean-burn conditions, a TWC or a diesel oxidation catalyst (DOC) is used to control HC and CO emissions. NOx is removed by either lean NOx trap catalyst (LNT) that can store NOx under lean conditions and reduce NOx under rich conditions, or selective catalytic reduction catalyst (SCR) that can selectively remove NOx with a reducing agent. Among the NOx reduction catalyst technologies, SCR offers a number of advantages, including excellent NOx reduction efficiency over a wide range of temperatures and overall lower system cost. In fact, the SCR technology using ammonia (NH3) as reductant has been proven effective and used commercially for the removal of NOx emissions from stationary sources since the 1970s. Currently, SCR is being used to meet the NOx emission standards for diesel engines in Europe and North America, and also being considered for meeting the future NOx emission standards for lean-burn gasoline engines. Because of the challenges associated with storage, handling and transportation of ammonia on a vehicle, aqueous urea solution (e.g., Diesel Exhaust Fluid, AdBlue) has been developed as ammonia storage compound for mobile applications. When the aqueous urea solution is sprayed into exhaust gas stream, urea is decomposed to release ammonia, which then reduces NOx over the downstream SCR catalyst. Although aqueous urea solution technology has enabled automakers and engine manufacturers to meet the current NOx emission standards, this process of releasing ammonia requires a hot exhaust gas and sufficient mixing, creating challenges for low temperature NOx emission control and aftertreatment system packaging. For these reasons, alternative technologies have been developed as ammonia sources (e.g., solid urea, ammonium carbamate, metal ammine chloride) during the past few years. These technologies promise more convenient handling and distribution of ammonia sources, and help maximize the low-temperature performance of SCR catalysts and reduce the overall system volume and weight. However, none of these alternative technologies can be successfully implemented without the industry consensus. Therefore, the USCAR SCR work group, which is comprised of representatives from GM, Ford, and Chrysler, has decided to investigate the potential alternative ammonia carriers, define common standard vehicle interfaces, and address personal and environmental safety concerns with part suppliers and chemical companies. Under this CRADA Project, USCAR and Battelle will investigate alternative ammonia carrier materials that are currently under development. Based on the data and information derived under the CRADA project, the USCAR SCR work group plans to build the consensus and make recommendations for the industry.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
Investigation of Ammonia Carrier Materials for Next Generation Ammonia Dosing System - CRADA 334 (Abstract)
Lean-burn gasoline and diesel engines can offer substantially higher fuel efficiency, good driving performance, and reduced carbon dioxide emission compared to stoichiometric gasoline engines. Various catalyst technologies have been developed to remove the pollutants from these engines. For example, a three-way catalyst (TWC) is used to remove hydrocarbons (HC), carbon monoxide (CO), and nitrogen oxides (NOx) from gasoline engines during the stoichiometric conditions. During the lean-burn conditions, a TWC or a diesel oxidation catalyst (DOC) is used to control HC and CO emissions. NOx is removed by either lean NOx trap catalyst (LNT) that can store NOx under lean conditions and reduce NOx under rich conditions, or selective catalytic reduction catalyst (SCR) that can selectively remove NOx with a reducing agent. Among the NOx reduction catalyst technologies, SCR offers a number of advantages, including excellent NOx reduction efficiency over a wide range of temperatures and overall lower system cost. In fact, the SCR technology using ammonia (NH3) as reductant has been proven effective and used commercially for the removal of NOx emissions from stationary sources since the 1970s. Currently, SCR is being used to meet the NOx emission standards for diesel engines in Europe and North America, and also being considered for meeting the future NOx emission standards for lean-burn gasoline engines. Because of the challenges associated with storage, handling and transportation of ammonia on a vehicle, aqueous urea solution (e.g., Diesel Exhaust Fluid, AdBlue) has been developed as ammonia storage compound for mobile applications. When the aqueous urea solution is sprayed into exhaust gas stream, urea is decomposed to release ammonia, which then reduces NOx over the downstream SCR catalyst. Although aqueous urea solution technology has enabled automakers and engine manufacturers to meet the current NOx emission standards, this process of releasing ammonia requires a hot exhaust gas and sufficient mixing, creating challenges for low temperature NOx emission control and aftertreatment system packaging. For these reasons, alternative technologies have been developed as ammonia sources (e.g., solid urea, ammonium carbamate, metal ammine chloride) during the past few