Potential impacts of emissions associated with unconventional hydrocarbon extraction on UK air quality and human health

Here we report the first results of model sensitivity simulations to assess the potential impacts of emissions related to future activities linked to unconventional hydrocarbon extraction (fracking) in the UK on air pollution and human health. These simulations were performed with the Met Office Air Quality in the Unified Model, a new air quality forecasting model, and included a wide range of extra emissions of volatile organic compounds (VOCs) and nitrogen oxides (NOx) to reflect emissions from the full life-cycle of fracking related activities and simulate the impacts of these compounds on levels of nitrogen-dioxide (NO2) and ozone (O3). These model simulations highlight that increases in NOx and VOC emissions associated with unconventional hydrocarbon extraction could lead to large local increases in the monthly means of daily 1-hourly maximum NO2 of up to +30 ppb and decreases in the maximum daily 8-hourly mean O3 up to -6 ppb in the summertime. Broadly speaking, our simulations indicate increases in both of these compounds across the UK air shed throughout the year. Changes in the 1-hourly maximum of NO2 and 8-hourly mean of O3 are particularly important for their human health impacts. These respective changes in NO2 and O3 would contribute to approximately 110 (range 50-530) extra premature-deaths a year across the UK based on the use of recently reported concentration response functions for changes in annual average NO2 and O3 exposure. As such we conclude that the release of emissions of VOCs and NOx be highly controlled to prevent deleterious health impacts

On the Changing Role of the Stratosphere on the Tropospheric Ozone Budget: 1979–2010

We study the evolution of tropospheric ozone over the period 1979-2010 using a chemistry-climate model employing a stratosphere-troposphere chemistry scheme. By running with specified dynamics, the key feedback of composition on meteorology is suppressed, isolating the chemical response. By using historical forcings and emissions, interactions between processes are realistically represented. We use the model to assess how the ozone responds over time and to investigate model responses and trends. We find that the CFC-driven decrease in stratospheric ozone plays a significant role in the tropospheric ozone burden. Over the period 1979-1994, the decline in transport of ozone from the stratosphere, partially offsets an emissions-driven increase in tropospheric ozone production. From 1994-2010, despite a levelling off in emissions increased stratosphere-to-troposphere transport of ozone drives a small increase in the tropospheric ozone burden. These results have implications for the impact of future stratospheric ozone recovery on air quality and radiative forcing.European Community’s Seventh Framework Programme 10 (FP7/2007-2013) under grant agreement no. 603557 (StratoClim)

Atlantic multidecadal variability and the U.K. acsis program

Abstract Atlantic multidecadal variability (AMV) is the term used to describe the pattern of variability in North Atlantic sea surface temperatures (SSTs) that is characterized by decades of basinwide warm or cool anomalies, relative to the global mean. AMV has been associated with numerous climate impacts in many regions of the world including decadal variations in temperature and rainfall patterns, hurricane activity, and sea level changes. Given its importance, understanding the physical processes that drive AMV and the extent to which its evolution is predictable is a key challenge in climate science. A leading hypothesis is that natural variations in ocean circulation control changes in ocean heat content and consequently AMV phases. However, this view has been challenged recently by claims that changing natural and anthropogenic radiative forcings are critical drivers of AMV. Others have argued that changes in ocean circulation are not required. Here, we review the leading hypotheses and mechanisms for AMV and discuss the key debates. In particular, we highlight the need for a holistic understanding of AMV. This perspective is a key motivation for a major new U.K. research program: the North Atlantic Climate System Integrated Study (ACSIS), which brings together seven of the United Kingdom’s leading environmental research institutes to enable a broad spectrum approach to the challenges of AMV. ACSIS will deliver the first fully integrated assessment of recent decadal changes in the North Atlantic, will investigate the attribution of these changes to their proximal and ultimate causes, and will assess the potential to predict future changes.</jats:p

Long-term high frequency measurements of ethane, benzene and methyl chloride at Ragged Point, Barbados: Identification of long-range transport events

