Primary emissions and secondary production of organic aerosols from heated animal fats

Author(s):  
Liyuan Zhou ◽  
Tengyu Liu ◽  
Dawen Yao ◽  
Hai Guo ◽  
Chunlei Cheng ◽  
...  
2011 ◽  
Vol 11 (23) ◽  
pp. 12387-12420 ◽  
Author(s):  
K. S. Docherty ◽  
A. C. Aiken ◽  
J. A. Huffman ◽  
I. M. Ulbrich ◽  
P. F. DeCarlo ◽  
...  

Abstract. Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR) to investigate the chemical composition and potential sources of fine particles (PMf) in the inland region of Southern California. In this paper, we briefly summarize the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July–15 August), provide detailed intercomparisons of high-resolution aerosol mass spectrometer (HR-AMS) measurements against complementary measurements, and report the average composition of PMf including the composition of the organic fraction measured by the HR-AMS. Daily meteorology and gas-phase species concentrations were highly consistent, displaying clear diurnal cycles and weekday/weekend contrast. HR-AMS measurements of non-refractory submicron (NR-PM1) mass are consistent and highly correlated with those from a filter dynamics measurement system tapered-element oscillating microbalance (TEOM), while the correlation between HR-AMS and heated TEOM measurements is lower due to loss of high volatility species including ammonium nitrate from the heated TEOM. Speciated HR-AMS measurements are also consistent with complementary measurements as well as with measurements from a collocated compact AMS while HR-AMS OC is similar to standard semi-continuous Sunset measurements within the combined uncertainties of both instruments. A correction intended to account for the loss of semi-volatile OC from the Sunset, however, yields measurements ~30% higher than either HR-AMS or standard Sunset measurements. On average, organic aerosol (OA) was the single largest component of PMf. OA composition was investigated using both elemental analysis and positive matrix factorization (PMF) of HR-AMS OA spectra. Oxygen is the main heteroatom during SOAR-1, with O/C exhibiting a diurnal minimum of 0.28 during the morning rush hour and maximum of 0.42 during the afternoon. O/C is broadly anti-correlated with H/C, while N/C and S/C (excluding organonitrate (ON) and organosulfate (OS) functionalities) are far lower than O/C at about 0.015 and ~0.001, respectively. When ON and OS estimates are included O/C, N/C, and S/C increase by factors of 1.21, 2, and 30, respectively, while H/C changes are insignificant. The increase in these ratios implies that ON accounts for ~1/2 of the organic nitrogen while OS dominate organic sulfur at this location. Accounting for the estimated ON and OS also improves the agreement between anions and cations measured by HR-AMS by ~8%, while amines have only a very small impact (1%) on this balance. Finally, a number of primary and secondary OA components were resolved by PMF. Among these a hydrocarbon-like OA and two minor, local OA components, one of which was associated with amines, were attributed to primary emissions and contributed a minor fraction (~20%) of OA mass. The remaining OA mass was attributed to a number of secondary oxidized OA (OOA) components including the previously-identified low-volatility and semi-volatile OOA components. In addition, we also report for the first time the presence of two additional OOA components.


2012 ◽  
Vol 12 (7) ◽  
pp. 3273-3288 ◽  
Author(s):  
D. D. Parrish ◽  
T. B. Ryerson ◽  
J. Mellqvist ◽  
J. Johansson ◽  
A. Fried ◽  
...  

Abstract. We evaluate the rates of secondary production and primary emission of formaldehyde (CH2O) from petrochemical industrial facilities and on-road vehicles in the Houston Texas region. This evaluation is based upon ambient measurements collected during field studies in 2000, 2006 and 2009. The predominant CH2O source (92 ± 4% of total) is secondary production formed during the atmospheric oxidation of highly reactive volatile organic compounds (HRVOCs) emitted from the petrochemical facilities. Smaller contributions are primary emissions from these facilities (4 ± 2%), and secondary production (~3%) and primary emissions (~1%) from vehicles. The primary emissions from both sectors are well quantified by current emission inventories. Since secondary production dominates, control efforts directed at primary CH2O emissions cannot address the large majority of CH2O sources in the Houston area, although there may still be a role for such efforts. Ongoing efforts to control alkene emissions from the petrochemical facilities, as well as volatile organic compound emissions from the motor vehicle fleet, will effectively reduce the CH2O concentrations in the Houston region. We do not address other emission sectors, such as off-road mobile sources or secondary formation from biogenic hydrocarbons. Previous analyses based on correlations between ambient concentrations of CH2O and various marker species have suggested much larger primary emissions of CH2O, but those results neglect confounding effects of dilution and loss processes, and do not demonstrate the causes of the observed correlations. Similar problems must be suspected in any source apportionment analysis of secondary species based upon correlations of ambient concentrations of pollutants.


2014 ◽  
Vol 48 (15) ◽  
pp. 8491-8497 ◽  
Author(s):  
Pingqing Fu ◽  
Kimitaka Kawamura ◽  
Jing Chen ◽  
Yuzo Miyazaki

2013 ◽  
Vol 13 (6) ◽  
pp. 3379-3392 ◽  
Author(s):  
L. Hu ◽  
D. B. Millet ◽  
S. Y. Kim ◽  
K. C. Wells ◽  
T. J. Griffis ◽  
...  

