Indoor terpene emissions from cooking with herbs and pepper and their secondary organic aerosol production potential

Cooking is widely recognized as an important source of indoor and outdoor particle and volatile organic compound emissions with potential deleterious effects on human health. Nevertheless, cooking emissions remain poorly characterized. Here the effect of herbs and pepper on cooking emissions was investigated for the first time to the best of our knowledge using state of the art mass spectrometric analysis of particle and gas-phase composition. Further, the secondary organic aerosol production potential of the gas-phase emissions was determined by smog chamber aging experiments. The emissions of frying meat with herbs and pepper include large amounts of mono-, sesqui- and diterpenes as well as various terpenoids and p-cymene. The average total terpene emission rate from the use of herbs and pepper during cooking is estimated to be 46 ± 5 gg-1 Herbs min-1. These compounds are highly reactive in the atmosphere and lead to significant amounts of secondary organic aerosol upon aging. In summary we demonstrate that cooking with condiments can constitute an important yet overlooked source of terpenes in indoor air

Brown Carbon in Primary and Aged Coal Combustion Emission

Smog chamber experiments were conducted to characterize the light absorption of brown carbon (BrC) from primary and photochemically aged coal combustion emissions. Light absorption was measured by the UV-visible spectrophotometric analysis of water and methanol extracts of filter samples. The single-scattering albedo at 450 nm was 0.73 ± 0.10 for primary emissions and 0.75 ± 0.13 for aged emissions. The light absorption coefficient at 365 nm of methanol extracts was higher than that of water extracts by a factor of 10 for primary emissions and a factor of 7 for aged emissions. This suggests that the majority of BrC is water-insoluble even after aging. The mass absorption efficiency of this BrC (MAE365) for primary OA (POA) was dependent on combustion conditions, with an average of 0.84 ± 0.54 m2 g-1, which was significantly higher than that for aged OA (0.24 ± 0.18 m2 g-1). Secondary OA (SOA) dominated aged OA and the decreased MAE365 after aging indicates that SOA is less light absorbing than POA and/or that BrC is bleached (oxidized) with aging. The estimated MAE365 of SOA (0.14 ± 0.08 m2 g-1) was much lower than that of POA. A comparison of MAE365 of residential coal combustion with other anthropogenic sources suggests that residential coal combustion emissions are among the strongest absorbing BrC organics

Characterization of Gas-Phase Organics Using Proton Transfer Reaction Time-of-Flight Mass Spectrometry : Cooking Emissions

Cooking processes produce gaseous and particle emissions that are potentially deleterious to human health. Using a highly controlled experimental setup involving a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS), we investigate the emission factors and the detailed chemical composition of gas phase emissions from a broad variety of cooking styles and techniques. A total of 95 experiments were conducted to characterize nonmethane organic gas (NMOG) emissions from boiling, charbroiling, shallow frying, and deep frying of various vegetables and meats, as well as emissions from vegetable oils heated to different temperatures. Emissions from boiling vegetables are dominated by methanol. Significant amounts of dimethyl sulfide are emitted from cruciferous vegetables. Emissions from shallow frying, deep frying and charbroiling are dominated by aldehydes of differing relative composition depending on the oil used. We show that the emission factors of some aldehydes are particularly large which may result in considerable negative impacts on human health in indoor environments. The suitability of some of the aldehydes as tracers for the identification of cooking emissions in ambient air is discussed

Formation of Highly Oxygenated Organic Molecules from alpha-Pinene Ozonolysis : Chemical Characteristics, Mechanism, and Kinetic Model Development

Terpenes are emitted by vegetation, and their oxidation in the atmosphere is an important source of secondary organic aerosol (SOA). A part of this oxidation can proceed through an autoxidation process, yielding highly oxygenated organic molecules (HOMs) with low saturation vapor pressure. They can therefore contribute, even in the absence of sulfuric acid, to new particle formation (NPF). The understanding of the autoxidation mechanism and its kinetics is still far from complete. Here, we present a mechanistic and kinetic analysis of mass spectrometry data from α-pinene (AP) ozonolysis experiments performed during the CLOUD 8 campaign at CERN. We grouped HOMs in classes according to their identified chemical composition and investigated the relative changes of these groups and their components as a function of the reagent concentration. We determined reaction rate constants for the different HOM peroxy radical reaction pathways. The accretion reaction between HOM peroxy radicals was found to be extremely fast. We developed a pseudo-mechanism for HOM formation and added it to the AP oxidation scheme of the Master Chemical Mechanism (MCM). With this extended model, the observed concentrations and trends in HOM formation were successfully simulated.Peer reviewe

