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31.
Atmospheric chemistry and physics in the atmosphere of a developed megacity (London): An overview of the REPARTEE experiment and its conclusions
Gavin J Phillips, Carole Helfter, Chiara F Di Marco, Eiko Nemitz, Fay Davies, Janet F Barlow, Tyrone Dunbar, Iain R White, Dudley E Shallcross, Stephen J Henshaw, K Fredrik Peterson, Brian Davison, Damien Martin, Ben Langford, C Nicholas Hewitt, Stephen M Ball, Justin M Langridge, A K Benton, Roderick L Jones, Paul I Williams, John Whitehead, Martin W Gallagher, Claire Martin, James R Dorsey, Hugh Coe, James D Allan, William J Bloss, Alistair J Thorpe, David C S Beddows, Manuel DallOsto, Roy M Harrison, Steven Smith, 2012, pregledni znanstveni članek

Opis: The Regents Park and Tower Environmental Experiment (REPARTEE) comprised two campaigns in London in October 2006 and October/November 2007. The experiment design involved measurements at a heavily trafficked roadside site, two urban background sites and an elevated site at 160-190 m above ground on the BT Tower, supplemented in the second campaign by Doppler lidar measurements of atmospheric vertical structure. A wide range of measurements of airborne particle physical metrics and chemical composition were made as well as measurements of a considerable range of gas phase species and the fluxes of both particulate and gas phase substances. Significant findings include (a) demonstration of the evaporation of traffic-generated nanoparticles during both horizontal and vertical atmospheric transport; (b) generation of a large base of information on the fluxes of nanoparticles, accumulation mode particles and specific chemical components of the aerosol and a range of gas phase species, as well as the elucidation of key processes and comparison with emissions inventories; (c) quantification of vertical gradients in selected aerosol and trace gas species which has demonstrated the important role of regional transport in influencing concentrations of sulphate, nitrate and secondary organic compounds within the atmosphere of London; (d) generation of new data on the atmospheric structure and turbulence above London, including the estimation of mixed layer depths; (e) provision of new data on trace gas dispersion in the urban atmosphere through the release of purposeful tracers; (f) the determination of spatial differences in aerosol particle size distributions and their interpretation in terms of sources and physico-chemical transformations; (g) studies of the nocturnal oxidation of nitrogen oxides and of the diurnal behaviour of nitrate aerosol in the urban atmosphere, and (h) new information on the chemical composition and source apportionment of particulate matter size fractions in the atmosphere of London derived both from bulk chemical analysis and aerosol mass spectrometry with two instrument types.
Ključne besede: megacity, trace gas, urban atmosphere, atmospheric transport, chemical composition, aerosol
Objavljeno: 18.07.2019; Ogledov: 71; Prenosov: 0
.pdf Polno besedilo (4,66 MB)

32.
Increased sensitivity in proton transfer reaction mass spectrometry by incorporation of a radio frequency ion funnel
Andrew M Ellis, Stephen Mullock, Fraser Reich, Paul S Monks, Iain R White, Robert S Blake, Shane Barber, 2012, izvirni znanstveni članek

Opis: A drift tube capable of simultaneously functioning as an ion funnel is demonstrated in proton transfer reaction mass spectrometry (PTR-MS) for the first time. The ion funnel enables a much higher proportion of ions to exit the drift tube and enter the mass spectrometer than would otherwise be the case. An increase in the detection sensitivity for volatile organic compounds of between 1 and 2 orders of magnitude is delivered, as demonstrated using several compounds. Other aspects of analytical performance explored in this study include the effective E/N (ratio of electric field to number density of the gas) and dynamic range over which the drift tube is operated. The dual-purpose drift tube/ion funnel can be coupled to various types of mass spectrometers to increase the detection sensitivity and may therefore offer considerable benefits in PTR-MS work.
Ključne besede: Analytical performance, Detection sensitivity, Drift tube, Dynamic range, Ion funnels, Proton-transfer reaction mass spectrometry, Volatile organic compounds
Objavljeno: 18.07.2019; Ogledov: 68; Prenosov: 0
.pdf Polno besedilo (799,47 KB)

33.
Investigating the use of secondary organic aerosol as seed particles in simulation chamber experiments
Jaqueline F Hamilton, M Rami Alfarra, Kevin P Wyche, Martyn W Ward, Alistair C Lewis, Gordon B McFiggans, Nicholas Good, Paul S Monks, Timo Carr, Iain R White, Ruth M Purvis, 2011, izvirni znanstveni članek