Abstract Here we present high frequency long-term observations of ethane, benzene and methyl chloride from the AGAGE Ragged Point, Barbados, monitoring station made using a custom built GC-MS system. Our analysis focuses on the first three years of data (2005–2007) and on the interpretation of periodic episodes of high concentrations of these compounds. We focus specifically on an exemplar episode during September 2007 to assess if these measurements are impacted by long-range transport of biomass burning and biogenic emissions. We use the Lagrangian Particle Dispersion model, NAME, run forwards and backwards in time to identify transport of air masses from the North East of Brazil during these events. To assess whether biomass burning was the cause we used hot spots detected using the MODIS instrument to act as point sources for simulating the release of biomass burning plumes. Excellent agreement for the arrival time of the simulated biomass burning plumes and the observations of enhancements in the trace gases indicates that biomass burning strongly influenced these measurements. These modelling data were then used to determine the emissions required to match the observations and compared with bottom up estimates based on burnt area and literature emission factors. Good agreement was found between the two techniques highlight the important role of biomass burning. The modelling constrained by in situ observations suggests that the emission factors were representative of their known upper limits, with the in situ data suggesting slightly greater emissions of ethane than the literature emission factors account for. Further analysis was performed concluding only a small role for biogenic emissions of methyl chloride from South America impacting measurements at Ragged Point. These results highlight the importance of long-term high frequency measurements of NMHC and ODS and highlight how these data can be used to determine sources of emissions 1000’s km away.ATA would like to thank the GWR and the Met Office for the PhD funding that was useful in the initiation of this research and the Herchel Smith foundation for a Postdoctoral fellowship, and NCAS for funding. The operation of the AGAGE station at Ragged Point is supported by the National Aeronautic and Space Administration (NASA, USA) (grants NNX07AE89G and NNX11AF17G to MIT) and the National Oceanic and Atmospheric Administration (NOAA, USA) (contract RA133R09CN0062).This is the final version of the article. It first appeared from BioOne via http://dx.doi.org/10.12952/journal.elementa.00006

Detection and identification of Criegee intermediates from the ozonolysis of biogenic and anthropogenic VOCs: comparison between experimental measurements and theoretical calculations

Ozonolysis of alkenes is a key reaction in the atmosphere, playing an important role in determining the oxidising capacity of the atmosphere and acting as a source of compounds that can contribute to local photochemical “smog”. The reaction products of the initial step of alkene-ozonolysis are Criegee intermediates (CIs), which have for many decades eluded direct experimental detection because of their very short lifetime. We use an innovative experimental technique, stabilisation of CIs with spin traps and analysis with proton transfer reaction mass spectrometry, to measure the gas phase concentration of a series of CIs formed from ozonolysis of a range of both biogenic and anthropogenic alkenes in flow tube experiments. Density functional theory (DFT) calculations were used to assess the stability of the CI-spin trap adducts and showed that the reaction of the investigated CIs with the spin trap occurs very rapidly except for the large β-pinene CI. Our measurement method was used successfully to measure all the expected CIs, emphasising that this new technique is applicable to a wide range of CIs with different molecular structures previously unidentified experimentally. In addition, for the first time it was possible to study CIs simultaneously in an even more complex reaction system consisting of more than one olefinic precursor. Comparison between our new experimental measurements, calculations of stability of the CI-spin trap adducts and results from numerical modelling, using the master chemical mechanism (MCM), showed that our new method can be used for quantification of CIs produced in situ in laboratory experiments.This work was funded by the European Research Council (ERC starting grant 279405) and NERC (NE/K008218/1). ATA thanks NERC for funding through NCAS

Description and Evaluation of the specified-dynamics experiment in the Chemistry-Climate Model Initiative

We provide an overview of the REF-C1SD specified-dynamics experiment that was conducted as part of phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly nudged general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and are evaluated in terms of how well they represent different measures of the dynamical and transport circulations. In the troposphere there are large (∼40 %) differences in the climatological mean distributions, seasonal cycle amplitude, and trends of the meridional and vertical winds. In the stratosphere there are similarly large (∼50 %) differences in the magnitude, trends and seasonal cycle amplitude of the transformed Eulerian mean circulation and among various chemical and idealized tracers. At the same time, interannual variations in nearly all quantities are very well represented, compared to the underlying reanalyses. We show that the differences in magnitude, trends and seasonal cycle are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. In most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models, which are also shown to be more dynamically consistent. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition

Lightning NOx, a key chemistry-climate interaction: impacts of future climate change and consequences for tropospheric oxidising capacity

Lightning is one of the major natural sources of NOx in the atmosphere. A suite of time slice experiments using a stratosphere-resolving configuration of the Unified Model (UM), containing the United Kingdom Chemistry and Aerosols sub-model (UKCA), has been performed to investigate the impact of climate change on emissions of NOx from lightning (LNOx) and to highlight its critical impacts on photochemical ozone production and the oxidising capacity of the troposphere. Two Representative Concentration Pathway (RCP) scenarios (RCP4.5 and RCP8.5) are explored. LNOx is simulated to increase in a year-2100 climate by 33% (RCP4.5) and 78% (RCP8.5), primarily as a result of increases in the depth of convection. The total tropospheric chemical odd oxygen production (P(Ox)) increases linearly with increases in total LNOx and consequently, tropospheric ozone burdens of 29 ± 4 Tg(O3) (RCP4.5) and 46 ± 4 Tg(O3) (RCP8.5) are calculated here. By prescribing a uniform surface boundary concentration for methane in these simulations, methane-driven feedbacks are essentially neglected. A simple estimate of the contribution of the feedback reduces the increase in ozone burden to 24 and 33 Tg(O3), respectively. We thus show that, through changes in LNOx, the effects of climate change counteract the simulated mitigation of the ozone burden, which results from reductions in ozone precursor emissions as part of air quality controls projected in the RCP scenarios. Without the driver of increased LNOx, our simulations suggest that the net effect of climate change would be to lower free tropospheric ozone. In addition, we identify large climate-change-induced enhancements in the concentration of the hydroxyl radical (OH) in the tropical upper troposphere (UT), particularly over the Maritime Continent, primarily as a consequence of greater LNOx. The OH enhancement in the tropics increases oxidation of both methane (with feedbacks onto chemistry and climate) and very short-lived substances (VSLS) (with implications for stratospheric ozone depletion). We emphasise that it is important to improve our understanding of LNOx in order to gain confidence in model projections of composition change under future climate

