Contributions Of Identified Sources Research Articles

Metal ratio mixing models clarify metal contamination sources to lake sediments in Yunnan, China

Contaminated legacy sediments contribute to modern pollution loadings, particularly trace metals. These contributions are challenging to quantify as metal histories reconstructed from sediment records cannot be easily divided into legacy and concurrent contamination. In particular, the contribution from re-mobilization and delivery of legacy metals stored in catchment soil, colluvial, and fluvial environments are rarely considered or quantified when interpreting sediment records. Here, extended records of metals accumulation for a set of three lakes in Yunnan, China are compared with endmember chemistries using Monte Carlo-Markov Chain mixing models to help identify source contributions to the sediments. This approach allows attribution of metals transported by atmospheric and fluvial mechanisms in a region with a history of mining and metallurgy spanning millennia. These analyses reveal distinct source mixtures and demonstrate the sensitivity of lake records to basin sediment dynamics. In particular, substantial proportions of elevated metal concentrations in these lake systems seem to arise from soil contributions more than from atmospheric deposition of smelting emissions. The largest soil contributions seem to be in Erhai, a lake with erosion prone soils closely “connected” to the lake. Moreover, these invesigations illustrate the potential for mixing approaches to accommodate and clarify uncertainties in metal source and extraction as differences in extraction efficiency can be incorporated into source uncertainty estimates. Ultimately, these approaches emphasize the need to account for fluvial metal transport in interpretation of sediment histories.

MABI - A multi-wavelength absorption black carbon instrument for the measurement of fine light absorbing carbon particles

Light absorbing carbon (LAC), also referred to as black carbon (BC) or more colloquially as soot; is generated from the partial combustion of fossil fuels and biomass. The significant research interest in BC is largely due to its aerodynamic diameter well within the 2.5 μm size fraction (known as PM2.5), as well as its abundance being a major constituent of atmospheric particulate matter, particularly in urban regions. Accurately measuring BC is crucial for researchers and regulators for identifying root causes, monitoring emission source concentrations and input into climate change models in order to identify approaches that can best mitigate its atmospheric abundance.This paper presents results from recent studies using a BC research instrument developed by ANSTO, the Multi-wavelength Absorption Black carbon Instrument (MABI). The paper describes in detail the instrument design, function and interpretation of data from measurement of filters collected from various geographical locations in Australia and Asia. This instrument measures the light absorption of LAC particles deposited on filters at seven different wavelengths ranging from 405 to 1050 nm to estimate the LAC concentration of different particle diameters in order to differentiate between LAC from high temperature fossil fuel combustion (such as diesel vehicle engines) and biomass burning. Providing a powerful tool for identifying source contributions and determining LAC content of filters using quantitative analysis.

Predicting carbonaceous aerosols and identifying their source contribution with advanced approaches

Organic carbon (OC) and elemental carbon (EC) play important roles in various atmospheric processes and health effects. Predicting carbonaceous aerosols and identifying source contributions are important steps for further epidemiological study and formulating effective emission control policies. However, we are not aware of any study that examined predictions of OC and EC, and this work is also the first study that attempted to use machine learning and hyperparameter optimization method to predict concentrations of specific aerosol contaminants. This paper describes an investigation of the characteristics and sources of OC and EC in fine particulate matter (PM2.5) from 2005 to 2010 in the City of Taipei. Respective hourly average concentrations of OC and EC were 5.2 μg/m3 and 1.6 μg/m3. We observed obvious seasonal variation in OC but not in EC. Hourly and daily OC and EC concentrations were predicted using generalized additive model and grey wolf optimized multilayer perceptron model, which could explain up to about 80% of the total variation. Subsequent clustering suggests that traffic emission was the major contribution to OC, accounting for about 80% in the spring, 65% in the summer, and 90% in the fall and winter. In the Taipei area, local emissions were the dominant sources of OC and EC in all seasons, and long-range transport had a significant contribution to OC and in PM2.5 in spring.