Urban case studies : general discussion

Urban case studies: general discussio

Biogenic carbon-enriched and pollutant depleted SRF from commercial and pretreated heterogeneous waste generated by NIR sensor-based sorting

Mechanical processing using predominantly particle size and density as separation criteria is currently applied in the production of solid-recovered fuel or refuse-derived fuel. It does not sufficiently allow for the optimization of the quality of heterogeneous solid waste for subsequent energy recovery. Material-specific processing, in contrast, allows the separation criterion to be linked to specific chemical constituents. Therefore, the technical applicability of material-specific sorting of heterogeneous waste, in order to optimize its routing options, was evaluated. Two sorting steps were tested on a pilot and a large scale. Near infrared multiplexed sensor-based sorting devices were used (1) to reduce the chlorine (Cl) respectively pollutant content, in order to broaden the utilization options of SRF in industrial co-incineration, and (2) to increase the biogenic carbon (Cbio) content, which is highly relevant in the light of the EU emission trading scheme on CO2. It was found that the technology is generally applicable for the heterogeneous waste fractions looked at, if the sensor systems are appropriately adjusted for the sorting task. The first sorting step allowed for the removal of up to 40% of the Cl freight by separating only 3 to 5% of the material mass. Very low Cl concentrations were achieved in the output stream to be used as solid-recovered fuel stream and additionally, the cadmium (Cd) and lead (Pb) concentration was decreased. A two- to four-fold enriched Cbio content was achieved by the second sorting step. Due to lower yields in the large-scale test further challenges need to be addressed.Energie-Umweltmanagemen

Analysis of regional CO2contributions at the high Alpine observatory Jungfraujoch by means of atmospheric transport simulations and δ13C

In this study, we investigated the regional contributions of carbon dioxide (CO2) at the location of the high Alpine observatory Jungfraujoch (JFJ, Switzerland, 3580ĝ€¯mĝ€¯a.s.l.). To this purpose, we combined receptor-oriented atmospheric transport simulations for CO2 concentration in the period 2009-2017 with stable carbon isotope (δ13C-CO2) information. We applied two Lagrangian particle dispersion models driven by output from two different numerical weather prediction systems (FLEXPART-COSMO and STILT-ECMWF) in order to simulate CO2 concentration at JFJ based on regional CO2 fluxes, to estimate atmospheric δ13C-CO2, and to obtain model-based estimates of the mixed source signatures (δ13Cm). Anthropogenic fluxes were taken from a fuel-type-specific version of the EDGAR v4.3 inventory, while ecosystem fluxes were based on the Vegetation Photosynthesis and Respiration Model (VPRM). The simulations of CO2, δ13C-CO2, and δ13Cm were then compared to observations performed by quantum cascade laser absorption spectroscopy. The models captured around 40ĝ€¯% of the regional CO2 variability above or below the large-scale background and up to 35ĝ€¯% of the regional variability in δ13C-CO2. This is according to expectations considering the complex Alpine topography, the low intensity of regional signals at JFJ, and the challenging measurements. Best agreement between simulations and observations in terms of short-term variability and intensity of the signals for CO2 and δ13C-CO2 was found between late autumn and early spring. The agreement was inferior in the early autumn periods and during summer. This may be associated with the atmospheric transport representation in the models. In addition, the net ecosystem exchange fluxes are a possible source of error, either through inaccuracies in their representation in VPRM for the (Alpine) vegetation or through a day (uptake) vs. night (respiration) transport discrimination to JFJ. Furthermore, the simulations suggest that JFJ is subject to relatively small regional anthropogenic contributions due to its remote location (elevated and far from major anthropogenic sources) and the limited planetary boundary layer influence during winter. Instead, the station is primarily exposed to summertime ecosystem CO2 contributions, which are dominated by rather nearby sources (within 100ĝ€¯km). Even during winter, simulated gross ecosystem respiration accounted for approximately 50ĝ€¯% of all contributions to the CO2 concentrations above the large-scale background. The model-based monthly mean δ13Cm ranged from -ĝ€¯22ĝ€¯‰ in winter to -ĝ€¯28ĝ€¯‰ in summer and reached the most depleted values of -ĝ€¯35ĝ€¯‰ at higher fractions of natural gas combustion, as well as the most enriched values of -ĝ€¯17ĝ€¯‰ to -ĝ€¯12ĝ€¯‰ when impacted by cement production emissions. Observation-based δ13Cm values were derived independently from the simulations by a moving Keeling-plot approach. While model-based estimates spread in a narrow range, observation-based δ13Cm values exhibited a larger scatter and were limited to a smaller number of data points due to the stringent analysis prerequisites

