Estimate of anthropogenic halocarbon emission based on measured ratio relative to CO in the Pearl River Delta region, China

被引:77
作者
Shao, M. [1 ]
Huang, D. [1 ]
Gu, D. [1 ]
Lu, S. [1 ]
Chang, C. [2 ]
Wang, J. [3 ]
机构
[1] Peking Univ, Coll Environm Sci & Engn, State Joint Key Lab Environm Simulat & Pollut Con, Beijing 100871, Peoples R China
[2] Acad Sinica, Res Ctr Environm Changes, Taipei 115, Taiwan
[3] Natl Cent Univ, Dept Chem, Chungli 320, Taiwan
关键词
METHYL CHLOROFORM EMISSIONS; MIXING RATIOS; EAST-ASIA; CHLORODIFLUOROMETHANE HCFC-22; CONCENTRATION VARIABILITY; ATMOSPHERIC CHEMISTRY; GLOBAL DISTRIBUTION; HISTORIC EMISSIONS; CHEMICAL-TRANSPORT; INTERNAL REFERENCE;
D O I
10.5194/acp-11-5011-2011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Using a GC/FID/MS system, we analyzed the mixing ratio of 16 halocarbon species in more than 100 air samples collected in 2004 from the Pearl River Delta (PRD) region of southern China. The results revealed that there are elevated mixing ratios for most of halocarbons, especially for HClC = CCl2 (trichloroethylene, TCE), CH2Cl2 (dichloromethane, DCM), CH3 Br (bromomethane), HCFC-22, CHCl3 (trichloromethane), CCl4 (tetrachloromethane), Cl2C = CCl2 (perchloroethylene, PCE), CH3CCl3 (methyl chloroform, MCF), and CFC-12. Comparisons were done with the data from TRACE-P and ALE/GAGE/AGAGE experiments, we found that the large variability in mixing ratios (relative standard deviation ranged from 9.31% to 96.55 %) of the halocarbons suggested substantial local emissions from the PRD region in 2004. Correlations between the mixing ratio of each species and carbon monoxide (CO) was examined, and then the emission of each halocarbon was quantified based on scaling the optimized CO emission inventory with the slope of the regression line fitted to each species relative to CO. The calculated results revealed that mass of CH2Cl2 (7.0 Gg), CH3CCl3 (6.7 Gg), and Cl2C = CCl2 (2.3 Gg) accounted for about 62.9% of total halocarbon emissions, it suggested a significant contribution from solvent use in the PRD region. Emissions of HCFC-22 (3.5 Gg), an alternative refrigerant to chlorofluorocarbons (CFCs), were about 2.3 times greater than those of CFC-12 (1.6 Gg). CFC-12 and HCFC-22 accounted for 21.5% of total emissions of halocarbons, so that the refrigerant would be the second largest source of halocarbons. However, the ratio approach found only minor emissions of CFCs, such as CFC-11, and the emission of CFC-114 and CFC-113 were close to zero. Emissions of other anthropogenic halocarbons, such as CCl4, CHCl3, CH3Br, and CH3Cl, were also estimated. Where possible, the emissions estimated from the measured ratios were compared with results from source inventory techniques, we found that both approaches gave emissions at similar magnitude for most of the halocarbons, except CFC-11. The comparison suggested that the ratio method may be a useful tool for assessing regional halocarbon emissions, and emission uncertainty could be further reduced by incorporating both longer-term and higher-frequency observations, as well as improving the accuracy of the CO inventory.
引用
收藏
页码:5011 / 5025
页数:15
相关论文
共 84 条
[1]   Evaluation of pollutant outflow and CO sources during TRACE-P using model-calculated, aircraft-based, and Measurements of Pollution in the Troposphere (MOPITT)-derived CO concentrations [J].
Allen, D ;
Pickering, K ;
Fox-Rabinovitz, M .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D15) :D15S031-19
[2]  
[Anonymous], 2000, MONTR PROT SUBST DEP
[3]  
[Anonymous], [No title captured]
[4]   Anthropogenic emissions of trichloromethane (chloroform, CHCl3) and chlorodifluoromethane (HCFC-22):: Reactive Chlorine Emissions Inventory [J].
Aucott, ML ;
McCulloch, A ;
Graedel, TE ;
Kleiman, G ;
Midgley, P ;
Li, YF .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D7) :8405-8415
[5]   Mixing ratios of volatile organic compounds (VOCs) in the atmosphere of Karachi, Pakistan [J].
Barletta, B ;
Meinardi, S ;
Simpson, IJ ;
Khwaja, HA ;
Blake, DR ;
Rowland, FS .
ATMOSPHERIC ENVIRONMENT, 2002, 36 (21) :3429-3443
[6]   Ambient halocarbon mixing ratios in 45 Chinese cities [J].
Barletta, Barbara ;
Meinardi, Simone ;
Simpson, Isobel J. ;
Rowland, F. Sherwood ;
Chan, Chuen-Yu ;
Wang, Xinming ;
Zou, Shichun ;
Chan, Lo Yin ;
Blake, Donald R. .
ATMOSPHERIC ENVIRONMENT, 2006, 40 (40) :7706-7719
[7]   Urban/industrial pollution for the New York City - Washington, DC, corridor, 1996-1998: 1. Providing independent verification of CO and PCE emissions inventories [J].
Barnes, DH ;
Wofsy, SC ;
Fehlau, BP ;
Gottlieb, EW ;
Elkins, JW ;
Dutton, GS ;
Montzka, SA .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D6)
[8]   NMHCs and halocarbons in Asian continental outflow during the Transport and Chemical Evolution over the Pacific (TRACE-P) Field Campaign: Comparison with PEM-West B [J].
Blake, NJ ;
Blake, DR ;
Simpson, IJ ;
Meinardi, S ;
Swanson, AL ;
Lopez, JP ;
Katzenstein, AS ;
Barletta, B ;
Shirai, T ;
Atlas, E ;
Sachse, G ;
Avery, M ;
Vay, S ;
Fuelberg, HE ;
Kiley, CM ;
Kita, K ;
Rowland, FS .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D20)
[9]   Technical Note: Review of methods for linear least-squares fitting of data and application to atmospheric chemistry problems [J].
Cantrell, C. A. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2008, 8 (17) :5477-5487
[10]   Mixing ratios and sources of halocarbons in urban, semi-urban and rural sites of the Pearl River Delta, South China [J].
Chan, C. Y. ;
Tang, J. H. ;
Li, Y. S. ;
Chan, L. Y. .
ATMOSPHERIC ENVIRONMENT, 2006, 40 (38) :7331-7345