scholarly journals Estimation of NO<sub><i>x</i></sub> and SO<sub>2</sub> Emissions from Sarnia, Ontario using Mobile-MAX-DOAS and a NO<sub><i>x</i></sub>-Analyzer

2019 ◽  
Author(s):  
Zoe Y. W. Davis ◽  
Sabour Baray ◽  
Chris A. McLinden ◽  
Aida Khanbabakhani ◽  
William Fujs ◽  
...  

Abstract. Sarnia, ON experiences pollutant emissions disproportionate to its relatively small size. The small size of the city limits traditional top-down emission estimate techniques (e.g., satellite) but a low-cost solution for emission monitoring is Mobile-MAX-DOAS. Measurements were made using this technique from 21/03/2017 to 23/03/2017 along various driving routes to retrieve vertical column densities (VCDs) of NO2 and SO2 and to estimate emissions of NOx and SO2 from the Sarnia region. A novel aspect of the current study was the installation of a NOx analyzer in the vehicle to allow real time measurement and characterization of near-surface NOx/NO2 ratios across the urban plumes, allowing improved accuracy of NOx emission estimates. Confidence in the use of near-surface measured NOx/NO2 ratios for estimation of NOx emissions was increased by relatively well-mixed boundary layer conditions. These conditions were indicated by similar temporal trends in NO2 VCDs and mixing ratios when measurements were sufficiently distant from the sources. Leighton ratios within transported plumes indicated peroxy radicals were likely disturbing the NO-NO2-O3 photostationary state through VOC oxidation. The average lower limit emission estimate of NOx from Sarnia was 1.60 ± 0.34 tonnes hr−1 using local 10 m elevation wind-speed measurements. Our estimates were larger than the downscaled annual 2017 NPRI reported industrial emissions of 0.9 tonnes NOx hr−1. Our lower limit estimate of SO2 emissions from Sarnia was 1.81 ± 0.83 tonnes SO2 hr−1, equal within uncertainty to the 2017 NPRI downscaled value of 1.85 tonnes SO2 hr−1. Satellite-derived NO2 VCDs over Sarnia from the Ozone Monitoring Instrument (OMI) were lower than Mobile-MAX-DOAS VCDs, likely due to the large pixel size relative to the city’s size. The results of this study support the utility of the Mobile-MAX-DOAS method for estimating NOx and SO2 emissions in relatively small, highly industrialized regions especially when supplemented with mobile NOx measurements.

2019 ◽  
Vol 19 (22) ◽  
pp. 13871-13889 ◽  
Author(s):  
Zoe Y. W. Davis ◽  
Sabour Baray ◽  
Chris A. McLinden ◽  
Aida Khanbabakhani ◽  
William Fujs ◽  
...  

Abstract. Sarnia, Ontario, experiences pollutant emissions disproportionate to its relatively small size. The small size of the city limits traditional top-down emission estimate techniques (e.g., satellite) but a low-cost solution for emission monitoring is the mobile MAX-DOAS (Multi-AXis Differential Optical Absorption Spectroscopy). Measurements were made using this technique from 21 March 2017 to 23 March 2017 along various driving routes to retrieve vertical column densities (VCDs) of NO2 and SO2 and to estimate emissions of NOx and SO2 from the Sarnia region. A novel aspect of the current study was the installation of a NOx analyzer in the vehicle to allow real time measurement and characterization of near-surface NOx∕NO2 ratios across the urban plumes, allowing improved accuracy of NOx emission estimates. Confidence in the use of near-surface-measured NOx∕NO2 ratios for estimation of NOx emissions was increased by relatively well-mixed boundary layer conditions. These conditions were indicated by similar temporal trends in NO2 VCDs and mixing ratios when measurements were sufficiently distant from the sources. Leighton ratios within transported plumes indicated peroxy radicals were likely disturbing the NO–NO2–O3 photostationary state through VOC (volatile organic compound) oxidation. The average lower-limit emission estimate of NOx from Sarnia was 1.60±0.34 t h−1 using local 10 m elevation wind-speed measurements. Our estimates were larger than the downscaled annual 2017 NPRI-reported (National Pollution Release Inventory) industrial emissions of 0.9 t NOx h−1. Our lower-limit estimate of SO2 emissions from Sarnia was 1.81±0.83 t SO2 h−1, equal within uncertainty to the 2017 NPRI downscaled value of 1.85 t SO2 h−1. Satellite-derived NO2 VCDs over Sarnia from the ozone monitoring instrument (OMI) were lower than mobile MAX-DOAS VCDs, likely due to the large pixel size relative to the city's size. The results of this study support the utility of the mobile MAX-DOAS method for estimating NOx and SO2 emissions in relatively small, highly industrialized regions, especially when supplemented with mobile NOx measurements.


