Average Mole Fraction Research Articles

Final report of CCQM-K129 Measurement of Mole Fractions of Cu, In, Ga and Se in Cu(In,Ga)Se2 Films

CCQM key comparison K-129 for the quantitative analysis of Cu(In,Ga)Se2 (CIGS) films has been performed by the Surface Analysis Working Group (SAWG) of the Consultative Committee for Amount of Substance (CCQM). The objective of this key comparison is to compare the equivalency of the National Metrology Institutes (NMIs) and Designated Institutes (DIs) for the measurement of mole fractions of Cu, In, Ga and Se in a thin CIGS film. The measurand of this key comparison is the average mole fractions of Cu, In, Ga and Se of a test CIGS alloy film in the unit of mole fraction (mol/mol). Mole fraction with the metrological unit of % mol/mol can be practically converted to atomic fraction with the unit of at %.In this key comparison, a CIGS film with certified mole fractions was supplied as a reference specimen to determine the relative sensitivity factors (RSFs) of Cu, In, Ga and Se. The mole fractions of the reference specimen were certified by isotope dilution - inductively coupled plasma/mass spectrometry (ID-ICP/MS). A total number counting (TNC) method was recommended as a method to determine the signal intensities of the constituent elements acquired in the depth profiles by Secondary Ion Mass Spectrometry (SIMS), X-ray Photoelectron Spectroscopy (XPS) and Auger Electron Spectroscopy (AES). Seven NMIs and one DI participated in this key comparison. The mole fractions of the CIGS films were measured by depth profiling based-SIMS, AES and XPS.In this key comparison, the average degrees of equivalence uncertainties for Cu, In, Ga and Se are 0.0093 mol/mol, 0.0123 mol/mol, 0.0047 mol/mol and 0.0228 mol/mol, respectively.Main textTo reach the main text of this paper, click on Final Report. Note that this text is that which appears in Appendix B of the BIPM key comparison database kcdb.bipm.org/.The final report has been peer-reviewed and approved for publication by the CCQM, according to the provisions of the CIPM Mutual Recognition Arrangement (CIPM MRA).

Comparison of the regional CO<sub>2</sub> mole fraction filtering approaches at a WMO/GAW regional station in China

Abstract. The identification of atmospheric CO2 observation data which are minimally influenced by very local emissions/removals is essential for trend analysis, for the estimation of regional sources and sinks, and for the modeling of long-range transport of CO2. In this study, four approaches are used to filter the atmospheric CO2 observation records from 2009 to 2011 at one World Meteorological Organization/Global Atmosphere Watch (WMO/GAW) regional station (Lin'an, LAN) in China. The methods are based on the concentration of atmospheric black carbon (BC), on a statistical approach (robust extraction of baseline signal, REBS), on CH4 as an auxiliary tracer (AUX), and on meteorological parameters (MET). All approaches do suitably well to capture the seasonal CO2 cycle at LAN. Differences are observed in the average regional mole fractions with annual values in the REBS method at least 1.7 ± 0.2 ppm higher than the other methods. The BC method may underestimate the regional CO2 mole fractions during the winter–spring period and should be treated with caution. The REBS method is a purely statistical method and it may also introduce errors on the regional CO2 mole fraction evaluations, as the filtered trend may be influenced by the "noisy" raw data series. Although there are correlations between CH4 and CO2 mole fractions at LAN, the different source/sink regimes may introduce bias on the regional CO2 estimation in the AUX method, typically in summer. Overall, the MET method seems to be the most favorable because it mainly focuses on the influence of potential local sources and sinks, and considers diurnal variations and meteorological conditions. Using the MET method, the annual growth rate of regional CO2 at LAN is determined to be 3.1 ± 0.01 ppm yr−1 (standard error) from 2009 to 2011.

