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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
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 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 OSTI2022

Historical Emissions - shipping emission perturbation data

Version of previously released anthropogenic SO2 emissions data re-generated with altered spatial distributions for shipping emissions for use in the Emissions-MIP model inter-comparison project. Also included are 30% and 60% global reductions in shipping SO2 emissions.

Ahsan, Hamza↗
DOE OSTI2025

The Co-Firing of Pine Biomass and Waste Coal in 100 and 600 MW Power Plants: A Sustainable Approach to Reduce GHG Emissions

Climate change is a global issue that has gained much attention recently. Co-firing biomass with coal/waste coal reduces the electricity sector’s GHG emissions sustainably. This study uses commercial software to model waste coal and biomass co-firing in 100 MW and 600 MW power plants. The objective is to assess the effects of fluid types (subcritical and supercritical), plant capacities (100 MW and 600 MW), boiler types (pulverized coal and circulating fluidized bed boilers), biomass and waste coal co-firing ratios (0:100, 20:80, 40:60, 60:40, 80:20, and 100:0), and carbon capture and storage efficiencies (0%, 90%, 95%, and 97%) on performance parameters such as net plant efficiency, heat rate, net plant CO2 and SO2, and particulate matter emissions. The feedstocks selected for this investigation include anthracite waste coal and loblolly pine biomass. As the biomass fraction increases from 0% to 100%, co-fired power plants net efficiency increases by 3–8%. Supercritical plants had a 6% higher net plant efficiency than the subcritical plants. The study found that the biomass’s high heating value decreased the fuel flow rate and reduced plant CO2 emissions by 10–16%. With 100% biomass power plant feed and 90% carbon capture and storage efficiency, CO2 emissions drop by 83% and SO2 and PM emissions drop to zero.

Bhoi, Prakashbhai R. (ORCID:0000000333104888)↗
DOE OSTI2014

Sensitivity of Tropospheric Chemical Composition to Halogen-Radical Chemistry Using a Fully Coupled Size-Resolved Multiphase Chemistry-Global Climate System: Halogen Distributions, Aerosol Composition, and Sensitivity of Climate-Relevant Gases

Observations and model studies suggest a significant but highly non-linear role for halogens, primarily Cl and Br, in multiphase atmospheric processes relevant to tropospheric chemistry and composition, aerosol evolution, radiative transfer, weather, and climate. The sensitivity of global atmospheric chemistry to the production of marine aerosol and the associated activation and cycling of inorganic Cl and Br was tested using a size-resolved multiphase coupled chemistry/global climate model (National Center for Atmospheric Research’s Community Atmosphere Model (CAM); v3.6.33). Simulation results showed strong meridional and vertical gradients in Cl and Br species. The simulation reproduced most available observations with reasonable confidence permitting the formulation of potential mechanisms for several previously unexplained halogen phenomena including the enrichment of Br- in submicron aerosol, and the presence of a BrO maximum in the polar free troposphere. However, simulated total volatile Br mixing ratios were generally high in the troposphere. Br in the stratosphere was lower than observed due to the lack of long-lived organobromine species in the simulation. Comparing simulations using chemical mechanisms with and without reactive Cl and Br species demonstrated a significant temporal and spatial sensitivity of primary atmospheric oxidants (O3, HOx, NOx), CH4, and non-methane hydrocarbons (NMHC’s) to halogen cycling. Simulated O3 and NOx were globally lower (65% and 35%, respectively, less in the planetary boundary layer based on median values) in simulations that included halogens. Globally, little impact was seen in SO2 and non-sea-salt SO42- processing due to halogens. Significant regional differences were evident: The lifetime of nss-SO42- was extended downwind of large sources of SO2. The burden and lifetime of DMS (and its oxidation products) were lower by a factor of 5 in simulations that included halogens, versus those without, leading to a 20% reduction in nss-SO42- in the southern hemisphere planetary boundary layer based on median values.

