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BackgroundMicroorganisms influence the chemical milieu of their environment, and chemical metabolites can affect ecological processes. In built environments, where people spend the majority of their time, very little is known about how surface-borne microorganisms influence the chemistry of the indoor spaces. Here, we applied multidisciplinary approaches to investigate aspects of chemical microbiology in a house.MethodsWe characterized the microbial and chemical composition of two common and frequently wet surfaces in a residential setting: kitchen sink and bathroom shower. Microbial communities were studied using culture-dependent and independent techniques, including targeting RNA for amplicon sequencing. Volatile and soluble chemicals from paired samples were analyzed using state-of-the-art techniques to explore the links between the observed microbiota and chemical exudates.ResultsMicrobial analysis revealed a rich biological presence on the surfaces exposed in kitchen sinks and bathroom shower stalls. Microbial composition, matched for DNA and RNA targets, varied by surface type and sampling period. Bacteria were found to have an average of 25× more gene copies than fungi. Biomass estimates based on qPCR were well correlated with measured total volatile organic compound (VOC) emissions. Abundant VOCs included products associated with fatty acid production. Molecular networking revealed a diversity of surface-borne compounds that likely originate from microbes and from household products.ConclusionsMicrobes played a role in structuring the chemical profiles on and emitted from kitchen sinks and shower stalls. Microbial VOCs (mVOCs) were predominately associated with the processing of fatty acids. The mVOC composition may be more stable than that of microbial communities, which can show temporal and spatial variation in their responses to changing environmental conditions. The mVOC output from microbial metabolism on kitchen sinks and bathroom showers should be apparent through careful measurement, even against a broader background of VOCs in homes, some of which may originate from microbes in other locations within the home. A deeper understanding of the chemical interactions between microbes on household surfaces will require experimentation under relevant environmental conditions, with a finer temporal resolution, to build on the observational study results presented here.

Despite decades of commercial harvest of bigmouth buffalo (Ictiobus cyprinellus) from Jamestown Reservoir, North Dakota, and the recent rapid growth of sport bowfishing that targets this species, there is a lack of biological information on this native catostomid. At present, no-limit recreational and commercial harvest of bigmouth buffalo occurs in North Dakota, with no harvest-reporting for recreational take. A long-lived life history was recently documented for this species, with a life-span exceeding 100 years. At Jamestown Reservoir, bigmouth buffalo were aged to 58 years of age, with onset of sexual maturity 10 years for females. Evidence for episodic recruitment over a 60-year period was in 1962-1979, 1993-2011, and 2017, with recruitment success more likely during non-drought periods. Annual commercial harvest data from this reservoir indicate bigmouth buffalo have declined significantly over the past 30 years, most precipitously since 2010 during the bowfishing era. The demographic patterns, episodic recruitment, and harvest changes observed in this population are relevant for informing management of bigmouth buffalo and other long-lived freshwater fishes. Malgre des decennies d'exploitation commerciale du buffalo a grande bouche (Ictiobus cyprinellus) dans le reservoir de Jamestown (Dakota du Nord) et, recemment, la croissance rapide de la peche sportive a l'arc visant cette espece, les donnees biologiques sur ce meunier indigene sont rares. A l'heure actuelle, une peche sportive et commerciale sans restriction au buffalo a grande bouche a cours au Dakota du Nord, ou la peche sportive n'est pas visee par une obligation de declaration des prises. Un long cycle biologique a recemment ete documente pour cette espece, sa longevite excedant 100 ans. Au reservoir de Jamestown, les ages determines de buffalos a grande bouche vont jusqu'a 58 ans, le debut de la maturite sexuelle etant a 10 ans pour les femelles. Les donnees temoignent de recrutement episodique sur une periode de 60 ans durant les intervalles de 1962 a 1979, de 1993 a 2011 et en 2017, la probabilite de succes du recrutement etant plus grande durant les periodes sans secheresse. Les donnees sur les prises commerciales annuelles de ce reservoir indiquent que les buffalos a grande bouche ont connu un declin significatif au cours des 30 dernieres annees, qui est particulierement prononce depuis 2010, soit la periode de la peche a l'arc. Les motifs demographiques, le recrutement episodique et les variations des prises observes dans cette population sont importants pour la gestion du buffalo a grande bouche et d'autres poissons d'eau douce longevifs. [Traduit par la Redaction], Introduction Bigmouth buffalo (Ictiobus cyprinellus) is a large-bodied freshwater fish belonging to the sucker family (Catostomidae) that is endemic to North America and is an integral component of native ecosystems. [...]

