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Ambient Elemental Signatures of Diesel and Automotive Particulate Matter by Size, Time, and Composition. 1 Thomas A. Cahill, 1 Earl Withycombe, Steven S. Cliff, Michael Jimenez-Cruz, Lee Portnoff, and 2 Kevin D. Perry, DELTA Group, University of California, Davis, http://delta.ucdavis.edu ,

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Ambient Elemental Signatures of Diesel and Automotive Particulate Matter by Size, Time, and Composition.

1Thomas A. Cahill, 1Earl Withycombe, Steven S. Cliff, Michael Jimenez-Cruz, Lee Portnoff, and 2Kevin D. Perry,

DELTA Group, University of California, Davis, http://delta.ucdavis.edu,

1The Health Effects Task Force, American Lung Association, Sacramento-Emigrant Trails,

2Dept. of Meteorology, University of Utah


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Sources of information – joint studies with the DELTA Group

  • Laboratory studies – NREL/U. Minnesota/DRI diesels; UCD S-XRF analysis –(Lawson, Watts, Zielenska et al.), plus DRI Lube oil (Fujita)

  • Prior field studies – prior ARB/UC Davis work; HEI/DRI Tuscarora Tunnel (Gertler et al 2002)

  • Quasi-ambient and ambient applications

    • Interstate 5 on downtown Sacramento and Watt Ave School – (Lung Assoc – Sacramento Emigrant Trails)

    • Fresno FACES studies (ARB)

    • Highway 50 in South Lake Tahoe – TRPA (Tahoe Regional Planning Agency)





Doe gasoline diesel pm split study particle phase pah in lubrication oil l.jpg
DOE Gasoline/Diesel PM Split Study Kelly, UC Davis) Particle-Phase PAH in Lubrication Oil


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Summary Kelly, UC Davis) of laboratory tests

  • Most diesel mass lies below 0.25 µm (very fine/ultra fine)

  • Sulfur correlates with emitted very fine/ultra fine mass, and is associated with the diesel fuel

  • Diesel tracers, some ultra-fine, comes from combustion of lubricating oil stabilized with zinc thiophosphate and CaCO3 ; the amounts are highly variable (factor of 3)

  • Ultra fine diesel particles have much more massive and less volatile organic components than coarser diesel components, as required by the Kelvin effect.

  • Lubricating oil for spark ignition vehicles has more and heavier PAHs than lubricating oil for diesels

  • Diesel particles are highly light absorbing at all wavelengths, 350 nm – 820 nm


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PM 0.25 ? Kelly, UC Davis)

PM 10

PM 2.5

Average Zn to mass, all DRI tests, 1800  1300



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Summary for prior field tests Kelly, UC Davis)

  • Diesel truck have roughly 10 (PM2.5) to 18 (PM10) times the mass emission rate of light duty vehicles

  • Diesels and light duty vehicles emit species seen in the laboratory tests, plus others in the PM2.5 mode.

  • There are a number of possible tracers that separate diesels from gasoline powered vehicles, including a few heavy PAHs

  • Gross emitting light duty vehicles, a few percent of all vehicles, can be as bad or worse per vehicle than the average heavy duty diesel.


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Current ambient/quasi-ambient studies Kelly, UC Davis)

  • Interstate 5 in downtown Sacramento

    • urban

  • Watt Avenue on Arden Middle School

    • suburban

  • Highway 50 in South Lake Tahoe

  • The Fresno Super-site

    • suburban


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Lung Assoc. Sacramento Transect Study Site Map and PM Kelly, UC Davis) 2.5 aggregated data

#1, #3 - light blue = rain, yellow = “clear”, rest = fogs, wet and dry

I-5

Hwy-50

I-80

I-80

Hwy-99


Sacramento a highway nexus i 5 i 80 hwy 50 hwy 99 and close to violations of pm 2 5 standards l.jpg
Sacramento – a highway nexus, (I-5, I-80, Hwy 50, Hwy 99) and close to violations of PM2.5 standards