2022 ◽  
Vol 14 (2) ◽  
pp. 323
Author(s):  
Pauline Verdurme ◽  
Simon Carn ◽  
Andrew J. L. Harris ◽  
Diego Coppola ◽  
Andrea Di Muro ◽  
...  

Five effusive eruptions of Piton de la Fournaise (La Réunion) are analyzed to investigate temporal trends of erupted mass and sulfur dioxide (SO2) emissions. Daily SO2 emissions are acquired from three ultraviolet (UV) satellite instruments (the Ozone Monitoring Instrument (OMI), the Ozone Mapping and Profiler Suite (OMPS), and the Tropospheric Monitoring Instrument (TROPOMI)) and an array of ground-based UV spectrometers (Network for Observation of Volcanic and Atmospheric Change (NOVAC)). Time-averaged lava discharge rates (TADRs) are obtained from two automatic satellite-based hot spot detection systems: MIROVA and MODVOLC. Assuming that the lava volumes measured in the field are accurate, the MIROVA system gave the best estimation of erupted volume among the methods investigated. We use a reverse petrological method to constrain pre-eruptive magmatic sulfur contents based on observed SO2 emissions and lava volumes. We also show that a direct petrological approach using SO2 data might be a viable alternative for TADR estimation during cloudy weather that compromises hot spot detection. In several eruptions we observed a terminal increase in TADR and SO2 emissions after initial emission of evolved degassed magma. We ascribe this to input of deeper, volatile-rich magma into the plumbing system towards the end of these eruptions. Furthermore, we find no evidence of volatile excess in the five eruptions studied, which were thus mostly fed by shallow degassed magma.


