Prediction of source contributions to urban background PM10 concentrations in European cities: a case study for an episode in December 2016 using EMEP/MSC-W rv4.15 and LOTOS-EUROS v2.0 – Part 1: The country contributions

A large fraction of the urban population in Europe is exposed to particulate matter levels above the WHO guideline value. To make more effective mitigation strategies, it is important to understand the influence on particulate matter (PM) from pollutants emitted in different European nations. In this study, we evaluate a country source contribution forecasting system aimed at assessing the domestic and transboundary contributions to PM in major European cities for an episode in December 2016. The system is composed of two models (EMEP/MSC-W rv4.15 and LOTOS-EUROS v2.0), which allows the consideration of differences in the source attribution. We also compared the PM10 concentrations, and both models present satisfactory agreement in the 4 d forecasts of the surface concentrations, since the hourly concentrations can be highly correlated with in situ observations. The correlation coefficients reach values of up to 0.58 for LOTOS-EUROS and 0.50 for EMEP for the urban stations; the values are 0.58 for LOTOS-EUROS and 0.72 for EMEP for the rural stations. However, the models underpredict the highest hourly concentrations measured by the urban stations (mean underestimation of 36 %), which is to be expected given the relatively coarse model resolution used (0.25∘ longitude × 0.125∘ latitude). For the source attribution calculations, LOTOS-EUROS uses a labelling technique, while the EMEP/MSC-W model uses a scenario having reduced anthropogenic emissions, and then it is compared to a reference run where no changes are applied. Different percentages (5 %, 15 %, and 50 %) for the reduced emissions in the EMEP/MSC-W model were used to test the robustness of the methodology. The impact of the different ways to define the urban area for the studied cities was also investigated (i.e. one model grid cell, nine grid cells, and grid cells covering the definition given by the Global Administrative Areas – GADM). We found that the combination of a 15 % emission reduction and a larger domain (nine grid cells or GADM) helps to preserve the linearity between emission and concentrations changes. The nonlinearity, related to the emission reduction scenario used, is suggested by the nature of the mismatch between the total concentration and the sum of the concentrations from different calculated sources. Even limited, this nonlinearity is observed in the NO-3, NH+4, and H2O concentrations, which is related to gas–aerosol partitioning of the species. The use of a 15 % emission reduction and of a larger city domain also causes better agreement on the determination of the main country contributors between both country source calculations. Over the 34 European cities investigated, PM10 was dominated by domestic emissions for the studied episode (1–9 December 2016). The two models generally agree on the dominant external country contributor (68 % on an hourly basis) to PM10 concentrations. Overall, 75 % of the hourly predicted PM10 concentrations of both models have the same top five main country contributors. Better agreement on the dominant country contributor for primary (emitted) species (70 % is found for primary organic matter (POM) and 80 % for elemental carbon – EC) than for the inorganic secondary component of the aerosol (50 %), which is predictable due to the conceptual differences in the source attribution used by both models. The country contribution calculated by the scenario approach depends on the chemical regime, which largely impacts the secondary components, unlike the calculation using the labelling approach

Source attribution of particulate matter in Berlin

The exposure to ambient particulate matter in metropolitan areas is a major health problem. A prerequisite for formulating effective mitigation strategies it to understand the origin of particulate matter in terms of source regions and sectors. We performed a source attribution of particulate matter (PM) for the Berlin agglomeration area covering the period from 2016 to 2018 using the LOTOS-EUROS chemistry transport model. The (3 year-) mean modelled urban background PM2.5 concentration (10.4 μg/m³) is largely explained by households (3.2 μg/m³) and industry & energy (2.0 μg/m³), while the remaining source sectors contribute the other half. The modelled annual mean urban increment for PM2.5 is mainly attributed to households (1.6 μg/m³) and traffic (0.5 μg/m³). With respect to its relative shares the PM10 source attribution looks similar to that of PM2.5 throughout the year, but with enhanced natural contributions. From a geographical perspective the main source area for the PM2.5 in Berlin is Germany (5.1 μg/m³) itself, followed by the contributions from transboundary transport (3.4 μg/m³). The German sources could be further split into Berlin (2.6 μg/m³), Brandenburg (0.7 μg/m³) and remaining states of Germany (1.8 μg/m³). About one third of the foreign shares can be attributed to Germany's neighbouring countries Poland and Czech Republic. During episodes these contributions can significantly differ, e.g. in February 2017 the Polish contribution is about 1/3rd. The sectoral contributions agree with previous findings except that our study indicates lower contributions for traffic. The model's underestimation of total PM is largely caused by an underestimation of the coarse mode PM. Both the coarse mode urban increment as well as the regional background concentrations are underestimated by the model, especially during summer. We suggest that the enhanced coarse material (in the city) during warm seasons is predominated by (road) resuspension processes which need more of our attention to further improve our models

Relaxed control of sugar utilization in Parageobacillus thermoglucosidasius DSM 2542

