ALBERT

Description: Residential solid biomass cookstoves are important sources of aerosol emissions in India. Cookstove emissions rates are largely based on laboratory experiments conducted using the standard water-boiling test, but real-world emissions are often higher owing to different stove designs, fuels, and cooking methods. Constraining mass emissions factors (EFs) for prevalent cookstoves is important because they serve as inputs to bottom-up emissions inventories used to evaluate health and climate impacts. Real-world EFs were measured during winter 2015 for a traditional cookstove (chulha) burning fuel wood, agricultural residue, and dung from different regions of India. Average (±95 % confidence interval) EFs for fuel wood, agricultural residue, and dung were (1) PM2.5 mass: 10.5 (7.7–13.4) g kg−1, 11.1 (7.7–15.5) g kg−1, and 22.6 (14.9–32.9) g kg−1, respectively; (2) elemental carbon (EC): 0.9 (0.6–1.4) g kg−1, 1.6 (0.6–3.0) g kg−1, and 1.0 (0.4–2.0) g kg−1, respectively; and (3) organic carbon (OC): 4.9 (3.2–7.1) g kg−1, 7.0 (3.5–12.5) g kg−1, and 12.9 (4.2–15.01) g kg−1, respectively. The mean (±95 % confidence interval) OC ∕ EC mass ratios were 6.5 (4.5–9.1), 7.6 (4.4–12.2), and 12.7 (6.5–23.3), respectively, with OC and EC quantified by the IMPROVE_A thermal-optical reflectance protocol. These real-world EFs are higher than those from previous laboratory-based measurements. Combustion conditions have larger effects on EFs than the fuel types. We also report the carbon mass fractions of our aerosol samples determined using the thermal-optical reflectance method. The mass fraction profiles are consistent between the three fuel categories but markedly different from those reported in past literature – including the source profiles for wood stove PM2.5 emissions developed as inputs to receptor modeling studies conducted by the Central Pollution Control Board of India. Thermally stable OC (OC3 in the IMPROVE_A protocol) contributed nearly 50 % of the total carbon mass for emissions from all fuels.

Description: In many parts of the developing world and economies in transition, small-scale traditional brick kilns are a notorious source of urban air pollution. Many are both energy inefficient and burn highly polluting fuels that emit significant levels of black carbon (BC), organic carbon (OC) and other atmospheric pollutants into local communities, resulting in severe health and environmental impacts. However, only a very limited number of studies are available on the emission characteristics of brick kilns; thus, there is a need to characterize their gaseous and particulate matter (PM) emission factors to better assess their overall contribution to emissions inventories and to quantify their ecological, human health, and climate impacts. In this study, the fuel-, energy-, and brick-based emissions factors and time-based emission ratios of BC, OC, inorganic PM components, CO, SO2, CH4, NOx, and selected volatile organic compounds (VOCs) from three artisanal brick kilns with different designs in Mexico were quantified using the tracer ratio sampling technique. Simultaneous measurements of PM components, CO, and CO2 were also obtained using a sampling probe technique. Additional measurements included the internal temperature of the brick kilns, mechanical resistance of bricks produced, and characteristics of fuels employed. Average fuel-based BC emission factors ranged from 0.15 to 0.58 g (kg fuel)−1, whereas BC∕OC mass ratios ranged from 0.9 to 5.2, depending on the kiln type. The results show that both techniques capture similar temporal profiles of the brick kiln emissions and produce comparable emission factors. A more integrated inter-comparison of the brick kilns' performances was obtained by simultaneously assessing emissions factors, energy efficiency, fuel consumption, and the quality of the bricks produced.