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A new analytical methodology combining comprehensive two-dimensional gas chromatography (GC×GC), dual ionization energies and high resolution time of flight mass spectrometry has been developed that improves molecular level identification of organic compounds in complex environmental samples. GC×GC maximizes compound separation providing cleaner mass spectra by minimizing erroneous fragments from interferences and co-eluting peaks. Traditional electron ionization (EI, 70 eV) provides MS fragmentation patterns that can be matched to published EI MS libraries while vacuum ultraviolet photoionization (VUV, 10.5 eV) yields MS with reduced fragmentation enhancing the abundance of the molecular ion providing molecular formulas when combined with high resolution mass spectrometry. We demonstrate this new approach by applying it to a sample of organic aerosol. In this sample, 238 peaks were matched to EI MS library data with FM ≥ 800 but a fifth (42 compounds) were determined to be incorrectly identified because the molecular formula was not confirmed by the VUV MS data. This highlights the importance of using a complementary technique to confirm compound identifications even for peaks with very good matching statistics. In total, 171 compounds were identified by EI MS matching to library spectra with confirmation of the molecular formula from the high resolution VUV MS data and were not dependent on the matching statistics being above a threshold value. A large number of unidentified peaks were still observed with FM < 800, which in routine analysis would typically be neglected. Where possible, these peaks were assigned molecular formulas from the VUV MS data (211 in total). In total, the combination of EI and VUV MS data provides more than twice as much molecular level peak information than traditional approaches and improves confidence in the identification of individual organic compounds. The molecular formula data from the VUV MS data was used, in conjunction with GC×GC retention times and the observed EI MS, to generate a new, searchable EI MS library compatible with the standard NIST MS search program. This library is deliberately dynamic and editable so that other end users can add new entries and update existing entries as new information becomes available.

On-road gasoline vehicles are a major source of secondary organic aerosol (SOA) in urban areas. We investigated SOA formation by oxidizing dilute, ambient-level exhaust concentrations from a fleet of on-road gasoline vehicles in a smog chamber. We measured less SOA formation from newer vehicles meeting more stringent emissions standards. This suggests that the natural replacement of older vehicles with newer ones that meet more stringent emissions standards should reduce SOA levels in urban environments. However, SOA production depends on both precursor concentrations (emissions) and atmospheric chemistry (SOA yields). We found a strongly nonlinear relationship between SOA formation and the ratio of nonmethane organic gas to oxides of nitrogen (NOx) (NMOG:NOx), which affects the fate of peroxy radicals. For example, changing the NMOG:NOx from 4 to 10 ppbC/ppbNOx increased the SOA yield from dilute gasoline vehicle exhaust by a factor of 8. We investigated the implications of this relationship for the Los Angeles area. Although organic gas emissions from gasoline vehicles in Los Angeles are expected to fall by almost 80% over the next two decades, we predict no reduction in SOA production from these emissions due to the effects of rising NMOG:NOx on SOA yields. This highlights the importance of integrated emission control policies for NOx and organic gases.

