Analysis of UK and European NOx and VOC emission scenarios in the Defra model intercomparison exercise

This is a PDF file of an unedited manuscript that has been accepted for publication. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertainSimple emission scenarios have been implemented in eight United Kingdom air quality models with the aim of assessing how these models compared when addressing whether photochemical ozone formation in southern England was NOx- or VOC-sensitive and whether ozone precursor sources in the UK or in the Rest of Europe (RoE) were the most important during July 2006. The suite of models included three Eulerian-grid models (three implementations of one of these models), a Lagrangian atmospheric dispersion model and two moving box air parcel models. The assignments as to NOx- or VOC-sensitive and to UK- versus RoE-dominant, turned out to be highly variable and often contradictory between the individual models. However, when the assignments were filtered by model performance on each day, many of the contradictions could be eliminated. Nevertheless, no one model was found to be the 'best' model on all days, indicating that no single air quality model could currently be relied upon to inform policymakers robustly in terms of NOx- versus VOC-sensitivity and UK- versus RoE-dominance on each day. It is important to maintain a diversity in model approaches.Peer reviewedFinal Accepted Versio

A comparison of atmospheric dispersion model predictions with observations of SO2 and sulphate aerosol from volcanic eruptions

The UK Met Office's Numerical Atmospheric-dispersion Modeling Environment (NAME) is used both operationally and for research investigations. It has previously been used to model volcanic ash at the London Volcanic Ash Advisory Centre (VAAC), including that from the eruptions in Iceland of Eyjafjallajökull in 2010 and Grímsvtn in 2011. In this paper, the ability of NAME to model the release and dispersion of volcanic SO2, the chemical processes leading to the production of sulphate aerosol, and the subsequent dispersion of sulphate aerosol, has been investigated. Sensitivity tests were carried out to investigate the suitability of the NAME chemistry scheme for use in both the troposphere and the stratosphere. The eruptions of Sarychev in 2009, Kasatochi in 2008 and Eyjafjallajökull in 2010 were simulated and results for SO2 column density and sulphate aerosol optical depth (AOD) were compared with satellite retrievals. NAME results compare favorably with available observations in terms of both geographical distribution and magnitude for all three cases. The NAME modeled values of SO2 show a correlation of 0.8 with the corresponding observations for Sarychev. Ninety percent of modeled values of northern hemisphere averaged sulphate AOD are within a factor of 2 of those observed for Kasatochi and 71% are within a factor of 2 of those observed for Sarychev. Although significant uncertainties are present in both the model and observations, this work demonstrates that NAME's current chemistry scheme shows promise as a tool for modeling SO2 and sulphate from volcanoes. © 2012 by the American Geophysical Union.SCOPUS: ar.jinfo:eu-repo/semantics/publishe

Western European emission estimates of CFC-11, CFC-12 and CCl4 derived from atmospheric measurements from 2008 to 2021