1995 ◽  
Vol 85 (5) ◽  
pp. 1359-1372
Author(s):  
Hsi-Ping Liu

Abstract Because of its simple form, a bandlimited, four-parameter anelastic model that yields nearly constant midband Q for low-loss materials is often used for calculating synthetic seismograms. The four parameters used in the literature to characterize anelastic behavior are τ1, τ2, Qm, and MR in the relaxation-function approach (s1 = 1/τ1 and s2 = 1/τ2 are angular frequencies defining the bandwidth, MR is the relaxed modulus, and Qm is approximately the midband quality factor when Qm ≫ 1); or τ1, τ2, Qm, and MR in the creep-function approach (s1 = 1/τ1 and s2 = 1/τ2 are angular frequencies defining the bandwidth, and Qm is approximately the midband quality factor when Qm ≫ 1). In practice, it is often the case that, for a particular medium, the quality factor Q(ω0) and phase velocity c(ω0) at an angular frequency ω0 (s1 &lt; ω0 &lt; s2; s1 &lt; ω0 &lt; s2) are known from field measurements. If values are assigned to τ1 and τ2 (τ2 &lt; τ1), or to τ1 and τ2 (τ2 &lt; τ1), then the two remaining parameters, Qm and MR, or Qm and MR, can be obtained from Q(ω0). However, for highly attenuative media, e.g., Q(ω0) ≦ 5, Q(ω) can become highly skewed and negative at low frequencies (for the relaxation-function approach) or at high frequencies (for the creep-function approach) if this procedure is followed. A negative Q(ω) is unacceptable because it implies an increase in energy for waves propagating in a homogeneous and attenuative medium. This article shows that given (τ1, τ2, ω0) or (τ1, τ2, ω0), a lower limit of Q(ω0) exists for a bandlimited, four-parameter anelastic model. In the relaxation-function approach, the minimum permissible Q(ω0) is given by ln [(1 + ω20τ21)/(1 + ω20τ22)]/{2 arctan [ω0(τ1 − τ2)/(1 + ω20τ1τ2)]}. In the creep-function approach, the minimum permissible Q(ω0) is given by {2 ln (τ1/τ2) − ln [(1 + ω20τ21)/(1 + ω20τ22)]}/{2 arctan [ω0(τ1 − τ2)/(1 + ω20τ1τ2)]}. The more general statement that, for a given set of relaxation mechanisms, a lower limit exists for Q(ω0) is also shown to hold. Because a nearly constant midband Q cannot be achieved for highly attenuative media using a four-parameter anelastic model, a bandlimited, six-parameter anelastic model that yields a nearly constant midband Q for such media is devised; an expression for the minimum permissible Q(ω0) is given. Six-parameter anelastic models with quality factors Q ∼ 5 and Q ∼ 16, constant to 6% over the frequency range 0.5 to 200 Hz, illustrate this result. In conformity with field observations that Q(ω) for near-surface earth materials is approximately constant over a wide frequency range, the bandlimited, six-parameter anelastic models are suitable for modeling wave propagation in highly attenuative media for bandlimited time functions in engineering and exploration seismology.


2017 ◽  
Author(s):  
Vitali Fioletov ◽  
Chris A. McLinden ◽  
Shailesh K. Kharol ◽  
Nickolay A. Krotkov ◽  
Can Li ◽  
...  

Abstract. Reported sulfur dioxide (SO2) emissions from U.S. and Canadian sources have declined dramatically since the 1990s as a result of emissions control measures. Observations from the Ozone Monitoring Instrument (OMI) on NASA's Aura satellite and ground-based in-situ measurements are examined to verify whether the observed changes from SO2 abundance measurements are quantitatively consistent with the reported changes in emissions. To make this connection, a new method to link SO2 emissions and satellite SO2 measurements was developed. The method is based on fitting satellite SO2 vertical column densities (VCDs) to a set of functions of OMI pixel coordinates and wind speeds, where each function represents a statistical model of a plume from a single point source. The concept is first demonstrated using sources in North America, and then applied to Europe. The correlation coefficient between OMI-measured VCDs (with a local bias removed) and SO2 VCDs derived here using reported emissions for 1° by 1° gridded data is 0.91 and the best-fit line has a slope near unity, confirming a very good agreement between observed SO2 VCDs and reported emissions. Having demonstrated their consistency, seasonal and annual mean SO2 VCD distributions are calculated, based on reported point-source emissions for the period 1980–2015, as would have been seen by OMI. This consistency is further substantiated as the emissions-derived VCDs also show a high correlation with annual mean SO2 surface concentrations at 50 regional monitoring stations.


2017 ◽  
Vol 10 (11) ◽  
pp. 4403-4419 ◽  
Author(s):  
Joshua L. Laughner ◽  
Ronald C. Cohen