Secondary organic aerosol (SOA), formed in the photooxidation of diesel fuel, biodiesel fuel, and 20% biodiesel fuel/80% diesel fuel mixture, are prepared under high-NOx conditions in the presence and absence of sulfur dioxide (SO2), ammonia (NH3), and relative humidity (RH). The composition of condensed-phase organic compounds in SOA is measured using several complementary techniques including aerosol mass spectrometry (AMS), high-resolution nanospray desorption electrospray ionization mass spectrometry (nano-DESI/HRMS), and ultrahigh resolution and mass accuracy 21T Fourier transform ion cyclotron resonance mass spectrometry (21T FT-ICR MS). Results demonstrate that sulfuric acid and condensed organosulfur species formed in photooxidation experiments with SO2 are present in the SOA particles. Fewer organosulfur species are formed in the high humidity experiments, performed at RH 90%, in comparison with experiments done under dry conditions. There is a strong overlap of organosulfur species observed in this study with previous field and chamber studies of SOA. Many MS peaks of organosulfates (R-OS(O)2OH) previously designated as biogenic or of unknown origin in field studies might have originated from anthropogenic sources, such as photooxidation of hydrocarbons present in diesel and biodiesel fuel.

Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM/OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM/OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH > SRH led to increased SOA concentrations,· particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties· such as the OM/OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model-measurement gap. When taking into account deviations from ideality, including both inorganic (when RH > SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from this work will be released in CMAQ v5.2.

Research on the sources of indoor airborne chemicals has traditionally focused on outdoor air, building materials, furnishings, and activities such as smoking, cooking, and cleaning. Relatively little research has examined the direct role of occupant emissions, even though this source clearly contributes to indoor volatile organic compounds (VOCs) and influences indoor chemistry. In this work, we quantify occupant-related gaseous VOC emissions in a university classroom using a proton-transfer-reaction time-of-flight mass spectrometer. Time-resolved concentrations of VOCs in room air and supply air were measured continuously during occupied and unoccupied periods. The emission factor for each human-emitted VOC was determined by dividing the occupant-associated source rate by the corresponding occupancy. Among the most abundant species detected were compounds associated with personal care products. Also prominent were human metabolic emissions, such as isoprene, methanol, acetone, and acetic acid. Additional sources included human skin oil oxidation by ozone, producing compounds such as 4-oxopentanal (4-OPA) and 6-methyl-5-hepten-2-one (6-MHO). By mass, human-emitted VOCs were the dominant source (57%) during occupied periods in a well-ventilated classroom, with ventilation supply air the second most important (35%), and indoor nonoccupant emissions the least (8%). The total occupant-associated VOC emission factor was 6.3 mg h-1 per person.

Tennessee began its movement toward Middle Level Licensure during the 2002-2003 school year. Only 14 years later, in 2016, Middle Level Licensure in Tennessee will change. In this article, the background and experiences of seven middle level education teacher candidates at the University of Memphis who were the first candidates to complete the Residency model for student teaching and the program's evolution from traditional to the new program are described. From its inception until today, the middle level teacher preparation program has adapted to state mandates and made changes to better meet the needs of teacher candidates committed to educating young adolescents. Tailoring to the needs of the students, the new program offers a year-long residency allowing candidates to spend more time in the classroom, a balanced assessment course, and adoption of the edTPA to assess candidates' overall aptitude for teaching. These changes have added rigor to the program. This qualitative case study discusses the "how and why" associated with changes, and what the course of action was in order to meet candidates' needs. Despite its growth and success, the future of the program and how middle level licensure will be awarded in the state of Tennessee remains unknown.

We assessed the relative importance of environmental filtering and dispersal limitation in structuring foliage- and ground-dwelling arthropod communities in central North Carolina. We hypothesized that differences in both local environment and dispersal distance between sites would predict differences in community composition, but that dispersal distance would be more important for ground arthropods than for foliage arthropods. We used variance partitioning to quantify the relative explanatory power of differences in the local environment and dispersal distance between sampling plots. For foliage arthropods, the full set of predictors explained 37–39% of the variance in community dissimilarity, while the full set of predictors explained 42–56% of the variance for ground arthropods. Environmental predictors alone consistently explained more variance in community dissimilarity than geographic predictors alone for ground arthropods, but the variance explained by each predictor set alone varied for foliage arthropods depending on the metric of community dissimilarity. Examining communities of multiple arthropod groups across the same spatial gradient highlights the scale-dependence of these processes and illustrates how variation in the environment can alter the relative abundance of specialist and generalist taxa. [ABSTRACT FROM AUTHOR]

