Characterization of the δ 13 C signatures of anthropogenic CO 2 emissions in the Greater Toronto Area, Canada

Pugliese, Stephanie C.; Murphy, J. G.; Vogel, Felix; Worthy, D.

doi:10.1016/j.apgeochem.2016.11.003

Cited by 13 publications

(7 citation statements)

References 21 publications

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“…Our data were similar to δ 13 C of EC in PM previously reported for Alert (−27.9 ± 0.8‰, 5 March 2014 to 18 March 2015) (Winiger et al, 2019). Additionally, these data fall within the range of reported δ 13 C values of particles produced by fossil fuel combustion (−24‰ to −28‰) (Andersson et al, 2015;Mašalaitė et al, 2012;Pugliese et al, 2017;Widory, 2006) and overlaps with δ 13 C values found in biomass burning aerosols (−21‰ to −29‰) (Agnihotri et al, 2011;Garbaras et al, 2015;Mouteva et al, 2015;Sang et al, 2012).…”

Section: 1029/2020jd033125supporting

confidence: 90%

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Seasonal Cycle of Isotope‐Based Source Apportionment of Elemental Carbon in Airborne Particulate Matter and Snow at Alert, Canada

et al. 2020

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Elemental carbon (EC) is a major light-absorbing component of atmospheric aerosol particles. Here, we report the seasonal variation in EC concentrations and sources in airborne particulate matter (PM) and snow at Alert, Canada, from March 2014 to June 2015. We isolated the EC fraction with the EnCan-Total-900 (ECT9) protocol and quantified its stable carbon isotope composition (δ 13 C) and radiocarbon content (Δ 14 C) to apportion EC into contributions from fossil fuel combustion and biomass burning (wildfires and biofuel combustion). Ten-day backward trajectories show EC aerosols reaching Alert by traveling over the Arctic Ocean from the Russian Arctic during winter and from North America (>40°N) during summer. EC concentrations range from 1.8-135.3 ng C m −3 air (1.9-41.2% of total carbon [TC], n = 48), with lowest values in summer (1.8-44.5 ng C m −3 air, n = 9). EC in PM (Δ 14 C =-532 ± 114‰ [ave. ± SD, n = 20]) and snow (−257 ± 131‰, n = 7) was depleted in 14 C relative to current ambient CO 2 year-round. EC in PM mainly originated from liquid and solid fossil fuels from fall to spring (47-70% fossil), but had greater contributions from biomass burning in summer (48-80% modern carbon). EC in snow was mostly from biomass burning (53-88%). Our data show that biomass burning EC is preferentially incorporated into snow because of scavenging processes within the Arctic atmosphere or long-range transport in storm systems. This work provides a comprehensive view of EC particles captured in the High Arctic through wet and dry deposition and demonstrates that surface stations monitoring EC in PM might underestimate biomass burning and transport. Plain Language Summary Elemental carbon (EC) aerosols are produced during combustion processes and impact Arctic climate because they absorb light, warm the atmosphere, and accelerate snow and ice melt. Here, we measured the concentration and isotopic composition of EC suspended in the atmosphere and in snow at Alert, Canada, between March 2014 and May 2015. We found that concentrations were lowest during the summer and increased throughout the winter and early spring. This pattern is typical, because EC is removed from the atmosphere by precipitation, which happens more frequently during summer. Our isotope data and meteorological analyses revealed that fossil fuel burning in the Russian Arctic was an important source of EC to Alert from September to May, while forest fires in the North American boreal region were major sources of EC during the summer. We also found that snow contained a greater proportion of EC derived from biomass burning than the suspended aerosols. Snow might be preferentially capturing biomass burning EC from the local atmosphere or be transporting them to the Arctic from lower latitudes. Since EC surface observing networks routinely measure EC in PM but not snow, the impact of biomass burning EC sources on Arctic climate might be underestimated.

