Articles | Volume 19, issue 17
https://doi.org/10.5194/acp-19-11071-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Special issue:
https://doi.org/10.5194/acp-19-11071-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
02 Sep 2019
Research article |
| 02 Sep 2019
| 02 Sep 2019
High time-resolved measurement of stable carbon isotope composition in water-soluble organic aerosols: method optimization and a case study during winter haze in eastern China
Wenqi Zhang
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Fang Cao
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Yankun Xiang
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Yuanyuan Zhang
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Mengying Bao
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Xiaoyan Liu
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
Yu-Chi Lin
Yale–NUIST Center on Atmospheric Environment, International Joint
Laboratory on Climate and Environment Change (ILCEC), Nanjing University of
Information Science and Technology, Nanjing 210044, China
Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological
Disasters (CIC-FEMD), Nanjing University of Information Science and
Technology, Nanjing 210044, China
Jiangsu Provincial Key Laboratory of Agricultural Meteorology, College of
Applied Meteorology, Nanjing University of Information Science and
Technology, Nanjing 210044, China
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Yunhua Chang, Yanlin Zhang, Chongguo Tian, Shichun Zhang, Xiaoyan Ma, Fang Cao, Xiaoyan Liu, Wenqi Zhang, Thomas Kuhn, and Moritz F. Lehmann
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Di Liu, Matthias Vonwiller, Jun Li, Junwen Liu, Sönke Szidat, Yanlin Zhang, Chongguo Tian, Yinjun Chen, Zhineng Cheng, Guangcai Zhong, Pingqing Fu, and Gan Zhang
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Revised manuscript not accepted
Yan-Lin Zhang, Imad El-Haddad, Ru-Jin Huang, Kin-Fai Ho, Jun-Ji Cao, Yongming Han, Peter Zotter, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Gary Salazar, André S. H. Prévôt, and Sönke Szidat
Atmos. Chem. Phys., 18, 4005–4017, https://doi.org/10.5194/acp-18-4005-2018, https://doi.org/10.5194/acp-18-4005-2018, 2018
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Yunhua Chang, Congrui Deng, Fang Cao, Chang Cao, Zhong Zou, Shoudong Liu, Xuhui Lee, Jun Li, Gan Zhang, and Yanlin Zhang
Atmos. Chem. Phys., 17, 9945–9964, https://doi.org/10.5194/acp-17-9945-2017, https://doi.org/10.5194/acp-17-9945-2017, 2017
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Peter Zotter, Hanna Herich, Martin Gysel, Imad El-Haddad, Yanlin Zhang, Griša Močnik, Christoph Hüglin, Urs Baltensperger, Sönke Szidat, and André S. H. Prévôt
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Yan-Lin Zhang, Kimitaka Kawamura, Ping Qing Fu, Suresh K. R. Boreddy, Tomomi Watanabe, Shiro Hatakeyama, Akinori Takami, and Wei Wang
Atmos. Chem. Phys., 16, 6407–6419, https://doi.org/10.5194/acp-16-6407-2016, https://doi.org/10.5194/acp-16-6407-2016, 2016
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Junwen Liu, Jun Li, Di Liu, Ping Ding, Chengde Shen, Yangzhi Mo, Xinming Wang, Chunling Luo, Zhineng Cheng, Sönke Szidat, Yanlin Zhang, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 16, 2985–2996, https://doi.org/10.5194/acp-16-2985-2016, https://doi.org/10.5194/acp-16-2985-2016, 2016
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Many Chinese cities now are suffering the high loadings of fine particular matters, which can bring a lot of negative impacts on air quality, human health, and the climate system. The Chinese government generally focuses on the control of the emissions from vehicles and industry. Our results evidently show that the burning of biomass materials such as wood and agricultural residues can lead to the urban air pollution in China. The characteristic of haze covering China is distinct from regions.
K. R. Daellenbach, C. Bozzetti, A. Křepelová, F. Canonaco, R. Wolf, P. Zotter, P. Fermo, M. Crippa, J. G. Slowik, Y. Sosedova, Y. Zhang, R.-J. Huang, L. Poulain, S. Szidat, U. Baltensperger, I. El Haddad, and A. S. H. Prévôt
Atmos. Meas. Tech., 9, 23–39, https://doi.org/10.5194/amt-9-23-2016, https://doi.org/10.5194/amt-9-23-2016, 2016
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In this study, we developed an offline technique using the AMS for the characterization of the chemical fingerprints of aerosols collected on quartz filters, and evaluated the suitability of the organic mass spectral data for source apportionment. This technique may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.