Description: Smoke from laboratory chamber burning of peat fuels from Russia, Siberia, the USA (Alaska and Florida), and Malaysia representing boreal, temperate, subtropical, and tropical regions was sampled before and after passing through a potential-aerosol-mass oxidation flow reactor (PAM-OFR) to simulate intermediately aged (∼2 d) and well-aged (∼7 d) source profiles. Species abundances in PM2.5 between aged and fresh profiles varied by several orders of magnitude with two distinguishable clusters, centered around 0.1 % for reactive and ionic species and centered around 10 % for carbon. Organic carbon (OC) accounted for 58 %–85 % of PM2.5 mass in fresh profiles with low elemental carbon (EC) abundances (0.67 %–4.4 %). OC abundances decreased by 20 %–33 % for well-aged profiles, with reductions of 3 %–14 % for the volatile OC fractions (e.g., OC1 and OC2, thermally evolved at 140 and 280 ∘C). Ratios of organic matter (OM) to OC abundances increased by 12 %–19 % from intermediately aged to well-aged smoke. Ratios of ammonia (NH3) to PM2.5 decreased after intermediate aging. Well-aged NH4+ and NO3- abundances increased to 7 %–8 % of PM2.5 mass, associated with decreases in NH3, low-temperature OC, and levoglucosan abundances for Siberia, Alaska, and Everglades (Florida) peats. Elevated levoglucosan was found for Russian peats, accounting for 35 %–39 % and 20 %–25 % of PM2.5 mass for fresh and aged profiles, respectively. The water-soluble organic carbon (WSOC) fractions of PM2.5 were over 2-fold higher in fresh Russian peat (37.0±2.7 %) than in Malaysian (14.6±0.9 %) peat. While Russian peat OC emissions were largely water-soluble, Malaysian peat emissions were mostly water-insoluble, with WSOC ∕ OC ratios of 0.59–0.71 and 0.18–0.40, respectively. This study shows significant differences between fresh and aged peat combustion profiles among the four biomes that can be used to establish speciated emission inventories for atmospheric modeling and receptor model source apportionment. A sufficient aging time (∼7 d) is needed to allow gas-to-particle partitioning of semi-volatilized species, gas-phase oxidation, and particle volatilization to achieve representative source profiles for regional-scale source apportionment.

Description: Peat fuels representing four biomes of boreal (western Russia and Siberia), temperate (northern Alaska, USA), subtropical (northern and southern Florida, USA), and tropical (Borneo, Malaysia) regions were burned in a laboratory chamber to determine gas and particle emission factors (EFs). Tests with 25 % fuel moisture were conducted with predominant smoldering combustion conditions (average modified combustion efficiency (MCE) =0.82±0.08). Average fuel-based EFCO2 (carbon dioxide) are highest (1400 ± 38 g kg−1) and lowest (1073 ± 63 g kg−1) for the Alaskan and Russian peats, respectively. EFCO (carbon monoxide) and EFCH4 (methane) are ∼12 %–15 % and ∼0.3 %–0.9 % of EFCO2, in the range of 157–171 and 3–10 g kg−1, respectively. EFs for nitrogen species are at the same magnitude as EFCH4, with an average of 5.6 ± 4.8 and 4.7 ± 3.1 g kg−1 for EFNH3 (ammonia) and EFHCN (hydrogen cyanide); 1.9±1.1 g kg−1 for EFNOx (nitrogen oxides); and 2.4±1.4 and 2.0 ± 0.7 g kg−1 for EFNOy (total reactive nitrogen) and EFN2O (nitrous oxide). An oxidation flow reactor (OFR) was used to simulate atmospheric aging times of ∼2 and ∼7 d to compare fresh (upstream) and aged (downstream) emissions. Filter-based EFPM2.5 varied by 〉 4-fold (14–61 g kg−1) without appreciable changes between fresh and aged emissions. The majority of EFPM2.5 consists of EFOC (organic carbon), with EFOC ∕ EFPM2.5 ratios in the range of 52 %–98 % for fresh emissions and ∼14 %–23 % degradation after aging. Reductions of EFOC (∼7–9 g kg−1) after aging are most apparent for boreal peats, with the largest degradation in low-temperature OC1 that evolves at  95 %) of the total emitted carbon is in the gas phase, with 54 %–75 % CO2, followed by 8 %–30 % CO. Nitrogen in the measured species explains 24 %–52 % of the consumed fuel nitrogen, with an average of 35 ± 11 %, consistent with past studies that report ∼1/3 to 2∕3 of the fuel nitrogen measured in biomass smoke. The majority (〉 99 %) of the total emitted nitrogen is in the gas phase, with an average of 16.7 % as NH3 and 9.5 % as HCN. N2O and NOy constituted 5.7 % and 2.9 % of consumed fuel nitrogen. EFs from this study can be used to refine current emission inventories.