Chemistry-driven changes strongly influence climate forcing from vegetation emissions

Biogenic volatile organic compounds (BVOCs) affect climate via changes to aerosols, aerosol-cloud interactions (ACI), ozone and methane. BVOCs exhibit dependence on climate (causing a feedback) and land use but there remains uncertainty in their net climatic impact. One factor is the description of BVOC chemistry. Here, using the earth-system model UKESM1, we quantify chemistry’s influence by comparing the response to doubling BVOC emissions in the pre-industrial with standard and state-of-science chemistry. The net forcing (feedback) is positive: ozone and methane increases and ACI changes outweigh enhanced aerosol scattering. Contrary to prior studies, the ACI response is driven by cloud droplet number concentration (CDNC) reductions from suppression of gas-phase SO2 oxidation. With state-of-science chemistry the feedback is 43% smaller as lower oxidant depletion yields smaller methane increases and CDNC decreases. This illustrates chemistry’s significant influence on BVOC’s climatic impact and the more complex pathways by which BVOCs influence climate than currently recognised

Projected changes in seasonal and extreme summertime temperature and precipitation in India in response to COVID-19 recovery emissions scenarios

Funder: Cambridge STEAM InitiativeFunder: Centre for Environmental Data Analysis, Science and Technology Facilities CouncilFunder: Harvard Global Institute; doi: http://dx.doi.org/10.13039/100016486Abstract Fossil fuel and aerosol emissions have played important roles on climate over the Indian subcontinent over the last century. As the world transitions toward decarbonization in the next few decades, emissions pathways could have major impacts on India’s climate and people. Pathways for future emissions are highly uncertain, particularly at present as countries recover from COVID-19. This paper explores a multimodel ensemble of Earth system models leveraging potential global emissions pathways following COVID-19 and the consequences for India’s summertime (June–July–August–September) climate in the near- and long-term. We investigate specifically scenarios which envisage a fossil-based recovery, a strong renewable-based recovery and a moderate scenario in between the two. We find that near-term climate changes are dominated by natural climate variability, and thus likely independent of the emissions pathway. By 2050, pathway-induced spatial patterns in the seasonally-aggregated precipitation become clearer with a slight drying in the fossil-based scenario and wetting in the strong renewable scenario. Additionally, extreme temperature and precipitation events in India are expected to increase in magnitude and frequency regardless of the emissions scenario, though the spatial patterns of these changes as well as the extent of the change are pathway dependent. This study provides an important discussion on the impacts of emissions recover pathways following COVID-19 on India, a nation which is likely to be particularly susceptible to climate change over the coming decades.</jats:p

Cloud impacts on photochemistry: Building a climatology of photolysis rates from the Atmospheric Tomography mission

Abstract. Measurements from actinic flux spectroradiometers on board the NASA DC-8 during the Atmospheric Tomography (ATom) mission provide an extensive set of statistics on how clouds alter photolysis rates (J values) throughout the remote Pacific and Atlantic Ocean basins. J values control tropospheric ozone and methane abundances, and thus clouds have been included for more than three decades in tropospheric chemistry modeling. ATom made four profiling circumnavigations of the troposphere capturing each of the seasons during 2016–2018. This work examines J values from the Pacific Ocean flights of the first deployment, but publishes the complete Atom-1 data set (29 July to 23 August 2016). We compare the observed J values (every 3 s along flight track) with those calculated by nine global chemistry–climate/transport models (globally gridded, hourly, for a mid-August day). To compare these disparate data sets, we build a commensurate statistical picture of the impact of clouds on J values using the ratio of J-cloudy (standard, sometimes cloudy conditions) to J-clear (artificially cleared of clouds). The range of modeled cloud effects is inconsistently large but they fall into two distinct classes: (1) models with large cloud effects showing mostly enhanced J values aloft and or diminished at the surface and (2) models with small effects having nearly clear-sky J values much of the time. The ATom-1 measurements generally favor large cloud effects but are not precise or robust enough to point out the best cloud-modeling approach. The models here have resolutions of 50–200 km and thus reduce the occurrence of clear sky when averaging over grid cells. In situ measurements also average scattered sunlight over a mixed cloud field, but only out to scales of tens of kilometers. A primary uncertainty remains in the role of clouds in chemistry, in particular, how models average over cloud fields, and how such averages can simulate measurements. NERC ACSIS LTSM projec