Though carbon catabolite repression (CCR) has been intensively studied in some more characterised organisms, there is a lack of information of CCR in thermophiles. In this work, CCR in the thermophile, Parageobacillus thermoglucosidasius DSM 2542 has been studied during growth on pentose sugars in the presence of glucose. Physiological studies under fermentative conditions revealed a loosely controlled CCR when DSM 2542 was grown in minimal medium supplemented with a mixture of glucose and xylose. This atypical CCR pattern was also confirmed by studying xylose isomerase expression level by qRT-PCR. Fortuitously, the pheB gene, which encodes catechol 2, 3-dioxygenase was found to have a cre site highly similar to the consensus catabolite-responsive element (cre) at its 3′ end and was used to confirm that expression of pheB from a plasmid was under stringent CCR control. Bioinformatic analysis suggested that the CCR regulation of xylose metabolism in P. thermoglucosidasius DSM 2542 might occur primarily via control of expression of pentose transporter operons. Relaxed control of sugar utilization might reflect a lower affinity of the CcpA-HPr (Ser46-P) or CcpA-Crh (Ser46-P) complexes to the cre(s) in these operons

Characterization of sporulation dynamics of Pseudoclostridium thermosuccinogenes using flow cytometry

Single-cell analysis of microbial population heterogeneity is a fast growing research area in microbiology due to its potential to identify and quantify the impact of subpopulations on microbial performance in, for example, industrial biotechnology, environmental biology, and pathogenesis. Although several tools have been developed, determination of population heterogenity in anaerobic bacteria, especially spore-forming clostridia species has been amply studied. In this study we applied single cell analysis techniques such as flow cytometry (FCM) and fluorescence-assisted cell sorting (FACS) on the spore-forming succinate producer Pseudoclostridium thermosuccinogenes. By combining FCM and FACS with fluorescent staining, we differentiated and enriched all sporulation-related morphologies of P. thermosuccinogenes. To evaluate the presence of metabolically active vegetative cells, a blend of the dyes propidium iodide (PI) and carboxy fluorescein diacetate (cFDA) tested best. Side scatter (SSC-H) in combination with metabolic indicator cFDA dye provided the best separation of sporulation populations. Based on this protocol, we successfully determined culture heterogeneity of P. thermosuccinogenes by discriminating between mature spores, forespores, dark and bright phase endospores, and vegetative cells populations. Henceforth, this methodology can be applied to further study sporulation dynamics and its impact on fermentation performance and product formation by P. thermosuccinogenes.</p

Genetic Tool Development for a New Host for Biotechnology, the Thermotolerant Bacterium Bacillus coagulans

Bacillus coagulans has good potential as an industrial production organism for platform chemicals from renewable resources but has limited genetic tools available. Here, we present a targeted gene disruption system using the Cre-lox system, development of a LacZ reporter assay for monitoring gene transcription, and heterologous D-lactate dehydrogenase expression

Forest–atmosphere exchange of reactive nitrogen in a remote region – Part II: Modeling annual budgets

To monitor the effect of current nitrogen emissions and mitigation strategies, total (wet + dry) atmospheric nitrogen deposition to forests is commonly estimated using chemical transport models or canopy budget models in combination with throughfall measurements. Since flux measurements of reactive nitrogen (Nr) compounds are scarce, dry deposition process descriptions as well as the calculated flux estimates and annual budgets are subject to considerable uncertainties. In this study, we compared four different approaches to quantify annual dry deposition budgets of total reactive nitrogen (ΣNr) at a mixed forest site situated in the Bavarian Forest National Park, Germany. Dry deposition budgets were quantified based on (I) 2.5 years of eddy covariance flux measurements with the Total Reactive Atmospheric Nitrogen Converter (TRANC); (II) an in situ application of the bidirectional inferential flux model DEPAC (Deposition of Acidifying Compounds), here called DEPAC-1D; (III) a simulation with the chemical transport model LOTOS-EUROS (Long-Term Ozone Simulation – European Operational Smog) v2.0, using DEPAC as dry deposition module; and (IV) a canopy budget technique (CBT). Averaged annual ΣNr dry deposition estimates determined from TRANC measurements were 4.7 ± 0.2 and 4.3 ± 0.4 kg N ha−1 a−1, depending on the gap-filling approach. DEPAC-1D-modeled dry deposition, using concentrations and meteorological drivers measured at the site, was 5.8 ± 0.1 kg N ha−1 a−1. In comparison to TRANC fluxes, DEPAC-1D estimates were systematically higher during summer and in close agreement in winter. Modeled ΣNr deposition velocities (vd) of DEPAC-1D were found to increase with lower temperatures and higher relative humidity and in the presence of wet leaf surfaces, particularly from May to September. This observation was contrary to TRANC-observed fluxes. LOTOS-EUROS-modeled annual dry deposition was 6.5 ± 0.3 kg N ha−1 a−1 for the site-specific weighting of land-use classes within the site's grid cell. LOTOS-EUROS showed substantial discrepancies to measured ΣNr deposition during spring and autumn, which was related to an overestimation of ammonia (NH3) concentrations by a factor of 2 to 3 compared to measured values as a consequence of a mismatch between gridded input NH3 emissions and the site's actual (rather low) pollution climate. According to LOTOS-EUROS predictions, ammonia contributed most to modeled input ΣNr concentrations, whereas measurements showed NOx as the prevailing compound in ΣNr concentrations. Annual deposition estimates from measurements and modeling were in the range of minimum and maximum estimates determined from CBT being at 3.8 ± 0.5 and 6.7 ± 0.3 kg N ha−1 a−1, respectively. By adding locally measured wet-only deposition, we estimated an annual total nitrogen deposition input between 11.5 and 14.8 kg N ha−1 a−1, which is within the critical load ranges proposed for deciduous and coniferous forests