Opis: The use of β-caryophyllene secondary organic aerosol particles as seeds for smog chamber simulations has been investigated. A series of experiments were carried out in the Manchester photochemical chamber as part of the Aerosol Coupling in the Earth System (ACES) project to study the effect of seed particles on the formation of secondary organic aerosol (SOA) from limonene photo-oxidation. Rather than use a conventional seed aerosol containing ammonium sulfate or diesel particles, a method was developed to use in-situ chamber generated seed particles from β-caryophyllene photo-oxidation, which were then diluted to a desired mass loading (in this case 4-13 μg m-3). Limonene was then introduced into the chamber and oxidised, with the formation of SOA seen as a growth in the size of oxidised organic seed particles from 150 to 325 nm mean diameter. The effect of the partitioning of limonene oxidation products onto the seed aerosol was assessed using aerosol mass spectrometry during the experiment and the percentage of m/z 44, an indicator of degree of oxidation, increased from around 5 to 8 %. The hygroscopicity of the aerosol also changed, with the growth factor for 200 nm particles increasing from less than 1.05 to 1.25 at 90 % RH. The detailed chemical composition of the limonene SOA could be extracted from the complex β-caryophyllene matrix using two-dimensional gas chromatography (GC× GC) and liquid chromatography coupled to mass spectrometry. High resolution Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS) was used to determine exact molecular formulae of the seed and the limonene modified aerosol. The average O:C ratio was seen to increase from 0.32 to 0.37 after limonene oxidation products had condensed onto the organic seed.
Ključne besede: Aerosol, Aerosol formation, Smog chamber
Objavljeno: 18.07.2019; Ogledov: 60; Prenosov: 0
.pdf Polno besedilo (1,96 MB)

34.
Development of an adaptable headspace sampling method for metabolic profiling of the fungal volatome
Stephen J Fowler, Nicholas D Read, Royston Goodacre, Michael J Bromley, Tamara M Nijsen, Oluwasola Lawal, Iain R White, Pavlos Geranios, Waqar M Ahmed, 2018, izvirni znanstveni članek

Opis: Pulmonary aspergillosis can cause serious complications in people with a suppressed immune system. Volatile metabolites emitted by Aspergillus spp. have shown promise for early detection of pathogenicity. However, volatile profiles require further research, as effective headspace analysis methods are required for extended chemical coverage of the volatome; in terms of both very volatile and semi-volatile compounds. In this study, we describe a novel adaptable sampling method in which fungal headspace samples can be sampled continuously throughout a defined time period using both active (pumped) and passive (diffusive) methods, with the capability for samples to be stored for later off-line analysis. For this method we utilise thermal desorption-gas chromatography-mass spectrometry to generate volatile metabolic profiles using Aspergillus fumigatus as the model organism. Several known fungal-specific volatiles associated with secondary metabolite biosynthesis (including α-pinene, camphene, limonene, and several sesquiterpenes) were identified. A comparison between the wild-type A. fumigatus with a phosphopantetheinyl transferase null mutant strain (ΔpptA) that is compromised in secondary metabolite synthesis, revealed reduced production of sesquiterpenes. We also showed the lack of terpene compounds production during the early growth phase, whilst pyrazines were identified in both early and late growth phases. We have demonstrated that the fungal volatome is dynamic and it is therefore critically necessary to sample the headspace across several time periods using a combination of active and passive sampling techniques to analyse and understand this dynamism.
Ključne besede: Volatile Organic Compounds, Fungi, Mycelial growth
Objavljeno: 18.07.2019; Ogledov: 59; Prenosov: 0
.pdf Polno besedilo (712,24 KB)

35.
TD/GC–MS analysis of volatile markers emitted from mono- and co-cultures of Enterobacter cloacae and Pseudomonas aeruginosa in artificial sputum
Craig Portsmouth, Pedro Povoa, Jan H Leopold, Pouline M P van Oort, Emili Diaz, Gemma Goma, Timothy Felton, Paul Dark, Alan Davie, Luis Coelho, Lieuwe D Bos, Marta Camprubi, Antonio Artigas, Jonathan Barnard-Smith, Waqar M Ahmed, Stephen J Fowler, Tamara M E Nijsen, Royston Goodacre, Weda Hans, Hugo knobel, Oluwasola Lawal, Iain R White, 2018, izvirni znanstveni članek

