Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-18-7757-2018 |
Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region | |
Amiri, Neda1; Ghahremaninezhad, Roghayeh2; Rempillo, Ofelia3; Tokarek, Travis W.4; Odame-Ankrah, Charles A.4,5; Osthoff, Hans D.4; Norman, Ann-Lise1 | |
2018-06-04 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS |
ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2018 |
卷号 | 18期号:11页码:7757-7780 |
文章类型 | Article |
语种 | 英语 |
国家 | Canada; Philippines |
英文摘要 | Concentrations and delta S-34 values for SO2 and size-segregated sulfate aerosols were determined for air monitoring station 13 (AMS 13) at Fort MacKay in the Athabasca oil sands region, northeastern Alberta, Canada as part of the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring (JOSM) campaign from 13 August to 5 September 2013. Sulfate aerosols and SO2 were collected on filters using a high-volume sampler, with 12 or 24 h time intervals. Sulfur dioxide (SO2) enriched in S-34 was exhausted by a chemical ionization mass spectrometer (CIMS) operated at the measurement site and affected isotope samples for a portion of the sampling period. It was realized that this could be a useful tracer and samples collected were divided into two sets. The first set includes periods when the CIMS was not running (CIMS-OFF) and no (SO2)-S-34 was emitted. The second set is for periods when the CIMS was running (CIMS-ON) and (SO2)-S-34 was expected to affect SO2 and sulfate high-volume filter samples. delta S-34 values for sulfate aerosols with diameter D > 0.49 mu m during CIMS-OFF periods (no tracer (SO2)-S-34 present) indicate the sulfur isotope characteristics of secondary sulfate in the region. Such aerosols had delta S-34 values that were isotopically lighter (down to -5.3%) than what was expected according to potential sulfur sources in the Athabasca oil sands region (+3.9 to +11.5 %). Lighter delta S-34 values for larger aerosol size fractions are contrary to expectations for primary unrefined sulfur from untreated oil sands (+6.4%) mixed with secondary sulfate from SO2 oxidation and ac-companied by isotope fractionation in gas phase reactions with OH or the aqueous phase by H2O2 or O-3. Furthermore, analysis of S-34 enhancements of sulfate and SO2 during CIMS-ON periods indicated rapid oxidation of SO2 from this local source at ground level on the surface of aerosols before reaching the high-volume sampler or on the collected aerosols on the filters in the high-volume sampler. Anti-correlations between delta S-34 values of dominantly secondary sulfate aerosols with D < 0.49 mu m and the concentrations of Fe and Mn (r = -0.80 and r = -0.76, respectively) were observed, suggesting that SO2 was oxidized by a transition metal ion (TMI) catalyzed pathway involving O-2 and Fe3+ and/or Mn2+, an oxidation pathway known to favor lighter sulfur isotopes. Correlations between SO2 to sulfate conversion ratio (F(s)) and the concentrations of alpha-pinene (r = 0.85), beta-pinene (r = 0.87), and limonene (r = 0.82) during daytime suggests that SO2 oxidation by Criegee biradicals may be a potential oxidation pathway in the study region. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000434114200001 |
WOS关键词 | STABILIZED CRIEGEE INTERMEDIATE ; CONNECTED FLOW CONDITIONS ; GLOBAL-MODEL ; SULFATE PRODUCTION ; FRASER VALLEY ; OXIDATION ; AEROSOL ; EMISSIONS ; RADICALS ; ALBERTA |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/30767 |
专题 | 地球科学 |
作者单位 | 1.Univ Calgary, Dept Phys & Astron, Calgary, AB, Canada; 2.Environm & Climate Change Canada, Toronto, ON, Canada; 3.De La Salle Univ, Phys Dept, Manila, Philippines; 4.Univ Calgary, Dept Chem, Calgary, AB, Canada; 5.Global Analyzer Syst Ltd, Calgary, AB, Canada |
推荐引用方式 GB/T 7714 | Amiri, Neda,Ghahremaninezhad, Roghayeh,Rempillo, Ofelia,et al. Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2018,18(11):7757-7780. |
APA | Amiri, Neda.,Ghahremaninezhad, Roghayeh.,Rempillo, Ofelia.,Tokarek, Travis W..,Odame-Ankrah, Charles A..,...&Norman, Ann-Lise.(2018).Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region.ATMOSPHERIC CHEMISTRY AND PHYSICS,18(11),7757-7780. |
MLA | Amiri, Neda,et al."Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region".ATMOSPHERIC CHEMISTRY AND PHYSICS 18.11(2018):7757-7780. |
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