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Observations of C1-C5 Alkyl Nitrates in the Yellow River Delta, Northern China: Effects of Biomass Burning and Oil Field Emissio

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Observations of C1-C5 Alkyl Nitrates in the Yellow River Delta, Northern China: Effects of Biomass Burning and Oil Field Emissio Science of the Total Environment 656 (2019) 129–139 Contents lists available at ScienceDirect Science of the Total Environment journal homepage: www.elsevier.com/locate/scitotenv Observations of C1–C5 alkyl nitrates in the Yellow River Delta, northern China: Effects of biomass burning and oil field emissions Yingnan Zhang a, Jingjing Sun a,PenggangZhenga, Tianshu Chen a, Yuhong Liu a, Guangxuan Han b, Isobel J. Simpson c, Xinfeng Wang a,DonaldR.Blakec,ZeyuanLia, Xue Yang a,YanbinQid,e,QiWangd,e, Wenxing Wang a, Likun Xue a,f,⁎ a Environment Research Institute, Shandong University, Ji'nan, Shandong, China b Key Laboratory of Coastal Environmental Process and Ecology Remediation, Yantai Institute of Coastal Zone Research, Chinese Academy of Sciences, Yantai, Shandong, China c Department of Chemistry, University of California at Irvine, Irvine, CA, United States d Jilin Weather Modification Office, Changchun, Jilin, China e Joint Laboratory of Weather Modification for Chinese Meteorological Administration and People's Government of Jilin Province (Key Laboratory of Jilin Province), Changchun, Jilin, China f Ji'nan Institute of Environmental Science, Ji'nan, Shandong, China HIGHLIGHTS GRAPHICAL ABSTRACT • The tempo-spatial variations of C1-C5 alkyl nitrates and parent hydrocarbons were examined in the Yellow River Delta. • Oil field emissions and biomass burning are important sources of hydrocarbons and alkyl nitrates in this region. • Besides parent hydrocarbons, longer alkanes are important precursors of alkyl nitrates in oil fields. article info abstract Article history: Alkyl nitrates (RONO2) are important reservoirs of nitrogen oxides and play key roles in the tropospheric chem- Received 26 September 2018 istry. Two phases of intensive campaigns were conducted during February–April and June–July of 2017 at a rural Received in revised form 14 November 2018 coastal site and in open oil fields of the Yellow River Delta region, northern China. C1–C5 alkyl nitrates showed Accepted 14 November 2018 higher concentration levels in summer than in winter-spring (p b 0.01), whilst their parent hydrocarbons Available online 15 November 2018 showed an opposite seasonal variation pattern. The C3–C5 RONO2 levels in the oil fields were significantly higher fi Editor: Jianmin Chen than those in the ambient rural air. Alkyl nitrates showed well-de ned diurnal variations, elucidating the effects of in-situ photochemical production and regional transport of aged polluted plumes. Backward trajectory analy- Keywords: sis and fire maps revealed the significant contribution of biomass burning to the observed alkyl nitrates and hy- Alkyl nitrate drocarbons. A simplified sequential reaction model and an observation-based chemical box model were fi Oil eld deployed to diagnose the formation mechanisms of C1–C5 RONO2. The C3–C5 RONO2 were mainly produced Biomass burning from the photochemical oxidation of their parent hydrocarbons (i.e., C3–C5 alkanes), whilst C1–C2 RONO2 com- Observation-based model pounds have additional sources. In addition to parent hydrocarbons, longer alkanes with N4 carbon atoms were also important precursors of alkyl nitrates in the oil fields. This study demonstrates the significant effects ⁎ Corresponding author at: Environment Research Institute, Shandong University, Ji'nan, Shandong, China. E-mail address: [email protected] (L. Xue). https://doi.org/10.1016/j.scitotenv.2018.11.208 0048-9697/© 2018 Elsevier B.V. All rights reserved. 130 Y. Zhang et al. / Science of the Total Environment 656 (2019) 129–139 Sequential reaction model of oil field emissions and biomass burning on the volatile organic compounds and alkyl nitrate formation, and Yellow River Delta provides scientific support for the formulation of control strategies against photochemical air pollution in the Yel- low River Delta region. © 2018 Elsevier B.V. All rights reserved. 1. Introduction circumstances. In coastal areas, for example, marine emissions are an important source of shorter-chain RONO2, especially methyl nitrate Alkyl nitrates (RONO2) are an important family member of the reac- (Atlas et al., 1993; Blake et al., 2003; Song et al., 2018). Biomass burning tive odd nitrogen (NOy =NO+NO2 +NO3 +N2O5 + HONO + HNO3 has been also recognized as a significant source contributing to the am- − +NO3 + PANs + RONO2 + etc.), which are crucial players of atmo- bient RONO2 (Simpson et al., 2002). Identification of the principal spheric chemistry and have significant consequences to regional air sources and secondary formation mechanisms is fundamental to formu- quality, ecosystem, and climate change (Jenkin and Clemitshaw, lating the control strategies against alkyl nitrate pollution in a specific 2000). They have relatively low chemical reactivity, and can release region. NO2 via photolysis (Atkinson et al., 2006; Sommariva et al., 2008). Due In