Climate Forcing and Trends of Organic Aerosols in the Community Earth System Model (CESM2)

AbstractThe Community Earth System Model version 2 (CESM2) includes three main atmospheric configurations: the Community Atmosphere Model version 6 (CAM6) with simplified chemistry and a simplified organic aerosol (OA) scheme, CAM6 with comprehensive tropospheric and stratospheric chemistry representation (CAM6‐chem), and the Whole Atmosphere Community Climate Model version 6 (WACCM6). Both, CAM6‐chem and WACCM6 include a more comprehensive secondary organic aerosols (SOA) approach using the Volatility Basis Set (VBS) scheme and prognostic stratospheric aerosols. This paper describes the different OA schemes available in the different atmospheric configurations of CESM2 and discusses differences in aerosol burden and resulting climate forcings. Derived OA burden and trends differ due to differences in OA formation using the different approaches. Regional differences in Aerosol Optical Depth with larger values using the comprehensive approach occur over SOA source regions. Stronger increasing SOA trends between 1960 and 2015 in WACCM6 compared to CAM6 are due to increasing biogenic emissions aligned with increasing surface temperatures. Using the comprehensive SOA approach further leads to improved comparisons to aircraft observations and SOA formation of ≈143 Tg/yr. We further use WACCM6 to identify source contributions of OA from biogenic, fossil fuel, and biomass burning emissions, to quantify SOA amounts and trends from these sources. Increasing SOA trends between 1960 and 2015 are the result of increasing biogenic emissions aligned with increasing surface temperatures. Biogenic emissions are at least two thirds of the total SOA burden. In addition, SOA source contributions from fossil fuel emissions become more important, with largest values over Southeast Asia. The estimated total anthropogenic forcing of OA in WACCM6 for 1995–2010 conditions is −0.43 W/m2, mostly from the aerosol direct effect.

Improving microplastics source apportionment: a role for microplastic morphology and taxonomy?

Paul Helm discusses the need for a more detailed level of classification to aid in identifying source contributions of microplastics, providing direction on the implementation of management activities to reduce the occurrence of microplastics in the environment and enabling monitoring of the effectiveness of those actions.

New Insights from Zinc and Copper Isotopic Compositions into the Sources of Atmospheric Particulate Matter from Two Major European Cities.

This study reports spatial and temporal variability of Zn and Cu isotopes in atmospheric particulate matter (PM) collected in two major European cities with contrasting atmospheric pollution, Barcelona and London. We demonstrate that nontraditional stable isotopes identify source contributions of Zn and Cu and can play a major role in future air quality studies. In Barcelona, samples of fine PM were collected at street level at sites with variable traffic density. The isotopic signatures ranged between -0.13 ± 0.09 and -0.51 ± 0.05‰ for δ(66)ZnIRMM and between +0.04 ± 0.20 and +0.33 ± 0.15‰ for δ(65)CuAE633. Copper isotope signatures similar to those of Cu sulfides and Cu/Sb ratios within the range typically found in brake wear suggest that nonexhaust emissions from vehicles are dominant. Negative Zn isotopic signatures characteristic for gaseous emissions from smelting and combustion and large enrichments of Zn and Cd suggest contribution from metallurgical industries. In London, samples of coarse PM collected on the top of a building over 18 months display isotope signatures ranging between +0.03 ± 0.04 and +0.49 ± 0.02‰ for δ(66)ZnIRMM and between +0.37 ± 0.17 and +0.97 ± 0.21‰ for δ(65)CuAE633. Heavy Cu isotope signatures (up to +0.97 ± 0.21‰) and higher enrichments and Cu/Sb ratios during winter time indicate important contribution from fossil fuel combustion. The positive δ(66)ZnIRMM signatures are in good agreement with signatures characteristic for ore concentrates used for the production of tires and galvanized materials, suggesting nonexhaust emissions from vehicles as the main source of Zn pollution.

Airborne PCDD/F profiles in rural and urban areas of Buenos Aires Province, Argentina

Passive air samplers were deployed in 18 rural and urban locations in the densely populated Buenos Aires district to investigate airborne polychlorinated dibenzo-p-dioxin and polychlorinated-dibenzofuran (PCDD/Fs) profiles, sources and spatial patterns. Atmospheric concentrations reported as total toxic equivalents (TEQs), 2378-substituted (∑17PCDD/F) and 4–8 homologous groups (∑4–8PCDD/F) were highly variable and significantly correlated to urban scale. The rural average (3.0±2.7fgTEQm−3) was thirty times less than metropolitan values (90±51fgTEQm−3), with urban cluster (5.4±4.0fgTEQm−3) and urbanized area (33±50fgTEQm−3) in an intermediate position. A rural outlier exhibited the highest TEQ values (295–296fgTEQm−3) suggesting a local source. Principal component analyses (PCA) performed for ∑17PCDD/F and ∑4-8PCDD/F to identify source contributions showed more significant results for homologue groups compared to 17 congeners (83 and 45% of total variability explained, respectively) pointing to dominant diesel emissions enriched in TeCDF in rural areas, and open burning and industrial sources characterized by TeCDD, PeCDD contributing most in urbanized and metropolitan areas. Homologue group PCA also performed better clustering samples according to sources and TEQ concentrations. The PCDD/Fs profile of the rural outlier dominated by HxCDF and HpCDD/F showed a typical municipal incineration signature confirming the presence of local source.