CCQM pilot study CCQM-P140: quantitative surface analysis of multi-element alloy films

A pilot study for a quantitative surface analysis of multi-element alloy films has been performed by the Surface Analysis Working Group (SAWG) of the Consultative Committee for Amount of Substance (CCQM). The aim of this pilot study is to evaluate a protocol for a key comparison to demonstrate the equivalence of measures by National Metrology Institutes (NMIs) and Designated Institutes (DI) for the mole fractions of multi-element alloy films.A Cu(In,Ga)Se2 (CIGS) film with non-uniform depth distribution was chosen as a representative multi-element alloy film. The mole fractions of the reference and the test CIGS films were certified by isotope dilution—inductively coupled plasma/mass spectrometry. A total number counting (TNC) method was used as a method to determine the signal intensities of the constituent elements acquired in SIMS, XPS and AES depth profiling. TNC method is comparable with the certification process because the certified mole fractions are the average values of the films.The mole fractions of the CIGS films were measured by Secondary Ion Mass Spectrometry (SIMS), Auger Electron Spectroscopy (AES), X-ray Photoelectron Spectroscopy (XPS), X-Ray Fluorescence (XRF) Analysis and Electron Probe Micro Analysis (EPMA) with Energy Dispersive X-ray Spectrometry (EDX). Fifteen laboratories from eight NMIs, one DI, and six non-NMIs participated in this pilot study.The average mole fractions of the reported data showed relative standard deviations from 5.5 % to 6.8 % and average relative expanded uncertainties in the range from 4.52 % to 4.86 % for the four test CIGS specimens. These values are smaller than those in the key comparison CCQM-K67 for the measurement of mole fractions of Fe-Ni alloy films. As one result it can be stated that SIMS, XPS and AES protocols relying on the quantification of CIGS films using the TNC method are mature to be used in a CCQM key comparison. Main text.To reach the main text of this paper, click on Final Report. The final report has been peer-reviewed and approved for publication by CCQM.

Comparisons of satellite (GOSAT) and ground-based spectroscopic measurements of CO2 content near St. Petersburg

The column-average mole fractions of atmospheric carbon dioxide measured with ground-based Fourier-transform spectroscopy at the Peterhof station of St. Petersburg State University (59.9° N, 29.8° E) in 2009–2011 are compared with similar data obtained with the Japanese GOSAT satellite. The comparison shows that the average mole fractions of CO2 from satellite data version V01.xx are lower by −9.8 ± 3 ppm than the corresponding values obtained from the ground-based measurements. For the GOSAT data version V02.xx, this difference is −4.7 ± 2.6 ppm on the average. Some overestimation of CO2 values in measurements near St. Petersburg in comparison with the ground-based TCCON network data has been revealed indirectly, the causes of which require further explanation.

Comparisons of satellite (GOSAT) and ground-based Fourier spectroscopic measurements of methane content near St. Petersburg

The column-average mole fraction of methane measured with hyperspectral methods of ground-based Fourier transform spectroscopy at the Physical Department of St. Petersburg State University (59.9° N, 29.8° E) in 2009–2012 is compared with similar data measured from the Japanese GOSAT satellite. The average mole fraction of methane \(X_{CH_4 } \) from GOSAT data version V01.xx are lower by 17–21 ppb than the corresponding value obtained from ground-based measurements with a standard deviation of about 13 ppb. For the GOSAT data version V02.xx, this difference is about 2 ppb on average, with a standard deviation of about 18 ppb. This corresponds to differences between data on \(X_{CH_4 } \) from the GOSAT satellite and from the TCCON and NDACC networks.

Epitaxial single-crystal thin films of MnxTi1 − xO2 − δ grown on (rutile)TiO2 substrates with pulsed laser deposition: Experiment and theory

Epitaxial rutile-structured single-crystal MnxTi1−xO2−δ films were synthesized on rutile- (110) and -(001) substrates using pulsed laser deposition. The films were characterized by reflection high-energy electron diffraction (RHEED), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and aberration-corrected transmission electron microscopy (ACTEM). Under the present conditions, 400°C and PO2=20mTorr, single crystal epitaxial thin films were grown for x=0.13, where x is the nominal average mole fraction of Mn. In fact, arbitrarily thick films could be grown with near invariant Mn/Ti concentration profiles from the substrate/film interface to the film surface. In contrast, at x=0.25, Mn became enriched towards the surface and a secondary nano-scale phase formed which appeared to maintain the basic rutile structure but with enhanced z-contrast in the tunnels, or interstitial sites. Ab initio thermodynamic calculations provided quantitative estimates for the destabilizing effect of expanding the β-MnO2 lattice parameters to those of TiO2-rutile, the stabilizing effect of diluting Mn with increasing Ti concentration, and competing reaction pathways for surface oxide formation.