years. These technologies promise more convenient handling and distribution of ammonia sources, and help maximize the low-temperature performance of SCR catalysts and reduce the overall system volume and weight. However, none of these alternative technologies can be successfully implemented without the industry consensus. Therefore, the USCAR SCR work group, which is comprised of representatives from GM, Ford, and Chrysler, has decided to investigate the potential alternative ammonia carriers, define common standard vehicle interfaces, and address personal and environmental safety concerns with part suppliers and chemical companies. Under this CRADA Project, USCAR and Battelle will investigate alternative ammonia carrier materials that are currently under development. Based on the data and information derived under the CRADA project, the USCAR SCR work group plans to build the consensus and make recommendations for the industry.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
The NO(x)-HNO3 System in the Lower Stratosphere: Insights from In Situ Measurements and Implications of the J(HNO3)-[OH] Relationship
During the 1997 Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) mission, simultaneous in situ observations of NOx and HOx radicals, their precursors, and the radiation field were obtained in the lower stratosphere. We use these observations to evaluate the primary mechanisms that control NOx-HNO3 exchange and to understand their control over the partitioning between NO2 and HNO3 in regions of continuous sunlight. We calculate NOx production (PNOx) and loss (LNOx) in a manner directly constrained by the in situ measurements and current rate constant recommendations, using approaches for representing albedo, overhead O3 and [OH] that reduce model uncertainty. We find a consistent discrepancy of 18% between modeled rates of NOx production and loss (LNOx = 1.18P(sub NOx)), which is within the measurement uncertainty of +/- 27%. The partitioning between NOx production processes is [HNO3 + OH (41 +/- 2)%; HNO3 + hv (59 +/- 2)%] and between NOx loss processes is [NO2 + OH, 90% to >97%; BrONO2 + H2O, 10% to <3%]. The steady-state description of NOx-HNO3 exchange reveals the significant influence of the tight correlation between the photolysis rate of HNO3 and [OH] established by in situ measurements throughout the lower stratosphere. Parametrizing this relationship, we find: (1) the steady-state value of [NO2](sub 24h-avg)/[HNO3] in the continuously sunlit, lower stratosphere is a function only of temperature and number density; and (2) the partitioning of NOx production between HNO3 + OH and HNO3 + hv is nearly constant throughout most of the lower stratosphere. We describe a methodology (functions of latitude, day, temperature, and pressure) for accurately predicting the steady-state value of [NO2](sub 24h-avg)/[HNO3] and the partitioning of NOx production within these regions. The results establish a metric to compare observations of [NO2](sub 24h-avg)/[HNO3] within the continuously sunlit region and provide a simple diagnostic for evaluating the accuracy of models that attempt to describe the coupled NOx-HOx photochemistry in the lower stratosphere.
Perkins, K. K.↗
Exploiting OMI NO2 Satellite Observations to Infer Fossil-fuel CO2 Emissions from U.S. Megacities
Fossil-fuel CO2 emissions and their trends in eight U.S. megacities during 2006–2017 are inferred by combining satellite-derived NOX emissions with bottom-up city-specific NOX-to-CO2 emission ratios. A statistical model is fit to a collection NO2 plumes observed from the Ozone Monitoring Instrument (OMI), and is used to calculate top-down NOX emissions. Decreases in OMI-derived NOX emissions are observed across the eight cities from 2006 to 2017 (−17% in Miami to −58% in Los Angeles), and are generally consistent with long-term trends of bottom-up inventories (−25% in Miami to −49% in Los Angeles), but there are some interannual discrepancies. City-specific NOX-to-CO2 emission ratios, used to calculate inferred CO2, are estimated through annual bottom-up inventories of NOX and CO2 emissions disaggregated to 1 × 1 km2 resolution. Over the study period, NOX-to-CO2 emission ratios have decreased by ~40% nationwide (−24% to −51% for our studied cities), which is attributed to a faster reduction in NOX when compared to CO2 due to policy regulations and fuel type shifts. Combining top-down NOX emissions and bottom-up NOX-to-CO2 emission ratios, annual fossil-fuel CO2 emissions are derived. Inferred OMI-based top-down CO2 emissions trends vary between +7% in Dallas to −31% in Phoenix. For 2017, we report annual fossil-fuel CO2 emissions to be: Los Angeles 113 ± 49 Tg/yr; New York City 144 ± 62 Tg/yr; and Chicago 55 ± 24 Tg/yr. A study in the Los Angeles area, using independent methods, reported a 2013–2016 average CO2 emissions rate of 104 Tg/yr and 120 Tg/yr, which suggests that the CO2 emissions from our method are in good agreement with other studies' top-down estimates. We anticipate future remote sensing instruments – with better spatial and temporal resolution – will better constrain the NOX-to-CO2 ratio and reduce the uncertainty in our method.