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Section: 1029/2020jd033125supporting

confidence: 90%

“…For nongaseous sources, we estimate a δ 13 C of −27 ± 4‰. These include the combustion of coal with a δ 13 C of −23.4 ± 1.3‰ and of liquid fuels (gasoline, diesel, and kerosene) with estimated ranges from −23.8‰ to −31.3‰ (Andersson et al, 2015; Mašalaitė et al, 2012; Pugliese et al, 2017).…”

Section: Methodsmentioning

confidence: 99%

Seasonal Cycle of Isotope‐Based Source Apportionment of Elemental Carbon in Airborne Particulate Matter and Snow at Alert, Canada

et al. 2020

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“…Detailed descriptions of pre-requisites and limitations of these models are available 675 elsewhere (Keeling, 1958;Keeling, 1961;Miller and Tans, 2003;Pataki et al, 2003;Zobitz et al, 2006;Ballantyne et al, 2011;Vardag et al, 2016), thus we provide only a brief discussion. Previous δ 13 Cs studies have been successful in deriving observation-based δ 13 Cm primarily under the following conditions: First, when measurements were taken rather close to a well-defined source location and using instrumentation with high precision (e.g., Pugliese et al, 2017). Second, when a pronounced regional signal (referred to as ΔCO2 and computed as the difference between 680 the CO2 concentration at the site and background) with stable source composition was observed during stable background conditions and the regional ecosystem contribution to the observed ΔCO2 was comparatively low (e.g., Vardag et al, 2016).…”

Section: Observation-based Source Signature Estimatesmentioning

confidence: 99%

“…However, the current instrumental capability of high precision δ 13 C-CO2 observations at high temporal resolution (e.g., Sturm et al (2013) or Vogel et al (2013)) opens up new opportunities to disentangle CO2 in a more complex setting. For instance, Pugliese et al (2017) and Vardag et al (2016) recently studied urban air masses, and Ghasemifard et al (2019) and Tuzson et al (2011) attempted to characterise specific regional scale CO2 signals at remote sites. These 95 studies used hourly to daily resolution, and compared observation-based (mixed) isotope source signatures (δ 13 Cm) with literature information on source-specific signatures (δ 13 Cs); often, however, reducing the data to few particular pollution events, as this method is applicable only under very stringent conditions (see e.g., Zobitz et al, 2006).…”

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confidence: 99%

Analysis of regional CO<sub>2</sub> contributions at the high Alpine observatory Jungfraujoch by means of atmospheric transport simulations and δ<sup>13</sup>C

Pieber

Tuzson

Henne

et al. 2021

Preprint

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Abstract. Understanding of regional greenhouse gas emissions into the atmosphere is a prerequisite to mitigate climate change. In this study, we investigated the regional contributions of carbon dioxide (CO2) at the location of the high Alpine observatory Jungfraujoch ("JFJ", Switzerland, 3580 m a.s.l.). To this purpose, we combined receptor-oriented atmospheric transport simulations for CO2 concentration in the period of 2009–2017 with stable carbon isotope (δ13C-CO2) information. We applied two Lagrangian particle dispersion models driven by output from two different numerical weather prediction systems (FLEXPART-COSMO and STILT-ECMWF) in order to simulate CO2 concentration at JFJ based on regional CO2 fluxes, to estimate atmospheric δ13C-CO2, and to obtain model-based estimates of the mixed source signatures (δ13Cm). Anthropogenic fluxes were taken from a fuel type-specific version of the EDGAR v4.3 inventory and ecosystem fluxes were based on the Vegetation Photosynthesis and Respiration Model (VPRM). The simulations of CO2, δ13C-CO2 and δ13Cm were then compared to observations performed by quantum cascade laser absorption spectroscopy. Around 40 % of the regional CO2 variability above or below the large-scale background was captured by the models, and up to 35 % of the regional variability in δ13C-CO2. This is remarkable considering the complex Alpine topography, the low intensity of regional signals at JFJ, and the challenging measurements. Best agreement between simulations and observations in terms of short-term variability and intensity of the signals for CO2 and δ13C-CO2 was found between late autumn and early spring. The agreement was inferior in the early autumn periods and during summer. This may be associated with the atmospheric transport representation in the models. In addition, the net ecosystem exchange fluxes are a possible source of error, either through inaccuracies in their representation in VPRM for the (Alpine) vegetation or through a day (uptake) vs. night (respiration) transport discrimination to JFJ. Furthermore, the simulations suggest that JFJ is subject to relatively small regional anthropogenic contributions, due to its remote location (elevated and far from major anthropogenic sources), and the limited planetary boundary layer-influence during winter. Instead, the station is primarily exposed to summer-time ecosystem CO2 contributions, which are dominated by rather nearby sources (within 100 km). Even during winter, simulated gross ecosystem respiration accounted for approximately 50 % of all contributions to the CO2 concentrations above the largescale background. The model-based monthly mean δ13Cm ranged from −22 ‰ in winter to −28 ‰ in summer and reached the most depleted values of −35 ‰ at higher fractions of natural gas combustion, and the most enriched values of −17 to −12 ‰ when impacted by cement production emissions. Observation-based δ13Cm values derived by a moving Keeling-plot approach were in good agreement with the model-based estimates. They exhibited a larger scatter, while model-based estimates spread in a more narrow range. Overall, observation-based δ13Cm were limited to a smaller number of data points compared to model-based estimates owing to the stringent analysis prerequisites in combination with the low regional signal at JFJ.

