Modern and Fossil Contributions to Polycyclic Aromatic Hydrocarbons in PM2.5 from North Birmingham, Alabama in the Southeastern U.S.Click to copy article linkArticle link copied!
Abstract

Analyzing the radiocarbon (14C) content of polycyclic aromatic hydrocarbons (PAHs) in atmospheric particulate matter can provide estimates on the source contributions from biomass burning versus fossil fuel. The relative importance of these two sources to ambient PAHs varies considerably across regions and even countries, and hence there is a pressing need to apportion these sources. In this study, we advanced the radiocarbon analysis from bulk carbon to compound class specific radiocarbon analysis (CCSRA) to determine Δ14C and δ13C values of PAHs in PM2.5 samples for investigating biomass burning and fossil fuel source contributions to PAHs from one of the Southeastern Aerosol Research and Characterization (SEARCH) sites in North Birmingham (BHM), Alabama during winter (December 2004-February 2005) and summer (June-August 2005) by accelerator mass spectrometry. To compare our ambient samples to known sources, we collected and analyzed fenceline samples from the vicinity of a coke plant in BHM. As expected, PAHs from the coke plant fenceline samples had very low radiocarbon levels. Its Δ14C varied from −990 to −970‰, indicating that 97 to 99% were of fossil source. PAHs in the ambient PM2.5 had Δ14C from −968 to −911 ‰, indicating that 92–97% of PAHs were from fossil fuel combustion. These levels indicated the dominance of fossil sources of ambient PAHs. The radiocarbon level of ambient PAHs was higher in winter than in summer. Winter samples exhibited depleted δ13C value and enriched Δ14C value because of the increased contribution of PAHs from biomass burning source. However, biomass burning contributed more to heavier PAHs (modern source accounting for 6–8%) than lighter ones with a modern contribution of 3%.
Cited By
Smart citations by scite.ai include citation statements extracted from the full text of the citing article. The number of the statements may be higher than the number of citations provided by ACS Publications if one paper cites another multiple times or lower if scite has not yet processed some of the citing articles.
This article is cited by 27 publications.
- Tiangang Tang, Zhineng Cheng, Buqing Xu, Bolong Zhang, Sanyuan Zhu, Hairong Cheng, Jun Li, Yingjun Chen, Gan Zhang. Triple Isotopes (δ13C, δ2H, and Δ14C) Compositions and Source Apportionment of Atmospheric Naphthalene: A Key Surrogate of Intermediate-Volatility Organic Compounds (IVOCs). Environmental Science & Technology 2020, 54
(9)
, 5409-5418. https://doi.org/10.1021/acs.est.0c00075
- Miaolei Ya, Li Xu, Yuling Wu, Yongyu Li, Songhe Zhao, Xinhong Wang. Fossil Fuel-Derived Polycyclic Aromatic Hydrocarbons in the Taiwan Strait, China, and Fluxes across the Air–Water Interface. Environmental Science & Technology 2018, 52
(13)
, 7307-7316. https://doi.org/10.1021/acs.est.8b01331
- Hong-Xi Zhang . Determination of Aromatic Structures of Bituminous Coal Using Sequential Oxidation. Industrial & Engineering Chemistry Research 2016, 55
(10)
, 2798-2805. https://doi.org/10.1021/acs.iecr.5b04899
- Josué J. Jautzy, Jason M. E. Ahad, Roland I. Hall, Johan A. Wiklund, Brent B. Wolfe, Charles Gobeil, and Martine M. Savard . Source Apportionment of Background PAHs in the Peace-Athabasca Delta (Alberta, Canada) Using Molecular Level Radiocarbon Analysis. Environmental Science & Technology 2015, 49
(15)
, 9056-9063. https://doi.org/10.1021/acs.est.5b01490