Opis: Introduction: Infections such as ventilator-associated pneumonia (VAP) can be caused by one or more pathogens. Current methods for identifying these pathogenic microbes often require invasive sampling, and can be time consuming, due to the requirement for prolonged cultural enrichment along with selective and differential plating steps. This results in delays in diagnosis which in such critically ill patients can have potentially life-threatening consequences. Therefore, a non-invasive and timely diagnostic method is required. Detection of microbial volatile organic compounds (VOCs) in exhaled breath is proposed as an alternative method for identifying these pathogens and may distinguish between mono- and poly-microbial infections. Objectives: To investigate volatile metabolites that discriminate between bacterial mono- and co-cultures. Methods: VAP-associated pathogens Enterobacter cloacae and Pseudomonas aeruginosa were cultured individually and together in artificial sputum medium for 24 h and their headspace was analysed for potential discriminatory VOCs by thermal desorption gas chromatography–mass spectrometry. Results: Of the 70 VOCs putatively identified, 23 were found to significantly increase during bacterial culture (i.e. likely to be released during metabolism) and 13 decreased (i.e. likely consumed during metabolism). The other VOCs showed no transformation (similar concentrations observed as in the medium). Bacteria-specific VOCs including 2-methyl-1-propanol, 2-phenylethanol, and 3-methyl-1-butanol were observed in the headspace of axenic cultures of E. cloacae, and methyl 2-ethylhexanoate in the headspace of P. aeruginosa cultures which is novel to this investigation. Previously reported VOCs 1-undecene and pyrrole were also detected. The metabolites 2-methylbutyl acetate and methyl 2-methylbutyrate, which are reported to exhibit antimicrobial activity, were elevated in co-culture only. Conclusion: The observed VOCs were able to differentiate axenic and co-cultures. Validation of these markers in exhaled breath specimens could prove useful for timely pathogen identification and infection type diagnosis.
Ključne besede: Bacteria, Enterobacter cloacae, Gas Chromatography-Mass Spectrometry, Infection, Pseudomonas aeruginosa, Volatile organic compounds
Objavljeno: 18.07.2019; Ogledov: 68; Prenosov: 3
.pdf Polno besedilo (1,29 MB)

36.
Tracer concentration profiles measured in central London as part of the REPARTEE campaign
Damien Martin, K Fredrik Petersson, Iain R White, Stephen H Henshaw, Graham Nickless, Amy Lovelock, Janet F Barlow, Tyrone Dunbar, Curtis R Wood, Dudley E. Shallcross, 2011, izvirni znanstveni članek

Opis: There have been relatively few tracer experiments carried out that have looked at vertical plume spread in urban areas. In this paper we present results from two tracer (cyclic perfluorocarbon) experiments carried out in 2006 and 2007 in central London centred on the BT Tower as part of the REPARTEE (Regent's Park and Tower Environmental Experiment) campaign. The height of the tower gives a unique opportunity to study vertical dispersion profiles and transport times in central London. Vertical gradients are contrasted with the relevant Pasquill stability classes. Estimation of lateral advection and vertical mixing times are made and compared with previous measurements. Data are then compared with a simple operational dispersion model and contrasted with data taken in central London as part of the DAPPLE campaign. This correlates dosage with non-dimensionalised distance from source. Such analyses illustrate the feasibility of the use of these empirical correlations over these prescribed distances in central London.
Ključne besede: advection, concentration (composition), dispersion, tracer, urban atmosphere, vertical mixing, vertical profile
Objavljeno: 18.07.2019; Ogledov: 64; Prenosov: 0
.pdf Polno besedilo (1,49 MB)

37.
Use of reactive tracers to determine ambient OH radical concentrations: Application within the indoor environment
Dudley E. Shallcross, Keven C Clemitshaw, Guy C Lloyd-Jones, Graham Nickless, Stephen J Henshaw, Fredrik K Petersson, Maria Paz Muñoz, Damien Martin, Iain R White, 2010, izvirni znanstveni članek

Opis: The hydroxyl radical (OH) plays a key role in determining indoor air quality. However, its highly reactive nature and low concentration indoors impede direct analysis. This paper describes the techniques used to indirectly quantify indoor OH, including the development of a new method based on the instantaneous release of chemical tracers into the air. This method was used to detect ambient OH in two indoor seminar rooms following tracer detection by gas chromatography- mass spectrometry (GCMS). The results from these tests add to the small number of experiments that have measured indoor OH which are discussed with regard to future directions within air quality research.
Ključne besede: Ozone, Indoor air pollution, Indoor ozone, chemical tracers
Objavljeno: 18.07.2019; Ogledov: 72; Prenosov: 0
.pdf Polno besedilo (153,74 KB)

38.
Headspace volatile organic compounds from bacteria implicated in ventilator-associated pneumonia analysed by TD-GC/MS
Stephen J Fowler, Roy Goodacre, Iain R White, Tamara M E Nijsen, Waqar M Ahmed, Howbeer Muhamadali, Oluwasola Lawal, 2018, izvirni znanstveni članek