Mitigation of Secondary Organic Aerosol Formation from Log Wood Burning Emissions by Catalytic Removal of Aromatic Hydrocarbons

Log wood burning is a significant source of volatile organic compounds including aromatic hydrocarbons (ArHC). ArHC are harmful, are reactive in the ambient atmosphere, and are important secondary organic aerosol (SOA) precursors. Consequently, SOA represents a major fraction of the sub-micron organic aerosol pollution from log wood burning. ArHC reduction is thus critical in the mitigation of adverse health and environmental effects of log wood burning. In this study, two Pt-based catalytic converters were prepared and tested for the mitigation of real-world log wood burning emissions, including ArHC and SOA formation, as well as toxic carbon monoxide and methane, a greenhouse gas. Substantial removal of mono- and polycyclic ArHC and phenolic compounds was achieved with both catalysts operated at realistic chimney temperatures (50% conversion was achieved at 200 and 300 degrees C for non-methane hydrocarbons in our experiments for Pt/Al2O3 and Pt/CeO2-Al2O3, respectively). The catalytically cleaned emissions exhibited a substantially reduced SOA formation already at temperatures as low as 185-310 degrees C. This reduces the sub-micron PM burden of log wood burning significantly. Thus, catalytic converters can effectively reduce primary and secondary log wood burning pollutants and, thereby, their adverse health impacts and environmental effects

Primary emissions and secondary aerosol production potential from woodstoves for residential heating: Influence of the stove technology and combustion efficiency

International audienc

Carbonaceous aerosol composition in air masses influenced by large-scale biomass burning: a case study in northwestern Vietnam

We investigated concentrations of organic carbon (OC), elemental carbon (EC), and a wide range of particle-bound organic compounds in daily sampled PM2.5 at the remote Pha Din (PDI) - Global Atmosphere Watch (GAW) monitoring station in northwestern Vietnam during an intense 3-week sampling campaign from 23 March to 12 April 2015. The site is known to receive trans-regional air masses during large-scale biomass burning (BB) episodes. BB is a globally widespread phenomenon and BB emission characterization is of high scientific and societal relevance. Emissions composition is influenced by multiple factors (e.g., fuel and thereby vegetation type, fuel moisture, fire temperature, available oxygen). Due to regional variations in these parameters, studies in different world regions are needed. OC composition provides valuable information regarding the health- and climate-relevant properties of PM2.5. Yet, OC composition studies from PDI are missing in the scientific literature to date. Therefore, we quantified 51 organic compounds simultaneously by in situ derivatization thermal desorption gas chromatography and time-of-flight mass spectrometry (IDTD-GC-TOFMS). Anhydrosugars, methoxyphenols, nalkanes, fatty acids, polycyclic aromatic hydrocarbons, oxygenated polycyclic aromatic hydrocarbons, nitrophenols, and OC were used in a hierarchical cluster analysis highlighting distinctive patterns for periods under low, medium, and high BB influence. The highest particle phase concentration of the typical primary organic aerosol (POA) and possible secondary organic aerosol (SOA) constituents, especially nitrophenols, were found on 5 and 6 April. We linked the trace gas mixing ratios of methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), and ozone (O-3) to the statistical classification of BB events based on OA composition and found increased CO and O-3 levels during medium and high BB influence. Likewise, a backward trajectory analysis indicates different source regions for the identified periods based on the OA clusters, with cleaner air masses arriving from the northeast, i.e., mainland China and the Yellow Sea. The more polluted periods are characterized by trajectories from the southwest, with more continental recirculation of the medium cluster and more westerly advection for the high cluster. These findings highlight that BB activities in northern Southeast Asia significantly enhance the regional organic aerosol loading and also affect the carbonaceous PM2.5 constituents and the trace gases in northwestern Vietnam. The presented analysis adds valuable data on the carbonaceous and chemical composition of PM2.5, in particular of OC, in a region of scarce data availability, and thus offers a reference dataset from Southeast Asian large-scale BB for future studies. Such a reference dataset may be useful for the evaluation of atmospheric transport simulation models, or for comparison with other world regions and BB types, such as Australian bush fires, African savannah fires, or tropical peatland fires