Ozone Monitoring Instrument (OMI)↗
Diagnostic methods for a high efficiency exhaust aftertreatment system
A method includes acquiring nitrogen oxide (NOx) data indicative of a first amount of NOx in an exhaust flow exiting an engine and a second amount of NOx in the exhaust flow exiting an exhaust aftertreatment system coupled to the engine where the exhaust aftertreatment system including a selective catalytic reduction (SCR) system including a SCR catalyst; determining a NOx conversion efficiency fault is present within the exhaust aftertreatment system based on the first amount of NOx and the second amount of NOx; monitoring an actual amount of NOx in the exhaust flow downstream of the SCR catalyst; determining an expected amount of NOx downstream of the SCR catalyst; and determining the SCR catalyst is responsible for the NOx conversion efficiency fault in response to the actual amount of NOx differing from the expected amount of NOx by more than a threshold amount.
Gupta, Aniket↗
Partitioning the LIS/OTD Lightning Climatological Dataset into Separate Ground and Cloud Flash Distributions
Presently, it is not well understood how to best model nitrogen oxides (NOx) emissions from lightning because lightning is highly variable. Peak current, channel length, channel altitude, stroke multiplicity, and the number of flashes that occur in a particular region (i.e., flash density) all influence the amount of lightning NOx produced. Moreover, these 5 variables are not the same for ground and cloud flashes; e.g., cloud flashes normally have lower peak currents, higher altitudes, and higher flash densities than ground flashes [see (Koshak, 2009) for additional details]. Because the existing satellite observations of lightning (Fig. 1) from the Lightning Imaging Sensor/Optical Transient Detector (LIS/OTD) do not distinguish between ground and cloud fashes, which produce different amounts of NOx, it is very difficult to accurately account for the regional/global production of lightning NOx. Hence, the ability to partition the LIS/OTD lightning climatology into separate ground and cloud flash distributions would substantially benefit the atmospheric chemistry modeling community. NOx indirectly influences climate because it controls the concentration of ozone and hydroxyl radicals in the atmosphere. The importance of lightning-produced NOx is empasized throughout the scientific literature (see for example, Huntrieser et al. 1998). In fact, lightning is the most important NOx source in the upper troposphere with a global production rate estimated to vary between 2 and 20 Tg (N)yr(sup -1) (Lee et al., 1997), with more recent estimates of about 6 Tg(N)yr(sup -1) (Martin et al., 2007). In order to make accurate predictions, global chemistry/climate models (as well as regional air quality modells) must more accurately account for the effects of lightning NOx. In particular, the NASA Goddard Institute for Space Studies (GISS) Model E (Schmidt et al., 2005) and the GEOS-CHEM global chemical transport model (Bey et al., 2001) would each benefit from a partitioning of the LIS/OTD lightning climatology. In this study, we introduce a new technique for retrieving the ground flash fraction in a set of N lightning observed from space and that occur within a specific latitude/longitude bin. The method is briefly described and applied to CONUS lightning that have already been partitioned into ground and cloud flashes using independent ground-based observations, in order to assess the accuracy of the retrieval method. The retrieval errors are encouragingly small.
Koshak, W. J.↗
Diagnostic methods for a high efficiency exhaust aftertreatment system
A method includes interpreting NOx data indicative of an amount of NOx exiting an engine and an amount of NOx exiting an exhaust aftertreatment system coupled to the engine, determining a NOx conversion efficiency fault is present based on the amount of NOx exiting the engine and the amount of NOx exiting the exhaust aftertreatment system, and determining at least one of a selective catalytic reduction (SCR) catalyst of the exhaust aftertreatment system and a diesel particulate filter having a coating of a SCR reaction catalyst (DPF-SCR) of the exhaust aftertreatment system are responsible for the NOx conversion efficiency fault based on at least one of a reductant slip amount and a NOx conversion value across at least one of the SCR catalyst and the DPF-SCR.
