scholarly journals Calibration of an airborne HO<sub>X</sub> instrument using the All Pressure Altitude based Calibrator for HO<sub>X</sub> Experimentation (APACHE)

2019 ◽  
Author(s):  
Daniel Marno ◽  
Cheryl Ernest ◽  
Korbinian Hens ◽  
Umar Javed ◽  
Thomas Klimach ◽  
...  
Keyword(s):  
Water Vapor ◽  
Atmospheric Chemistry ◽  
Ambient Pressure ◽  
Chemical Species ◽  
External Pressure ◽  
Controlled Environment ◽  
Instrument Response ◽  
Flow Speeds ◽  
Instrument Sensitivity ◽  
Pressure Altitude

Abstract. Laser induced fluorescence (LIF) is a widely used technique for both laboratory-based and ambient atmospheric chemistry measurements. However, LIF instruments require calibrations in order to translate instrument response into concentrations of chemical species. Calibration of LIF instruments measuring OH and HO2 (HOX), typically involves the photolysis of water vapor by 184.9 nm light thereby producing quantitative amounts of OH and HO2. For ground-based systems HOX instruments, this method of calibration is done at one pressure (typically ambient pressure) at the instrument inlet. However, airborne HOX instruments can experience varying cell pressures, internal residence times, temperatures, and humidity during flight. Therefore, replication of such variances when calibrating are essential to acquire the appropriate sensitivities. This requirement resulted in the development of the APACHE (All Pressure Altitude-based Calibrator for HOX Experimentation) chamber. It utilizes photolysis of water vapor, but has the additional ability to alter the pressure at the inlet of the HOX instrument thus relating instrument sensitivity to the external pressure ranges experienced during flight (275 to 1000 mbar). Measurements supported by COMSOL multiphysics and its computational fluid dynamics calculations revealed that, for all pressures explored in this study, APACHE is capable of initializing homogenous flow and maintain near uniform flow speeds across the internal cross-section of the chamber. This reduces the uncertainty regarding average exposure times across the mercury (Hg) UV ring lamp. Two different actinometrical approaches characterized the APACHE UV ring lamp flux as 6.3 x 1014 (± 0.9 x 1014) s-1 depending on pressure. Data presented in this study are the first direct calibrations, performed in a controlled environment using APACHE of an airborne HOX system instrument.

scholarly journals Calibration of an airborne HO<sub><i>x</i></sub> instrument using the All Pressure Altitude-based Calibrator for HO<sub><i>x</i></sub> Experimentation (APACHE)

2020 ◽  
Vol 13 (5) ◽  
pp. 2711-2731
Author(s):  
Daniel Marno ◽  
Cheryl Ernest ◽  
Korbinian Hens ◽  
Umar Javed ◽  
Thomas Klimach ◽  
...  
Keyword(s):  
Water Vapor ◽  
Atmospheric Chemistry ◽  
Ambient Pressure ◽  
Chemical Species ◽  
External Pressure ◽  
Ozone Production ◽  
Flow Speeds ◽  
Gas Expansion ◽  
Pressure Altitude ◽  
Ground Calibration