Interstate 5 in sacramento l.jpg
Interstate 5 in Sacramento and close to violations of PM

  • Impact of I-5 on Downtown Sacramento

    • 10,500 light duty, 1125 heavy duty (> 5 axel) vehicles/hr,

    • 10 traffic lanes, nearest 100 m to Crocker Art Museum site

    • Sound wall; some trees but not a barrier

    • Prevailing wind in daytime from southwest, across I-80; stagnation low winds from southeast

    • Cut section freeway; complex terrain prevents direct line source modeling; use very fine diesel tracers


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DELTA Group slotted 8 DRUM Impactor and close to violations of PM

  • 8 size ranges:

    • Inlet ( ~ 12) to 5.0 μm

    • 5.0 to 2.5 μm

    • 2.5 to 1.15 μm

    • 1.15 to 0.75 μm

    • 0.75 to 0.56 μm

    • 0.56 to 0.34 μm

    • 0.34 to 0.26 μm

    • 0.26 to 0.09 μm

  • 10.4 l/min, critical orifice control, ¼ hp pump

  • 6.5 x 168 mm Mylar strips

  • For 42 day run, 4 mm/day,

    time resolution = 3 hr.

  • Field portable

    • 10 kg, 43 × 22× 13 cm

43 cm


Very fine 0 26 d p 0 09 m drum sample 3 weeks south lake tahoe 1cm high true color l.jpg
Very fine (0.26 > D and close to violations of PMp > 0.09 µm) DRUM sample, 3 weeks, South Lake Tahoe; 1cm high, true color



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Crocker blank subtraction Art Museum site

Predict 4.3  2.9µg/m3 diesel mass (U. Minn.)

rain

rain

rain

Fog and haze


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rain blank subtraction

Observe  6  1 µg/m3 mass


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Impact of Watt Avenue on Arden Middle School blank subtraction

  • 3800 light duty, 53 heavy (> 5 axel) vehicles/hr

  • Stop light at NW corner of school grounds

  • 9 traffic lanes, nearest 15 m to school buildings

  • Prevailing wind in daytime from southwest, across Watt Avenue; stagnation winds weak from southeast

  • No wall or vegetation barrier; line source modeling easy from Tuscarora PM2.5 data


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Watt Ave blank subtraction

HETF Site

Arden Way

Sebastian Way site



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Application of Tuscarora data concentrations of lead

  • Sliding box model on roadway

  • Upwind regional PM2.5 data (CARB)

  • Regional meteorology (NOAA’s ARL HYSPLIT 4)

  • PM2.5 inlet (IMPROVE); 3 stage rotating DRUM impactor at 1.15, 0.34, and <0.15 μm diameter

  • Line source model, neutral stability

  • Soft beta gauge PM2.5 mass ~ 7.0 ± 1.5 µg/m3 ( ~8µg/m3 with uf correction)

  • Calculated mass, 3.7 µg/m3 light, 1.7 µg/m3 trucks, for 5.4 µg/m3; with literature values, 7.7 µg/m3


Summary of watt avenue impacts l.jpg
Summary of Watt Avenue impacts concentrations of lead

  • Mass numbers calculated are in fair to good agreement with observed values, car and truck

  • About 1/3 of the mass is diesel, even through diesels were only about 1.5% of the average vehicle mix

  • Very fine aerosols at the downwind school site have many of the elements predicted from the laboratory and Tuscarora studies,

  • Very fine aerosols 300 m upwind (Sebastian Way) are much lower that downwind at the school, and much lower than downtown Sacramento.