Global freight distribution patterns have been affected by trading policies and the pandemic outbreak. The Belt and Road Initiative, trade conflicts, and the COVID-19 pandemic have changed the global logistics flow, shifting cargos from maritime and air transport to railway transport along the countries in the Eurasian Landbridge. Though railway freight emits less carbon than road truck transportation, the increased use of railway freight brings in a higher volume of carbon emissions to cities located along the landbridges. Achieving net zero carbon emission is becoming more important, but there is a lack of literature in assessing the environmental impact of cross-border railway logistics transportation among Belt and Road countries. A novel two-stage multilateral trade-based prediction model is developed, integrating a modified gravity model and nonlinear autoregressive neural network for trade and emission forecasting. The model evaluates railway freight along the landbridge over ten years and forecasts the impact of carbon emissions from trading and logistics along the corridor in the subsequent five years. It further analyses the emissions impact of the proposed Third Eurasian Landbridge and the extended Second Eurasian Landbridge. The findings provide insights for the development of railway freight transport, considering trade and logistics flow, carbon emission mitigation strategies, and sustainability impact between China and other Belt and Road countries. While countries such as India and Kazakhstan were forecast to have significant amounts of carbon emissions in the projected period, the rapid growths in locations with smaller emission amounts such as Kunming and Georgia should draw attention and require continuous monitoring. [ABSTRACT FROM AUTHOR]

Background: Having a haematological condition can adversely affect the quality of life (QoL) of family members/partners of patients. It is important to measure this often ignored burden in order to implement appropriate supportive interventions. Objective: To measure current impact of haematological conditions on the QoL of family members/partners of patients, using the Family Reported Outcome Measure‐16 (FROM‐16). Methods: A cross‐sectional study, recruited online through patient support groups, involved UK family members/partners of people with haematological conditions completing the FROM‐16. Results: 183 family members/partners (mean age = 60.5 years, SD = 13.2; females = 62.8%) of patients (mean age = 64.1, SD = 12.8; females = 46.4%) with 12 haematological conditions completed the FROM‐16. The FROM‐16 mean total score was 14.0 (SD = 7.2), meaning 'a moderate effect on QoL'. The mean FROM‐16 scores of family members of people with multiple myeloma (mean = 15.8, SD = 6.3, n = 99) and other haematological malignancies (mean = 13.9, SD = 7.8, n = 29) were higher than of people with pernicious anaemia (mean = 10.7, SD = 7.5, n = 47) and other non‐malignant conditions (mean = 11, SD = 7.4, n = 56, p <.01). Over one third (36.1%, n = 183) of family members experienced a 'very large effect' (FROM‐16 score>16) on their quality of life. Conclusions: Haematological conditions, in particular those of malignant type, impact the QoL of family members/partners of patients. Healthcare professionals can now, using FROM‐16, identify those most affected and should consider how to provide appropriate holistic support within routine practice. [ABSTRACT FROM AUTHOR]

Isoprene photooxidation is a major driver of atmospheric chemistry over forested regions. Isoprene reacts with hydroxyl radicals (OH) and molecular oxygen to produce isoprene peroxy radicals (ISOPOO). These radicals can react with hydroperoxyl radicals (HO2) to dominantly produce hydroxyhydroperoxides (ISOPOOH). They can also react with nitric oxide (NO) to largely produce methyl vinyl ketone (MVK) and methacrolein (MACR). Unimolecular isomerization and bimolecular reactions with organic peroxy radicals are also possible. There is uncertainty about the relative importance of each of these pathways in the atmosphere and possible changes because of anthropogenic pollution. Herein, measurements of ISOPOOH and MVK + MACR concentrations are reported over the central region of the Amazon basin during the wet season. The research site, downwind of an urban region, intercepted both background and polluted air masses during the GoAmazon2014/5 Experiment. Under background conditions, the confidence interval for the ratio of the ISOPOOH concentration to that of MVK + MACR spanned 0.4-0.6. This result implies a ratio of the reaction rate of ISOPOO with HO2 to that with NO of approximately unity. A value of unity is significantly smaller than simulated at present by global chemical transport models for this important, nominally low-NO, forested region of Earth. Under polluted conditions, when the concentrations of reactive nitrogen compounds were high (>1 ppb), ISOPOOH concentrations dropped below the instrumental detection limit (