G. O. Mouteva, S. M. Fahrni, G. M. Santos, J. T. Randerson, Y.-L. Zhang, S. Szidat, and C. I. Czimczik
Atmos. Meas. Tech., 8, 3729–3743, https://doi.org/10.5194/amt-8-3729-2015, https://doi.org/10.5194/amt-8-3729-2015, 2015
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We describe a stepwise uncertainty analysis of 14C measurements of organic (OC) and elemental (EC) carbon fractions of aerosols. Using the Swiss_4S thermal-optical protocol with a newly established trapping setup, we show that we can efficiently isolate and trap each carbon fraction and perform 14C analysis of ultra-small OC and EC samples with high accuracy and low 14C blanks. Our study presents a first step towards the development of a common protocol for OC and EC 14C measurements.
J. Gabbi, M. Huss, A. Bauder, F. Cao, and M. Schwikowski
The Cryosphere, 9, 1385–1400, https://doi.org/10.5194/tc-9-1385-2015, https://doi.org/10.5194/tc-9-1385-2015, 2015
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Light-absorbing impurities in snow and ice increase the absorption of solar radiation and thus enhance melting. We investigated the effect of Saharan dust and black carbon on the mass balance of an Alpine glacier over 1914-2014. Snow impurities increased melt by 15-19% depending on the location on the glacier. From the accumulation area towards the equilibrium line, the effect of impurities increased as more frequent years with negative mass balance led to a re-exposure of dust-enriched layers.
Y.-L. Zhang, R.-J. Huang, I. El Haddad, K.-F. Ho, J.-J. Cao, Y. Han, P. Zotter, C. Bozzetti, K. R. Daellenbach, F. Canonaco, J. G. Slowik, G. Salazar, M. Schwikowski, J. Schnelle-Kreis, G. Abbaszade, R. Zimmermann, U. Baltensperger, A. S. H. Prévôt, and S. Szidat
Atmos. Chem. Phys., 15, 1299–1312, https://doi.org/10.5194/acp-15-1299-2015, https://doi.org/10.5194/acp-15-1299-2015, 2015
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Source apportionment of fine carbonaceous aerosols using radiocarbon and other organic markers measurements during 2013 winter haze episodes was conducted at four megacities in China. Our results demonstrate that fossil emissions predominate EC with a mean contribution of 75±8%, whereas non-fossil sources account for 55±10% of OC; and the increment of TC on heavily polluted days was mainly driven by the increase of secondary OC from both fossil-fuel and non-fossil emissions.
P. Zotter, V. G. Ciobanu, Y. L. Zhang, I. El-Haddad, M. Macchia, K. R. Daellenbach, G. A. Salazar, R.-J. Huang, L. Wacker, C. Hueglin, A. Piazzalunga, P. Fermo, M. Schwikowski, U. Baltensperger, S. Szidat, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 13551–13570, https://doi.org/10.5194/acp-14-13551-2014, https://doi.org/10.5194/acp-14-13551-2014, 2014
Related subject area
Subject: Isotopes | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
On the potential fingerprint of the Antarctic ozone hole in ice-core nitrate isotopes: a case study based on a South Pole ice core
Quantifying the nitrogen isotope effects during photochemical equilibrium between NO and NO2: implications for δ15N in tropospheric reactive nitrogen
Temporal variation in 129I and 127I in aerosols from Xi'an, China: influence of East Asian monsoon and heavy haze events
Dependence between the photochemical age of light aromatic hydrocarbons and the carbon isotope ratios of atmospheric nitrophenols
Evidence for a major missing source in the global chloromethane budget from stable carbon isotopes
Atmospheric Δ17O(NO3−) reveals nocturnal chemistry dominates nitrate production in Beijing haze
Mass spectrometric measurement of hydrogen isotope fractionation for the reactions of chloromethane with OH and Cl
Stable carbon isotope ratios of ambient aromatic volatile organic compounds
Kinetic isotope effects of 12CH3D + OH and 13CH3D + OH from 278 to 313 K
Investigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputs
Chlorine isotope composition in chlorofluorocarbons CFC-11, CFC-12 and CFC-113 in firn, stratospheric and tropospheric air
NOx cycle and the tropospheric ozone isotope anomaly: an experimental investigation
Fractionation of sulfur isotopes during heterogeneous oxidation of SO2 on sea salt aerosol: a new tool to investigate non-sea salt sulfate production in the marine boundary layer
Sulfur isotope fractionation during oxidation of sulfur dioxide: gas-phase oxidation by OH radicals and aqueous oxidation by H2O2, O3 and iron catalysis
Molecular hydrogen (H2) emissions and their isotopic signatures (H/D) from a motor vehicle: implications on atmospheric H2
Isotope effect in the formation of H2 from H2CO studied at the atmospheric simulation chamber SAPHIR
Pressure dependence of the deuterium isotope effect in the photolysis of formaldehyde by ultraviolet light
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Jianghanyang Li, Xuan Zhang, John Orlando, Geoffrey Tyndall, and Greg Michalski
Atmos. Chem. Phys., 20, 9805–9819, https://doi.org/10.5194/acp-20-9805-2020, https://doi.org/10.5194/acp-20-9805-2020, 2020
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Nitrogen isotopic compositions of atmospheric reactive nitrogen are widely used to infer their sources. However, the reactions between NO and NO2 strongly impact their isotopes, which was not well understood. We conducted a series of experiments in an atmospheric simulation chamber to determine the isotopic effects of (1) direct isotopic exchange between NO and NO2 and (2) the isotopic fractionations during NOx photochemistry, then developed an equation to quantify the overall isotopic effect.