Abstract. Space-borne measurements of tropospheric nitrogen dioxide (NO2) columns are up to 10x more sensitive to upper tropospheric (UT) NO2 than near-surface NO2 over low-reflectivity surfaces. Here, we quantify the effect of adding simulated lightning NO2 to the a priori profiles for NO2 observations from the Ozone Monitoring Instrument (OMI) using modeled NO2 profiles from the Weather Research and Forecasting–Chemistry (WRF-Chem) model. With observed NO2 profiles from the Deep Convective Clouds and Chemistry (DC3) aircraft campaign as observational truth, we quantify the bias in the NO2 column that occurs when lightning NO2 is not accounted for in the a priori profiles. Focusing on late spring and early summer in the central and eastern United States, we find that a simulation without lightning NO2 underestimates the air mass factor (AMF) by 25 % on average for common summer OMI viewing geometry and 35 % for viewing geometries that will be encountered by geostationary satellites. Using a simulation with 500 to 665 mol NO flash−1 produces good agreement with observed NO2 profiles and reduces the bias in the AMF to  <  ±4 % for OMI viewing geometries. The bias is regionally dependent, with the strongest effects in the southeast United States (up to 80 %) and negligible effects in the central US. We also find that constraining WRF meteorology to a reanalysis dataset reduces lightning flash counts by a factor of 2 compared to an unconstrained run, most likely due to changes in the simulated water vapor profile.


2017 ◽  
Vol 17 (14) ◽  
pp. 8903-8922 ◽  
Author(s):  
Yang Yang ◽  
Hailong Wang ◽  
Steven J. Smith ◽  
Richard Easter ◽  
Po-Lun Ma ◽  
...  

Abstract. The global source–receptor relationships of sulfate concentrations, and direct and indirect radiative forcing (DRF and IRF) from 16 regions/sectors for years 2010–2014 are examined in this study through utilizing a sulfur source-tagging capability implemented in the Community Earth System Model (CESM) with winds nudged to reanalysis data. Sulfate concentrations are mostly contributed by local emissions in regions with high emissions, while over regions with relatively low SO2 emissions, the near-surface sulfate concentrations are primarily attributed to non-local sources from long-range transport. Regional source efficiencies of sulfate concentrations are higher over regions with dry atmospheric conditions and less export, suggesting that lifetime of aerosols, together with regional export, is important in determining regional air quality. The simulated global total sulfate DRF is −0.42 W m−2, with −0.31 W m−2 contributed by anthropogenic sulfate and −0.11 W m−2 contributed by natural sulfate, relative to a state with no sulfur emissions. In the Southern Hemisphere tropics, dimethyl sulfide (DMS) contributes 17–84 % to the total DRF. East Asia has the largest contribution of 20–30 % over the Northern Hemisphere mid- and high latitudes. A 20 % perturbation of sulfate and its precursor emissions gives a sulfate incremental IRF of −0.44 W m−2. DMS has the largest contribution, explaining −0.23 W m−2 of the global sulfate incremental IRF. Incremental IRF over regions in the Southern Hemisphere with low background aerosols is more sensitive to emission perturbation than that over the polluted Northern Hemisphere.


2012 ◽  
Vol 12 (8) ◽  
pp. 19529-19570 ◽  
Author(s):  
M. D. Andrés-Hernández ◽  
D. Kartal ◽  
J. N. Growley ◽  
V. Sinha ◽  
E. Regelin ◽  
...  

Abstract. Peroxy radicals were measured by a PeRCA (Peroxy Radical Chemical Amplifier) instrument in the boundary layer during the DOMINO (Diel Oxidant Mechanisms In relation to Nitrogen Oxides) campaign at a coastal, forested site influenced by urban-industrial emissions in Southern Spain in late autumn. Total peroxy radicals (RO2* = HO2 + ΣRO2) generally showed a daylight maximum between 10 and 50 pptv at 13:00 UTC, with an average of 18 pptv over the 15 days of measurements. Emissions from the industrial area of Huelva often impacted the measurement site at night during the campaign. The processing of significant levels of anthropogenic organics leads to an intense nocturnal radical chemistry accompanied by formation of organic peroxy radicals at comparable levels to those of summer photochemical conditions with peak events up to 60–80 pptv. The RO2 production initiated by reactions of NO3 with organic trace gases was estimated to be significant but not sufficient to account for the concentrations of RO2* observed in air masses carrying high pollutant loading. The nocturnal production of peroxy radicals seems therefore to be dominated by ozonolysis of volatile organic compounds. RO2* diurnal variations were consistent with other HO2 measurements available at the site. HO2/RO2* ratios generally varied between 0.3 and 0.4 in all wind directions. Occasional HO2/RO2* ≥ 1 seemed to be associated with periods of high RO2* variability and with RO2 interferences in the HO2 measurement in air masses with high RO2 load.