- Carme Bosch, August Andersson, Martin Kruså, Cecilia Bandh, Ivana Hovorková, Jana Klánová, Timothy D. J. Knowles, Richard D. Pancost, Richard P. Evershed, and Örjan Gustafsson . Source Apportionment of Polycyclic Aromatic Hydrocarbons in Central European Soils with Compound-Specific Triple Isotopes (δ13C, Δ14C, and δ2H). Environmental Science & Technology 2015, 49
(13)
, 7657-7665. https://doi.org/10.1021/acs.est.5b01190
- G. F. Slater, A. A. Benson, C. Marvin, and D. Muir . PAH Fluxes to Siskiwit Revisted: Trends in Fluxes and Sources of Pyrogenic PAH and Perylene Constrained via Radiocarbon Analysis. Environmental Science & Technology 2013, 47
(10)
, 5066-5073. https://doi.org/10.1021/es400272z
- Yu Fu, Rui Zhang, Shaopeng Rong, Yuling Wu, Ying Wu, Miaolei Ya. A methodological review of compound-specific radiocarbon analysis for polycyclic aromatic hydrocarbons in environmental matrices. Environmental Pollution 2024, 350 , 124050. https://doi.org/10.1016/j.envpol.2024.124050
- Jianjun Li, Xiaoqing Wang, Wenting Dai, Weining Qi, Haijiao Liu, Minxia Shen, Yali Liu, Xiao Guo, Yifan Zhang, Lu Li, Yue Cao, Lijuan Li, Yukun Chen, Qiao Feng. Molecular compositions and stable carbon isotopes (δ13C) of PAHs in wintertime PM2.5 in urban Xi'an, China: Implications for source distribution and atmospheric oxidation. Atmospheric Research 2023, 292 , 106890. https://doi.org/10.1016/j.atmosres.2023.106890
- Xin Yi, Xiaofei Geng, Yangzhi Mo, Guangcai Zhong, Jiao Tang, Sanyuan Zhu, Zhineng Cheng, Shizhen Zhao, Jun Li, Örjan Gustafsson, Ping'an Peng, Gan Zhang. Compound-specific radiocarbon analysis of benzene polycarboxylic acids for source apportionment of polyaromatic organic matter in ambient aerosols. Atmospheric Environment 2023, 307 , 119832. https://doi.org/10.1016/j.atmosenv.2023.119832
- Lian Duan, Huimin Yu, Qiongzhen Wang, Yibo Cao, Guochen Wang, Xueshi Sun, Hao Li, Tian Lin, Zhigang Guo. PM2.5-bound polycyclic aromatic hydrocarbons of a megacity in eastern China: Source apportionment and cancer risk assessment. Science of The Total Environment 2023, 869 , 161792. https://doi.org/10.1016/j.scitotenv.2023.161792
- Boyang Tian, Shutao Gao, Zhanjun Zhu, Xiangying Zeng, Yi Liang, Zhiqiang Yu, Ping'an Peng. Two-dimensional gas chromatography coupled to isotope ratio mass spectrometry for determining high molecular weight polycyclic aromatic hydrocarbons in sediments. Journal of Chromatography A 2023, 1693 , 463879. https://doi.org/10.1016/j.chroma.2023.463879
- Di Huang, Lirong Gao, Minghui Zheng, Lin Qiao, Chi Xu, Kunran Wang, Shuang Wang. Screening organic contaminants in soil by two-dimensional gas chromatography high-resolution time-of-flight mass spectrometry: A non-target analysis strategy and contaminated area case study. Environmental Research 2022, 205 , 112420. https://doi.org/10.1016/j.envres.2021.112420
- Miaolei Ya, Yuling Wu, Xinhong Wang, Yongyu Li, Guanyong Su. The importance of compound-specific radiocarbon analysis in source identification of polycyclic aromatic hydrocarbons: A critical review. Critical Reviews in Environmental Science and Technology 2022, 52
(6)
, 937-978. https://doi.org/10.1080/10643389.2020.1843305
- Miaolei Ya, Yuling Wu, Li Xu, Yongyu Li, Hanzhe Chen, Xinhong Wang. Compound-specific radiocarbon reveals sources and land–sea transport of polycyclic aromatic hydrocarbons in an urban estuary. Water Research 2021, 198 , 117134. https://doi.org/10.1016/j.watres.2021.117134
- Gan Zhang, Junwen Liu, Jing Li, Pingyang Li, Nannan Wei, Buqing Xu. Radiocarbon isotope technique as a powerful tool in tracking anthropogenic emissions of carbonaceous air pollutants and greenhouse gases: A review. Fundamental Research 2021, 1
(3)
, 306-316. https://doi.org/10.1016/j.fmre.2021.03.007