chemical composition↗
DOE OSTI2022

Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO 2 regimes

Abstract. The atmospheric oxidation of dimethyl sulfide (DMS) represents a major natural source of atmospheric sulfate aerosols. However, there remain large uncertainties in our understanding of the underlying chemistry that governs the product distribution and sulfate yield from DMS oxidation. Here, chamber experiments were conducted to simulate gas-phase OH-initiated oxidation of DMS under a range of reaction conditions. Most importantly, the bimolecular lifetime (τbi) of the peroxy radical CH3SCH2OO was varied over several orders of magnitude, enabling the examination of the role of peroxy radical isomerization reactions on product formation. An array of analytical instruments was used to measure nearly all sulfur-containing species in the reaction mixture, and results were compared with a near-explicit chemical mechanism. When relative humidity was low, “sulfur closure” was achieved under both high-NO (τbi<0.1 s) and low-NO (τbi>10 s) conditions, though product distributions were substantially different in the two cases. Under high-NO conditions, approximately half the product sulfur was in the particle phase, as methane sulfonic acid (MSA) and sulfate, with most of the remainder as SO2 (which in the atmosphere would eventually oxidize to sulfate or be lost to deposition). Under low-NO conditions, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), formed from CH3SCH2OO isomerization, dominates the sulfur budget over the course of the experiment, suppressing or delaying the formation of SO2 and particulate matter. The isomerization rate constant of CH3SCH2OO at 295 K is found to be 0.13±0.03 s−1, in broad agreement with other recent laboratory measurements. The rate constants for the OH oxidation of key first-generation oxidation products (HPMTF and methyl thioformate, MTF) were also determined (kOH+HPMTF=2.1×10-11 cm3 molec.−1 s−1, kOH+MTF=1.35×10-11 cm3 molec.−1 s−1). Product measurements agree reasonably well with mechanistic predictions in terms of total sulfur distribution and concentrations of most individual species, though the mechanism overpredicts sulfate and underpredicts MSA under high-NO conditions. Lastly, results from high-relative-humidity conditions suggest efficient heterogenous loss of at least some gas-phase products.

Ye, Qing (ORCID:0000000337978988)↗
DOE OSTI2024

Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism

Abstract. The oxidation of dimethyl sulfide (DMS) in the marine atmosphere represents an important natural source of non-sea-salt sulfate aerosol, but the chemical mechanisms underlying this process remain uncertain. While recent studies have focused on the role of the peroxy radical isomerization channel in DMS oxidation, this work revisits the impact of the other channels (OH addition and OH abstraction followed by bimolecular RO2 reaction) on aerosol formation from DMS. Due to the presence of common intermediate species, the oxidation of dimethyl sulfoxide (DMSO) and dimethyl disulfide (DMDS) can shed light on these two DMS reaction channels; they are also both atmospherically relevant species in their own right. This work examines the OH oxidation of DMSO and DMDS, using chamber experiments monitored by chemical ionization mass spectrometry and aerosol mass spectrometry to study the full range of sulfur-containing products across a range of NO concentrations. The oxidation of both compounds is found to lead to rapid aerosol formation (which does not involve the intermediate formation of SO2), with a substantial fraction (14 %–47 % S yield for DMSO and 5 %–21 % for DMDS) of reacted sulfur ending up in the particle phase and the highest yields observed under elevated NO conditions. Aerosol is observed to consist mainly of sulfate, methanesulfonic acid, and methanesulfinic acid. In the gas phase, the NOx dependence of several products, including SO2 and S2-containing organosulfur species, suggest reaction pathways not included in current mechanisms. Based on the commonalities with the DMS oxidation mechanism, DMSO and DMDS results are used to reconstruct DMS aerosol yields; these reconstructions roughly match DMS aerosol yield measurements from the literature but differ in composition, underscoring remaining uncertainties in sulfur chemistry. This work indicates that both the abstraction and addition channels contribute to rapid aerosol formation from DMS and highlights the need for more study into the fate of small sulfur radical intermediates (e.g., CH3S, CH3SO2, and CH3SO3) that are thought to play central roles in the DMS oxidation mechanism.