42 ENGINEERING↗
Reburning of Animal Waste Based Biomass with Coals for NO x Reduction, Part II: Dairy Biomass (DB) and Coal–DB Blends
Concentrated animal feeding operations (both slaughter and dairy cattle) lead to land, water, and air pollution if waste storage and handling systems are not effectively managed. At the same time, cattle biomass (CB), which includes both slaughter/feedlot biomass (FB) and dairy biomass (DB), have the potential to be a source of green energy at coal-fired power plants. Part I presented results on NOx reductions with pure FB or Coal: FB blends as reburn fuels. Part II deals with results from reburning with pure DB or Coal: DB blends as reburn fuels. A mixture of NG with a small amount of NH3 was used to generate the baseline NOx of 400–420 ppm (or 185–194 g/GJ). NOx emissions were found to be reduced by as much as 96% when reburning with FB. The effects of reburn fuel type, equivalence ratio (ER RBZ ) in the reburn zone, vitiated air, several injection configurations of reburn fuel and initial NO concentrations on NOx emissions were investigated. The ER RBZ shows a significant effect on the NOx reduction. The 20% heat input by reburning was the better operating condition for the long-term operation due to its ash production. The results reveal that reburn with DB fuels is an effective technology for NOx emission control when the initial NOx emission is higher than 275 ppm (or 127 g/GJ or 0.3 lb/MMBtu).
09 BIOMASS FUELS↗
Advanced Low Emissions Subsonic Combustor Study
Recent advances in commercial and military aircraft gas turbines have yielded significant improvements in fuel efficiency and thrust-to-weight ratio, due in large part to increased combustor operating pressures and temperatures. However, the higher operating conditions have increased the emission of oxides of nitrogen (NOx), which is a pollutant with adverse impact on the atmosphere and environment. Since commercial and military aircraft are the only important direct source of NOx emissions at high altitudes, there is a growing consensus that considerably more stringent limits on NOx emissions will be required in the future for all aircraft. In fact, the regulatory communities have recently agreed to reduce NOx limits by 20 percent from current requirements effective in 1996. Further reductions at low altitude, together with introduction of limits on NOx at altitude, are virtual certainties. In addition, the U.S. Government recently conducted hearings on the introduction of federal fees on the local emission of pollutants from all sources, including aircraft. While no action was taken regarding aircraft in this instance, the threat of future action clearly remains. In these times of intense and growing international competition, the U.S. le-ad in aerospace can only be maintained through a clear technological dominance that leads to a product line of maximum value to the global airline customer. Development of a very low NOx combustor will be essential to meet the future needs of both the commercial and military transport markets, if additional economic burdens and/or operational restrictions are to be avoided. In this report, Pratt & Whitney (P&W) presents the study results with the following specific objectives: Development of low-emissions combustor technologies for advances engines that will enter into service circa 2005, while producing a goal of 70 percent lower NOx emissions, compared to 1996 regulatory levels. Identification of solution approaches to barriers to the productization and economic viability of the low-emissions technologies. Preparation of these technologies to facilitate an annular rig high-pressure demonstration.
Smith, Reid↗
The plasma membrane-associated NADH oxidase of spinach leaves responds to blue light
The plasma membrane-associated NADH oxidase (NOX) of spinach leaf disks is characterized by oscillations in activity with a regular period length of ca. 24 min. Within a single population of plants exposed to light at the same time, NOX activities of all plants function synchronously. Exposure of plants transferred from darkness to blue light (495 nm, 2 min, 50 micromoles m-2 s-1) resulted in a complex response pattern but with a new maximum in the rate of NOX activity 36 (24+12) min after illumination and then with maxima in the rate of NOX activity every 24 min thereafter. Transient maxima in NOX activity were observed as well after 9.3 + /- 1.4 and 20.7 +/- 2.1 min. The blue light response differed from the response to red (650 nm, 10 min, 50 micromoles m-2 s-1) or white light where activity maxima were initiated 12 min after the light exposure followed by maxima every 24 min thereafter. Green or yellow light was ineffective. The light response was independent of the time in the 24-min NOX cycle when the light was given. The net effects of blue and red light were ultimately the same with a new maximum in the rate of NOX activity at 12+24=36 min (and every 24 min thereafter), but the mechanisms appear to be distinct.