Luyuan Zhang, Xiaolin Hou, Sheng Xu, Tian Feng, Peng Cheng, Yunchong Fu, and Ning Chen
Atmos. Chem. Phys., 20, 2623–2635, https://doi.org/10.5194/acp-20-2623-2020, https://doi.org/10.5194/acp-20-2623-2020, 2020
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To trace the long-range transport of air pollutants and understand the atmospheric effect of iodine, the daily-resolution temporal variations of 129I and 127I in aerosols from a monsoonal city indicate the East Asian monsoon and fossil fuel combustion plays crucial roles on transport of 129I from Europe to East Asia and on elevated 127I concentrations. Through linking iodine isotopes with five major air pollutants, this study proposes the possible role of iodine in urban air pollution.
Marina Saccon, Anna Kornilova, Lin Huang, and Jochen Rudolph
Atmos. Chem. Phys., 19, 5495–5509, https://doi.org/10.5194/acp-19-5495-2019, https://doi.org/10.5194/acp-19-5495-2019, 2019
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As compound are emitted into the atmosphere, they can undergo chemical reactions to produce secondary products. This paper investigates the relations of compounds' unique chemical characteristics to the processes that formed them from emissions in the atmosphere. A model is applied to help with this investigation. The complexity of the atmosphere, including mixing of air masses and variability in precursor reactivity, is taken into consideration, and results are presented.
Enno Bahlmann, Frank Keppler, Julian Wittmer, Markus Greule, Heinz Friedrich Schöler, Richard Seifert, and Cornelius Zetzsch
Atmos. Chem. Phys., 19, 1703–1719, https://doi.org/10.5194/acp-19-1703-2019, https://doi.org/10.5194/acp-19-1703-2019, 2019
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Chloromethane is the most important natural carrier of chlorine to the stratosphere. From a newly determined carbon isotope effect of −11.2 ‰ for the tropospheric loss of CH3Cl we derive a tropical rainforest CH3Cl source of 670 ± 200 Gg a−1, 60 % smaller than previous estimates. A revision of previous bottom-up estimates using above-ground biomass instead of rainforest area strongly supports this lower estimate. Our results suggest a large unknown tropical value of 1530 ± 200 Gg a−1.
Pengzhen He, Zhouqing Xie, Xiyuan Chi, Xiawei Yu, Shidong Fan, Hui Kang, Cheng Liu, and Haicong Zhan
Atmos. Chem. Phys., 18, 14465–14476, https://doi.org/10.5194/acp-18-14465-2018, https://doi.org/10.5194/acp-18-14465-2018, 2018
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We present the first observations of the oxygen-17 excess of atmospheric nitrate (Δ17O(NO−3)) collected in Beijing haze to reveal the relative importance of different nitrate formation pathways. We found that nocturnal pathways (N2O5 + H2O/Cl– and NO3 + HC) dominated nitrate production during polluted days (PM2.5 ≥ 75 μg m–3), with a mean possible fraction of 56–97 %.
Frank Keppler, Enno Bahlmann, Markus Greule, Heinz Friedrich Schöler, Julian Wittmer, and Cornelius Zetzsch
Atmos. Chem. Phys., 18, 6625–6635, https://doi.org/10.5194/acp-18-6625-2018, https://doi.org/10.5194/acp-18-6625-2018, 2018
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Chloromethane is involved in stratospheric ozone depletion, but detailed knowledge of its global budget is missing. In this study stable hydrogen isotope analyses were performed to investigate the dominant loss process for atmospheric chloromethane with photochemically produced hydroxyl radicals. The findings might have significant implications for the use of stable isotope signatures in elucidation of global chloromethane cycling.