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Very fine aerosols characteristic of diesels/smoking cars in Fresno > 1 km from freeways

Predicted diesel vf/uf mass 11/25 – 12/17, 9 ± 6 µg/m3


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Nov 25 – Dec. 17, measured mass = 4.8 Fresno > 1 km from freeways± 1.0, predicted mass = 6.6 ± 4.8,

estimated total very fine mass = 8.8 μg/m3


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Persistence of very fine/ultra fine particles Fresno > 1 km from freeways

  • We find high concentrations of very fine particles near freeways in periods of stagnation,

  • We also find significant concentrations (6 µg/m3) over large areas of downtown Sacramento well away (> 400 m) from the nearest freeway source

  • Even higher levels are seen in Fresno in winter, in a residential neighborhood > 1 km away from the nearest freeway.

  • Recent work in Los Angeles finds ultra fines falling off from freeways roughly as rapidly as diffusion-limited CO, so coagulation appears to be limited and lifetimes long (for the non H2SO4 fraction).


Study of ultrafine particles near a major highway with heavy duty diesel traffic zhu et al 2002 l.jpg
Study of ultrafine particles near a major highway with heavy-duty diesel traffic Zhu et al (2002)


Study of ultrafine particles near a major highway zhu et al 2002 lead from cahill et al arb 1974 l.jpg
Study of ultrafine particles near a major highway Zhu et al (2002); Lead from Cahill et al (ARB, 1974)

BC, number -diesels

CO, Pb - cars


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Conclusions (2002); Lead from Cahill et al (ARB, 1974)

  • Diesel exhaust mass lies almost entirely in the very fine mode < 0.25 µm; ultra-fine mode misses ~ ½ of the diesel mass.

  • Laboratory and field studies are consistent in composition and particle size, allowing calculation of diesel impacts.

  • Separation of diesel and smoking car exhaust is difficult, organic tracers unstable and uncertain, and costs high.

  • Smoking car exhaust appears to be as toxic as diesel exhaust per unit mass.

  • Diesel and smoking car exhaust represents most of the very fine mass in Sacramento and Fresno, even well away from freeways.

  • Diesel and smoking car exhaust must be measured in ambient urban and sub-urban sites where it is a significant and toxic fraction of PM2.5 mass.


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Proposals for California (2002); Lead from Cahill et al (ARB, 1974)

  • We propose getting automobile smoke listed as a Toxic Air Contaminant (TAC) under California Prop 65, joining diesel

    • Diesel is presently 70% of the cancer risk of all current California TACs, combined.

  • We have initiated PM0.25 mass measurements in the CA Central Valley, using High Schools and air district support.

    • We have deployed robust, simple and inexpensive monitors to begin generating data on possible PM0.25 – health associations

  • We propose that these urgent but unmet needs can be addressed via a new California PM0.25 mass standard

    • It would include diesels, smoking cars, and other high temperature processes (coal fired power plants, smelting, welding, ….) that generate very fine and ultra fine particles of suspected health impacts.

    • It avoids the difficulty and expense of routinely resolving the diesel-smoking car overlap, since it appears both are toxic and both must be controlled

    • It could in the future allow the possibility of US EPA re-evaluating the PM2.5 standard if it turns out that 2.5 μm – 0.25 μm mode aerosols prove less harmful to human health.


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Acknowledgements (2002); Lead from Cahill et al (ARB, 1974)

  • American Lung Association – Sacramento Emigrant Trails Health Effects Task Force – many volunteers, modest funding, excellent oversight

  • National Renewable Energy Laboratory – DRI diesel tests

  • Health Effects Institute – Tuscarora Tunnel studies

  • California Air Resources Board – Fresno FACES study

  • Tahoe Regional Planning Agency and CalTrans – Tahoe Studies

  • Department of Energy - Lawrence Berkeley NL and the Advanced Light Source – S-XRF capabilities

  • National Science Foundation – ACE-Asia DRUM samplers


Ultra fine particles near a busy road gramotnev and ristovski atm env 2003 l.jpg
“…ultra-fine particles near a busy road” (2002); Lead from Cahill et al (ARB, 1974) – (Gramotnev and Ristovski Atm. Env. 2003)


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Wood Smoke at South Lake Tahoe (2002); Lead from Cahill et al (ARB, 1974)

Oregon fire smoke


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