DOI: 10.1016/j.atmosenv.2020.117578
论文题名: Variable ethanol concentrations and stable carbon isotopes reveal anthropogenic ethanol contributions to rainwater
作者: Shimizu M.S. ; Summerlin S.L. ; Felix J.D. ; Halls J. ; Avery G.B. ; Kieber R.J. ; Lane C.S. ; Mead R.N. ; Willey J.D.
刊名: Atmospheric Environment
ISSN: 1352-2310
出版年: 2020
卷: 234 语种: 英语
英文关键词: Air quality
; Automotive fuels
; Biofuels
; Carbon
; Isotopes
; Rain
; Air mass back trajectories
; Anthropogenic emissions
; Ethanol concentrations
; Mean and standard deviations
; Partial oxidation of ethanol
; Stable carbon isotope ratio
; Stable carbon isotopes
; Volume-weighted averages
; Ethanol
; acetaldehyde
; alcohol
; biofuel
; carbon 13
; rain
; stable isotope
; acetaldehyde
; air mass
; air quality
; anthropogenic source
; biofuel
; C3 plant
; C4 plant
; carbon isotope
; concentration (composition)
; continental interior
; droplet
; ethanol
; GIS
; isotopic composition
; rainwater
; air
; alcohol oxidation
; Article
; Atlantic Ocean
; atmospheric dispersion
; concentration (parameter)
; geographic information system
; limit of detection
; mass
; North Carolina
; priority journal
; water sampling
; wet deposition
; Atlantic Ocean
; North Carolina
; United States
; Wilmington [North Carolina]
学科: Biofuel
; Ethanol
; Precipitation
; Rainwater
; Volatile organic carbon
中文摘要: The recent rapid increase in ethanol use as a biofuel and emission to the atmosphere may impact air quality and oxidizing capacity in the atmosphere. However, the global models show large uncertainties on sources of atmospheric ethanol. Concentrations and compound-specific stable carbon isotope ratios of ethanol (δ13Cethanol) in rainwater were measured in samples collected in six countries and 16 different locations over a two-year period (n = 270 for concentration; n = 111 for δ13Cethanol). Ethanol concentrations ranged from below the limit of detection (<28 nM) to 12 μM, while δ13Cethanol values ranged between −31 and −11‰. The higher the percent ethanol in automotive fuel, the higher the volume-weighted average ethanol concentration in rain, with the exception of Asian countries where there may be significant alternative sources. The wide range of δ13Cethanol values indicates that mixtures of sources contribute to atmospheric ethanol and the relative proportion of sources differs among rain events. Another explanation of variable δ13Cethanol values is partial oxidation of ethanol to acetaldehyde in the atmosphere. In Wilmington NC, USA, air mass back trajectory appeared to be the primary factor controlling ethanol concentrations and δ13Cethanol values with air masses originating over the Atlantic Ocean containing significantly 13C-enriched ethanol with lower concentrations compared to air masses from the continental interior (p < 0.03). A two-endmember isotope mixing model was applied for samples collected in Wilmington in order to quantify contributions from biofuels and natural biogenic emissions. The δ13Cethanol value of the biogenic endmember was determined to be −33‰ using measurements of ethanol isotopic composition in local plants combined with land coverage of C3 and C4 plants estimated by geographic information system with USDA Crop Data Layer, National Land Cover Dataset, and National Wetland Inventory. The relative contribution of biofuel ethanol in rainwater ranged from 11% to 97% at the Wilmington site, with a mean and standard deviation of 76 ± 17% (n = 97). The average concentrations of biofuel-sourced ethanol were similar among air mass back trajectories (p > 0.15), indicating that biofuel ethanol in rainwater is locally supplied during rain droplet formation. The results of this study are significant because they shed new insight into the role of anthropogenic emission of ethanol to the atmosphere. This study is particularly relevant as ethanol production and usage as a biofuel continues to increase globally. © 2020 Elsevier Ltd Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/160281
Appears in Collections: 气候变化与战略
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作者单位: Department of Chemistry and Biochemistry, University of North Carolina Wilmington, Wilmington, NC, United States; Department of Physical and Environmental Science, Texas A&M University – Corpus Christi, Corpus Christi, TX, United States; Department of Earth and Ocean Sciences, University of North Carolina Wilmington, Wilmington, NC, United States
Recommended Citation:
Shimizu M.S.,Summerlin S.L.,Felix J.D.,et al. Variable ethanol concentrations and stable carbon isotopes reveal anthropogenic ethanol contributions to rainwater[J]. Atmospheric Environment,2020-01-01,234