Abstract. Laser-induced fluorescence (LIF) is a widely used technique for both laboratory-based and ambient atmospheric chemistry measurements. However, LIF instruments require calibrations in order to translate instrument response into concentrations of chemical species. Calibration of LIF instruments measuring OH and HO2 (HOx) typically involves the photolysis of water vapor by 184.9 nm light, thereby producing quantitative amounts of OH and HO2. For ground-based HOx instruments, this method of calibration is done at one pressure (typically ambient pressure) at the instrument inlet. However, airborne HOx instruments can experience varying cell pressures, internal residence times, temperatures, and humidity during flight. Therefore, replication of such variances when calibrating in the lab is essential to acquire the appropriate sensitivities. This requirement resulted in the development of the APACHE (All Pressure Altitude-based Calibrator for HOx Experimentation) chamber to characterize the sensitivity of the airborne LIF-FAGE (fluorescence assay by gas expansion) HOx instrument, HORUS, which took part in an intensive airborne campaign, OMO-Asia 2015. It utilizes photolysis of water vapor but has the additional ability to alter the pressure at the nozzle of the HORUS instrument. With APACHE, the HORUS instrument sensitivity towards OH (26.1–7.8 cts s−1 pptv−1 mW−1, ±22.6 % 1σ; cts stands for counts by the detector) and HO2 (21.2–8.1 cts s−1 pptv−1 mW−1, ±22.1 % 1σ) was characterized to the external pressure range at the instrument nozzle of 227–900 mbar. Measurements supported by a computational fluid dynamics model, COMSOL Multiphysics, revealed that, for all pressures explored in this study, APACHE is capable of initializing a homogenous flow and maintaining near-uniform flow speeds across the internal cross section of the chamber. This reduces the uncertainty regarding average exposure times across the mercury (Hg) UV ring lamp. Two different actinometrical approaches characterized the APACHE UV ring lamp flux as 6.37×1014(±1.3×1014) photons cm−2 s−1. One approach used the HORUS instrument as a transfer standard in conjunction with a calibrated on-ground calibration system traceable to NIST standards, which characterized the UV ring lamp flux to be 6.9(±1.1)×1014 photons cm−2 s−1. The second approach involved measuring ozone production by the UV ring lamp using an ANSYCO O3 41 M ozone monitor, which characterized the UV ring lamp flux to be 6.11(±0.8)×1014 photons cm−2 s−1. Data presented in this study are the first direct calibrations of an airborne HOx instrument, performed in a controlled environment in the lab using APACHE.

Effect of Water Vapor and SOx in Air on the Cathodes of Solid Oxide Fuel Cells

2007 ◽  
Vol 1041 ◽  
Author(s):  
Seon Hye Kim ◽  
Toshihiro Ohshima ◽  
Yusuke Shiratori ◽  
Kohei Itoh ◽  
Kazunari Sasaki
Keyword(s):  
Water Vapor ◽  
Solid Oxide Fuel Cells ◽  
Degradation Mechanism ◽  
Chemical Species ◽  
Cell Voltage ◽  
Ambient Air ◽  
Open Circuit ◽  
Constant Current ◽  
Constant Current Density

AbstractAmbient air is used as an oxygen source in SOFCs to be commercialized. Various chemical species which can lead to poisoning of SOFC cathodes are included as minor constitutions in air, such as water vapor, SOx, NOx and NaCl etc. However, their effects on the cathode performance have not yet well known, even though they are expected to cause a degradation of the electrode performance and to reduce the long-term durability of SOFCs. Therefore, in this study, we focused on the poisoning caused by water vapor and SOx in the oxygen source to clarify their effects on SOFCs performances and to reveal the degradation mechanism of cathodes. SOFCs with typical electrolyte-supported structure were used in this work, which were composed with ScSZ (10 mol% Sc2O3, 1mol% CeO2, 89 mol% ZrO2) plate with the thickness of 200 µm as electrolyte, NiO-ScSZ (mixture of 56 wt% NiO and 44 wt% ScSZ) porous layer as anode, and two cathode layers of LSM ((La0.8Sr0.2)0.98MnO3) and LSM-ScSZ (mixture of 50 wt% LSM and 50 wt% ScSZ). Power generation characteristics of the cells had been analyzed by measuring cell voltage at a constant current density (200 mA/cm2) and by comparing changes in cell impedance, upon supplying the artificially-contaminated air with water vapor or SOx, to the SOFC cathodes at various operational temperatures. High-resolution FESEM (S-5200, Hitachi) was used to analyze microstructural changes caused by the impurities. Mg Kα radiation from a monochromatized X-ray source was used for XPS measurements (ESCA-3400, KRATOS). AC impedance was measured at various temperatures under the open circuit voltage condition by an impedance analyzer (Solatron 1255B/SI 1287, Solatron), in a frequency range from 0.1 to 105 Hz with an amplitude of 10 mV.