Functional Analysis of the ComK Protein of Bacillus coagulans

The genes for DNA uptake and recombination in Bacilli are commonly regulated by the transcriptional factor ComK. We have identified a ComK homologue in Bacillus coagulans, an industrial relevant organism that is recalcitrant for transformation. Introduction of B. coagulans comK gene under its own promoter region into Bacillus subtilis comK strain results in low transcriptional induction of the late competence gene comGA, but lacking bistable expression. The promoter regions of B. coagulans comK and the comGA genes are recognized in B. subtilis and expression from these promoters is activated by B. subtilis ComK. Purified ComK protein of B. coagulans showed DNA-binding ability in gel retardation assays with B. subtilis- and B. coagulans-derived probes. These experiments suggest that the function of B. coagulans ComK is similar to that of ComK of B. subtilis. When its own comK is overexpressed in B. coagulans the comGA gene expression increases 40-fold, while the expression of another late competence gene, comC is not elevated and no reproducible DNA-uptake could be observed under these conditions. Our results demonstrate that B. coagulans ComK can recognize several B. subtilis comK-responsive elements, and vice versa, but indicate that the activation of the transcription of complete sets of genes coding for a putative DNA uptake apparatus in B. coagulans might differ from that of B. subtilis

Data assimilation of CrIS NH3 satellite observations for improving spatiotemporal NH3 distributions in LOTOS-EUROS

Atmospheric levels of ammonia (NH3) have substantially increased during the last century, posing a hazard to both human health and environmental quality. The atmospheric budget of NH3, however, is still highly uncertain due to an overall lack of observations. Satellite observations of atmospheric NH3 may help us in the current observational and knowledge gaps. Recent observations of the Cross-track Infrared Sounder (CrIS) provide us with daily, global distributions of NH3. In this study, the CrIS NH3 product is assimilated into the LOTOS-EUROS chemistry transport model using two different methods aimed at improving the modeled spatiotemporal NH3 distributions. In the first method NH3 surface concentrations from CrIS are used to fit spatially varying NH3 emission time factors to redistribute model input NH3 emissions over the year. The second method uses the CrIS NH3 profile to adjust the NH3 emissions using a local ensemble transform Kalman filter (LETKF) in a top-down approach. The two methods are tested separately and combined, focusing on a region in western Europe (Germany, Belgium and the Netherlands). In this region, the mean CrIS NH3 total columns were up to a factor 2 higher than the simulated NH3 columns between 2014 and 2018, which, after assimilating the CrIS NH3 columns using the LETKF algorithm, led to an increase in the total NH3 emissions of up to approximately 30 %. Our results illustrate that CrIS NH3 observations can be used successfully to estimate spatially variable NH3 time factors and improve NH3 emission distributions temporally, especially in spring (March to May). Moreover, the use of the CrIS-based NH3 time factors resulted in an improved comparison with the onset and duration of the NH3 spring peak observed at observation sites at hourly resolution in the Netherlands. Assimilation of the CrIS NH3 columns with the LETKF algorithm is mainly advantageous for improving the spatial concentration distribution of the modeled NH3 fields. Compared to in situ observations, a combination of both methods led to the most significant improvements in modeled monthly NH3 surface concentration and NH4+ wet deposition fields, illustrating the usefulness of the CrIS NH3 products to improve the temporal representativity of the model and better constrain the budget in agricultural areas

Estimating particulate matter health impact related to the combustion of different fossil fuels

International audienceExposure to particulate matter (PM) in ambient air leads to adverse health effects. To design cost effective mitigation strategies, a thorough understanding of the sources of particulate matter is crucial. We have successfully generated a web map service that allows to access information on fuel dependent health effects due to particulate matter. For this purpose, the LOTOS-EUROS air pollution model was equipped with a source apportionment module that tracks the origin of the modelled particulate matter distributions throughout a simulation. Combined with a dedicated emission inventory PM2.5 maps specified by fuel type were generated for 2007-2009. These maps were combined with a health impact calculation to estimate Lost of Life Expectancy for each fuel categories. An user friendly web client was generated to access the results and use the web mapping service in an easy manner