CO2 Monitoring and Background Mole Fraction at Zhongshan Station, Antarctica

Background CO2 mole fraction and seasonal variations, measured at Zhongshan station, Antarctica, for 2010 through 2013, exhibit the expected lowest mole fraction in March with a peak in November. Irrespective of wind direction, the mole fraction of CO2 distributes evenly after polluted air from station operations is removed from the data sets. The daily range of average CO2 mole fraction in all four seasons is small. The monthly mean CO2 mole fraction at Zhongshan station is similar to that of other stations in Antarctica, with seasonal CO2 amplitudes in the order of 384–392 µmol∙mol−1. The annual increase in recent years is about 2 µmol∙mol−1∙yr−1. There is no appreciable difference between CO2 mole fractions around the coast of Antarctica and in the interior, showing that CO2 observed in Antarctica has been fully mixed in the atmosphere as it moves from the north through the southern hemisphere.

Detailed simulation of dual-reflux pressure swing adsorption process

A model for the detailed simulation of dual-reflux pressure swing adsorption process developed in the frame of the commercial software Aspen Adsim® is presented. For validation purposes, simulations were performed and model predictions were compared with published experimental results. At cyclic steady-state, model predictions were found to be in good agreement with reported experimental results in terms of (i) average ethane mole fraction in heavy product, (ii) average nitrogen mole fraction in light product, (iii) instantaneous heavy product composition profiles, and (iv) instantaneous column composition profiles. The predicted and experimental trends obtained by analyzing the effect of various operating parameters (light reflux flowrate, duration of feed/purge step, heavy product flowrate and mole fraction of heavy component in binary feed gas mixture) on process performance are also comparable. Overall, this simulation technique of dual-reflux pressure swing adsorption can serve as an effective tool for process design, cost reduction of laboratory and/or plant trails, and enhanced process understanding.

Global emissions of HFC-143a (CH<sub>3</sub>CF<sub>3</sub>) and HFC-32 (CH<sub>2</sub>F<sub>2</sub>) from in situ and air archive atmospheric observations

Abstract. High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant hydrofluorocarbons (HFCs) respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 ± 0.04 and 0.7 ± 0.02 mW m−2 in 2012 respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1σ) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing by 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.

Model‐data comparison of MCI field campaign atmospheric CO2 mole fractions

AbstractAtmospheric transport model errors are a major contributor to uncertainty in CO2 inverse flux estimates. Our study compares CO2 mole fraction observations from the North American Carbon Program Mid‐Continental Intensive (MCI) field campaign and modeled mole fractions from two atmospheric transport models: the global Transport Model 5 from NOAA's CarbonTracker system and the mesoscale Weather Research and Forecasting model. Both models are coupled to identical CO2 fluxes and lateral boundary conditions from CarbonTracker (CT2009 release). Statistical analyses were performed for two periods of 2007 using observed daily daytime average mole fractions of CO2 to test the ability of these models to reproduce the observations and to infer possible causes of the discrepancies. TM5‐CT2009 overestimates midsummer planetary boundary layer CO2 for sites in the U.S. corn belt by 10 ppm. Weather Research and Forecasting (WRF)‐CT2009 estimates diverge from the observations with similar magnitudes, but the signs of the differences vary from site to site. The modeled mole fractions are highly correlated with the observed seasonal cycle (r ≥ 0.7) but less correlated in the growing season, where weather‐related changes in CO2 dominate the observed variability. Spatial correlations in residuals from TM5‐CT2009 are higher than WRF‐CT2009 perhaps due to TM5's coarse horizontal resolution and shallow vertical mixing. Vertical mixing appears to have influenced CO2 residuals from both models. TM5‐CT2009 has relatively weak vertical mixing near the surface limiting the connection between local CO2 surface fluxes and boundary layer. WRF‐CT2009 has stronger vertical mixing that may increase the connections between local surface fluxes and the boundary layer.

CarbonTracker-CH<sub>4</sub>: an assimilation system for estimating emissions of atmospheric methane