scholarly journals The Detailed Emissions Scaling, Isolation, and Diagnostic (DESID) module in the Community Multiscale Air Quality (CMAQ) Modeling System version 5.3

2020 ◽  
Author(s):  
Benjamin N. Murphy ◽  
Christopher G. Nolte ◽  
Fahim Sidi ◽  
Jesse O. Bash ◽  
K. Wyat Appel ◽  
...  
Keyword(s):  
Air Quality ◽  
Atmospheric Chemistry ◽  
Chemical Species ◽  
Energy System ◽  
Reduced Form ◽  
Chemistry Research ◽  
Control Interface ◽  
Source Contributions ◽  
Areas Of Interest ◽  
Multiple Chemical

Abstract. Air quality modeling for research and regulatory applications often involves executing many emissions sensitivity cases to quantify impacts of hypothetical scenarios, estimate source contributions or quantify uncertainties. Despite the prevalence of this task, conventional approaches for perturbing emissions in chemical transport models like the Community Multiscale Air Quality (CMAQ) model require extensive offline creation and finalization of alternative emissions input files. This workflow tends to be time-consuming, error-prone, inconsistent among model users and difficult to document while consuming increased computer storage space. The Detailed Emissions Scaling, Isolation, and Diagnostic (DESID) module, a component of CMAQv5.3 and beyond, addresses these limitations by performing these modifications online during the air quality simulation. Further, the model contains an Emission Control Interface which allows users to prescribe both simple and highly complex emissions scaling operations with control over individual or multiple chemical species, emissions sources, and spatial areas of interest. DESID further enhances the transparency of its operations with extensive error-checking and optional gridded output of processed emission fields. These new features are of high value to many air quality applications including routine perturbation studies, atmospheric chemistry research, and coupling with external models (e.g. energy system models, reduced-form models).

scholarly journals Effects of temperature on the heterogeneous oxidation of sulfur dioxide by ozone on calcium carbonate

2011 ◽  
Vol 11 (13) ◽  
pp. 6593-6605 ◽  
Author(s):  
L. Y. Wu ◽  
S. R. Tong ◽  
W. G. Wang ◽  
M. F. Ge
Keyword(s):  
Sulfur Dioxide ◽  
Atmospheric Chemistry ◽  
Ambient Pressure ◽  
Oxidation Reactions ◽  
Heterogeneous Oxidation ◽  
Fourier Transform Spectrometry ◽  
Different Temperatures ◽  
Chemistry Modeling ◽  
Sulfate Formation ◽  
Diffuse Reflectance Infrared

Abstract. The heterogeneous oxidation of sulfur dioxide by ozone on CaCO3 was studied as a function of temperature (230 to 298 K) at ambient pressure. Oxidation reactions were followed in real time using diffuse reflectance infrared Fourier transform spectrometry (DRIFTS) to obtain kinetic and mechanistic data. From the analysis of the spectral features, the formation of sulfate was identified on the surface in the presence of O3 and SO2 at different temperatures from 230 to 298 K. The results showed that the heterogeneous oxidation and the rate of sulfate formation were sensitive to temperature. An interesting stage-transition region was observed at temperatures ranging from 230 to 257 K, but it became ambiguous gradually above 257 K. The reactive uptake coefficients at different temperatures from 230 to 298 K were acquired for the first time, which can be used directly in atmospheric chemistry modeling studies to predict the formation of secondary sulfate aerosol in the troposphere. Furthermore, the rate of sulfate formation had a turning point at about 250 K. The sulfate concentration at 250 K was about twice as large as that at 298 K. The rate of sulfate formation increased with decreasing temperature at temperatures above 250 K, while there is a contrary temperature effect at temperatures below 250 K. The activation energy for heterogeneous oxidation at temperatures from 245 K to 230 K was determined to be 14.63 ± 0.20 kJ mol−1. A mechanism for the temperature dependence was proposed and the atmospheric implications were discussed.