Tagged ozone mechanism for MOZART-4, CAM-chem and other chemical transport models

Abstract. A procedure for tagging ozone produced from NO sources through updates to an existing chemical mechanism is described, and results from its implementation in the Model for Ozone and Related chemical Tracers (MOZART-4), a global chemical transport model, are presented. Artificial tracers are added to the mechanism, thus, not affecting the standard chemistry. The results are linear in the troposphere, i.e., the sum of ozone from individual tagged sources equals the ozone from all sources to within 3% in zonal mean monthly averages. In addition, the tagged ozone is shown to equal the standard ozone, when all tropospheric sources are tagged and stratospheric input is turned off. The stratospheric ozone contribution to the troposphere determined from the difference between total ozone and ozone from all tagged sources is significantly less than estimates using a traditional stratospheric ozone tracer (8 vs. 20 ppbv at the surface). The commonly used technique of perturbing NO emissions by 20% in a region to determine its ozone contribution is compared to the tagging technique, showing that the tagged ozone is 2–4 times the ozone contribution that was deduced from perturbing emissions. The ozone tagging described here is useful for identifying source contributions based on NO emissions in a given state of the atmosphere, such as for quantifying the ozone budget.

Ft. McHenry tunnel study: Source profiles and mercury emissions from diesel and gasoline powered vehicles

During the fall of 1998, the US Environmental Protection Agency and the Florida Department of Environmental Protection sponsored a 7-day study at the Ft. McHenry tunnel in Baltimore, MD with the objective of obtaining PM 2.5 vehicle source profiles for use in atmospheric mercury source apportionment studies. PM 2.5 emission profiles from gasoline and diesel powered vehicles were developed from analysis of trace elements, polycyclic aromatic hydrocarbons (PAH), and condensed aliphatic hydrocarbons. PM 2.5 samples were collected using commercially available sampling systems and were extracted and analyzed using conventional well-established methods. Both inorganic and organic profiles were sufficiently unique to mathematically discriminate the contributions from each source type using a chemical mass balance source apportionment approach. However, only the organic source profiles provided unique PAH tracers (e.g., fluoranthene, pyrene, and chrysene) for diesel combustion that could be used to identify source contributions generated using multivariate statistical receptor modeling approaches. In addition, the study found significant emission of gaseous elemental mercury (Hg 0), divalent reactive gaseous mercury (RGM), and particulate mercury (Hg(p)) from gasoline but not from diesel powered motor vehicles. Fuel analysis supported the tunnel measurement results showing that total mercury content in all grades of gasoline (284±108 ng L −1) was substantially higher than total mercury content in diesel fuel (62±37 ng L −1) collected contemporaneously at local Baltimore retailers.

Fingerprinting of bed sediment in the Tay Estuary, Scotland: an environmental magnetism approach

Abstract. Sediment fingerprinting is commonly used for sediment provenance studies in lakes, rivers and reservoirs and on hillslopes and floodplains. This investigation explores the mixing of terrestrial and marine-derived sediment in the Tay Estuary, Scotland, using mineral magnetic attributes for fingerprinting. Samples representative of the estuary sediments and of four sources (end-members) were subjected to a suite of magnetic susceptibility and remanence measurements. Sediment samples from the beds of the Rivers Tay and Earn represented fluvial inputs while samples from the Angus and Fife coasts represented marine input. Multivariate discriminant and factor analysis showed that the sources could be separated on the basis of six magnetic parameters in a simple multivariate unmixing model to identify source contributions to estuarine bed sediments. Multi-domain magnetite signatures, characteristic of unweathered bedrock, dominate the magnetic measurements. Overall contributions of 3% from the River Earn, 17% from the River Tay, 29% from the Angus coast and 51% from the Fife coast source end-members, demonstrated the present-day regime of marine sediment derivation in the Tay Estuary. However, this conceals considerable spatial variability both along-estuary and in terms of sub-environments, with small-scale variations in sediment provenance reflecting local morphology, particularly areas of channel convergence. Keywords: bed sediment, environmental magnetism, fingerprinting, Tay Estuary, Scotland