Abstract. We describe an assimilation system for atmospheric methane (CH4), CarbonTracker-CH4, and demonstrate the diagnostic value of global or zonally averaged CH4 abundances for evaluating the results. We show that CarbonTracker-CH4 is able to simulate the observed zonal average mole fractions and capture inter-annual variability in emissions quite well at high northern latitudes (53–90° N). In contrast, CarbonTracker-CH4 is less successful in the tropics where there are few observations and therefore misses significant variability and is more influenced by prior flux estimates. CarbonTracker-CH4 estimates of total fluxes at high northern latitudes are about 81 ± 7 Tg CH4 yr−1, about 12 Tg CH4 yr−1 (13%) lower than prior estimates, a result that is consistent with other atmospheric inversions. Emissions from European wetlands are decreased by 30%, a result consistent with previous work by Bergamaschi et al. (2005); however, unlike their results, emissions from wetlands in boreal Eurasia are increased relative to the prior estimate. Although CarbonTracker-CH4 does not estimate an increasing trend in emissions from high northern latitudes for 2000 through 2010, significant inter-annual variability in high northern latitude fluxes is recovered. Exceptionally warm growing season temperatures in the Arctic occurred in 2007, a year that was also anonymously wet. Estimated emissions from natural sources were greater than the decadal average by 4.4 ± 3.8 Tg CH4 yr−1 in 2007. CarbonTracker-CH4 estimates for temperate latitudes are only slightly increased over prior estimates, but about 10 Tg CH4 yr−1 is redistributed from Asia to North America. This difference exceeds the estimated uncertainty for North America (±3.5 Tg CH4 yr−1). We used time invariant prior flux estimates, so for the period from 2000 to 2006, when the growth rate of global atmospheric CH4 was very small, the assimilation does not produce increases in natural or anthropogenic emissions in contrast to bottom-up emission data sets. After 2006, when atmospheric CH4 began its recent increases, CarbonTracker-CH4 allocates some of the increases to anthropogenic emissions at temperate latitudes, and some to tropical wetland emissions. For temperate North America the prior flux increases by about 4 Tg CH4 yr−1 during winter when biogenic emissions are small. Examination of the residuals at some North American observation sites suggests that increased gas and oil exploration may play a role since sites near fossil fuel production are particularly hard for the inversion to fit and the prior flux estimates at these sites are apparently lower and lower over time than what the atmospheric measurements imply. The tropics are not currently well resolved by CarbonTracker-CH4 due to sparse observational coverage and a short assimilation window. However, there is a small uncertainty reduction and posterior emissions are about 18% higher than prior estimates. Most of this increase is allocated to tropical South America rather than being distributed among the global tropics. Our estimates for this source region are about 32 ± 4 Tg CH4 yr−1, in good agreement with the analysis of Melack et al. (2004) who obtained 29 Tg CH4 yr−1 for the most productive region, the Amazon Basin.

Comparisons of satellite (GOSAT) and ground-based spectroscopic measurements of CH4 content near Saint Petersburg: influence of data collocation

We compared atmospheric column average mole fractions of methane measured with ground-based Fourier transform spectroscopy at the Physical Department of Saint Petersburg State University (59.9° N, 29.8° E) in years 2009–2012 with similar data obtained from the Japanese Greenhouse Gases Observing Satellite (GOSAT) satellite. For the GOSAT data version V02.xx, average and median values of biases between satellite and ground-based methane mole fractions are −(1.7–4.1) ppb and their standard deviations are 10–13 ppb. These values are similar to biases between the GOSAT satellite and the ground-based Total Carbon Column Observation Network and Network for the Detection of Atmospheric Composition Change making Fourier transform spectroscopic observations. Average and median biases for satellite data selected within α = ±1° latitude–longitude vicinity from the ground-based observations site are smaller than those for α = ±3° and α = ±5°.

Comparisons of CH<sub>4</sub> ground-based FTIR measurements near Saint Petersburg with GOSAT observations

Abstract. Atmospheric column-average methane mole fractions measured with ground-based Fourier-transform spectroscopy near Saint Petersburg, Russia (59.9° N, 29.8° E, 20 m a.s.l.) are compared with similar data obtained with the Japanese GOSAT (Greenhouse gases Observing SATellite) in the years 2009–2012. Average CH4 mole fractions for the GOSAT data version V01.xx are −15.0 ± 5.4 ppb less than the corresponding values obtained from ground-based measurements (with the standard deviations of biases at 13.0 ± 4.2 ppb). For the GOSAT data version V02.xx, the average values of the differences are −1.9 ± 1.8 ppb with standard deviations of 14.5 ± 1.3 ppb. This verifies that FTIR (Fourier transform infrared) spectroscopic observations near Saint Petersburg have similar biases with GOSAT satellite data as FTIR measurements at other ground-based networks and aircraft CH4 estimations.