Anna Kornilova, Lin Huang, Marina Saccon, and Jochen Rudolph
Atmos. Chem. Phys., 16, 11755–11772, https://doi.org/10.5194/acp-16-11755-2016, https://doi.org/10.5194/acp-16-11755-2016, 2016
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The photochemical oxidation of organic compounds in the atmosphere results in the formation of important secondary pollutants such as ozone and fine particles. The extent of oxidation the organic compounds have been subjected too since there emissions is essential is key for understanding the formation of secondary pollutants. This paper demonstrates that measurements of the carbon isotope ratios allow determining the extent of photochemical processing for individual compounds.
L. M. T. Joelsson, J. A. Schmidt, E. J. K. Nilsson, T. Blunier, D. W. T. Griffith, S. Ono, and M. S. Johnson
Atmos. Chem. Phys., 16, 4439–4449, https://doi.org/10.5194/acp-16-4439-2016, https://doi.org/10.5194/acp-16-4439-2016, 2016
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We present experimental kinetic isotope effects (KIE) for the OH oxidation of CH3D and 13CH3D and their temperature dependence. Our determination of the 13CH3D + OH KIE is novel and we find no "clumped" isotope effect within the experimental uncertainty.
G. Shi, A. M. Buffen, M. G. Hastings, C. Li, H. Ma, Y. Li, B. Sun, C. An, and S. Jiang
Atmos. Chem. Phys., 15, 9435–9453, https://doi.org/10.5194/acp-15-9435-2015, https://doi.org/10.5194/acp-15-9435-2015, 2015
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We evaluate isotopic composition of NO3- in different environments across East Antarctica. At high snow accumulation sites, isotopic ratios are suggestive of preservation of NO3- deposition. At low accumulation sites, isotopes are sensitive to both the loss of NO3- due to photolysis and secondary formation of NO3- within the snow. The imprint of post-depositional alteration is not uniform with depth, making it difficult to predict the isotopic composition at depth from near-surface data alone.
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
G. Michalski, S. K. Bhattacharya, and G. Girsch
Atmos. Chem. Phys., 14, 4935–4953, https://doi.org/10.5194/acp-14-4935-2014, https://doi.org/10.5194/acp-14-4935-2014, 2014
E. Harris, B. Sinha, P. Hoppe, S. Foley, and S. Borrmann
Atmos. Chem. Phys., 12, 4619–4631, https://doi.org/10.5194/acp-12-4619-2012, https://doi.org/10.5194/acp-12-4619-2012, 2012
E. Harris, B. Sinha, P. Hoppe, J. N. Crowley, S. Ono, and S. Foley
Atmos. Chem. Phys., 12, 407–423, https://doi.org/10.5194/acp-12-407-2012, https://doi.org/10.5194/acp-12-407-2012, 2012
M. K. Vollmer, S. Walter, S. W. Bond, P. Soltic, and T. Röckmann
Atmos. Chem. Phys., 10, 5707–5718, https://doi.org/10.5194/acp-10-5707-2010, https://doi.org/10.5194/acp-10-5707-2010, 2010
T. Röckmann, S. Walter, B. Bohn, R. Wegener, H. Spahn, T. Brauers, R. Tillmann, E. Schlosser, R. Koppmann, and F. Rohrer
Atmos. Chem. Phys., 10, 5343–5357, https://doi.org/10.5194/acp-10-5343-2010, https://doi.org/10.5194/acp-10-5343-2010, 2010
E. J. K. Nilsson, V. F. Andersen, H. Skov, and M. S. Johnson
Atmos. Chem. Phys., 10, 3455–3462, https://doi.org/10.5194/acp-10-3455-2010, https://doi.org/10.5194/acp-10-3455-2010, 2010
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Short summary
A novel method to determine the concentration and the isotopes of WSOC in aerosols is established and applied in the analysis of a severe haze in eastern China. The results show that the studied site is affected by the photochemical aging, biomass burning and dust aerosols in different episodes during the sampling period. The analysis of WSOC and its isotopes offers a great potential to better understand the source emission, the atmospheric aging and the secondary production of WSOC.
A novel method to determine the concentration and the isotopes of WSOC in aerosols is...
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