Surface-Promoted Redox Reactions Occurs Spontaneously on Solvating Salt Surfaces

2021 ◽  
Author(s):  
Xiangrui Kong ◽  
Ivan Gladich ◽  
Dimitri Castarede ◽  
Erik Thomson ◽  
Anthony Boucly ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Photoelectron Spectroscopy ◽  
Ambient Pressure ◽  
Species Abundance ◽  
Ammonium Oxidation ◽  
Gas Uptake ◽  
Sulfate Reducing ◽  
Interfacial Processes ◽  
Key Species ◽  
Halogen Chemistry

&lt;p&gt;Gas-particle interfaces play essential roles in the atmosphere and directly influence many atmospheric processes, including gas uptake, halogen chemistry, ozone depletion, and heterogeneous ice nucleation. However, because interfacial processes take place on molecular scales, classical bulk thermodynamic theories are often insufficient to describe interfaces. Also, interfacial processes are challenging to characterize and are often overlooked in current atmospheric chemistry.&lt;/p&gt;&lt;p&gt;For this study, ambient pressure X-ray photoelectron spectroscopy (APXPS) experiments were performed. A surface-promoted sulfate-reducing ammonium oxidation reaction is discovered to spontaneously take place on common inorganic aerosol surfaces undergoing solvation. Several key intermediate species including, S&lt;sup&gt;0&lt;/sup&gt;, HS&lt;sup&gt;-&lt;/sup&gt;, HONO, and NH&lt;sub&gt;3(aq)&lt;/sub&gt;&amp;#160;are identified as reaction components associated with the solvation process. Depth profiles of relative species abundance show the surface propensity of key species. The species assignments and depth profile features are supported by classical and first-principle molecular dynamics calculations. A detailed mechanism is proposed to describe the processes that lead to unexpected products during salt solvation. This discovery reveals novel chemistry that is uniquely linked to a solvating surface and has great potential to illuminate current puzzles within heterogeneous chemistry. Lastly, natural salts sampled from saline lakes and playas are examined for this behavior, and provide further evidence of the important roles this surface-promoted redox mechanism may play in nature.&lt;/p&gt;

Measurement of alveolar gas volume by ambient pressure changes in isolated lungs

1988 ◽  
Vol 65 (3) ◽  
pp. 1281-1285
Author(s):  
R. R. Martin ◽  
R. Peslin ◽  
C. Duvivier ◽  
C. Gallina
Keyword(s):  
Water Vapor ◽  
Ambient Pressure ◽  
Water Vapor Pressure ◽  
Volumetric Method ◽  
The Body ◽  
Highly Correlated ◽  
Isolated Lungs ◽  
Pressure Changes ◽  
Gas Volume ◽  
The Relationship

Alveolar gas volume (AGV) may be measured in humans (Peslin et al., J. Appl. Physiol. 62: 359-363, 1987) by applying very slow sinusoidal variations of ambient pressure (delta Pam) around the body and studying the relationship between delta Pam and the resulting gas displacement at the mouth (delta Vaw): AGVapc = (PB.delta Vaw)/(delta Pam.cos phi), where AGVapc is AGV measured by ambient pressure changes, PB is barometric minus alveolar water vapor pressure, and phi is the phase angle between Pam and Vaw. The applicability of this method to excised lungs at various transpulmonary pressures was assessed in six rabbit lungs and three dog lobes by reference to AGV measurements by He dilution (AGVdil) and by a volumetric method (AGVvol). Except in one instance, AGVapc did not change significantly when the frequency of delta Pam was varied from 0.02 to 0.2 Hz. AGVapc was highly correlated (P less than 0.001) to both AGVdil and AGVvol. It did not differ significantly from AGVdil (81.4 +/- 50.6 vs. 80.2 +/- 44.2 ml) and was only marginally higher than AGVvol (64.6 +/- 26.9 vs. 62.4 +/- 24.4 ml, P less than 0.05). We conclude that the method usually provides accurate results in excised lung preparations. Its main advantages are that it does not require manipulating the lung or changing its volume and that the measurement takes less than 1 min.

scholarly journals Characterization of a boreal convective boundary layer and its impact on atmospheric chemistry during HUMPPA-COPEC-2010