NASA Discipline Cell Biology↗
An Overview of the Impact of Energetic Particle Precipitation on the Mesosphere and Stratosphere
Energetic precipitating particles (EPPs) can cause significant constituent changes in the polar mesosphere and stratosphere (middle atmosphere) during certain periods. Both protons and electrons can influence the polar middle atmosphere through ionization and dissociation processes. EPPs can enhance HOx (H, OH, HO2) through the formation of positive ions followed by complex ion chemistry and NOx (N, NO, NO2) through the dissociation of molecular nitrogen. The HO, increases can lead to ozone destruction in the mesosphere and upper stratosphere via several catalytic loss cycles. Such middle atmospheric HOx,-caused ozone loss is rather short-lived due to the relatively short lifetime (hours) of the HOx constituents. The HOx,-caused ozone depletion has been observed during several solar proton events (SPEs) in the past 40 years. HOx enhancements due to SPEs were confirmed by observations in the past solar cycle. A number of modeling studies have been undertaken over this time period that show predictions of enhanced HO, accompanied by decreased ozone due to energetic particles. The NO, family has a longer lifetime than the HOx family and can also lead to catalytic ozone destruction. EPP-caused enhancements of the NOx family can affect ozone promptly, if produced in the stratosphere, or subsequently, if produced in the 1ow.er thermosphere or mesosphere and transported to the stratosphere. NOx enhancements due to auroral electrons, medium and high energy electrons, relativistic electron precipitation (REP) events, and SPEs have been measured and/or modeled for decades Only a small number of SPEs (less than 10) in each solar cycle have sufficient flux of high energy protons (greater than 30 MeV) to produce a significant amount of NOx directly in the stratosphere to cause a measurable ozone destruction. Very high energy electrons (greater than 1500 keV) during REP events can also produce NOx directly in the stratosphere, however, the frequency and intensity of these electrons is uncertain. Indirect stratospheric EPP effects result when NO, is produced in the mesosphere and lower thermosphere and transported to the stratosphere during the late fall or winter. Such EPP-produced NOx may last up to months beyond its initial production. This EPP-produced mesospheric and lower thermospheric NOx primarily results from auroral electrons (approx. 1- 30 keV), medium- and high-energy electrons (approx. 30-1500 keV), and medium energy protons (approx. 1-30 MeV). The EPP-caused direct and indirect effects on the stratosphere are important in the polar regions during particular years, especially near solar maximum. This talk will attempt to provide an overview of several of the EPP-related important processes and their impact on the mesosphere and stratosphere. Much progress has been made in this field in the past several years and it is anticipated that other workshop participants will address aspects of this topic in their presentations.
Jackman, Charles H.↗
Reactive Nitrogen, Ozone and Ozone Production in the Arctic Troposphere and the Impact of Stratosphere-Troposphere Exchange
We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of approximately 60 ppbv and NOx of approximately 25 pptv throughout spring and summer with CO decreases from approximately 145 ppbv in spring to approximately 100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140-160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (approximately 800 pptv in spring and approximately 1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of approximately 120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.
