Particle Measurements Understanding and Reducing Residential Wood Combustion Emissions November 30, 2016 Albany, NY Track 2A - Test Methods for Residential Wood Heating Technologies Methods (Stoves and Boilers) Brian P. Frank, Ph.D., P.E. Emissions Measurement Research Group Bureau of Mobile Sources and Technology Development Division of Air Resources New York State Department of Environmental Conservation Pat Mason Fritz, M. Eng. Exposure Characterization and Response Section Bureau of Toxic Substance Assessment Division of Environmental Health New York State Department of Health April 20, 2016 DRAFT

Project Partners NYSDEC Emissions Measurement Research Group Division of Air Resources, Bureau of Mobile Sources and Technology Development NYSDOH Exposure Characterization & Response Section Division of Environmental Health Assessment, Bureau of Toxic Substance Assessment Brookhaven National Laboratories Sustainable Energy Technology System NYSERDA Contract 63033 DRAFT

Why a Mobile Source Group? Relative contributions of mobile sources vs. other sources Source apportionment Focus on emissions which are currently unregulated Ultrafines Elemental Carbon/Organic Carbon Particle morphology Toxics (PAHs, carbonyls) Adapt source measurement methodology from mobile source to biomass Sampling and dilution Real-time instrumentation DRAFT

Ultrafines Sampling Mobile Source DRAFT

Proposed BNL Ultrafines Sampling Stack View from Mezzanine Start of BNL Sampling Biomass Appliance DRAFT

Source Measurement for Ultrafines Ultrafines are emitted from combustion sources at high Particle concentration Temperature Humidity Co-pollutant(s) concentration Source conditions Are unmanageable for instrumentation Lead to complex formation processes Need to address Sampling Isokinetic Dilution High Variable DRAFT

Isokinetic Sampling Exhaust flow velocity = Sampling inlet velocity Exhaust flow velocity measurement always nontrivial Sampling inlet velocity range ~ 0.4 to 1.48 fps http://www.airflowsciences.com/Services/FieldTesting/Isokinetic DRAFT

Source Measurement Dilution Effects < 30: 1 dilution – particle size distribution is altered and unsteady-state > 30:1 dilution – particle size distribution is unaltered and stable Investigations into Diesel Particulate Morphology: Part 1, DEC Internal Report, 9/10/04, Frank. DRAFT

Source Sampling Dilution System Differential pressure transducer Dilution air mass flow meter Primary dilution pressure regulator Secondary dilution pressure regulator Overflow port Secondary dilution manifold Dilution chamber Sampling chamber Inlet flow control orifice Primary dilution manifold DRAFT

Dilution System Variability Dilution as a function of primary and secondary pressure. Inlet flow as a function of primary and secondary pressure. Standard deviation (sigma value) of dilution. Standard deviation (sigma value) of inlet flow DRAFT

Why a Mobile Source Group? Relative contributions of mobile sources vs. other sources Source apportionment Focus on emissions which are currently unregulated Ultrafines Elemental Carbon/Organic Carbon Particle morphology Toxics (PAHs, carbonyls) Adapt source measurement methodology from mobile source to biomass Sampling and dilution Real-time instrumentation DRAFT

Real-Time (1 Hz) Instrumentation + Sampling Dilution air Overflow DRAFT

Electrical Low Pressure Impactor (ELPI+) Multistage impactor Aerodynamic size range from ultrafine to PM10 6, 16, 30, 54, 94, 150, 250, 380, 600, 940 nm; 1.6, 2.5, 3.6, 5.3, 10 microns 1 Hz time resolution Buffer for obtaining steady-state measurements Ability to measure transients Size-resolved sample capture for analysis DRAFT

Mobile Source Cold Starts ELPI Data A. Engine Out B. Diesel Oxidation Catalyst A B C D C. Continuously Regenerating Diesel Particulate Filter D. Exhaust Gas Recirculation – Diesel Particulate Filter Brian P. Frank, Shida Tang, Thomas Lanni, Jillian Grygas, Greg Rideout, Norman Meyer, Chris Beregszaszy, “The Effect of Fuel Type and Aftertreatment Method on Ultrafine Particle Emissions from a Heavy-Duty Diesel Engine”, Aerosol Science and Technology, 41:1029-1039, 2007. DRAFT

Size-Resolved Sampling ELPI (left) and SMPS (above) Display of Particle Distribution Centered on ELPI Stage 1, D50 = 30 nm, SMPS Geometric Mean = 37.1 nm Particle deposition centered on various stages; bottom left is stage1, upper right is stage 12; heaviest loading on stage 5. ELPI (left) and SMPS (above) Display of Particle Distribution Centered on ELPI Stage 3, D50 = 109 nm SMPS Geometric Mean = 90.1 nm Patricia M. Fritz, Brian P. Frank, David Guerrieri, Shida Tang, and Daniel Hershey, Poster: “Determination of Chemical and Morphological Properties of Size-Segregated Aerosol Particles Using the Electrical Low Pressure Impactor”, 2013 American Association for Aerosol Research 32nd Annual Conference, Portland, OR, September 30 - October 4, 2013. DRAFT