There remains considerable uncertainty in how anthropogenic gas phase emissions alter the oxidative aging of organic aerosols in the troposphere. Here we observe a 10-20 fold acceleration in the effective heterogeneous OH oxidation rate of organic aerosol in the presence of SO2. This acceleration originates from the radical chain reactions propagated by alkoxy radicals, which are formed efficiently inside the particle by the reaction of peroxy radicals with SO2. As the OH approaches atmospheric concentrations, the radical chain length increases, transforming the aerosol at rates predicted to be up to 10 times the OH-aerosol collision frequency. Model predictions, constrained by experiments over orders of magnitude changes in [OH] and [SO2], suggest that in polluted regions the heterogeneous processing of organic aerosols by OH ([SO2] ≥ 40 ppb) occur on similar time scales as analogous gas-phase oxidation reactions. These results provide evidence for a previously unidentified mechanism by which organic aerosol oxidation is enhanced by anthropogenic gas phase emissions.

Earth's atmosphere contains a multitude of organic compounds, which differ by orders of magnitude regarding fundamental properties such as volatility, reactivity, and propensity to form cloud droplets, affecting their impact on global climate and human health. Despite recent major research efforts and advances, there are still substantial gaps in understanding of atmospheric organic chemistry, hampering efforts to understand, model, and mitigate environmental problems such as aerosol formation in both polluted urban and more pristine regions. The analytical toolbox available for chemists to study atmospheric organic components has expanded considerably during the past decade, opening new windows into speciation, time resolution and detection of reactive and semivolatile compounds at low concentrations. This has provided unprecedented opportunities, but also unveiled new scientific challenges. Specific groundbreaking examples include the role of epoxides in aerosol formation especially from isoprene, the importance of highly oxidized, reactive organics in air-surface processes (whether atmosphere-biosphere exchange or aerosols), as well as the extent of interactions of anthropogenic and biogenic emissions and the resulting impact on atmospheric organic chemistry.

Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene- and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas-particle equilibrium and (ii) have a short particle-phase lifetime (∼2-4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment.

The emission, dispersion, and photochemistry of isoprene (C5H8) and related chemical species in the convective boundary layer (CBL) during sunlit daytime were studied over a mixed forest in the southeastern United States by combining ground-based and aircraft observations. Fluxes of isoprene and monoterpenes were quantified at the top of the forest canopy using a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). Snapshot (2 min sampling duration) vertical profiles of isoprene, methyl vinyl ketone (MVK)Cmethacrolein (MACR), and monoterpenes were collected from aircraft every hour in the CBL (100-1000 m). Both ground-based and airborne collected volatile organic compound (VOC) data are used to constrain the initial conditions of a mixed-layer chemistry model (MXLCH), which is applied to examine the chemical evolution of the O3-NOx-HOx-VOC system and how it is affected by boundary layer dynamics in the CBL. The chemical loss rate of isoprene (1 h) is similar to the turbulent mixing timescale (0.1-0.5 h), which indicates that isoprene concentrations are equally dependent on both photooxidation and boundary layer dynamics. Analysis of a modelderived concentration budget suggests that diurnal evolution of isoprene inside the CBL is mainly controlled by surface emissions and chemical loss; the diurnal evolution of O3 is dominated by entrainment. The NO to HO2 ratio (NO :HO2) is used as an indicator of anthropogenic impact on the CBL chemical composition and spans a wide range (1-163). The fate of hydroxyl-substituted isoprene peroxyl radical (HOC5H8OO q; ISOPOO) is strongly affected by NO:HO2, shifting from NO-dominant to NO-HO2-balanced conditions from early morning to noontime. This chemical regime change is reflected in the diurnal evolution of isoprene hydroxynitrates (ISOPN) and isoprene hydroxy hydroperoxides (ISOPOOH).