Description: Carbonaceous aerosol is a major contributor to the total aerosol load and being monitored by diverse measurement approaches. Here, 10 years (2005–2015) of continuous carbonaceous aerosol measurements collected at the Centre of Atmospheric Research Experiments (CARE) in Egbert, Ontario, Canada, on quartz-fiber filters by three independent networks (Interagency Monitoring of Protected Visual Environments, IMPROVE; Canadian Air and Precipitation Monitoring Network, CAPMoN; and Canadian Aerosol Baseline Measurement, CABM) were compared. Specifically, the study evaluated how differences in sample collection and analysis affected the concentrations of total carbon (TC), organic carbon (OC), and elemental carbon (EC). Results show that different carbonaceous fractions measured by various networks were consistent and comparable in general among the three networks over the 10-year period, even with different sampling systems/frequencies, analytical protocols, and artifact corrections. The CAPMoN TC, OC, and EC obtained from the DRI model 2001 thermal–optical carbon analyzer following the IMPROVE-TOR protocol (denoted as DRI-TOR) method were lower than those determined from the IMPROVE_A TOR method by 17 %, 14 %, and 18 %, respectively. When using transmittance for charring correction, the corresponding carbonaceous fractions obtained from the Sunset-TOT were lower by as much as 30 %, 15 %, and 75 %, respectively. In comparison, the CABM TC, OC, and EC obtained from a thermal method, EnCan-Total-900 (ECT9), were higher than the corresponding fractions from IMPROVE_A TOR by 20 %–30 %, 0 %–15 %, and 60 %–80 %, respectively. Ambient OC and EC concentrations were found to increase when ambient temperature exceeded 10 ∘C. These increased ambient concentrations of OC during summer were possibly attributed to secondary organic aerosol (SOA) formation and forest fire emissions, while elevated EC concentrations were potentially influenced by forest fire emissions and increased vehicle emissions. Results also show that the pyrolyzed organic carbon (POC) obtained from the ECT9 protocol could provide additional information on SOA although more research is still needed.

Description: Residential solid biomass cookstoves are important sources of aerosol emissions in India. Cookstove emission rates are largely based on laboratory experiments conducted using the standard water-boiling test, but real-world emissions are often higher owing to different stove designs, fuels, and cooking methods. Constraining mass emission factors (EFs) for prevalent cookstoves is important because they serve as inputs to bottom-up emission inventories used to evaluate health and climate impacts. Real-world EFs were measured during winter, 2015, for a traditional cookstove (chulha) burning fuel-wood (FW), agricultural residue (AG) and dung (DG) from different regions of India. Average (±95 % confidence interval) EFs for FW, AG, and DG were: 1) PM2.5 mass: 6.8 (4.7–9.4) g kg−1, 7.1 (3.9–11.8) g kg−1, and 14.5 (7.5–25.3) g kg−1, respectively; 2) elemental carbon (EC): 0.6 (0.4–0.9) g kg−1, 1.0 (0.4–2.0) g kg−1, and 0.6 (0.3–1.3) g kg−1, respectively; and 3) Organic carbon (OC): 3.1 (2.0–4.6) g kg−1, 4.5 (2.3–8.0) g kg−1, and 8.2 (4.2–15.01) g kg−1, respectively. The mean (±95 % confidence interval) OC-to-EC mass ratios were 6.5 (4.5–9.1), 7.6 (4.4–12.2), and 12.7 (8.8–17.8), respectively, with OC and EC quantified by the IMPROVE_A thermal/optical reflectance protocol. These real-world EFs are higher than those from laboratory-based measurements. Combustion conditions have larger effects on EFs than the fuel-types. We also report the carbon mass fractions of our aerosol samples determined using the thermal-optical reflectance method. The mass fraction profiles are consistent between the three fuel categories, but markedly different from those reported in past literature.