Abstract. We apply a full year of continuous atmospheric acetone measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), with a 0.5° × 0.667° GEOS-Chem nested grid simulation to develop quantitative new constraints on seasonal acetone sources over North America. Biogenic acetone emissions in the model are computed based on the MEGANv2.1 inventory. An inverse analysis of the tall tower observations implies a 37% underestimate of emissions from broadleaf trees, shrubs, and herbaceous plants, and an offsetting 40% overestimate of emissions from needleleaf trees plus secondary production from biogenic precursors. The overall result is a small (16%) model underestimate of the total primary + secondary biogenic acetone source in North America. Our analysis shows that North American primary + secondary anthropogenic acetone sources in the model (based on the EPA NEI 2005 inventory) are accurate to within approximately 20%. An optimized GEOS-Chem simulation incorporating the above findings captures 70% of the variance (R = 0.83) in the hourly measurements at the KCMP tall tower, with minimal bias. The resulting North American acetone source is 11 Tg a−1, including both primary emissions (5.5 Tg a−1) and secondary production (5.5 Tg a−1), and with roughly equal contributions from anthropogenic and biogenic sources. The North American acetone source alone is nearly as large as the total continental volatile organic compound (VOC) source from fossil fuel combustion. Using our optimized source estimates as a baseline, we evaluate the sensitivity of atmospheric acetone and peroxyacetyl nitrate (PAN) to shifts in natural and anthropogenic acetone sources over North America. Increased biogenic acetone emissions due to surface warming are likely to provide a significant offset to any future decrease in anthropogenic acetone emissions, particularly during summer.


2012 ◽  
Vol 12 (11) ◽  
pp. 30869-30908
Author(s):  
L. Hu ◽  
D. B. Millet ◽  
S. Y. Kim ◽  
K. C. Wells ◽  
T. J. Griffis ◽  
...  

Abstract. We apply a full year of continuous atmospheric acetone measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), with a 0.5° × 0.667° GEOS-Chem nested grid simulation to develop quantitative new constraints on seasonal acetone sources over North America, and assess the corresponding impacts on atmospheric chemistry. Biogenic acetone emissions in the model are computed based on the MEGANv2.1 inventory. An inverse analysis of the tall tower observations implies a 37% underestimate of emissions from broadleaf trees, shrubs, and herbaceous plants, and an offsetting 40% overestimate of emissions from needleleaf trees plus secondary production from biogenic precursors. The overall result is a small (16%) model underestimate of the total primary + secondary biogenic acetone source in North America. Our analysis shows that North American primary + secondary anthropogenic acetone sources in the model (based on the EPA NEI 2005 inventory) are accurate to within approximately 20%. An optimized GEOS-Chem simulation incorporating the above findings captures 70% of the variance (R=0.83) in the hourly measurements at the KCMP tall tower, with minimal bias. The resulting North American acetone source is 10.9 Tg a−1, including both primary emissions (5.5 Tg a−1) and secondary production (5.5 Tg a−1), and with roughly equal contributions from anthropogenic and biogenic sources. The North American acetone source alone is nearly as large as the total continental volatile organic compound (VOC) source from fossil fuel combustion. Using our optimized source estimates as a baseline, we evaluate the atmospheric impact of some potential future shifts in acetone sources over North America. Increased biogenic acetone emissions due to surface warming are likely to provide a significant offset to any future decrease in anthropogenic acetone emissions, particularly during summer.


2021 ◽  
Author(s):  
Amir Yazdani ◽  
Satoshi Takahama ◽  
Jack K. Kodros ◽  
Marco Paglione ◽  
Mauro Masiol ◽  
...  

<p>Fine particulate matter (PM) affects visibility, climate and public health. Organic matter (OM), which is hard to characterize due to its complex chemical composition, can constitute more than half of the PM. Biomass burning from residential wood burning, wildfires, and prescribed burning is a major source of OM with an ever-increasing importance.</p><p>    Aerosol mass spectrometry (AMS) and Fourier transform infrared spectroscopy (FTIR) are two complementary methods of identifying the chemical composition of OM. AMS measures the bulk composition of OM with relatively high temporal resolution but provides limited parent compound information. FTIR, carried out on samples collected on Teflon filters, provides detailed functional groupinformation at the expense of relatively low temporal resolution.</p><p>    In this study, we used these two methods to better understand the evolution of biomass burning OM in the atmosphere with aging. For this purpose, primary emissions from wood and pellet stoves were injected into the Center for Studies of Air Qualities and Climate Change (C-STACC) environmental chamber at ICE-HT/FORTH. Primary emissions were aged using hydroxyl and nitrate radicals (with atmospherically relevant exposures) simulating atmospheric day-time and night-time oxidation.  A time-of-flight (ToF) AMS reported the composition of non-refractory PM<sub>1 </sub>every three minutes and PM<sub>1 </sub>was collected on PTFE filters over 20-minute periods before and after aging for off-line FTIR analysis.</p><p>    We found that AMS and FTIR measurements agreed well in terms of measured OM mass concentration, the OM:OC ratio, and concentration of biomass burning tracers – lignin and levoglucosan. AMS OM concentration was used to estimate chamber wall loss rates which were then used separate the contribution of primary and secondary organic aerosols (POA and SOA) to the aged OM. AMS mass spectra and FTIR spectra of biomass burning SOA and estimates of bulk composition were obtained by this procedure. FTIR and AMS spectra of SOA produced by OH oxidation of biomass burning volatile organic compounds (VOCs) were dominated by acid signatures. Organonitrates, on the other hand, appeared to be important in the SOA aged by the nitrate radical. The spectra from the two instruments also indicated that the signatures of certain compounds such as levoglucosan, lignin and hydrocarbons, which are abundant in biomass burning POA, diminish with aging significantly more than what can be attributed to chamber wall losses. The latter suggests biomass burning POA chemical composition might change noticeably due to heterogeneous reactions or partitioning in the atmosphere. Therefore, the common assumption of stable POA composition is only partially true. In addition, more stable biomass burning tracers should be used to be able to identify highly aged biomass burning aerosols in the atmosphere.</p>


