Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments
<p><span id="page3066"/>Molecular markers in organic aerosol (OA) provide specific source information on PM<span class="inline-formula"><sub>2.5</sub></span>, and the contribution of cooking organic aerosols to OA is significant, especially in...
| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Copernicus Publications
2023-03-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/23/3065/2023/acp-23-3065-2023.pdf |
| _version_ | 1811157671026360320 |
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| author | R. Li R. Li K. Zhang K. Zhang Q. Li Q. Li L. Yang L. Yang S. Wang S. Wang Z. Liu Z. Liu Z. Liu X. Zhang X. Zhang X. Zhang H. Chen H. Chen Y. Yi Y. Yi J. Feng J. Feng Q. Wang L. Huang L. Huang W. Wang W. Wang Y. Wang Y. Wang J. Z. Yu J. Z. Yu L. Li L. Li |
| author_facet | R. Li R. Li K. Zhang K. Zhang Q. Li Q. Li L. Yang L. Yang S. Wang S. Wang Z. Liu Z. Liu Z. Liu X. Zhang X. Zhang X. Zhang H. Chen H. Chen Y. Yi Y. Yi J. Feng J. Feng Q. Wang L. Huang L. Huang W. Wang W. Wang Y. Wang Y. Wang J. Z. Yu J. Z. Yu L. Li L. Li |
| author_sort | R. Li |
| collection | DOAJ |
| description | <p><span id="page3066"/>Molecular markers in organic aerosol (OA) provide specific source
information on PM<span class="inline-formula"><sub>2.5</sub></span>, and the contribution of cooking organic aerosols
to OA is significant, especially in urban environments. However, the low
time resolution of offline measurements limits the effectiveness when
interpreting the tracer data, the diurnal variation in cooking emissions and
the oxidation process. In this study, we used online thermal desorption
aerosol gas chromatography and mass spectrometry (TAG) to measure organic
molecular markers in fine particulate matter (PM<span class="inline-formula"><sub>2.5</sub></span>) at an urban site
in Changzhou, China. The concentrations of saturated fatty acids (sFAs),
unsaturated fatty acids (uFAs) and oxidative decomposition products (ODPs) of
unsaturated fatty acids were measured every 2 h to investigate
the temporal variations and the oxidative decomposition characteristics of
uFAs in urban environments. The average concentration of total fatty acids
(TFAs, sum of sFAs and uFAs) was measured to be
<span class="inline-formula">105.70±230.28</span> ng m<span class="inline-formula"><sup>−3</sup></span>. The average concentration of TFAs in the polluted period (PM<span class="inline-formula"><sub>2.5</sub>≥35</span> <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) was 147.06 ng m<span class="inline-formula"><sup>−3</sup></span>, which was 4.2
times higher than that in the clean period
(PM<span class="inline-formula"><sub>2.5</sub><35</span> <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) and higher than the enhancement of PM<span class="inline-formula"><sub>2.5</sub></span> (2.2 times) and
organic carbon (OC) (2.0 times) concentrations when comparing the polluted period to the
clean period. The mean concentration of cooking aerosol in the polluted
period (4.0 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) was about 5.3 times higher than that in the
clean period (0.75 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>), which was similar to the trend of fatty
acids. Fatty acids showed a clear diurnal variation. Linoleic acid <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M17" display="inline" overflow="scroll" dspmath="mathml"><mo>/</mo></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="8pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="a3a809672b156f3719eee3cbaf593ee5"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-3065-2023-ie00001.svg" width="8pt" height="14pt" src="acp-23-3065-2023-ie00001.png"/></svg:svg></span></span> stearic
acid and oleic acid <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M18" display="inline" overflow="scroll" dspmath="mathml"><mo>/</mo></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="8pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="62d2c8208bbdf49afb8db19c9f7b6b50"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-3065-2023-ie00002.svg" width="8pt" height="14pt" src="acp-23-3065-2023-ie00002.png"/></svg:svg></span></span> stearic acid ratios were significantly higher at
dinnertime and closer to the cooking source profile. By performing
backward trajectory clustering analysis, under the influence of
short-distance air masses from surrounding areas, the concentrations of TFAs
and PM<span class="inline-formula"><sub>2.5</sub></span> were relatively high, while under the influence of air masses
from easterly coastal areas, the oxidation degree of uFAs emitted from local