2016 ◽  
Author(s):  
Can Li ◽  
Nickolay A. Krotkov ◽  
Simon Carn ◽  
Yan Zhang ◽  
Robert J. D. Spurr ◽  
...  

Abstract. Since the fall of 2004, the Ozone Monitoring Instrument (OMI) has been providing global monitoring of volcanic SO2 emissions, helping to understand their climate impacts and to mitigate aviation hazards. Here we introduce a new generation OMI volcanic SO2 dataset based on a principal component analysis (PCA) retrieval technique. To reduce retrieval noise and artifacts as seen in the current operational linear fit (LF) algorithm, the new algorithm, OMSO2VOLCANO, uses characteristic features extracted directly from OMI radiances in the spectral fitting, thereby helping to minimize interferences from various geophysical processes (e.g., O3 absorption) and measurement details (e.g., wavelength shift). To solve the problem of low bias for large SO2 total columns in the LF product, the OMSO2VOLCANO algorithm employs a table lookup approach to estimate SO2 Jacobians (i.e., the instrument sensitivity to a perturbation in the SO2 column amount) and iteratively adjusts the spectral fitting window to exclude shorter wavelengths where the SO2 absorption signals are saturated. To first order, the effects of clouds and aerosols are accounted for using a simple Lambertian equivalent reflectivity approach. As with the LF algorithm, OMSO2VOLCANO provides total column retrievals based on a set of pre-defined SO2 profiles from the lower troposphere to the lower stratosphere, including a new profile peaked at 13 km for plumes in the upper troposphere. Examples given in this study indicate that the new dataset shows significant improvement over the LF product, with at least 50 % reduction in retrieval noise over the remote Pacific. For large eruptions such as Kasatochi in 2008 (~ 1700 kt total SO2) and Sierra Negra in 2005 (> 1100 DU maximal SO2), OMSO2VOLCANO generally agrees well with other algorithms that also utilize the full spectral content of satellite measurements, while the LF algorithm tends to underestimate SO2. We also demonstrate that, despite the coarser spatial and spectral resolution of the Suomi National Polar-orbiting Partnership (Suomi-NPP) Ozone Mapping and Profiler Suite (OMPS) instrument, application of the new PCA algorithm to OMPS data produces highly consistent retrievals between OMI and OMPS. The new PCA algorithm is therefore capable of continuing the volcanic SO2 data record well into the future using current and future hyperspectral UV satellite instruments.


