Emission measurements of alkenes, alkanes, SO2, and NO2 from stationary sources in Southeast Texas over a 5 year period using SOF and mobile DOAS

被引:33
作者
Johansson, John K. E. [1 ]
Mellqvist, Johan [1 ]
Samuelsson, Jerker [1 ]
Offerle, Brian [1 ]
Lefer, Barry [2 ]
Rappenglueck, Bernhard [2 ]
Flynn, James [2 ]
Yarwood, Greg [3 ]
机构
[1] Chalmers Univ Technol, Dept Earth & Space Sci, S-41296 Gothenburg, Sweden
[2] Univ Houston, Dept Earth & Atmospher Sci, Houston, TX USA
[3] ENVIRON Int Corp, Novato, CA USA
基金
奥地利科学基金会;
关键词
VOC; Alkanes; Ethene; Propene; Emissions; Flux; ABSORPTION CROSS-SECTIONS; AIR-QUALITY; NM; HOUSTON;
D O I
10.1002/2013JD020485
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
A mobile platform for flux measurements of VOCs (alkanes and alkenes), SO2, and NO2 emissions using the Solar Occultation Flux (SOF) method and mobile differential optical absorption spectroscopy (DOAS) was used in four different studies to measure industrial emissions. The studies were carried out in several large conglomerates of oil refineries and petrochemical industries in Southeast and East Texas in 2006, 2009, 2011, and 2012. The measured alkane emissions from the Houston Ship Channel (HSC) have been fairly stable between 2006 and 2011, averaging about 11,500kg/h, while the alkene emissions have shown greater variations. The ethene and propene emissions measured from the HSC were 1511kg/h and 878kg/h, respectively, in 2006, while dropping to roughly 600kg/h for both species in 2009 and 2011. The results were compared to annual inventory emissions, showing that measured VOC emissions were typically 5-15 times higher, while for SO2 and NO2 the ratio was typically 0.5-2. AP-42 emission factors were used to estimate meteorological effects on alkane emissions from tanks, showing that these emissions may have been up to 35-45% higher during the studies than the annual average. A more focused study of alkene emissions from a petrochemical complex in Longview in 2012 identified two upset episodes, and the elevation of the total emissions during the measurement period due to the upsets was estimated to be approximately 20%. Both meteorological and upset effects were small compared to the factor of 5-15, suggesting that VOC emissions are systematically and substantially underestimated in current emission inventories.
引用
收藏
页码:1973 / 1991
页数:19
相关论文
共 36 条
[1]   A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network [J].
Angelbratt, J. ;
Mellqvist, J. ;
Blumenstock, T. ;
Borsdorff, T. ;
Brohede, S. ;
Duchatelet, P. ;
Forster, F. ;
Hase, F. ;
Mahieu, E. ;
Murtagh, D. ;
Petersen, A. K. ;
Schneider, M. ;
Sussmann, R. ;
Urban, J. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (13) :6167-6183
[2]   Ship emissions of SO2 and NO2: DOAS measurements from airborne platforms [J].
Berg, N. ;
Mellqvist, J. ;
Jalkanen, J. -P. ;
Balzani, J. .
ATMOSPHERIC MEASUREMENT TECHNIQUES, 2012, 5 (05) :1085-1098
[3]   Measurements of molecular absorption spectra with the SCIAMACHY pre-flight model: instrument characterization and reference data for atmospheric remote-sensing in the 230-2380 nm region [J].
Bogumil, K ;
Orphal, J ;
Homann, T ;
Voigt, S ;
Spietz, P ;
Fleischmann, OC ;
Vogel, A ;
Hartmann, M ;
Kromminga, H ;
Bovensmann, H ;
Frerick, J ;
Burrows, JP .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 2003, 157 (2-3) :167-184
[4]   Atmospheric remote-sensing reference data from GOME -: 2.: Temperature-dependent absorption cross sections of O3 in the 231-794 nm range [J].
Burrows, JP ;
Richter, A ;
Dehn, A ;
Deters, B ;
Himmelmann, S ;
Orphal, J .
JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER, 1999, 61 (04) :509-517
[5]   TEMPERATURE-DEPENDENT FORMALDEHYDE CROSS-SECTIONS IN THE NEAR-ULTRAVIOLET SPECTRAL REGION [J].
CANTRELL, CA ;
DAVIDSON, JA ;
MCDANIEL, AH ;
SHETTER, RE ;
CALVERT, JG .
JOURNAL OF PHYSICAL CHEMISTRY, 1990, 94 (10) :3902-3908
[6]   Airborne Measurements of Ethene from Industrial Sources Using Laser Photo-Acoustic Spectroscopy [J].
De Gouw, J. A. ;
Hekkert, S. Te Lintel ;
Mellqvist, J. ;
Warneke, C. ;
Atlas, E. L. ;
Fehsenfeld, F. C. ;
Fried, A. ;
Frost, G. J. ;
Harren, F. J. M. ;
Holloway, J. S. ;
Lefer, B. ;
Lueb, R. ;
Meagher, J. F. ;
Parrish, D. D. ;
Patel, M. ;
Pope, L. ;
Richter, D. ;
Rivera, C. ;
Ryerson, T. B. ;
Samuelsson, J. ;
Walega, J. ;
Washenfelder, R. A. ;
Weibring, P. ;
Zhu, X. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2009, 43 (07) :2437-2442
[7]  
Fayt C., 2011, QDOAS 1 00
[8]   A miniaturised ultraviolet spectrometer for remote sensing of SO2 fluxes:: a new tool for volcano surveillance [J].
Galle, B ;
Oppenheimer, C ;
Geyer, A ;
McGonigle, AJS ;
Edmonds, M ;
Horrocks, L .
JOURNAL OF VOLCANOLOGY AND GEOTHERMAL RESEARCH, 2003, 119 (1-4) :241-254
[9]   Measurements of volatile organic compounds during the 2006 TexAQS/GoMACCS campaign: Industrial influences, regional characteristics, and diurnal dependencies of the OH reactivity [J].
Gilman, Jessica B. ;
Kuster, William C. ;
Goldan, Paul D. ;
Herndon, Scott C. ;
Zahniser, Mark S. ;
Tucker, Sara C. ;
Brewer, W. Alan ;
Lerner, Brian M. ;
Williams, Eric J. ;
Harley, Robert A. ;
Fehsenfeld, Fred C. ;
Warneke, Carsten ;
de Gouw, Joost A. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2009, 114
[10]   Absorption cross-sections of atmospheric constituents:: NO2, O2, and H2O [J].
Hermans, C ;
Vandaele, AC ;
Carleer, M ;
Fally, S ;
Colin, R ;
Jenouvrier, A ;
Coquart, B ;
Mérienne, MF .
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH, 1999, 6 (03) :151-158