culinary sources was higher. The effective rate constants (<span class="inline-formula"><i>k</i><sub>O</sub></span>) for the
oxidative degradation of oleic acid were estimated to be 0.08–0.57 h<span class="inline-formula"><sup>−1</sup></span>,
which were lower than <span class="inline-formula"><i>k</i><sub>L</sub></span> (the estimated effective rate constants of
linoleic acid, 0.16–0.80 h<span class="inline-formula"><sup>−1</sup></span>). Both <span class="inline-formula"><i>k</i><sub>O</sub></span> and <span class="inline-formula"><i>k</i><sub>L</sub></span> showed a
significant positive correlation with O<span class="inline-formula"><sub>3</sub></span>, indicating that O<span class="inline-formula"><sub>3</sub></span> was
the main nighttime oxidant for uFAs in the city of Changzhou. Using fatty
acids as tracers, cooking was estimated to contribute an average of 4.6 %
to PM<span class="inline-formula"><sub>2.5</sub></span> concentrations, increasing to 7.8 % at 20:00 UTC<span class="inline-formula">+</span>8 h. Cooking was an
important source of OC, contributing 8.1 %, higher than the
contribution of PM<span class="inline-formula"><sub>2.5</sub></span>. This study investigates the variation in the
concentrations and oxidative degradation of fatty acids and corresponding
oxidation products in ambient air, which can be a guide for the refinement
of aerosol source apportionment and provide scientific support for the
development of cooking source control policies.</p> |
| first_indexed | 2024-04-10T05:11:15Z |
| format | Article |
| id | doaj.art-236657b6d96044f1bcfda4ea8287b7a4 |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-04-10T05:11:15Z |
| publishDate | 2023-03-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-236657b6d96044f1bcfda4ea8287b7a42023-03-09T07:23:06ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242023-03-01233065308110.5194/acp-23-3065-2023Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environmentsR. Li0R. Li1K. Zhang2K. Zhang3Q. Li4Q. Li5L. Yang6L. Yang7S. Wang8S. Wang9Z. Liu10Z. Liu11Z. Liu12X. Zhang13X. Zhang14X. Zhang15H. Chen16H. Chen17Y. Yi18Y. Yi19J. Feng20J. Feng21Q. Wang22L. Huang23L. Huang24W. Wang25W. Wang26Y. Wang27Y. Wang28J. Z. Yu29J. Z. Yu30L. Li31L. Li32School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaJiangsu Changhuan Environment Technology Co., Ltd., Jiangsu, Changzhou, 213004, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaJiangsu Changhuan Environment Technology Co., Ltd., Jiangsu, Changzhou, 213004, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental Studies, China University of Geosciences, Wuhan, 430074, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, ChinaDepartment of Chemistry, Hong Kong University of Science and Technology, Hong Kong SAR, 999077, ChinaDivision of Environment and Sustainability, Hong Kong University of Science and Technology, Hong Kong SAR, 999077, ChinaSchool of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, ChinaKey Laboratory of Organic Compound Pollution Control Engineering (MOE), Shanghai University, Shanghai, 200444, China<p><span id="page3066"/>Molecular markers in organic aerosol (OA) provide specific source information on PM<span class="inline-formula"><sub>2.5</sub></span>, and the contribution of cooking organic aerosols to OA is significant, especially in urban environments. However, the low time resolution of offline measurements limits the effectiveness when interpreting the tracer data, the diurnal variation in cooking emissions and the oxidation process. In this study, we used online thermal desorption aerosol gas chromatography and mass spectrometry (TAG) to measure organic molecular markers in fine particulate matter (PM<span class="inline-formula"><sub>2.5</sub></span>) at an urban site in Changzhou, China. The concentrations of saturated fatty acids (sFAs), unsaturated fatty acids (uFAs) and oxidative decomposition products (ODPs) of unsaturated fatty acids were measured every 2 h to investigate the temporal variations and the oxidative decomposition characteristics of uFAs in urban environments. The average concentration of total fatty acids (TFAs, sum of sFAs and uFAs) was measured to be <span class="inline-formula">105.70±230.28</span> ng m<span class="inline-formula"><sup>−3</sup></span>. The average concentration of TFAs in the polluted period (PM<span class="inline-formula"><sub>2.5</sub>≥35</span> <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) was 147.06 ng m<span class="inline-formula"><sup>−3</sup></span>, which was 4.2 times higher than that in the clean period (PM<span