Size-Resolved Sampling: OC/EC Two similar Combustion Aerosol Standard (CAST) particle size distributions: Rich Lean OC/EC ratios are not uniform across the entire distribution and do not correlate to the overall rich or lean condition. Smaller particles have higher OC/EC ratios Surface area (size) Surface area (morphology) Affinities Varying OC/EC ratios may also have a direct effect on particle density Has potential implications for both health and climate change. Patricia M. Fritz, Shida D. Tang, David Guerrieri, Brian P. Frank, Marilyn Wurth, William Chien, Gerald T. Willson, and Malissa Kramer, Poster: “Evaluating Elemental and Organic Carbon Composition of Size-Segregated Combustion Particles Using the Electrical Low Pressure Impactor”, 2014 American Association for Aerosol Research 33rd Annual Conference, Orlando, FL, October 20 – 24, 2014. DRAFT

Basic Particle Information for Monitoring and Health Consideration Particle transport behavior in air differs, depending on physical size, shape, density, and surface characteristics For Fine and Coarse PM fractions, gravitational forces Settling Impaction & interception For UFP it is diffusion and agglomeration (concentration, electrostatic, thermal and radiometric forces) Sampling equipment exploits particle characteristics, but we need multiple instruments, using multiple technologies to explore the particle size distribution from UFP to Coarse. Health considerations probably hinge on particle characteristics, but we are a long way from completely understanding which characteristics matter most, much less which characteristics matter most for a specific health endpoint. DRAFT

surface characteristics solubility particle numbers Factors influencing how it gets there, versus factors for behavior, hence biological effects, once there. Getting there: aerodynamic size geometric size, shape hydrophobicity surface charge Behavior once there: where deposited geometric size shape surface characteristics solubility particle numbers Sampling equipment exploits particle characteristics, but we need multiple instruments, using multiple technologies to explore the particle size distribution from UFP to Coarse. DRAFT

Human Respiratory Tract and Particle Exposure Implications DRAFT

DRAFT How likely are particles, based on aerodynamic diameter, likely to enter and be retained in the human respiratory tract The EPA and OSHA have balanced the info in this illustration along with the sampling tools the had, to develop standards. As far as deposition probability there isn’t much difference for particles that are 2.5 vs 4 micrometers in diameter- above 10 deposition is almost entirely upper airways- with deflection downward somewhere around maybe 20 micrometers. Using this curve and assuming that deposition matters, the least interesting portion of the curve with respect to health appears to be for particles in the 200 -400 nanometer size range. My personal bias, is to include measurement of particles at this end of the particle size distribution and to begin to consider health endpoints beyond respiratory and cardiovascular. If you are small enough, and deposit in the head airways there is a pathway directly to the brain without interference from the blood/brain barrier. DRAFT DRAFT

Research on the Role and Effects of Particulates in Exposure and Disease is Unfolding Quickly (and may not be keeping up with technologies that generate UFP) Toxicological cell culture and animals studies and epidemiological studies of fine particulates and ultrafine particulates in humans find unique and overlapping effects, including cardiovascular, pulmonary, and central nervous system effects, and mortality. Previous mass based potency differences for different particle sizes may be due to how dose is expressed. UFP particles may appear less or more potent on a mass basis, but have equivalent potency with larger PM fractions, if the dose metric is surface area or number concentration. Particle concentrations, characteristics and ultimate deposition location all are likely to influence exposure and health outcomes. DRAFT

DRAFT EPA: 2009 PM ISA for 2012 NAAQS 24-Hr NAAQS The Integrated Science Assessment (ISA) did not find enough evidence to determine that UFPs (in isolation) were Causal: (proven to cause a negative health outcome) Annual NAAQS The strength of the associations vary with particle size- and to date without being able to attribute observed health effects to a specific PM component. Inflammatory effects may be a common feature though. Source: Integrated Science Assessment for Particulate Mat (US EPA 2009) DRAFT DRAFT

Collecting Emissions Data to Inform Industry and Policy makers Characterization of the particle size distribution, carbon emissions profile and gaseous composition of biomass smoke emissions across different technologies, operation conditions, and stack configurations can inform: Policies that consider energy efficiency and low emissions when selecting biomass-fueled heating appliances Environmentally responsible operation that minimizes environmental impacts and fuel costs. Selection of mitigation approaches to comprehensively address exposure concerns DRAFT

Thank You Pat Mason Fritz, M. Eng. Brian P. Frank, Ph.D., P.E. Section Chief, Emissions Measurement Research Group Bureau of Mobile Sources and Technology Development Division of Air Resources brian.frank@dec.ny.gov 518-402-8355 Pat Mason Fritz, M. Eng. Exposure Characterization and Response Section Bureau of Toxic Substance Assessment Division of Environmental Health Assessment patricia.fritz@health.ny.gov 518-402-7800 DRAFT