Liang, Q.↗
The Influence of Ozone Precursor Emissions from Four World Regions on Tropospheric Composition and Radiative Climate Forcing
Ozone (O3) precursor emissions influence regional and global climate and air quality through changes in tropospheric O3 and oxidants, which also influence methane (CH4) and sulfate aerosols (SO4 (sup 2-)). We examine changes in the tropospheric composition of O3, CH4, SO4 (sup 2-) and global net radiative forcing (RF) for 20% reductions in global CH4 burden and in anthropogenic O3 precursor emissions (NOx, NMVOC, and CO) from four regions (East Asia, Europe and Northern Africa, North America, and South Asia) using the Task Force on Hemispheric Transport of Air Pollution Source-Receptor global chemical transport model (CTM) simulations, assessing uncertainty (mean plus or minus 1 standard deviation) across multiple CTMs. We evaluate steady state O3 responses, including long-term feedbacks via CH4. With a radiative transfer model that includes greenhouse gases and the aerosol direct effect, we find that regional NOx reductions produce global, annually averaged positive net RFs (0.2 plus or minus 0.6 to 1.7 2 mWm(sup -2)/Tg N yr(sup -1), with some variation among models. Negative net RFs result from reductions in global CH4 (-162.6 plus or minus 2 mWm(sup -2) for a change from 1760 to 1408 ppbv CH4) and regional NMVOC (-0.4 plus or minus 0.2 to 0.7 plus or minus 0.2 mWm(sup -2)/Tg C yr(sup -1) and CO emissions (-0.13 plus or minus 0.02 to -0.15 plus or minus 0.02 mWm(sup-2)/Tg CO yr(sup-1). Including the effect of O3 on CO2 uptake by vegetation likely makes these net RFs more negative by -1.9 to- 5.2 mWm(sup -2)/Tg N yr(sup -1), -0.2 to -0.7 mWm(sup -2)/Tg C yr(sup -1), and -0.02 to -0.05 mWm(sup -2)/ Tg CO yr(sup -1). Net RF impacts reflect the distribution of concentration changes, where RF is affected locally by changes in SO4 (sup -2), regionally to hemispherically by O3, and globally by CH4. Global annual average SO4 2 responses to oxidant changes range from 0.4 plus or minus 2.6 to -1.9 plus or minus 1.3 Gg for NOx reductions, 0.1 plus or minus 1.2 to -0.9 plus or minus 0.8 Gg for NMVOC reductions, and -0.09 plus or minus 0.5 to -0.9 plus or minus 0.8 Gg for CO reductions, suggesting additional research is needed. The 100-year global warming potentials (GWP(sub 100)) are calculated for the global CH4 reduction (20.9 plus or minus 3.7 without stratospheric O3 or water vapor, 24.2 plus or minus 4.2 including those components), and for the regional NOx, NMVOC, and CO reductions (18.7 plus or minus 25.9 to 1.9 plus or minus 8.7 for NOx, 4.8 plus or minus 1.7 to 8.3 plus or minus 1.9 for NMVOC, and 1.5 plus or minus 0.4 to 1.7 plus or minus 0.5 for CO). Variation in GWP(sub 100) for NOx, NMVOC, and CO suggests that regionally specific GWPs may be necessary and could support the inclusion of O3 precursors in future policies that address air quality and climate change simultaneously. Both global net RF and GWP100 are more sensitive to NOx and NMVOC reductions from South Asia than the other three regions.
ozone↗
Analysis of Ion-Exchanged ZSM-5, BEA, and SSZ-13 Zeolite Trapping Materials under Realistic Exhaust Conditions
An industry-defined evaluation protocol was used to evaluate the hydrocarbon trapping (HCT) and passive NOx adsorption (PNA) potential for BEA, ZSM-5, and SSZ-13 zeolites with ion-exchanged Pd or Ag. All materials underwent 700 °C degreening prior to exposure to an industry-derived protocol gas stream, which included NOx, ethylene, toluene, and decane as measured trapping species as well as common exhaust gasses CO, H2O, O2, CO2, and H2. Evaluation showed that BEA and ZSM-5 zeolites were effective at trapping hydrocarbons (HCs), as saturation was not achieved after 30 min of exposure. SSZ-13 also stored HCs but was only able to adsorb 20–25% compared to BEA and ZSM-5. The presence of Ag or Pd did not impact the overall HC uptake, particularly in the first three minutes. Pd/zeolites had significantly lower THC release temperature, and it aided in the conversion of the released HCs; Ag only had a moderate effect in both areas. With respect to NOx adsorption, the level of uptake was much lower than HCs on all samples, and Ag or Pd was necessary with Pd being notably more effective. Additionally, only Pd/ZSM-5 and Pd/SSZ-13 continue to store a portion of the NOx above 200 °C, which is critical for downstream selective catalytic NOx reduction (SCR). Hydrothermal aging (800 °C for 50 h) of a subset of the samples were performed: BEA, Pd/BEA, ZSM-5, Pd/ZSM-5, and Pd/SSZ-13. There was a minimal effect on the HC storage, ~10% reduction in capacity with no effect on release temperature; however, only Pd/SSZ-13 showed significant NOx storage after aging.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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↗