class="inline-formula"><sub>2.5</sub><35</span> <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) and higher than the enhancement of PM<span class="inline-formula"><sub>2.5</sub></span> (2.2 times) and organic carbon (OC) (2.0 times) concentrations when comparing the polluted period to the clean period. The mean concentration of cooking aerosol in the polluted period (4.0 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>) was about 5.3 times higher than that in the clean period (0.75 <span class="inline-formula">µ</span>g m<span class="inline-formula"><sup>−3</sup></span>), which was similar to the trend of fatty acids. Fatty acids showed a clear diurnal variation. Linoleic acid <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M17" display="inline" overflow="scroll" dspmath="mathml"><mo>/</mo></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="8pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="a3a809672b156f3719eee3cbaf593ee5"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-3065-2023-ie00001.svg" width="8pt" height="14pt" src="acp-23-3065-2023-ie00001.png"/></svg:svg></span></span> stearic acid and oleic acid <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M18" display="inline" overflow="scroll" dspmath="mathml"><mo>/</mo></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="8pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="62d2c8208bbdf49afb8db19c9f7b6b50"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-3065-2023-ie00002.svg" width="8pt" height="14pt" src="acp-23-3065-2023-ie00002.png"/></svg:svg></span></span> stearic acid ratios were significantly higher at dinnertime and closer to the cooking source profile. By performing backward trajectory clustering analysis, under the influence of short-distance air masses from surrounding areas, the concentrations of TFAs and PM<span class="inline-formula"><sub>2.5</sub></span> were relatively high, while under the influence of air masses from easterly coastal areas, the oxidation degree of uFAs emitted from local culinary sources was higher. The effective rate constants (<span class="inline-formula"><i>k</i><sub>O</sub></span>) for the oxidative degradation of oleic acid were estimated to be 0.08–0.57 h<span class="inline-formula"><sup>−1</sup></span>, which were lower than <span class="inline-formula"><i>k</i><sub>L</sub></span> (the estimated effective rate constants of linoleic acid, 0.16–0.80 h<span class="inline-formula"><sup>−1</sup></span>). Both <span class="inline-formula"><i>k</i><sub>O</sub></span> and <span class="inline-formula"><i>k</i><sub>L</sub></span> showed a significant positive correlation with O<span class="inline-formula"><sub>3</sub></span>, indicating that O<span class="inline-formula"><sub>3</sub></span> was the main nighttime oxidant for uFAs in the city of Changzhou. Using fatty acids as tracers, cooking was estimated to contribute an average of 4.6 % to PM<span class="inline-formula"><sub>2.5</sub></span> concentrations, increasing to 7.8 % at 20:00 UTC<span class="inline-formula">+</span>8 h. Cooking was an important source of OC, contributing 8.1 %, higher than the contribution of PM<span class="inline-formula"><sub>2.5</sub></span>. This study investigates the variation in the concentrations and oxidative degradation of fatty acids and corresponding oxidation products in ambient air, which can be a guide for the refinement of aerosol source apportionment and provide scientific support for the development of cooking source control policies.</p>https://acp.copernicus.org/articles/23/3065/2023/acp-23-3065-2023.pdf |
| spellingShingle | R. Li R. Li K. Zhang K. Zhang Q. Li Q. Li L. Yang L. Yang S. Wang S. Wang Z. Liu Z. Liu Z. Liu X. Zhang X. Zhang X. Zhang H. Chen H. Chen Y. Yi Y. Yi J. Feng J. Feng Q. Wang L. Huang L. Huang W. Wang W. Wang Y. Wang Y. Wang J. Z. Yu J. Z. Yu L. Li L. Li Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments Atmospheric Chemistry and Physics |
| title | Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments |
| title_full | Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments |
| title_fullStr | Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments |
| title_full_unstemmed | Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments |
| title_short | Characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments |
| title_sort | characteristics and degradation of organic aerosols from cooking sources based on hourly observations of organic molecular markers in urban environments |
| url | https://acp.copernicus.org/articles/23/3065/2023/acp-23-3065-2023.pdf |
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