Goss, Matthew B. (ORCID:0000000226885463)↗
DOE OSTI2024

HSW-V v1.0: localized injections of interactive volcanic aerosols and their climate impacts in a simple general circulation model

Abstract. A new set of standalone parameterizations is presented for simulating the injection, evolution, and radiative forcing by stratospheric volcanic aerosols against an idealized Held–Suarez–Williamson (HSW) atmospheric background in the Energy Exascale Earth System Model version 2 (E3SMv2). In this model configuration (HSW with enabled volcanism, HSW-V), sulfur dioxide (SO2) and ash are injected into the atmosphere with a specified profile in the vertical, and they proceed to follow a simple exponential decay. The SO2 decay is modeled as a perfect conversion to a long-living sulfate aerosol which persists in the stratosphere. All three species are implemented as tracers in the model framework and are transported by the dynamical core's advection algorithm. The aerosols contribute simultaneously to local heating of the stratosphere and cooling of the surface by a simple plane-parallel Beer–Lambert law applied on two zonally symmetric radiation broadbands in the longwave and shortwave ranges. It is shown that the implementation parameters can be tuned to produce realistic temperature anomaly signatures of large volcanic events. In particular, results are shown for an ensemble of runs that mimic the volcanic eruption of Mt. Pinatubo in 1991. The design requires no coupling to microphysical subgrid-scale parameterizations and thus approaches the computational affordability of prescribed aerosol forcing strategies. The idealized simulations contain a single isolated volcanic event against a statistically uniform climate, where no background aerosols or other sources of externally forced variability are present. HSW-V represents a simpler-to-understand tool for the development of climate source-to-impact attribution methods.

Hollowed, Joseph P. (ORCID:0000000286581672)↗
DOE OSTI2026

Local Air Quality Impacts of a Peak-Shaving Diesel Generator Unit in Waynesville, North Carolina

The Waynesville Electric Department in Waynesville, North Carolina, operates a 2,000-kW diesel generator with a 4% capacity factor, emitting less than 1 ton annually of PM2.5, VOCs, carbon monoxide (CO), and sulfur dioxide (SO2), and approximately 1.8 tons of NO. The National Laboratory of the Rockies (NLR) conducted high-resolution, near-source air-quality modeling to evaluate the generator's impacts. Results indicate minimal effects on ambient pollutant concentrations: annual PM2.5 increases are below 0.0004 microgrm/m3 for local census tracts, while CO and SO2 levels increase by less than 0.00004 ppm and 0.0002 ppb, respectively. Estimated annual premature mortality attributable to PM2.5 exposure is less than 0.001 cases across Haywood County, with an associated economic impact of approximately $12,000. This report complements a separate technoeconomic analysis to inform Waynesville's investment strategies for demand reduction.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2017

Field Testing of Cryogenic Carbon Capture

Sustainable Energy Solutions has been developing Cryogenic Carbon Capture™ (CCC) since 2008. In that time two processes have been developed, the External Cooling Loop and Compressed Flue Gas Cryogenic Carbon Capture processes (CCC ECL™ and CCC CFG™ respectively). The CCC ECL™ process has been scaled up to a 1TPD CO2 system. In this process the flue gas is cooled by an external refrigerant loop. SES has tested CCC ECL™ on real flue gas slip streams from subbituminous coal, bituminous coal, biomass, natural gas, shredded tires, and municipal waste fuels at field sites that include utility power stations, heating plants, cement kilns, and pilot-scale research reactors. The CO2 concentrations from these tests ranged from 5 to 22% on a dry basis. CO2 capture ranged from 95-99+% during these tests. Several other condensable species were also captured including NO2, SO2 and PMxx at 95+%. NO was also captured at a modest rate. The CCC CFG™ process has been scaled up to a .25 ton per day system. This system has been tested on real flue gas streams including subbituminous coal, bituminous coal and natural gas at field sites that include utility power stations, heating plants, and pilot-scale research reactors. CO2 concentrations for these tests ranged from 5 to 15% on a dry basis. CO2 capture ranged from 95-99+% during these tests. Several other condensable species were also captured including NO2, SO2 and PMxx at 95+%. NO was also captured at 90+%. Hg capture was also verified and the resulting effluent from CCC CFG™ was below a 1ppt concentration. This paper will focus on discussion of the capabilities of CCC, the results of field testing and the future steps surrounding the development of this technology.