- Lujie Ren, Yiyun Wang, Kimitaka Kawamura, Srinivas Bikkina, Negar Haghipour, Lukas Wacker, Chandra Mouli Pavuluri, Zhimin Zhang, Siyao Yue, Yele Sun, Zifa Wang, Yanli Zhang, Xiaojuan Feng, Cong-Qiang Liu, Timothy I Eglinton, Pingqing Fu. Source forensics of n-alkanes and n-fatty acids in urban aerosols using compound specific radiocarbon/stable carbon isotopic composition. Environmental Research Letters 2020, 15
(7)
, 074007. https://doi.org/10.1088/1748-9326/ab8333
- Peng Gao, Hongbo Li, Chris P. Wilson, Timothy G. Townsend, Ping Xiang, Yungen Liu, Lena Q. Ma. Source identification of PAHs in soils based on stable carbon isotopic signatures. Critical Reviews in Environmental Science and Technology 2018, 48
(13-15)
, 923-948. https://doi.org/10.1080/10643389.2018.1495983
- U M Hanke, L Wacker, N Haghipour, M W I Schmidt, T I Eglinton, C P McIntyre. Comprehensive radiocarbon analysis of benzene polycarboxylic acids (BPCAs) derived from pyrogenic carbon in environmental samples. Radiocarbon 2017, 59
(4)
, 1103-1116. https://doi.org/10.1017/RDC.2017.44
- Yue Liu, Caiqing Yan, Xiang Ding, Xinming Wang, Qingyan Fu, Qianbiao Zhao, Yihua Zhang, Yusen Duan, Xinghua Qiu, Mei Zheng. Sources and spatial distribution of particulate polycyclic aromatic hydrocarbons in Shanghai, China. Science of The Total Environment 2017, 584-585 , 307-317. https://doi.org/10.1016/j.scitotenv.2016.12.134
- Jing-Sha Xu, Hong-Hui Xu, Hang Xiao, Lei Tong, Colin E. Snape, Cheng-Jun Wang, Jun He. Aerosol composition and sources during high and low pollution periods in Ningbo, China. Atmospheric Research 2016, 178-179 , 559-569. https://doi.org/10.1016/j.atmosres.2016.05.006
- Ye Li, Xinran Liu, Min Liu, Xiaofei Li, Fei Meng, Juan Wang, Wenjun Yan, Xianbiao Lin, Junmin Zhu, Yukun Qin. Investigation into atmospheric PM
2.5
-borne PAHs in Eastern cities of China: concentration, source diagnosis and health risk assessment. Environmental Science: Processes & Impacts 2016, 18
(5)
, 529-537. https://doi.org/10.1039/C6EM00012F
- Danilo Sciarrone, Sebastiano Pantò, Carla Ragonese, Paola Dugo, Luigi Mondello. Evolution and status of preparative gas chromatography as a green sample-preparation technique. TrAC Trends in Analytical Chemistry 2015, 71 , 65-73. https://doi.org/10.1016/j.trac.2015.02.024
- Daniel B. Wiedemeier, Sonja Brodowski, Guido L.B. Wiesenberg. Pyrogenic molecular markers: Linking PAH with BPCA analysis. Chemosphere 2015, 119 , 432-437. https://doi.org/10.1016/j.chemosphere.2014.06.046
- Gui-Rong Liu, Guo-Liang Shi, Ying-Ze Tian, Yi-Nan Wang, Cai-Yan Zhang, Yin-Chang Feng. Physically constrained source apportionment (PCSA) for polycyclic aromatic hydrocarbon using the Multilinear Engine 2-species ratios (ME2-SR) method. Science of The Total Environment 2015, 502 , 16-21. https://doi.org/10.1016/j.scitotenv.2014.09.011
- Mathew R. Heal. The application of carbon-14 analyses to the source apportionment of atmospheric carbonaceous particulate matter: a review. Analytical and Bioanalytical Chemistry 2014, 406
(1)
, 81-98. https://doi.org/10.1007/s00216-013-7404-1
- Xinyu Zhang, Liang Zhao, Yexin Wang, Yunping Xu, Liping Zhou. Optimization of programmed‐temperature vaporization injection preparative capillary GC for compound specific radiocarbon analysis. Journal of Separation Science 2013, 36
(13)
, 2136-2144. https://doi.org/10.1002/jssc.201300088
- A.J. Buczyńska, B. Geypens, R. Van Grieken, K. De Wael. Stable carbon isotopic ratio measurement of polycyclic aromatic hydrocarbons as a tool for source identification and apportionment—A review of analytical methodologies. Talanta 2013, 105 , 435-450. https://doi.org/10.1016/j.talanta.2012.10.075
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.