2020 ◽  
Vol 13 (7) ◽  
pp. 3521-3542
Author(s):  
Ian Ashpole ◽  
Aldona Wiacek

Abstract. We compare MOPITT Version 7 (V7) Level 2 (L2) and Level 3 (L3) carbon monoxide (CO) products for the 1∘×1∘ L3 grid box containing the coastal city of Halifax, Canada (longitude −63.58∘, latitude 44.65∘), with a focus on the seasons DJF and JJA, and highlight a limitation in the L3 products that has significant consequences for the temporal trends in near-surface CO identified using those data. Because this grid box straddles the coastline, the MOPITT L3 products are created from the finer spatial resolution L2 products that are retrieved over both land and water, with a greater contribution from retrievals over water because more of the grid box lies over water than land. We create alternative L3 products for this grid box by separately averaging the bounded L2 retrievals over land (L3L) and water (L3W) and demonstrate that profile and total column CO (TCO) concentrations, retrieved at the same time, differ depending on whether the retrieval took place over land or water. These differences (ΔRET) are greatest in the lower troposphere (LT), where mean retrieved volume mixing ratios (VMRs) are greater in L3W than L3L, with maximum mean differences of 11.6 % (14.3 ppbv, p=0.001) at the surface level in JJA. Retrieved CO concentrations are more similar, on average, in the middle and upper troposphere (MT and UT), although large differences (in excess of 40 %) do infrequently occur. TCO is also greater in L3W than L3L in both seasons. By analysing L3L and L3W retrieval averaging kernels and simulations of these retrievals, we demonstrate that, in JJA, ΔRET is strongly influenced by differences in retrieval sensitivity over land and water, especially close to the surface where L3L has significantly greater information content than L3W. In DJF, land–water differences in retrieval sensitivity are much less pronounced and appear to have less of an impact on ΔRET, which analysis of wind directions suggests is more likely to reflect differences in true profile concentrations (i.e. real differences). The original L3 time series for the 1∘×1∘ grid box containing Halifax (L3O) corresponds much more closely to L3W than L3L, owing to the greater contribution from L2 retrievals over water than land. Thus, in JJA, variability in retrieved CO concentrations close to the surface in L3O is suppressed compared to L3L, and a declining trend detected using weighted least squares (WLS) regression analysis is significantly slower in L3O (strongest surface level trend identifiable is −1.35 (±0.35) ppbv yr−1) than L3L (−2.85 (±0.60) ppbv yr−1). This is because contributing L2 retrievals over water are closely tied to a priori CO concentrations used in the retrieval, owing to their lack of near-surface sensitivity in JJA, and these are based on monthly climatological CO profiles from a chemical transport model and therefore have no yearly change (surface level trend in L3W is −0.60 (±0.33) ppbv yr−1). Although our analysis focuses on DJF and JJA, we demonstrate that the findings also apply to MAM and SON. The results that we report here suggest that similar analyses be performed for other coastal cities before using MOPITT surface CO.


2018 ◽  
Vol 11 (3) ◽  
pp. 1817-1832 ◽  
Author(s):  
Maria Elissavet Koukouli ◽  
Nicolas Theys ◽  
Jieying Ding ◽  
Irene Zyrichidou ◽  
Bas Mijling ◽  
...  

Abstract. The main aim of this paper is to update existing sulfur dioxide (SO2) emission inventories over China using modern inversion techniques, state-of-the-art chemistry transport modelling (CTM) and satellite observations of SO2. Within the framework of the EU Seventh Framework Programme (FP7) MarcoPolo (Monitoring and Assessment of Regional air quality in China using space Observations) project, a new SO2 emission inventory over China was calculated using the CHIMERE v2013b CTM simulations, 10 years of Ozone Monitoring Instrument (OMI)/Aura total SO2 columns and the pre-existing Multi-resolution Emission Inventory for China (MEIC v1.2). It is shown that including satellite observations in the calculations increases the current bottom-up MEIC inventory emissions for the entire domain studied (15–55° N, 102–132° E) from 26.30 to 32.60 Tg annum−1, with positive updates which are stronger in winter ( ∼  36 % increase). New source areas were identified in the southwest (25–35° N, 100–110° E) as well as in the northeast (40–50° N, 120–130° E) of the domain studied as high SO2 levels were observed by OMI, resulting in increased emissions in the a posteriori inventory that do not appear in the original MEIC v1.2 dataset. Comparisons with the independent Emissions Database for Global Atmospheric Research, EDGAR v4.3.1, show a satisfying agreement since the EDGAR 2010 bottom-up database provides 33.30 Tg annum−1 of SO2 emissions. When studying the entire OMI/Aura time period (2005 to 2015), it was shown that the SO2 emissions remain nearly constant before the year 2010, with a drift of −0.51 ± 0.38 Tg annum−1, and show a statistically significant decline after the year 2010 of −1.64 ± 0.37 Tg annum−1 for the entire domain. Similar findings were obtained when focusing on the greater Beijing area (30–40° N, 110–120° E) with pre-2010 drifts of −0.17 ± 0.14 and post-2010 drifts of −0.47 ± 0.12 Tg annum−1. The new SO2 emission inventory is publicly available and forms part of the official EU MarcoPolo emission inventory over China, which also includes updated NOx, volatile organic compounds and particulate matter emissions.


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