Description: Peat fuels representing four biomes of boreal (western Russia and Siberia), temperate (northern Alaska, U.S.A.), subtropical (northern and southern Florida, U.S.A), and tropical (Borneo, Malaysia) regions were burned in a laboratory chamber to determine gas and particle emission factors (EFs). Tests with 25 % fuel moisture were conducted with predominant smoldering combustion conditions (average modified combustion efficiency [MCE] = 0.82 ± 0.08). Average fuel-based EFCO2 (carbon dioxide) are highest (1400 ± 38 g kg−1) and lowest (1073 ± 63 g kg−1) for the Alaskan and Russian peats, respectively. EFCO (carbon monoxide) and EFCH4 (methane) are ~12 %‒15 % and ~0.3 %‒0.9  % of EFCO2, in the range of 157‒171 g kg−1 and 3‒10 g kg−1, respectively. EFs for nitrogen species are at the same magnitude of EFCH4, with an average of 5.6 ± 4.8 and 4.7 ± 3.1 g kg−1 for EFNH3 (ammonia) and EFHCN (hydrogen cyanide); 1.9 ± 1.1 g kg−1 for EFNOx (nitrogen oxides); as well as 2.4 ± 1.4 and 2.0 ± 0.7 g kg−1 for EFNOy (reactive nitrogen) and EFN2O (nitrous oxide). An oxidation flow reactor (OFR) was used to simulate atmospheric aging times of ~2 and ~7 days to compare fresh (upstream) and aged (downstream) emissions. Filter-based EFPM2.5 varied by 〉4-fold (14‒61 g kg−1) without appreciable changes between fresh and aged emissions. The majority of EFPM2.5 consists of EFOC (organic carbon), with EFOC/EFPM2.5 ratios in the range of 52 %‒98 % for fresh emissions, and ~15 % degradation after aging. Reductions of EFOC (~7‒9 g kg−1) after aging are most apparent for boreal peats with the largest degradation in organic carbon that evolves at 〈140 °C, indicating the loss of high vapor pressure semi-volatile organic compounds upon aging. The highest EFLevoglucosan is found for Russian peat (~16 g kg−1), with ~35 %‒50 % degradation after aging. EFs for water-soluble OC (EFWSOC) accounts for ~20 %‒62 % of fresh EFOC. The majority (〉95 %) of the total emitted carbon is in the gas phase with 54 %‒75 % CO2, followed by 8 %‒30 % CO. Nitrogen in the measured species explains 24 %‒52 % of the consumed fuel nitrogen with an average of 35 ± 11 %, consistent with past studies that report ~one- to two-thirds of the fuel nitrogen measured in biomass smoke. The majority (〉99 %) of the total emitted nitrogen is in the gas phase, with an average of 16.7 % fuel N emitted as NH3 and 9.5 % of fuel N emitted as HCN. N2O and NOy constituted 5.7 % and 2.9 % of consumed fuel N. EFs from this study can be used to refine current emissions inventories.

Description: Smoke from laboratory chamber burning of peat fuels from Russia, Siberia, U.S.A. (Alaska and Florida), and Malaysia representing boreal, temperate, subtropical, and tropical regions was sampled before and after passing through a potential aerosol mass-oxidation flow reactor (PAM-OFR) to simulate ∼2- and 7-day atmospheric aging. Species abundances in PM2.5 between aged and fresh profiles varied by 〉5 orders of magnitude with two distinguishable clusters: around 0.1 % for reactive and ionic species and mostly 〉10 % for carbon. Organic carbon (OC) accounted for 58–85 % of PM2.5 mass in fresh profiles with low EC abundance (0.67–4.4 %). After a 7-day aging time, degradation was 20–33 % for OC, with apparent reductions (4–12 %) in low temperature OC1 and OC2 (thermally evolved at 140 and 280 °C), implying evaporation of higher vapor pressure semi-volatile organic compounds (SVOCs). Additional losses of OC from 2- to 7-days aging is somewhat offset by the formation of oxygenated organic compounds, as evidenced by the 12–19 % increase in organic mass (OM) to OC ratios. However, the reduction of OM abundances in PM2.5 by 3–18 % after 7 days, reconfirms that volatilization is the main loss mechanism of SVOCs. Although the ammonia (NH3) to PM2.5 ratio rapidly diminished with a 2-day aging time, it represents an intermediate profile – not sufficient for completed OC evaporation, levoglucosan degradation, organic acid oxidation, or secondary inorganic aerosol formation. Week-long aging resulted in an increase to ∼7–8 % of NH4+ and NO3− abundances, but with enhanced degradation of NH3, low temperature OC, and levoglucosan for Siberia, Alaska, and Everglasdes (FL) peats. Elevated levoglucosan was found for Russian peats, accounting for 35–39 % and 20–25 % of PM2.5 mass for fresh and aged profiles, respectively. Abundances of water-soluble organic carbon (WSOC) in PM2.5 was 〉2-fold higher in fresh Russian (37.0 ± 2.7 %) than Malaysian (14.6 ± 0.9 %) peats. While Russian peat OC emissions are largely water-soluble, Malaysian peat emissions are mostly water-insoluble, with WSOC/OC ratios of 0.59–0.71 and 0.18–0.40, respectively. Source profiles can change with aging during transport from source to receptor. This study shows significant differences between fresh and aged peat combustion profiles among the four biomes that can be used to establish speciated emission inventories for atmospheric modeling and receptor model source apportionment. A sufficient aging time (∼one week) is needed to allow gas-to-particle partitioning of semi-volatilized species, gas-phase oxidation, and particle volatilization to achieve representative source profiles for regional-scale source apportionment.