Passive ventilation of a sustained gaseous release in an enclosure with one vent

A model for prediction of steady-state uniform concentration of a sustained gaseous leak in an enclosure with passive ventilation through one vent is described. Theoretically natural ventilation models under-predict up to twice lower concentrations of releasing gas and over-predict up to twice higher concentrations compared to the model of passive ventilation. The distinctive feature of passive ventilation is positioning of the neutral plane anywhere below the half of the vent height whereas it is located at about half vent height in the case of natural ventilation. The model is compared against experimental data on uniform and non-uniform distribution of helium concentration in the enclosure with one vent of different size and various release flow rates. The model predictions of maximum concentrations of helium observed in the experiments with the conservative discharge coefficient value CD = 0.60 (the best fit range is from 0.60 to 0.95) are closer to measured data than calculation by a model based on the natural ventilation assumptions even with “tuned” CD = 0.25. The engineering nomogram to calculate a release mass flow rate leading to 100% concentration of gas in an enclosure as a function of vent width and height is presented. The equation behind the nomogram is verified by CFD simulations and the appropriate discharge coefficient is derived for use in the equation as CD = 0.85. Effectiveness of different vent configurations is compared based of the ventilation parameterAH. A new criterion for mixture uniformity in a ventilated enclosure is suggested and applied to available experimental data. It is concluded that the maximum and minimum mole fractions deviate from the average mole fraction by no more than 20% when the criterion is above 4.

The first submillimeter observation of CO in the stratosphere of Uranus

Context. Carbon monoxide (CO) has been detected in all Giant Planets and its origin is both internal and external in Jupiter and Neptune. Despite its first detection in Uranus a decade ago, the magnitude of its internal and external sources remains unconstrained. Aims. We targeted CO lines in Uranus in the submillimeter range to constrain its origin. Methods. We recorded disk-averaged spectra of Uranus with a very high spectral resolution at the frequencies of CO rotational lines in the submillimeter range in 2011-2012. We used empirical and diffusion models of the atmosphere of Uranus to constrain the origin of CO. We also used a thermochemical model of its troposphere to derive an upper limit on the O/H ratio in the deep atmosphere of Uranus. Results. We have detected the CO(8-7) rotational line for the first time, with Herschel-HIFI. Both empirical and diffusion model results show that CO has an external origin. An empirical profile in which CO is constant above the 100mbar level with a mole fraction of 7.1-9.0E-9 (depending on the adopted stratospheric thermal structure) reproduces the data. Sporadic and steady source models cannot be differentiated with our data. Taking Teanby & Irwin's internal source model upper limit of a mole fraction of 2.1E-9 [Teanby & Irwin 2013. ApJ, 775, L49], the deep O/H ratio of Uranus is lower than 500 times solar according to our thermochemical computations. Conclusions. Our work shows that the average mole fraction of CO decreases from the stratosphere to the troposphere and thus strongly advocates for an external source of CO in Uranus. Photochemical modeling of oxygen species in the atmosphere of Uranus and more sensitive observations are needed to reveal the nature of the external source.

A study on the scaling features for mixing and deflagration potential of stratified layer of hydrogen due to molecular diffusion

Hydrogen deflagration in confined spaces is an important safety issue. The dispersion of a stratified layer of hydrogen due to molecular diffusion is studied. It represents an important class of problems related to long term behaviour of hydrogen release in confined spaces. Diffusion being a slow process, gives an upper bound on the time taken for the stratified layer to mix with air below. A method, based on four indices, namely, average mole fraction (of hydrogen), non-uniformity index, deflagration volume fraction and deflagration pressure ratio, developed recently by the authors, is used to provide vital temporal information on mixing of the stratified layer with air below and formation of flammable cloud in the enclosure. In the present paper, stratified layers of different thickness are considered and the temporal evolutions of the above indices are plotted against diffusion Fourier number. The results in non-dimensional form provide an upper bound of the time that would be required to form a uniform mixture and to attain a state with respect to deflagration potential for enclosures of different sizes. This estimate is an important input for planning mitigation measures before the accident and for post accident investigations.

Coherent Growth of AlN/GaN Short-Period Superlattice with Average GaN Mole Fraction of up to 20% on 6H-SiC(0001) Substrates by Plasma-Assisted Molecular-Beam Epitaxy

To obtain a high-crystalline-quality AlN/GaN short-period superlattice with higher average GaN mole fraction, the effects of the thicknesses of AlN barrier and GaN well layers on the superlattice growth were investigated. Coherent growth with an average GaN mole fraction of 20% was realized by reducing the AlN barrier layer thickness to 8 bilayers (BL) while keeping the GaN well layer thickness at 2 BL. Further reduction in the AlN barrier layer thickness resulted in lattice relaxation and degradation of the crystalline quality. Grown layers with various well and barrier thicknesses were investigated by transmission electron microscopy, X-ray diffraction, and atomic force microscopy.

