Time-resolved analysis of particle emissions from residential biomass combustion – Emissions of refractory black carbon, PAHs and organic tracers
Time-resolved particle emissions from a conventional wood stove were investigated with aerosol mass spectrometry to provide links between combustion conditions, emission factors, mixing state of refractory black carbon and implications for organic tracer methods. The addition of a new batch of fuel results in low temperature pyrolysis as the fuel heats up, resulting in strong, short-lived, variable emission peaks of organic aerosol-containing markers of anhydrous sugars, such as levoglucosan (fragment at m/z 60). Flaming combustion results in emissions dominated by refractory black carbon co-emitted with minor fractions of organic aerosol and markers of anhydrous sugars. Full cycle emissions are an external mixture of larger organic aerosol-dominated and smaller thinly coated refractory black carbon particles. A very high burn rate results in increased full cycle mass emission factors of 66, 2.7, 2.8 and 1.3 for particulate polycyclic aromatic hydrocarbons, refractory black carbon, total organic aerosol and m/z 60, respectively, compared to nominal burn rate. Polycyclic aromatic hydrocarbons are primarily associated with refractory black carbon-containing particles. We hypothesize that at very high burn rates, the central parts of the combustion zone become air starved, leading to a locally reduced combustion temperature that reduces the conversion rates from polycyclic aromatic hydrocarbons to refractory black carbon. This facilitates a strong increase of polycyclic aromatic hydrocarbons emissions. At nominal burn rates, full cycle emissions based on m/z 60 correlate well with organic aerosol, refractory black carbon and particulate matter. However, at higher burn rates, m/z 60 does not correlate with increased emissions of polycyclic aromatic hydrocarbons, refractory black carbon and organic aerosol in the flaming phase. The new knowledge can be used to advance source apportionment studies, reduce emissions of genotoxic compounds and model the climate impacts of refractory black carbon, such as absorption enhancement by lensing.
Land-use and land-cover change carbon emissions between 1901 and 2012 constrained by biomass observations
The use of dynamic global vegetation models (DGVMs) to estimate CO2 emissions from land-use and land-cover change (LULCC) offers a new window to account for spatial and temporal details of emissions, and for ecosystem processes affected by LULCC. One drawback of DGVMs however is their large uncertainty. Here, we propose a new method of using satellite- and inventory-based biomass observations to constrain historical cumulative LULCC emissions (EcLUC) from an ensemble of nine DGVMs based on emerging relationships between simulated vegetation biomass and EcLUC. This method is applicable at global and regional scale. Compared to the large range of EcLUC in the original ensemble (94 to 273 Pg C) during 1901–2012, current biomass observations allow us to derive a new best estimate of 155 ± 50 (1-σ Gaussian error) Pg C. The constrained LULCC emissions are higher than prior DGVM values in tropical regions, but significantly lower in North America. Our approach of constraining cumulative LULCC emissions based on biomass observations reduces the uncertainty of the historical carbon budget, and can also be applied to evaluate the impact of land-based mitigation activities.
Organic matter drives high interannual variability in methylmercury concentrations in a subarctic coastal sea
Levels of neurotoxic methylmercury (MeHg) in phytoplankton are strongly associated to water MeHg concentrations. Because uptake by phytoplankton is the first and largest step of bioaccumulation in aquatic food webs many studies have investigated factors controlling seasonal changes in water MeHg concentrations. However organic matter (OM), widely accepted as an important driver of MeHg production and uptake by phytoplankton, is known for strong interannual variability in concentrations and composition within systems. In this study, we explore the role of OM on spatial and interannual variability of MeHg in a subarctic coastal sea, the northern Baltic Sea. Using MeHg (2014: 80±25 fM; 2015:
Decoupling of microbial carbon, nitrogen, and phosphorus cycling in response to extreme temperature events
Adductomic Screening of Hemoglobin Adducts and Monitoring of Micronuclei in School-Age Children
Electrophilic compounds/metabolites present in humans, originating from endogenous processes or exogenous exposure, pose a risk to health effects through their reactions with nucleophilic sites in proteins and DNA, forming adducts. Adductomic approaches are developed to screen for adducts to biomacromolecules in vivo by mass spectrometry (MS), with the aim to detect adducts corresponding to unknown exposures from electrophiles. In the present study, adductomic screening was performed using blood samples from healthy children about 12 years old (n = 51). The frequencies of micronuclei (MN) in erythrocytes in peripheral blood were monitored as a measure of genotoxic effect/genotoxic exposure. The applied adductomic approach has been reported earlier by us and is based on analysis of N-terminal valine adducts in hemoglobin (Hb) by liquid chromatography tandem mass spectrometry (LC-MS/MS). High resolution MS was introduced for refined screening of previously unknown N-terminal Hb adducts. Measured adduct levels were compared with MN frequencies using multivariate data analysis. In the 51 individuals, a total of 24 adducts (whereof 12 were previously identified) were observed and their levels quantified. Relatively large interindividual variations in adduct levels were observed. The data analysis (with partial least-squares regression) showed that as much as 60% of the MN variation could be explained by the adduct levels. This study, for the first time, applies the combination of these sensitive methods to measure the internal dose of potentially genotoxic chemicals and genotoxic effects, respectively. The results indicate that this is a valuable approach for the characterization of exposure to chemical risk factors for the genotoxic effects present in individuals of the general population.
