scholarly journals Real-Time Measurements of Engine-Out Trace Elements: Application of a Novel Soot Particle Aerosol Mass Spectrometer for Emissions Characterization

Author(s):  
E. S. Cross ◽  
A. Sappok ◽  
E. C. Fortner ◽  
J. F. Hunter ◽  
J. T. Jayne ◽  
...  

Lubricant-derived trace element emissions are the largest contributors to the accumulation of incombustible ash in diesel particulate filters (DPF), eventually leading to filter plugging and an increase in engine fuel consumption. Particulate trace element emissions also pose adverse health effects and are the focus of increasingly stringent air quality regulations. To date, the rates and physical and chemical properties of lubricant-derived additive emissions are not well characterized, largely due to the difficulties associated with conducting the measurements. This work investigated the potential for conducting real-time measurements of lubricant-derived particle emissions. The experiment used the Soot Particle Aerosol Mass Spectrometer (SP-AMS) developed by Aerodyne Research to measure the size, mass and composition of submicron particles in the exhaust. Results confirm the ability of the SP-AMS to measure engine-out emissions of calcium, zinc, magnesium, phosphorous, and sulfur. Further, emissions of previously difficult to detect elements, such as boron, and low-level engine wear metals, such as lead, were also measured. This paper provides an overview of the results obtained with the SP-AMS, and demonstrates the utility of applying real-time techniques to engine-out and tailpipe-out trace element emissions. The SP-AMS used in this study was developed for real-time characterization of refractory particles (i.e. black carbon or soot) in the ambient atmosphere. The instrument consists of an intra-cavity laser (1064 nm) for particle vaporization followed by electron impact ionization and ion detection via a time-of-flight mass spectrometer. Application of the SP-AMS for engine exhaust characterization followed a two-part approach: (1) measurement validation, and (2) measurement of engine-out exhaust. Measurement validation utilized a diesel burner with precise control of lubricant consumption. Results showed a good correlation between CJ-4 oil consumption and measured levels of lubricant-derived trace elements in the particle phase. Following measurement validation, the SP-AMS measured engine-out emissions from a medium-duty diesel engine, operated over a standard speed/load matrix. This work demonstrates the utility of state-of-the-art online techniques (such as the SP-AMS) to measure engine-out emissions, including trace species derived from lubricant additives. Results help optimize the combined engine-lubricant-aftertreatment system and provide a real-time characterization of emissions. As regulations become more stringent and emission controls more complex, advanced measurement techniques with high sensitivity and fast time response will become an increasingly important part of engine characterization studies.

Author(s):  
E. S. Cross ◽  
A. Sappok ◽  
E. C. Fortner ◽  
J. F. Hunter ◽  
J. T. Jayne ◽  
...  

Lubricant-derived trace element emissions are the largest contributors to the accumulation of incombustible ash in diesel particulate filters (DPF), eventually leading to filter plugging and an increase in engine fuel consumption. Particulate trace element emissions also pose adverse health effects and are the focus of increasingly stringent air quality regulations. To date, the rates and physical and chemical properties of lubricant-derived additive emissions are not well characterized, largely due to the difficulties associated with conducting the measurements. This work investigated the potential for conducting real-time measurements of lubricant-derived particle emissions. The experiment used the Soot Particle Aerosol Mass Spectrometer (SP-AMS) developed by Aerodyne Research to measure the size, mass and composition of submicron particles in the exhaust. Results confirm the ability of the SP-AMS to measure engine-out emissions of calcium, zinc, magnesium, phosphorous, and sulfur. Further, emissions of previously difficult to detect elements, such as boron, and low-level engine wear metals, such as lead, were also measured. This paper provides an overview of the results obtained with the SP-AMS, and demonstrates the utility of applying real-time techniques to engine-out and tailpipe-out trace element emissions. Application of the SP-AMS for engine exhaust characterization followed a two-part approach: (1) measurement validation, and (2) measurement of engine-out exhaust. Measurement validation utilized a diesel burner with precise control of lubricant consumption. Results showed a good correlation between CJ-4 oil consumption and measured levels of lubricant-derived trace elements in the particle phase. Following measurement validation, the SP-AMS measured engine-out emissions from a medium-duty diesel engine, operated over a standard speed/load matrix. This work demonstrates the utility of state-of-the-art online techniques (such as the SP-AMS) to measure engine-out emissions, including trace species derived from lubricant additives. Results help optimize the combined engine-lubricant-aftertreatment system and provide a real-time characterization of emissions. As regulations become more stringent and emission controls more complex, advanced measurement techniques with high sensitivity and fast time response will become an increasingly important part of engine characterization studies.


