Non-methane hydrocarbon (C2-C8) sources and sinks around the Arabian Peninsula

被引:42
作者
Bourtsoukidis, Efstratios [1 ]
Ernle, Lisa [1 ]
Crowley, John N. [1 ]
Lelieveld, Jos [1 ]
Paris, Jean-Daniel [2 ]
Pozzer, Andrea [1 ]
Walter, David [3 ]
Williams, Jonathan [1 ]
机构
[1] Max Planck Inst Chem, Dept Atmospher Chem, D-55128 Mainz, Germany
[2] UVSQ, CNRS, CEA, Lab Sci Climat & Environm,IPSL,UMR8212, Gif Sur Yvette, France
[3] Max Planck Inst Chem, Dept Multiphase Chem, D-55128 Mainz, Germany
关键词
VOLATILE ORGANIC-COMPOUNDS; GLOBAL ATMOSPHERIC ETHANE; NATURAL-GAS OPERATIONS; AIR-POLLUTION; REACTIVE CHLORINE; PHASE REACTIONS; TRACE GASES; VARIABILITY; EMISSIONS; METHANE;
D O I
10.5194/acp-19-7209-2019
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Atmospheric non-methane hydrocarbons (NMHCs) have been extensively studied around the globe due to their importance to atmospheric chemistry and their utility in emission source and chemical sink identification. This study reports on shipborne NMHC measurements made around the Arabian Peninsula during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign. The ship traversed the Mediterranean Sea, the Suez Canal, the Red Sea, the northern Indian Ocean, and the Arabian Gulf, before returning by the same route. The Middle East is one of the largest producers of oil and gas (O&G), yet it is among the least studied. Atmospheric mixing ratios of C-2-C-8 hydrocarbons ranged from a few ppt in unpolluted regions (Arabian Sea) to several ppb over the Suez Canal and Arabian Gulf (also known as the Persian Gulf), where a maximum of 166.5 ppb of alkanes was detected. The ratio between i -pentane and n-pentane was found to be 0.93 +/- 0.03 ppb ppb(-1) over the Arabian Gulf, which is indicative of widespread O&G activities, while it was 1.71 +/- 0.06 ppb ppb(-1) in the Suez Canal, which is a characteristic signature of ship emissions. We provide evidence that international shipping contributes to ambient C-3-C-8 hydrocarbon concentrations but not to ethane, which was not detected in marine traffic exhausts. NMHC relationships with propane differentiated between alkane-rich associated gas and methane-rich non-associated gas through a characteristic enrichment of ethane over propane atmospheric mixing ratios Utilizing the variability- lifetime relationship, we show that atmospheric chemistry governs the variability of the alkanes only weakly in the source-dominated areas of the Arabian Gulf (b(AG) = 0.16) and along the northern part of the Red Sea (b(RSN) = 0.22), but stronger dependencies are found in unpolluted regions such as the Gulf of Aden (b(GA) = 0.58) and the Mediterranean Sea (b(MS) = 0.48). NMHC oxidative pair analysis indicated that OH chemistry dominates the oxidation of hydrocarbons in the region, but along the Red Sea and the Arabian Gulf the NMHC ratios occasionally provided evidence of chlorine radical chemistry. These results demonstrate the utility of NMHCs as source/sink identification tracers and provide an overview of NMHCs around the Arabian Peninsula.
引用
收藏
页码:7209 / 7232
页数:24
相关论文
共 99 条
[41]  
HELMIG D, 1995, HRC-J HIGH RES CHROM, V18, P15
[42]  
Helmig D, 2016, NAT GEOSCI, V9, P490, DOI [10.1038/NGEO2721, 10.1038/ngeo2721]
[43]   Speciation of anthropogenic emissions of non-methane volatile organic compounds: a global gridded data set for 1970-2012 [J].
Huang, Ganlin ;
Brook, Rosie ;
Crippa, Monica ;
Janssens-Maenhout, Greet ;
Schieberle, Christian ;
Dore, Chris ;
Guizzardi, Diego ;
Muntean, Marilena ;
Schaaf, Edwin ;
Friedrich, Rainer .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2017, 17 (12) :7683-7701
[44]   Trace gas mixing ratio variability versus lifetime in the troposphere and stratosphere: Observations [J].
Jobson, BT ;
McKeen, SA ;
Parrish, DD ;
Fehsenfeld, FC ;
Blake, DR ;
Goldstein, AH ;
Schauffler, SM ;
Elkins, JC .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D13) :16091-16113
[45]   Hydrocarbon source signatures in Houston, Texas: Influence of the petrochemical industry [J].
Jobson, BT ;
Berkowitz, CM ;
Kuster, WC ;
Goldan, PD ;
Williams, EJ ;
Fesenfeld, FC ;
Apel, EC ;
Karl, T ;
Lonneman, WA ;
Riemer, D .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D24) :1-26
[46]   MEASUREMENTS OF C-2-C-6 HYDROCARBONS DURING THE POLAR SUNRISE 1992 EXPERIMENT - EVIDENCE FOR CL ATOM AND BR ATOM CHEMISTRY [J].
JOBSON, BT ;
NIKI, H ;
YOKOUCHI, Y ;
BOTTENHEIM, J ;
HOPPER, F ;
LEAITCH, R .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1994, 99 (D12) :25355-25368
[47]   Spatial and temporal variability of nonmethane hydrocarbon mixing ratios and their relation to photochemical lifetime [J].
Jobson, BT ;
Parrish, DD ;
Goldan, P ;
Kuster, W ;
Fehsenfeld, FC ;
Blake, DR ;
Blake, NJ ;
Niki, H .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1998, 103 (D11) :13557-13567
[48]   Development cycle 2 of the Modular Earth Submodel System (MESSy2) [J].
Joeckel, P. ;
Kerkweg, A. ;
Pozzer, A. ;
Sander, R. ;
Tost, H. ;
Riede, H. ;
Baumgaertner, A. ;
Gromov, S. ;
Kern, B. .
GEOSCIENTIFIC MODEL DEVELOPMENT, 2010, 3 (02) :717-752
[49]   RESIDENCE TIME AND VARIABILITY OF TROPOSPHERIC TRACE GASES [J].
JUNGE, CE .
TELLUS, 1974, 26 (04) :477-488
[50]   Composite global emissions of reactive chlorine from anthropogenic and natural sources: Reactive Chlorine Emissions Inventory [J].
Keene, WC ;
Khalil, MAK ;
Erickson, DJ ;
McCulloch, A ;
Graedel, TE ;
Lobert, JM ;
Aucott, ML ;
Gong, SL ;
Harper, DB ;
Kleiman, G ;
Midgley, P ;
Moore, RM ;
Seuzaret, C ;
Sturges, WT ;
Benkovitz, CM ;
Koropalov, V ;
Barrie, LA ;
Li, YF .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D7) :8429-8440