20 FOSSIL-FUELED POWER PLANTS↗
NASA NTRS1975

Reaction of sulfur dioxide with modified 440C, studied by Auger electron spectroscopy and depth profiling

Auger electron spectroscopy and sputtering were used to study the interaction of SO2 with modified 440C, which is a nominally 77-wt%-Fe, 14-wt%-Cr, and 4-wt%-Mo bearing steel with C, S, Si, Ni, V, P, and Mn making up the balance. The sample was polycrystalline. Three temperatures were used: room temperature, 500 C, and 600 C. The reaction time was varied from 30 minutes to 2 hours. A surface cleaned of oxides was the starting point for each reaction. For reactions at 500 C, the major constituents Cr, O, Fe, and S were present in the surface film. At 600 C, the principal constituents of the film were Cr, O, and S with no Fe present. Therefore, a transition in film composition occurred between 500 and 600 C. Oxides were the primary constituents of the films at both temperatures. Room-temperature reactions indicated that SO2 adsorbed dissociatively, with approximately equal quantities of S and O on the surface. For the same reaction time (1 hr) and pressure, a strong temperature dependence of film thickness was observed. The film formed at 600 C was approximately seven times thicker than that formed at 500 C.

Ferrante, J.↗
NASA NTRS1975

Sensitivity of gas filter correlation instrument to variations in optical balance

A computer program was used to simulate the response of the Gas Filter Correlation Radiometer (GFCR) to changing pollutant levels of CO, SO2, CH4, and NH3 in two model atmospheres. Positive and negative deviations of tau sub alpha of magnitudes 0.01, 0.1, and 1 percent were imposed upon the simulation and the resulting deviations in inferred concentrations were determined. For the CO, CH4, and the higher pressure cell of the NH3 channel, the deviations are less than + or - 12 percent for deviations in tau sub alpha of + or - 0.1 percent, but increase to significantly higher values for larger deviations. For the lower pressure cell of NH3 and for SO2, the deviations in inferred concentration begin to rise sharply between 0.01 and 0.1 percent deviation in tau sub alpha, suggesting that a tighter control on tau sub alpha may be required for these channels.

Orr, H. D., III↗
NASA NTRS1975

A theoretical/experimental program to develop active optical pollution sensors: Quantitative remote Raman lidar measurements of pollutants from stationary sources

Typical pollutant gas concentrations at the stack exits of stationary sources can be estimated to be about 500 ppm under the present emission standards. Raman lidar has a number of advantages which makes it a valuable tool for remote measurements of these stack emissions. Tests of the Langley Research Center Raman lidar at a calibration tank indicate that night measurements of SO2 concentrations and stack opacity are possible. Accuracies of 10 percent are shown to be achievable from a distance of 300 m within 30 min integration times for 500 ppm SO2 at the stack exits. All possible interferences were examined quantitatively (except for the fluorescence of aerosols in actual stack emissions) and found to have negligible effect on the measurements. An early test at an instrumented stack is strongly recommended.

