Browsing by Author "Connors, Sarah"
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Item Open Access Development of a low-maintenance measurement approach to continuously estimate methane emissions: a case study(Elsevier, 2016-12-18) Riddick, Stuart N.; Hancock, B. R.; Robinson, Andrew D.; Connors, Sarah; Davies, S.; Allen, Grant; Pitt, Joseph; Harris, Neil R. P.The chemical breakdown of organic matter in landfills represents a significant source of methane gas (CH4). Current estimates suggest that landfills are responsible for between 3% and 19% of global anthropogenic emissions. The net CH4 emissions resulting from biogeochemical processes and their modulation by microbes in landfills are poorly constrained by imprecise knowledge of environmental constraints. The uncertainty in absolute CH4 emissions from landfills is therefore considerable. This study investigates a new method to estimate the temporal variability of CH4 emissions using meteorological and CH4 concentration measurements downwind of a landfill site in Suffolk, UK from July to September 2014, taking advantage of the statistics that such a measurement approach offers versus shorter-term, but more complex and instantaneously accurate, flux snapshots. Methane emissions were calculated from CH4 concentrations measured 700 m from the perimeter of the landfill with observed concentrations ranging from background to 46.4 ppm. Using an atmospheric dispersion model, we estimate a mean emission flux of 709 μg m−2 s−1 over this period, with a maximum value of 6.21 mg m−2 s−1, reflecting the wide natural variability in biogeochemical and other environmental controls on net site emission. The emissions calculated suggest that meteorological conditions have an influence on the magnitude of CH4 emissions. We also investigate the factors responsible for the large variability observed in the estimated CH4 emissions, and suggest that the largest component arises from uncertainty in the spatial distribution of CH4 emissions within the landfill area. The results determined using the low-maintenance approach discussed in this paper suggest that a network of cheaper, less precise CH4 sensors could be used to measure a continuous CH4 emission time series from a landfill site, something that is not practical using far-field approaches such as tracer release methods. Even though there are limitations to the approach described here, this easy, low-maintenance, low-cost method could be used by landfill operators to estimate time-averaged CH4 emissions and their impact downwind by simultaneously monitoring plume advection and CH4 concentrations.Item Open Access Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols(Nature, 2016-10-13) Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil R. P.; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Back, Jaana; Petaja, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, MarkusSecondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.Item Open Access Estimating the size of a methane emission point source at different scales: from local to landscape(European Geosciences Union (EGU) / Copernicus Publications, 2017-06-29) Riddick, Stuart N.; Connors, Sarah; Robinson, Andrew D.; Manning, Alistair J.; Jones, Pippa S. D.; Lowry, David; Nisbet, Euan; Skelton, Robert L.; Allen, Grant; Pitt, Joseph; Harris, NeilHigh methane (CH4) mixing ratios (up to 4 ppm) have occurred sporadically at our measurement site in Haddenham, Cambridgeshire, since July 2012. Isotopic measurements and back trajectories show that the source is the Waterbeach Waste Management Park 7 km SE of Haddenham. To investigate this further, measurements were made on 30 June and 1 July 2015 at other locations nearer to the source. Landfill emissions have been estimated using three different approaches at different scales; near source using the WindTrax inversion dispersion model, middle distance using a Gaussian plume (GP) model and at the landscape scale using the Numerical Atmospheric Modelling Environment (NAME) Inversion Technique for Emission Modelling (InTEM) inversion. The emission estimates derived using the WindTrax and Gaussian plume (GP) approaches agree well for the period of intense observations. Applying the Gaussian plume approach to all periods of elevated measurements seen at Haddenham produces year-round and monthly landfill emission estimates with an estimated annual emission of 11.6 GgCH(4) yr(-1). The monthly emission estimates are highest in winter (2160 kg h(-1) in February) and lowest in summer (620 kg h(-1) in July). These data identify the effects of environmental conditions on landfill CH4 production and highlight the importance of year-round measurements to capture seasonal variability in CH4 emission.Item Open Access Estimating the size of a methane emission point-source at different scales: from local to landscape(Copernicus Publications, 2016-11-22) Riddick, Stuart N.; Connors, Sarah; Robinson, Andrew D.; Manning, Alistair J.; Jones, Pippa S. D.; Lowry, David; Nisbet, Euan; Skelton, Robert L.; Allen, Grant; Pitt, Joseph; Harris, NeilHigh methane (CH4) mixing ratios (up to 4 ppm) have occurred sporadically at our measurement site in Haddenham, Cambridgeshire since July 2012. Isotopic measurements and back trajectories show that the source is the Waterbeach Waste