Opis: Ventilator-associated pneumonia (VAP) is a healthcare-acquired infection arising from the invasion of the lower respiratory tract by opportunistic pathogens in ventilated patients. The current method of diagnosis requires the culture of an airway sample such as bronchoalveolar lavage, which is invasive to obtain and may take up to seven days to identify a causal pathogen, or indeed rule out infection. While awaiting results, patients are administered empirical antibiotics; risks of this approach include lack of effect on the causal pathogen, contribution to the development of antibiotic resistance and downstream effects such as increased length of intensive care stay, cost, morbidity and mortality. Specific biomarkers which could identify causal pathogens in a timely manner are needed as they would allow judicious use of the most appropriate antimicrobial therapy. Volatile organic compound (VOC) analysis in exhaled breath is proposed as an alternative due to its non-invasive nature and its potential to provide rapid diagnosis at the patient's bedside. VOCs in exhaled breath originate from exogenous, endogenous, as well as microbial sources. To identify potential markers, VAP-associated pathogens Escherichia coli, Klebsiella pneumoniae, Pseudomonas aeruginosa, and Staphylococcus aureus were cultured in both artificial sputum medium and nutrient broth, and their headspaces were sampled and analysed for VOCs. Previously reported volatile markers were identified in this study, including indole and 1-undecene, alongside compounds that are novel to this investigation, cyclopentanone and 1-hexanol. We further investigated media components (substrates) to identify those that are essential for indole and cyclopentanone production, with potential implications for understanding microbial metabolism in the lung.
Ključne besede: bacteria, exhaled breath, infection, ventilator-associated pneumonia, volatile organic compounds
Objavljeno: 18.07.2019; Ogledov: 53; Prenosov: 0

39.
Urban tracer dispersion experiments during the second DAPPLE field campaign in London 2004
Damien Martin, Catheryn S Price, Iain R White, Graham Nickless, K Fredrik Petersson, Rex E Britter, Alan G Robins, Stephen E Belcher, Janet F Barlow, Marie Neophytou, Samantha J Arnold, Alan S Tomlin, Robert J Smalley, Dudley E. Shallcross, 2010, izvirni znanstveni članek

Opis: As part of the DAPPLE programme two large scale urban tracer experiments using multiple simultaneous releases of cyclic perfluoroalkanes from fixed location point sources was performed. The receptor concentrations along with relevant meteorological parameters measured are compared with a three screening dispersion models in order to best predict the decay of pollution sources with respect to distance. It is shown here that the simple dispersion models tested here can provide a reasonable upper bound estimate of the maximum concentrations measured with an empirical model derived from field observations and wind tunnel studies providing the best estimate. An indoor receptor was also used to assess indoor concentrations and their pertinence to commonly used evacuation procedures.
Ključne besede: Dapple, dispersion
Objavljeno: 18.07.2019; Ogledov: 70; Prenosov: 0
.pdf Polno besedilo (1,69 MB)

40.
CityFlux perfluorocarbon tracer experiments
Fredrik K Petersson, Damien Martin, Iain R White, Stephen J Henshaw, Graham Nickless, Ian Longley, Carl J Percival, Martin Gallagher, Dudley E. Shallcross, 2010, izvirni znanstveni članek

Opis: In June 2006, two perfluorocarbon tracer experiments were conducted in central Manchester UK as part of the CityFlux campaign. The main aim was to investigate vertical dispersion in an urban area during convective conditions, but dispersion mechanisms within the street network were also studied. Paired receptors were used in most cases where one receptor was located at ground level and one at roof level. One receptor was located on the roof of Portland Tower which is an 80m high building in central Manchester. Source receptor distances in the two experiments varied between 120 and 600 m. The results reveal that maximum concentration was sometimes found at roof level rather than at ground level implying the effectiveness of convective forces on dispersion. The degree of vertical dispersion was found to be dependent on source receptor distance as well as on building height in proximity to the release site. Evidence of flow channelling in a street canyon was also found. Both a Gaussian profile and a street network model were applied and the results show that the urban topography may lead to highly effective flow channelling which therefore may be a very important dispersion mechanism should the right meteorological conditions prevail. The experimental results from this campaign have also been compared with a simple urban dispersion model that was developed during the DAPPLE framework and show good agreement with this. The results presented here are some of the first published regarding vertical dispersion. More tracer experiments are needed in order to further characterise vertical concentration profiles and their dependence on, for instance, atmospheric stability. The impact of urban topography on pollutant dispersion is important to focus on in future tracer experiments in order to improve performance of models as well as for our understanding of the relationship between air quality and public health.
Ključne besede: air quality, atmospheric chemistry, concentration (composition), convective system, dispersion, public health, street canyon, tracer, urban area
Objavljeno: 18.07.2019; Ogledov: 69; Prenosov: 0
.pdf Polno besedilo (1,07 MB)

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