Poultney, S. K.↗
NASA NTRS1977

Gaseous sodium sulfate formation in flames and flowing gas environments

Formation of Na2SO4(g) in flames and hot flowing gas systems was studied by high pressure, free-jet expansion, modulated molecular beam mass spectrometric sampling. Fuel-lean CH4-O2 flames doped with SO2, H2O and NaCl yielded the gaseous Na2SO4 molecule in residence times of less than one millisecond. Intermediate species NaSO2(g) and NaSO3(g) were also observed and measured. Composition profiles were obtained for all reaction products. Nonflame flowing gas experiments showed that Na2SO4 and NaSO3 gaseous molecules were formed at 1140 C in mixtures of O2, H2O(g), SO2 and NaCl(g). Experimental results are compared with calculated equilibrium thermodynamic predictions.

Stearns, C. A.↗
NASA NTRS1977

Atomic and molecular fluorescence as a stratospheric species monitor

The results of an investigation are presented evaluating the potential of atomic and molecular fluorescence as a stratospheric monitor of the concentrations of any one of 18 minor species: Cl, Cl2, ClO, ClO2, CO, H2, HCHO, HCl, HNO2, HNO3, H2S, NH3, NO, NO2, N2O, O, OH, and SO2. All spectral regions from the vacuum ultraviolet through the infrared were included. It was found that suitable systems can be constructed for the stratospheric monitoring of CO (5 ppb), NO2 (less than 1 ppb), OH (0.2 ppt), and O (50-200 ppt). The fluorescence sensitivities for Cl (0.5-1.0 ppt), H2 (0.2 ppm at 10 torr) and SO2 (1-10 ppb) are marginally insufficient with current technology.

Schofield, K.↗
NASA NTRS1977

Gaseous sodium sulfate formation in flames and flowing gas environments

Formation of Na2SO4(g) in flames and hot flowing gas systems was studied by high pressure, free-jet expansion, modulated molecular beam mass spectrometric sampling. Fuel-lean CH4-O2 flames doped with SO2, H2O and NaCl yielded the gaseous Na2SO4 molecule in residence times of less than one millisecond. Intermediate species NaSO2(g) and NaSO3(g) were also observed and measured. Composition profiles were obtained for all reaction products. Non-flame flowing gas experiments showed that Na2SO4 and NaSO3 gaseous molecules were formed at 1140 C in mixtures of O2, H2O(g), SO2 and and NaCl(g). Experimental results are compared with calculated equilibrium thermodynamic predictions.

Stearns, C. A.↗
NASA NTRS1977

Fluidized bed combustor modeling

A general mathematical model for the prediction of performance of a fluidized bed coal combustor (FBC) is developed. The basic elements of the model consist of: (1) hydrodynamics of gas and solids in the combustor; (2) description of gas and solids contacting pattern; (3) kinetics of combustion; and (4) absorption of SO2 by limestone in the bed. The model is capable of calculating the combustion efficiency, axial bed temperature profile, carbon hold-up in the bed, oxygen and SO2 concentrations in the bubble and emulsion phases, sulfur retention efficiency and particulate carry over by elutriation. The effects of bed geometry, excess air, location of heat transfer coils in the bed, calcium to sulfur ratio in the feeds, etc. are examined. The calculated results are compared with experimental data. Agreement between the calculated results and the observed data are satisfactory in most cases. Recommendations to enhance the accuracy of prediction of the model are suggested.

Horio, M.↗
NASA NTRS1977

Electrophoresis pattern of serum from mice exposed to different concentrations of sulfur dioxide

Three day old mice were continuously exposed to sulphur dioxide concentrations at 0ppm, 0.05ppm, 0.15ppm and 1ppm for eight weeks. At the end of the experiment, blood samples were collected and centrifuged for electrophoresis studies of the serum in 5 percent acrylamide gel. The length of bands of different serum proteins from the SO2 exposed mice was at a variance as compared with the length of bands from the control exposed mice and alpha-1 band seems to be missing from the serum of SO2 exposed mice.

Singh, J.↗