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“…Several studies have assessed GHG emissions in the GTA, including the creation of emission inventories, 2−4 observation-based flux estimates using continuous monitoring, 5 and source apportionment and atmospheric modeling studies using fixed site in situ observations. 6,7 In this study, we focus on methane (CH 4 ), the second most abundant anthropogenic GHG emitted. Reducing methane emissions is an important short-term climate change mitigation option because methane has a relatively short atmospheric lifetime (about 9 years 8 ) and its radiative forcing is between 28 and 32 times greater than that of carbon dioxide over a 100-year period and between 84 and 90 times greater over a 20 year period.…”

Section: Introductionmentioning

confidence: 99%

Investigation of the Spatial Distribution of Methane Sources in the Greater Toronto Area Using Mobile Gas Monitoring Systems

Ars

Vogel

Arrowsmith

et al. 2020

Environ. Sci. Technol.

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For methane emission reduction strategies in urban areas to be effective, large emitters must be identified. Recent studies in U.S. cities have highlighted the contribution of methane emissions from natural gas distribution networks and end use. We present a methane emission source identification and quantification method for the Greater Toronto Area (GTA), the largest metropolitan area in Canada, using mobile gas monitoring systems. From May 2018 to August 2019, we collected 77 surveys of methane mixing ratios, covering a distance of about 6400 km, and sampled emission plumes from sources such as closed landfills, natural gas compressor stations, and waterways. Our results indicate that inactive landfills emit less than inventory estimates. Despite this discrepancy, we confirm that the waste sector is the largest methane emitter in the GTA. We also report that the frequency of methane leaks from the local distribution system ranges between 4 and 22 leaks per 100 km of roadway in downtown Toronto, which is comparable to the range observed in U.S. cities, which have invested in modern natural gas distribution infrastructure. Last, we find that engineered waterways, whose emissions are currently not reported in inventories, may be a significant source of methane.

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Characterization of the δ 13 C signatures of anthropogenic CO 2 emissions in the Greater Toronto Area, Canada

Cited by 13 publications

References 21 publications

Seasonal Cycle of Isotope‐Based Source Apportionment of Elemental Carbon in Airborne Particulate Matter and Snow at Alert, Canada

Seasonal Cycle of Isotope‐Based Source Apportionment of Elemental Carbon in Airborne Particulate Matter and Snow at Alert, Canada

Analysis of regional CO<sub>2</sub> contributions at the high Alpine observatory Jungfraujoch by means of atmospheric transport simulations and δ<sup>13</sup>C

Investigation of the Spatial Distribution of Methane Sources in the Greater Toronto Area Using Mobile Gas Monitoring Systems

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Characterization of the δ 13 C signatures of anthropogenic CO 2 emissions in the Greater Toronto Area, Canada

Cited by 13 publications

References 21 publications

Seasonal Cycle of Isotope‐Based Source Apportionment of Elemental Carbon in Airborne Particulate Matter and Snow at Alert, Canada

Seasonal Cycle of Isotope‐Based Source Apportionment of Elemental Carbon in Airborne Particulate Matter and Snow at Alert, Canada

Analysis of regional CO&lt;sub&gt;2&lt;/sub&gt; contributions at the high Alpine observatory Jungfraujoch by means of atmospheric transport simulations and δ&lt;sup&gt;13&lt;/sup&gt;C

Investigation of the Spatial Distribution of Methane Sources in the Greater Toronto Area Using Mobile Gas Monitoring Systems

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Analysis of regional CO<sub>2</sub> contributions at the high Alpine observatory Jungfraujoch by means of atmospheric transport simulations and δ<sup>13</sup>C