recent decades, photochemical air pollution characterized by high to this nature, alkyl nitrates can serve as temporary reservoirs of nitro- concentrations of O3 and other secondary pollutants (such as PANs and gen oxides (NOx =NO+NO2) during long-range transport, re- RONO2, etc.) has become a major environmental concern in China, as a distribute NOx between urban and rural (or remote) areas, and hence result of its fast urbanization process (Wang et al., 2006; Wang et al., affect the regional and even global ozone (O3) formation (Day et al., 2017; Xue et al., 2014a). A number of field studies have been carried 2003). Thus, investigation of characteristics and sources of alkyl nitrates out to evaluate the characteristics and formation mechanisms of O3 pol- is an important step towards better understanding of the formation of lution in the fast developing regions of China, such as the Jing-Jin-Ji re- regional photochemical pollution. gion, Pearl River Delta, and Yangtze River Delta (Wang et al., 2017; In the troposphere, alkyl nitrates are mainly formed through photo- and references therein), whilst relatively limited efforts have focused chemical degradation of volatile organic compounds (VOCs) in the pres- on alkyl nitrates (Ling et al., 2016; Lyu et al., 2015; Sun et al., 2018; ence of NOx (Arey et al., 2001; Atkinson et al., 2006). Briefly, oxidation of Wang et al., 2013). The Yellow River Delta region (YelRD) is located in hydrocarbons by the hydroxyl radical (OH) produces a RO2 radical, the mouth of the Yellow River in Shandong province, and lies in be- which can then react with NO to yield RONO2 (Arey et al., 2001). For tween the Shandong Peninsula and Beijing-Tianjin area (see Fig. 1). each RONO2 species, there are only a small number of precursor hydro- With a population of 10 million, it is home to the second largest oil carbons, the degradation of which can exactly yield the specificRO2 rad- field (Shengli Oil Field) in China with numerous refinery and petro- ical (e.g., CH3O2 for methyl nitrate, C2H5O2 for ethyl nitrate, etc.). In chemical plants, and now is one of the most economically dynamic re- general, the longer and more complex is the chain of the RO2 radical, gions in China. It is also an important agricultural area and a coastal the fewer are the precursor hydrocarbons of the RONO2 species. For in- wetland in northern China. Given the above features, it can be expected stance, the formation of the longer-chain (e.g., ≥C3) RONO2 is usually that the YelRD region should be suffering from serious air pollution dominated by the oxidation of parent alkanes (e.g., propane for problems, especially photochemical pollution. To the best of our knowl- PrONO2, butane for BuONO2, pentane for PeONO2, etc.), whilst C1–C2 edge, however, there have been no previous studies to investigate the RONO2 can be formed from the other VOCs that can decompose to photochemical pollution in this region and evaluate the impacts of the CH3O2 and C2H5O2 radicals, in addition to their parent alkanes oil extraction and petrochemical industries. (i.e., methane and ethane) (Russo et al., 2010; Sunetal.,2018). Besides, To investigate the photochemical air pollution and its formation ambient alkyl nitrates are also subject to primary emissions in specific mechanisms in the YelRD region, intensive field campaigns were Fig. 1. Maps showing the Yellow River Delta region (YelRD) as well as the locations of the study site and oil field samples. The emission data of non-methane VOCs were taken from Li et al. (2017). Y. Zhang et al. / Science of the Total Environment 656 (2019) 129–139 131 conducted at a rural site surrounded by oil fields and directly in the Table 1 open oil fields during selected months of 2017. A large suite of air pollut- Detailed information of instrument techniques used in the present study. ants and meteorological parameters were measured in-situ. This paper Species Instrument techniques Detection limit (ppbv) Precision analyzes the tempo-spatial variations, sources, and secondary forma- a O3 T-API , model T400 0.4 0.5% tion regimes of C –C RONO in the YelRD region. Elevated concentra- a 1 5 2 NO & NOy T-API , model T200U 0.05 0.5% a tions of alkyl nitrates were observed in the oil fields, where longer NO2 T-API , model T500U 0.04 0.5% CO T-APIa, T300U 20 0.5% chain alkanes are important RONO2 precursors besides the well- b known short chain parent hydrocarbons. Oil field emissions and bio- SO2 TEI , model 43C 1 1% HONO QUMA, model LOPAP-03 0.003 1% mass burning are major sources of alkyl nitrates and photochemical a air pollution in the region. Overall, this study provides some new in- T-API: Teledyne Advanced Pollution Instrumentation. b TEI: Thermo Electron Instruments. sights into the characterization and sources of alkyl nitrates in the oil- extracting areas, and can support the formulation of control strategies against photochemical pollution in the YelRD region. Real-time measurements of related traces gases and meteorological parameters were also carried out. The detailed information of the in- 2. Methodology strument techniques and their corresponding detection limit and preci- sion is summarized in Table 1.
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