Abstract. Production and consumption of CFC-11 (trichlorofluoromethane, CCl3F), CFC-12 (dichlorodifluoromethane, CCl2F2) and CCl4 (carbon tetrachloride) are controlled under the regulations of the Montreal Protocol and have been phased out globally since 2010. Only CCl4 is still widely produced as a chemical feedstock. After 2010, emissions of CFC-11 and CFC-12 should therefore mostly originate from existing banks (e.g. from foams, mobile air conditioning units and refrigerators); however evidence has emerged of an increase in global emissions of CFC-11 in the last decade, some of which has not been fully accounted for. The motivation for this work was to assess the emissions of CFC-11, CFC-12 and CCl4 from western Europe. All countries in this region have been subject to the controls of the Montreal Protocol since the late 1980s and, as non-Article 5 Parties, have been prohibited from producing CFCs and CCl4 for dispersive use since 1996. Four different inverse modelling systems are used to estimate emissions of these gases from 2008 to 2021 using data from four atmospheric measurement stations: Mace Head (Ireland), Jungfraujoch (Switzerland), Monte Cimone (Italy) and Tacolneston (UK). The average of the four model studies found that western European emissions of CFC-11, CFC-12 and CCl4 between 2008 and 2021 were declining at 3.5 % yr−1 (2.7 % yr−1–4.8 % yr−1), 7.7 % yr−1 (6.3 % yr−1–8.0 % yr−1) and 4.4 % yr−1 (2.6 % yr−1–6.4 % yr−1), respectively. Even though the emissions were declining throughout the period, the area including northern France, Belgium, the Netherlands and Luxembourg showed consistently elevated emissions of CFC-11 compared with the surrounding regions. Emissions of CFC-12 were slightly elevated in the same region. CCl4 emissions were the highest in the south of France. France had the highest emissions of all three gases over the period 2008–2021. Emissions from western Europe (2008–2021) were on average 2.4 ± 0.4 Gg (CFC-11), 1.3 ± 0.3 Gg (CFC-12) and 0.9 ± 0.2 Gg (CCl4). Our estimated decline in emissions of CFC-11 is consistent with a western European bank release rate of 3.4 % (2.6 %–4.5 %). This study concludes that emissions of CFC-11, CFC-12 and CCl4 have all declined from 2008 to 2021 in western Europe. Therefore, no evidence is found that western European emissions contributed to the unexplained part of the global increase in atmospheric concentrations of CFC-11 observed in the last decade

Western European emission estimates of CFC-11, CFC-12 and CCl4 derived from atmospheric measurements 2008 to 2021

Production and consumption of CFC-11 (trichlorofluoromethane, CCl3F), CFC-12 (dichlorodifluoromethane, CCl2F2) and CCl4 (carbon tetrachloride) are controlled under the regulations of the Montreal Protocol and have been phased out globally since 2010. Only CCl4 is still widely produced as a chemical feedstock. After 2010, emissions of CFC-11 and CFC-12 should therefore mostly originate from existing banks (e.g. from foams, mobile air conditioning units and refrigerators); however evidence has emerged of an increase in global emissions of CFC-11 in the last decade, some of which has not been fully accounted for. The motivation for this work was to assess the emissions of CFC-11, CFC-12 and CCl4 from western Europe. All countries in this region have been subject to the controls of the Montreal Protocol since the late 1980s and, as non-Article 5 Parties, have been prohibited from producing CFCs and CCl4 for dispersive use since 1996. Four different inverse modelling systems are used to estimate emissions of these gases from 2008 to 2021 using data from four atmospheric measurement stations: Mace Head (Ireland), Jungfraujoch (Switzerland), Monte Cimone (Italy) and Tacolneston (UK). The average of the four model studies found that western European emissions of CFC-11, CFC-12 and CCl4 between 2008 and 2021 were declining at 3.5 % yr−1 (2.7 % yr−1–4.8 % yr−1), 7.7 % yr−1 (6.3 % yr−1–8.0 % yr−1) and 4.4 % yr−1 (2.6 % yr−1–6.4 % yr−1), respectively. Even though the emissions were declining throughout the period, the area including northern France, Belgium, the Netherlands and Luxembourg showed consistently elevated emissions of CFC-11 compared with the surrounding regions. Emissions of CFC-12 were slightly elevated in the same region. CCl4 emissions were the highest in the south of France. France had the highest emissions of all three gases over the period 2008–2021. Emissions from western Europe (2008–2021) were on average 2.4 ± 0.4 Gg (CFC-11), 1.3 ± 0.3 Gg (CFC-12) and 0.9 ± 0.2 Gg (CCl4). Our estimated decline in emissions of CFC-11 is consistent with a western European bank release rate of 3.4 % (2.6 %–4.5 %). This study concludes that emissions of CFC-11, CFC-12 and CCl4 have all declined from 2008 to 2021 in western Europe. Therefore, no evidence is found that western European emissions contributed to the unexplained part of the global increase in atmospheric concentrations of CFC-11 observed in the last decade