Description: In many parts of the developing world and economies in transition, small-scale traditional brick kilns are a notorious source of urban air pollution. Many are both energy inefficient and burn highly polluting fuels that emit significant levels of black carbon (BC), organic carbon (OC) and other atmospheric pollutants into local communities, resulting in severe health and environmental impacts. However, only a very limited number of studies are available on the emission characteristics of brick kilns; thus there is a need to characterize their gaseous and particulate matter (PM) emission factors to better assess their overall contribution to emissions inventories and to quantify their ecological, human health, and climate impacts. In this study, the fuel-, energy-, and brick-based emissions factors and time-based emission ratios of BC, OC, inorganic PM components, CO, SO2, CH4, NOx, and selected volatile organic compounds (VOCs) from two traditional artisanal kilns and one MK2 kiln in Mexico were quantified using the tracer ratio sampling technique. Simultaneous measurements of PM components, CO and CO2 were also obtained using a filter-based sampling probe technique. Additional measurements included the internal temperature of the brick kilns, mechanical resistance of bricks produced, and characteristics of fuels employed. The results show that both techniques capture similar temporal profiles of the brick kiln emissions and produce comparable emission factors, indicating that the tracer ratio technique can be an alternative option to the filter-based sampling probe technique in understanding the temporal profile of the chemical composition of brick kilns emissions. A more integrated inter-comparison of the brick kilns' performances was obtained by simultaneously assessing emissions factors, energy efficiency, fuel consumption, and the quality of the bricks produced. Overall, a well-designed and operated MK2 kiln produced lower PM2.5, BC, OC emission factors and higher energy efficiency than the traditional artisanal brick kilns. Average fuel-based BC emission factors ranged from 0.15–0.58 g/kg-fuel whereas BC / OC mass ratios ranged from 0.9–5.2, depending on the kiln type. The results from this study contribute to the limited number of databases available on the emission characteristics of the informal brick production sector.

Description: Carbonaceous aerosol is a major contributor to the total aerosol load and being monitored by diverse measurement approaches. Here, ten years of continuous carbonaceous aerosol measurements collected at the Centre of Atmospheric Research Experiments (CARE) in Egbert, Ontario, Canada on quartz filters by three independent networks (Interagency Monitoring of PROtected Visual Environments (IMPROVE), Canadian Air and Precipitation Monitoring Network (CAPMoN), and Canadian Aerosol Baseline Measurement (CABM)) were compared. Specifically, the study evaluated how differences in sample collection and analysis affected the yield of total carbon (TC), organic carbon (OC), and elemental carbon (EC). When all measurements were normalized with respect to concentration measured in a common reference year, OC measurements agreed to within 29–48 % and EC measurement to within 20 % amongst the different networks. Fitted with a sigmoid function, elevated OC and EC concentrations were found when ambient temperature exceeded 10 °C. These increased ambient concentrations of OC during summer were attributed to the secondary organic aerosol (SOA) formation and forest fire emissions, while elevated EC concentrations were attributed to forest fire emissions and increased vehicle emissions. The observations from this study suggest that carbonaceous aerosol measurements, especially EC, can be synchronized across networks if sample collection and analytical method in each network remain internally consistent. This study allows the generation of regional to continental-scale-harmonized concentration data sets for benchmarking of atmospheric chemical transport models that determine emission sources and sinks, and assess the effectiveness of government mitigation policies in improving air quality and reducing reliance on fossil fuel consumption.