2011 ◽  
Vol 11 (12) ◽  
pp. 32601-32645 ◽  
Author(s):  
D. D. Parrish ◽  
T. B. Ryerson ◽  
J. Mellqvist ◽  
J. Johansson ◽  
A. Fried ◽  
...  

Abstract. We evaluate the rates of secondary production and primary emission of formaldehyde (CH2O) from petrochemical industrial facilities and on-road vehicles in the Houston Texas region. This evaluation is based upon ambient measurements collected during field studies in 2000, 2006 and 2009. The predominant CH2O source (92 ± 4% of total) is secondary production formed during the atmospheric oxidation of highly reactive volatile organic compounds (HRVOCs) emitted from the petrochemical facilities. Smaller contributions are primary emissions from these facilities (4 ± 2%), and secondary production (~3%) and primary emissions (~1%) from vehicles. The primary emissions from both sectors are well quantified by current emission inventories. Since secondary production dominates, control efforts directed at primary CH2O emissions cannot address the large majority of CH2O sources in the Houston area, although there may still be a role for such efforts. Ongoing efforts to control alkene emissions from the petrochemical facilities, as well as volatile organic compound emissions from the motor vehicle fleet, will effectively reduce the CH2O concentrations in the Houston region. We have not addressed other emission sectors, such as off-road mobile sources or secondary formation from biogenic hydrocarbons. Previous analyses based on correlations between ambient concentrations of CH2O and various marker species have suggested much larger primary emissions of CH2O, but those results neglect confounding effects of dilution and loss processes, and do not demonstrate the causes of the observed correlations. Similar problems must be suspected in any source apportionment analysis of secondary species based upon correlations of ambient concentrations of pollutants.


2020 ◽  
pp. 149-159
Author(s):  
Jatinder Kataria ◽  
Saroj Kumar Mohapatra ◽  
Amit Pal

The limited fossil reserves, spiraling price and environmental impact due to usage of fossil fuels leads the world wide researchers’ interest in using alternative renewable and environment safe fuels that can meet the energy demand. Biodiesel is an emerging renewable alternative fuel to conventional diesel which can be produced from both edible and non-edible oils, animal fats, algae etc. The society is in dire need of using renewable fuels as an immediate control measure to mitigate the pollution level. In this work an attempt is made to review the requisite and access the capability of the biodiesel in improving the environmental degradation.


Author(s):  
Sosuke Otani ◽  
Sosuke Otani ◽  
Akira Umehara ◽  
Akira Umehara ◽  
Haruka Miyagawa ◽  
...  

Fish yields of Ruditapes philippinarum have been decreased and the resources have not yet recovered. It needs to clarify food sources of R. philippinarum, and relationship between primary and secondary production of it. The purpose on this study is to reveal transfer efficiency from primary producers to R. philippinarum and food sources of R. philippinarum. The field investigation was carried out to quantify biomass of R. philippinarum and primary producers on intertidal sand flat at Zigozen beach in Hiroshima Bay, Japan. In particular, photosynthetic rates of primary producers such as Zostera marina, Ulva sp. and microphytobenthos were determined in laboratory experiments. The carbon and nitrogen stable isotope ratios for R. philippinarum and 8 potential food sources (microphytobenthos, MPOM etc) growing in the tidal flat were also measured. In summer 2015, the primary productions of Z. marina, Ulva sp. and microphytobenthos were estimated to be 70.4 kgC/day, 43.4 kgC/day and 2.2 kgC/day, respectively. Secondary production of R. philippinarum was 0.4 kgC/day. Contribution of microphytobenthos to R. philippinarum as food source was 56-76% on the basis of those carbon and nitrogen stable isotope ratios. Transfer efficiency from microphytobenthos to R. philippinarum was estimated to be 10-14%. It was suggested that microphytobenthos might sustain the high secondary production of R. philippinarum, though the primary production of microphytobenthos was about 1/10 compared to other algae.


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