2015 ◽  
Vol 120 (6) ◽  
pp. 2575-2593 ◽  
Author(s):  
Paola Massoli ◽  
Timothy B. Onasch ◽  
Christopher D. Cappa ◽  
Ibraheem Nuamaan ◽  
Jani Hakala ◽  
...  

2020 ◽  
Vol 22 (8) ◽  
pp. 1616-1653 ◽  
Author(s):  
Wei Zhou ◽  
Weiqi Xu ◽  
Hwajin Kim ◽  
Qi Zhang ◽  
Pingqing Fu ◽  
...  

Aerosol mass spectrometer has been widely deployed in Asia for real-time characterization of aerosol chemistry, and has significantly improved our understanding of the sources, properties, and formation processes of aerosols in a complex environment.


2015 ◽  
Vol 15 (20) ◽  
pp. 11807-11833 ◽  
Author(s):  
W. W. Hu ◽  
P. Campuzano-Jost ◽  
B. B. Palm ◽  
D. A. Day ◽  
A. M. Ortega ◽  
...  

Abstract. Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.


2014 ◽  
Vol 7 (12) ◽  
pp. 4507-4516 ◽  
Author(s):  
M. D. Willis ◽  
A. K. Y. Lee ◽  
T. B. Onasch ◽  
E. C. Fortner ◽  
L. R. Williams ◽  
...  

Abstract. The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements are used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.


2012 ◽  
Vol 46 (7) ◽  
pp. 804-817 ◽  
Author(s):  
T. B. Onasch ◽  
A. Trimborn ◽  
E. C. Fortner ◽  
J. T. Jayne ◽  
G. L. Kok ◽  
...  

2013 ◽  
Vol 6 (11) ◽  
pp. 3271-3280 ◽  
Author(s):  
L. R. Williams ◽  
L. A. Gonzalez ◽  
J. Peck ◽  
D. Trimborn ◽  
J. McInnis ◽  
...  

Abstract. We have designed and characterized a new inlet and aerodynamic lens for the Aerodyne aerosol mass spectrometer (AMS) that transmits particles between 80 nm and more than 3 μm in vacuum aerodynamic diameter. The design of the inlet and lens was optimized with computational fluid dynamics (CFD) modeling of particle trajectories. Major changes include a redesigned critical orifice holder and valve assembly, addition of a relaxation chamber behind the critical orifice, and a higher lens operating pressure. The transmission efficiency of the new inlet and lens was characterized experimentally with size-selected particles. Experimental measurements are in good agreement with the calculated transmission efficiency.


2005 ◽  
Vol 39 (8) ◽  
pp. 760-770 ◽  
Author(s):  
N. Takegawa ◽  
Y. Miyazaki ◽  
Y. Kondo ◽  
Y. Komazaki ◽  
T. Miyakawa ◽  
...  

2015 ◽  
Vol 32 (6) ◽  
pp. 877-888 ◽  
Author(s):  
Junke Zhang ◽  
Yuesi Wang ◽  
Xiaojuan Huang ◽  
Zirui Liu ◽  
Dongsheng Ji ◽  
...  

2015 ◽  
Vol 299 ◽  
pp. 156-174 ◽  
Author(s):  
Stefanos Samaras ◽  
Doina Nicolae ◽  
Christine Böckmann ◽  
Jeni Vasilescu ◽  
Ioannis Binietoglou ◽  
...  

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