CO, NO<sub>x</sub> and <sup>13</sup>CO<sub>2</sub> as tracers for fossil fuel CO<sub>2</sub>: results from a pilot study in Paris during winter 2010

Abstract. Measurements of the mole fraction of the CO2 and its isotopes were performed in Paris during the MEGAPOLI winter campaign (January–February 2010). Radiocarbon (14CO2) measurements were used to identify the relative contributions of 77% CO2 from fossil fuel consumption (CO2ff from liquid and gas combustion) and 23% from biospheric CO2 (CO2 from the use of biofuels and from human and plant respiration: CO2bio). These percentages correspond to average mole fractions of 26.4 ppm and 8.2 ppm for CO2ff and CO2bio, respectively. The 13CO2 analysis indicated that gas and liquid fuel contributed 70% and 30%, respectively, of the CO2 emission from fossil fuel use. Continuous measurements of CO and NOx and the ratios CO/CO2ff and NOx/CO2ff derived from radiocarbon measurements during four days make it possible to estimate the fossil fuel CO2 contribution over the entire campaign. The ratios CO/CO2ff and NOx/CO2ff are functions of air mass origin and exhibited daily ranges of 7.9 to 14.5 ppb ppm−1 and 1.1 to 4.3 ppb ppm−1, respectively. These ratios are consistent with different emission inventories given the uncertainties of the different approaches. By using both tracers to derive the fossil fuel CO2, we observed similar diurnal cycles with two maxima during rush hour traffic.

Numerical simulation of hydrogen–air reacting flows in rectangular channels with catalytic surface reactions

In this work a prediction was numerically modeled for a catalytically stabilized thermal combustion of a lean homogeneous mixture of air and hydrogen. The mixture flows in a narrow rectangular channel lined with a thin coating of platinum catalyst. The solution using an in-house code is based on the steady state partial differential continuity, momentum and energy conservation equations for the mixture and species involved in the reactions. A marching technique is used along the streamwise direction to solve the 2-D plane-symmetric laminar flow of the gas. Two chemical kinetic reaction mechanisms were included; one for the gas phase reactions consisting of 17 elementary reactions; of which 7 are forward–backward reactions while the other mechanism is for the surface reactions—which are the prime mover of the combustion under a lean mixture condition—consisting of 16 elementary reactions. The results were compared with a former congruent experimental work where temperature was measured using thermocouples, while using PLIF laser for measuring water and hydrogen mole fractions. The comparison showed good agreement. More results for the velocities, mole fractions of other species were carried out across the transverse and along the streamwise directions providing a complete picture of overall mechanism—gas and surface—and on the production, consumptions and travel of the different species. The variations of the average OH mole fraction with the streamwise direction showed a sudden increase in the region where the ignition occurred. Also the rate of reactions of the entire surface species were calculated along the streamwise direction and a surface water production flux equation was derived by calculating the law of mass action’s constants from the concentrations of hydrogen, oxygen and the rate of formation of water near the surface.

Numerical indices for quantification of hydrogen mixing and deflagration potential in the nuclear reactor containment

Studies on hydrogen distribution in the nuclear reactor containment and the effect of a distribution on subsequent combustion are important to nuclear safety. Contour plots, concentration profiles and ternary diagrams are routinely used to represent a distribution. The significance to safety has to be qualitatively inferred from these representations. Thus, there is a need to quantify distributions in terms of gross parameters that are important to safety. In the present study, four numerical indices are developed to obtain quantitative information on the mixing and deflagration potential of a distribution of hydrogen, steam and air. Two indices, namely, Average mole fraction and Non-uniformity index can be used to give the state of mixing of hydrogen in an enclosure at any instant of time. Similarly, the other two indices, namely, deflagration volume fraction and deflagration pressure ratio can be used to indicate the relative size of combustible cloud and the expected pressure rise in case of deflagration in the cloud at any instant of time. The significance and utility of the indices are brought forth through simple illustrations and numerical studies on the influence of steam condensation on hydrogen distributions. The indices depict the rate of mixing and changes in deflagration potential for the situations considered. Results form the simple studies show that the indices can give useful integral information for comparison of mixing and mitigation measures deployed in the nuclear reactor containment.