management park 7 km SE of Haddenham. To investigate this further, measurements were made on June 30th and July 1st 2015 at other locations nearer to the source. Landfill emissions have been estimated using three different approaches (WindTrax, Gaussian plume, and NAME InTEM inversion) applied to the measurements made close to source and at Haddenham. The emission estimates derived using the WindTrax and Gaussian plume approaches agree well for the period of intense observations. Applying the Gaussian plume approach to all periods of elevated measurements seen at Haddenham produces year-round and monthly landfill emission estimates. The estimated annual emissions vary between 11.6 and 13.7 Gg CH4 yr−1. The monthly emission estimates are highest in winter (2160 kg hr−1 in February) and lowest in summer (620 kg hr−1 in July). These data identify the effects of environmental conditions on landfill CH4 production and highlight the importance of year-round measurement to capture seasonal variability in CH4 emission. We suggest the landscape inverse modelling approach described in this paper is in good agreement with more labour-intensive near-source approaches and can be used to identify point-sources within an emission landscape to provide high-quality emission estimates.Item Open Access A measurement-based verification framework for UK greenhouse gas emissions: an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) project(Elsevier, 2018-08-17) Palmer, Paul I.; O'Doherty, Simon; Allen, Grant; Bower, Keith; Bösch, Hartmut; Chipperfield, Martyn P.; Connors, Sarah; Dhomse, Sandip; Feng, Liang; Finch, Douglas P.; Gallagher, Martin W.; Gloor, Emanuel; Gonzi, Siegfried; Harris, Neil R. P.; Helfter, Carole; Humpage, Neil; Kerridge, Brian; Knappett, Diane; Jones, Roderic L.; Le Breton, Michael; Lunt, Mark F.; Manning, Alistair J.; Matthiesen, Stephan; Muller, Jennifer B. A.; Mullinger, Neil; Nemitz, Eiko; O'Shea, Sebastian; Parker, Robert J.; Percival, Carl J.; Pitt, Joseph; Riddick, Stuart N.; Rigby, Matthew; Sembhi, Harjinder; Siddans, Richard; Skelton, Robert L.; Smith, Paul; Sonderfeld, Hannah; Stanley, Kieran; Stavert, Ann R.; Wenger, Angelina; White, Emily; Wilson, Christopher; Young, DickonWe describe the motivation, design, and execution of the Greenhouse gAs Uk and Global Emissions (GAUGE) project. The overarching scientific objective of GAUGE was to use atmospheric data to estimate the magnitude, distribution, and uncertainty of the UK greenhouse gas (GHG, defined here as CO2, CH4, and N2O) budget, 2013–2015. To address this objective, we established a multi-year and interlinked measurement and data analysis programme, building on an established tall-tower GHG measurement network. The calibrated measurement network comprises ground-based, airborne, ship-borne, balloon-borne, and space-borne GHG sensors. Our choice of measurement technologies and measurement locations reflects the heterogeneity of UK GHG sources, which range from small point sources such as landfills to large, diffuse sources such as agriculture. Atmospheric mole fraction data collected at the tall towers and on the ships provide information on sub-continental fluxes, representing the backbone to the GAUGE network. Additional spatial and temporal details of GHG fluxes over East Anglia were inferred from data collected by a regional network. Data collected during aircraft flights were used to study the transport of GHGs on local and regional scales. We purposely integrated new sensor and platform technologies into the GAUGE network, allowing us to lay the foundations of a strengthened UK capability to verify national GHG emissions beyond the project lifetime. For example, current satellites provide sparse and seasonally uneven sampling over the UK mainly because of its geographical size and cloud cover. This situation will improve with new and future satellite instruments, e.g. measurements of CH4 from the TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5P. We use global, nested, and regional atmospheric transport models and inverse methods to infer geographically resolved CO2 and CH4 fluxes. This multi-model approach allows us to study model spread in a posteriori flux estimates. These models are used to determine the relative importance of different measurements to infer the UK GHG budget. Attributing observed GHG variations to specific sources is a major challenge. Within a UK-wide spatial context we used two approaches: (1) Δ14CO2 and other relevant isotopologues (e.g. δ13CCH4) from collected air samples to quantify the contribution from fossil fuel combustion and other sources, and (2) geographical separation of individual sources, e.g. agriculture, using a high-density measurement network. Neither of these represents a definitive approach, but they will provide invaluable information about GHG source attribution when they are adopted as part of a more comprehensive, long-term national GHG measurement programme. We also conducted a number of case studies, including an instrumented landfill experiment that provided a test bed for new technologies and flux estimation methods. We anticipate that results from the GAUGE project will help inform other countries on how to use atmospheric data to quantify their nationally determined contributions to the Paris Agreement.