2012 ◽  
Vol 12 (19) ◽  
pp. 9335-9353 ◽  
Author(s):  
H. G. Ouwersloot ◽  
J. Vilà-Guerau de Arellano ◽  
A. C. Nölscher ◽  
M. C. Krol ◽  
L. N. Ganzeveld ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Atmospheric Chemistry ◽  
Convective Boundary Layer ◽  
Large Scale ◽  
Spatial Scales ◽  
Potential Temperature ◽  
Chemical Species ◽  
Convective Boundary ◽  
The Impact

Abstract. We studied the atmospheric boundary layer (ABL) dynamics and the impact on atmospheric chemistry during the HUMPPA-COPEC-2010 campaign. We used vertical profiles of potential temperature and specific moisture, obtained from 132 radio soundings, to determine the main boundary layer characteristics during the campaign. We propose a classification according to several main ABL prototypes. Further, we performed a case study of a single day, focusing on the convective boundary layer, to analyse the influence of the dynamics on the chemical evolution of the ABL. We used a mixed layer model, initialized and constrained by observations. In particular, we investigated the role of large scale atmospheric dynamics (subsidence and advection) on the ABL development and the evolution of chemical species concentrations. We find that, if the large scale forcings are taken into account, the ABL dynamics are represented satisfactorily. Subsequently, we studied the impact of mixing with a residual layer aloft during the morning transition on atmospheric chemistry. The time evolution of NOx and O3 concentrations, including morning peaks, can be explained and accurately simulated by incorporating the transition of the ABL dynamics from night to day. We demonstrate the importance of the ABL height evolution for the representation of atmospheric chemistry. Our findings underscore the need to couple the dynamics and chemistry at different spatial scales (from turbulence to mesoscale) in chemistry-transport models and in the interpretation of observational data.

Observation of Oxygen Vacancy Filling under Water Vapor in Ceramic Proton Conductors in Situ with Ambient Pressure XPS

2013 ◽  
Vol 25 (23) ◽  
pp. 4690-4696 ◽  
Author(s):  
Qianli Chen ◽  
Farid El Gabaly ◽  
Funda Aksoy Akgul ◽  
Zhi Liu ◽  
Bongjin Simon Mun ◽  
...  
Keyword(s):  
Water Vapor ◽  
Oxygen Vacancy ◽  
Ambient Pressure ◽  
Proton Conductors ◽  
Ambient Pressure Xps

scholarly journals A review of operational, regional-scale, chemical weather forecasting models in Europe

2012 ◽  
Vol 12 (1) ◽  
pp. 1-87 ◽  
Author(s):  
J. Kukkonen ◽  
T. Olsson ◽  
D. M. Schultz ◽  
A. Baklanov ◽  
T. Klein ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Weather Forecasting ◽  
Numerical Models ◽  
Weather Prediction ◽  
Regional Scale ◽  
Chemical Species ◽  
Future Research ◽  
Physical Processes ◽  
Forecasting Models ◽  
Air Chemistry

Abstract. Numerical models that combine weather forecasting and atmospheric chemistry are here referred to as chemical weather forecasting models. Eighteen operational chemical weather forecasting models on regional and continental scales in Europe are described and compared in this article. Topics discussed in this article include how weather forecasting and atmospheric chemistry models are integrated into chemical weather forecasting systems, how physical processes are incorporated into the models through parameterization schemes, how the model architecture affects the predicted variables, and how air chemistry and aerosol processes are formulated. In addition, we discuss sensitivity analysis and evaluation of the models, user operational requirements, such as model availability and documentation, and output availability and dissemination. In this manner, this article allows for the evaluation of the relative strengths and weaknesses of the various modelling systems and modelling approaches. Finally, this article highlights the most prominent gaps of knowledge for chemical weather forecasting models and suggests potential priorities for future research directions, for the following selected focus areas: emission inventories, the integration of numerical weather prediction and atmospheric chemical transport models, boundary conditions and nesting of models, data assimilation of the various chemical species, improved understanding and parameterization of physical processes, better evaluation of models against data and the construction of model ensembles.

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