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For the results reported here, a collection efficiency value of 0.5 has been used for the March campaign, which is consistent with previous AMS measurements

Identification of the Mass Spectral Signature of Organic Aerosols from Wood Burning Emissions

ENVIRONMENTAL SCIENCE & TECHNOLOGY, no. 16 (2007): 5770-5777

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摘要

Throughout the winter months, the village of Roveredo, Switzerland, frequently experiences strong temperature inversions that contribute to elevated levels of particulate matter. Wood is used as fuel for 75% of the domestic heating installations in Roveredo, which makes it a suitable location to study wood burning emissions in the atmosph...更多

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简介
  • A better characterization of the chemical composition of organic aerosols is an important step to reduce the current uncertainty in their effect on the radiative forcing of the climate.
  • The time series of the total aerosol mass concentration measured by the AMS and the fractional contribution of the main chemical constituents of the nonrefractory aerosol are shown for both of the March and December periods in Figure 1a and b, respectively.
重点内容
  • A better characterization of the chemical composition of organic aerosols is an important step to reduce the current uncertainty in their effect on the radiative forcing of the climate
  • To interpret the results of these statistical methods, mass spectral signatures of various organic aerosol sources and components are needed. These may include mass spectral signatures of primary organic aerosols emitted from various combustion processes and secondary organic aerosols produced by various precursors
  • Organics were by far the most dominant component of the aerosol during the December period contributing more than 80% of the total AMS measured mass during the afternoon and evening hours
  • The concentration of the 14C isotope was measured in aerosol samples collected during morning and evening periods in order to quantify the contributions of fossil and nonfossil sources to the organic carbon (OC) and OM in Roveredo [15]
  • The results show that the individual mass fragments that were enhanced during the evening periods during March and December are consistent with those of the filter periods
结果
  • The diurnal patterns of the total AMS aerosol mass and the fractional contribution of the organics for both measurement periods are shown in Figure 2a and b.
  • Organics were by far the most dominant component of the aerosol during the December period contributing more than 80% of the total AMS measured mass during the afternoon and evening hours.
  • The concentration of the 14C isotope was measured in aerosol samples collected during morning and evening periods in order to quantify the contributions of fossil and nonfossil sources to the OC and OM in Roveredo [15].
  • The fraction of OC to the total carbon was quite similar between morning and evening samples, the contributions of fossil and nonfossil sources to the organic mass were drastically different.
  • The 14C analysis results showed that nonfossil sources were by far more dominant during the evening periods, when more wood burning was used for domestic heating, contributing up to 94% of the OM.
  • 16, 2007 during the times of the chosen filter examples, AMS organic spectra were averaged over morning and evening periods throughout both of the March and December campaigns.
  • The ratios of the averaged evening to morning organic mass spectra for the entire sampling periods of March and December are shown in panels B and C, respectively, of Figure 3.
结论
  • Normalized mass spectra of levoglucosan (A), organic aerosols emitted during the burning of chestnut wood sample in a small stove (B), ambient mass spectra of organic aerosols obtained in Roveredo during the sampling period of filter 2, Table 1 (C), the averaged evening time periods during the December campaign (D), and the averaged sampling period in Haerkingen (E).
  • Inspection of the chestnut mass spectrum and the ambient evening spectra from March and December reveals that m/z 29 is a feature of wood burning aerosols with the highest contribution to the total organic signal.
总结
  • A better characterization of the chemical composition of organic aerosols is an important step to reduce the current uncertainty in their effect on the radiative forcing of the climate.
  • The time series of the total aerosol mass concentration measured by the AMS and the fractional contribution of the main chemical constituents of the nonrefractory aerosol are shown for both of the March and December periods in Figure 1a and b, respectively.
  • The diurnal patterns of the total AMS aerosol mass and the fractional contribution of the organics for both measurement periods are shown in Figure 2a and b.
  • Organics were by far the most dominant component of the aerosol during the December period contributing more than 80% of the total AMS measured mass during the afternoon and evening hours.
  • The concentration of the 14C isotope was measured in aerosol samples collected during morning and evening periods in order to quantify the contributions of fossil and nonfossil sources to the OC and OM in Roveredo [15].
  • The fraction of OC to the total carbon was quite similar between morning and evening samples, the contributions of fossil and nonfossil sources to the organic mass were drastically different.
  • The 14C analysis results showed that nonfossil sources were by far more dominant during the evening periods, when more wood burning was used for domestic heating, contributing up to 94% of the OM.
  • 16, 2007 during the times of the chosen filter examples, AMS organic spectra were averaged over morning and evening periods throughout both of the March and December campaigns.
  • The ratios of the averaged evening to morning organic mass spectra for the entire sampling periods of March and December are shown in panels B and C, respectively, of Figure 3.
  • Normalized mass spectra of levoglucosan (A), organic aerosols emitted during the burning of chestnut wood sample in a small stove (B), ambient mass spectra of organic aerosols obtained in Roveredo during the sampling period of filter 2, Table 1 (C), the averaged evening time periods during the December campaign (D), and the averaged sampling period in Haerkingen (E).
  • Inspection of the chestnut mass spectrum and the ambient evening spectra from March and December reveals that m/z 29 is a feature of wood burning aerosols with the highest contribution to the total organic signal.
表格
  • Table1: Organic Carbon Contribution to the Total Carbon Mass Measured by an EC/OC Analyzer and Contributions of Fossil and Nonfossil Sources to the Organic Mass during Morning and Evening Periods in Roveredo Based on the 14C Isotope Analysis [<a class="ref-link" id="c15" href="#r15">15</a>]a
Download tables as Excel
基金
  • This work was supported by the Federal Office for the Environment and the Cantons of Graubunden, Ticino, and Zurich, Switzerland
研究对象与分析
kinds of wood samples: 5
A particular aim of this study was to obtain the mass spectral signatures of wood burning aerosols and compare them to ambient measurements. Five kinds of wood samples were used including beech, larch, oak, white fir, and chestnut. Each burning cycle lasted for 45 min and three cycles were performed for each type of wood

filter samples: 4
This assumption was supported by substantial nonfossil EC concentrations, which originate exclusively from burning of wood. Table 1 lists the results of OC/TC (total carbon) and 14C analyses for four filter samples collected during the March period. Results show that OC was the major component of the total carbon during morning and evening periods contributing between 80 and 86% to its total mass

cases: 3
However, m/z 29 is not a suitable marker for wood burning aerosols because it is not unique to this source and has been widely observed in mass spectra in various environments, albeit with lower contributions and where m/z 44 or 43 have the highest contributions to the total organic signal [3, 29, 30]. The wood burning spectra also show that m/z 44 (CO2+ from di- and polycarboxylic acids) can arise from primary wood combustion sources and it contributes about 5% to the total organic mass in these three cases (panels B, C, and D in Figure 4). This finding indicates that m/z 44, which is used as a marker for oxygenated organic aerosols (OOA) [8] does not only arise from secondary organic aerosol sources but can also be produced from primary sources such as wood burning

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