An academic researcher’s guide to increased impact on regulatory assessment of chemicals.
The interactions between academic research and regulatory assessment of chemicals may in theory seem straightforward: researchers perform studies, and these studies are used by regulators for decision-making. However, in practice the situation is more complex, and many factors decide a research study’s regulatory use. According to several EU chemical legislations, all available and relevant studies can be used in hazard and risk assessment of chemicals. However, in practice, standard tests conducted under GLP and sponsored and provided by industry are predominantly used. Peer-reviewed studies from independent sources are often disregarded or disputed since they often do not comply with regulatory data requirements and quality criteria. There are several possible reasons for this, one being that academic research is reported in a way that does not fit the regulatory requirements. To help bridge such a gap, the aim of this paper is to give an overview of the general workings of chemicals legislation and propose a set of actions to increase the usability of research data. In the end, this may increase the use of academic research for decision-making and ultimately result in more science-based policies. From a policy perspective, useful scientific evidence are those studies that are sufficiently reliable and relevant. This is not in contradiction to the aims of research and generally accepted scientific standards.
Export of calcium carbonate corrosive waters from the East Siberian Sea
The Siberian shelf seas are areas of extensive biogeochemical transformation of organic matter, both of marine and terrestrial origin. This in combination with brine production from sea ice formation results in a cold bottom water of relative high salinity and partial pressure of carbon dioxide (pCO2). Data from the SWERUS-C3 expedition compiled on the icebreaker Oden in July to September 2014 show the distribution of such waters at the outer shelf, as well as their export into the deep central Arctic basins. Very high pCO2 water, up to ∼ 1000 µatm, was observed associated with high nutrients and low oxygen concentrations. Consequently, this water had low saturation state with respect to calcium carbonate down to less than 0.8 for calcite and 0.5 for aragonite. Waters undersaturated in aragonite were also observed in the surface in waters at equilibrium with atmospheric CO2; however, at these conditions the cause of under-saturation was low salinity from river runoff and/or sea ice melt. The calcium carbonate corrosive water was observed all along the continental margin and well out into the deep Makarov and Canada basins at a depth from about 50 m depth in the west to about 150 m in the east. These waters of low aragonite saturation state are traced in historic data to the Canada Basin and in the waters flowing out of the Arctic Ocean north of Greenland and in the western Fram Strait, thus potentially impacting the marine life in the North Atlantic Ocean.
Carbon cycling on the East Siberian Arctic Shelf – a change in air-sea CO2 flux induced by mineralization of terrestrial organic carbon
Measurements from the SWERUS-C3 and ISSS-08 Arctic expeditions were used to calibrate and validate a new physical-biogeochemical model developed to quantify key carbon cycling processes on the East Siberian Arctic Shelf (ESAS). The model was used in a series of experimental simulations with the specific aim to investigate the pathways of terrestrial dissolved and particulate organic carbon (DOCter and POCter) supplied to the shelf. Rivers supply on average 8.5 Tg C yr−1 dissolved inorganic carbon (DIC), and further 8.5 and 1.1 Tg C yr−1 DOCter and POCter respectively. Based on observed and simulated DOC concentrations and stable isotope values (δ13CDOC) in shelf waters, we estimate that only some 20 % of the riverine DOCter is labile. According to our model results, an additional supply of approximately 14 Tg C yr−1 eroded labile POCter is however required to describe the observed stable isotope values of DIC (δ13CDIC). Degradation of riverine DOCter and POCter results in a 1.8 Tg C yr−1 reduction in the uptake of atmospheric CO2, while degradation of eroded POCter results in an additional 10 Tg C yr−1 reduction. Our calculations indicate nevertheless that the ESAS is an overall small net sink for atmospheric CO2 (1.7 Tg C yr−1). The external carbon sources are largely compensated by a net export from the shelf to the Arctic Ocean (31 Tg C yr−1), and to a smaller degree by a permanent burial in the sediments (2.7 Tg C yr−1)
NanoCRED: A transparent framework to assess’ the regulatory adequacy of ecotoxicity data for nanomaterials – Relevance and reliability revisited
Environmental hazard and risk assessment serve as the basis for regulatory decisions to protect the environment from unintentional adverse effects of chemical substances including nanomaterials. This process requires reliable and relevant environmental hazard data upon which classification and labelling can be based and Predicted No-Effect Concentration (PNEC) values can be estimated. In a regulatory context ecotoxicological data is often recommended to be generated according to accepted and validated test guidelines, preferably also following Good Laboratory Practice. However, engineered nanomaterials are known to behave very differently in ecotoxicity tests compared to the conventional soluble chemicals, for which most guidelines were developed. Therefore non-guideline tests, or tests following modified test guidelines, can provide valuable information and should not per se be considered less adequate for regulatory use. Here we propose a framework for reliability and relevance evaluation of ecotoxicity data for nanomaterials that take into account the challenges and characterisation requirements associated with testing of these substances. The nanoCRED evaluation criteria, and accompanying guidance, were developed to be used in combination with those developed through the ‘Criteria for Reporting and Evaluating Ecotoxicity Data (CRED)’ project. This approach can accommodate all types of nanomaterials, all types of aquatic ecotoxicity studies, and qualitative as well as quantitative data evaluation requirements. Furthermore, it is practically feasible to implement and directly applicable in European as well as international regulatory frameworks.