UK greenhouse gas measurements at two new tall towers for aiding emissions verification

Abstract. Under the UK focused Greenhouse gAs and Uk and Global Emissions (GAUGE) project, two new tall tower greenhouse gas (GHG) observation sites were established in the 2013/2014 Northern Hemispheric winter. These sites were located at two existing telecommunications towers, Heathfield (HFD) and Bilsdale (BSD), utilised a combination of cavity ring-down spectroscopy (CRDS) and gas chromatography (GC) to measure key GHGs (CO2, CH4, CO, N2O and SF6). Measurements were made at multiple intake heights on each tower. The inclusion of the two additional tower stations within the existing UK Deriving Emissions linked to Climate Change (DECC) network of four stations was found to reduce the uncertainty of CH4 UK emission estimates by between 10–20 %. CO2 and CH4 dry mole fractions were calculated from either CRDS measurements of wet air which were post corrected with an instrument specific empirical correction or samples dried to between 0.05 and 0.3 % H2O using a Nafion dryer, with a smaller correction applied for the residual H2O. The impact of these two drying strategies was examined. Drying with a Nafion drier was not found to have a significant effect on the observed CH4 mole fraction; however, Nafion drying did cause a 0.02 µmol mol−1 CO2 bias. This bias was stable with sample CO2 mole fractions between 373 and 514 µmol mol−1 and for sample H2O up to 3.5 %. As the calibration and standard gases are treated in the same manner, this error is mostly calibrated out with the residual error below the World Meteorological Organization’s (WMO) reproducibility requirements. Of more concern was the error associated with both default factory and empirical instrument specific water correction algorithms. These corrections are relatively stable and reproducible for samples with H2O between 0.2 and 2.5 %, CO2 between 345 and 449 µmol mol−1 and CH4 between 1743 and 2145 nmol mol−1. However, the residual errors in these corrections increase to &gt; 0.05 µmol mol−1 for CO2 and &gt; 1 nmol mol−1 for CH4 (greater than the WMO internal reproducibility guidelines) at higher humidities and for samples with very low ( </jats:p

Inter-model comparison of global hydroxyl radical (OH) distributions and their impact on atmospheric methane over the 2000–2016 period

The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolving discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields was analyzed and aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz (Laboratoire de Meteorologie Dynamique) with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8:7*10^5 and 12:8*10^5 molec cm-3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and volatile organic compound (VOC) chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0:3*10^5 molec cm-3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in the CH4 mixing ratio in 2010, which represents 7%–20% of the model-simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of > 30 ppbv. Over the full 2000–2016 time period, using a common stateof- the-art but nonoptimized emission scenario, the impact of [OH] changes tested here can explain up to 54% of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions

Quantifying the UK's carbon dioxide flux: An atmospheric inverse modelling approach using a regional measurement network

We present a method to derive atmosphericobservation-based estimates of carbon dioxide (CO 2 ) fluxes at the national scale, demonstrated using data from a network of surface tall-tower sites across the UK and Ireland over the period 2013-2014. The inversion is carried out using simulations from a Lagrangian chemical transport model and an innovative hierarchical Bayesian Markov chain Monte Carlo (MCMC) framework, which addresses some of the traditional problems faced by inverse modelling studies, such as subjectivity in the specification of model and prior uncertainties. Biospheric fluxes related to gross primary productivity and terrestrial ecosystem respiration are solved separately in the inversion and then combined a posteriori to determine net ecosystem exchange of CO 2 . Two different models, Data Assimilation Linked Ecosystem Carbon (DALEC) and Joint UK Land Environment Simulator (JULES), provide prior estimates for these fluxes. We carry out separate inversions to assess the impact of these different priors on the posterior flux estimates and evaluate the differences between the prior and posterior estimates in terms of missing model components. The Numerical Atmospheric dispersion Modelling Environment (NAME) is used to relate fluxes to the measurements taken across the regional network. Posterior CO2 estimates from the two inversions agree within estimated uncertainties, despite large differences in the prior fluxes from the different models. With our method, averaging results from 2013 and 2014, we find a total annual net biospheric flux for the UK of 8±79 TgCO 2 yr -1 (DALEC prior) and 64±85 TgCO 2 yr -1 (JULES prior), where negative values represent an uptake of CO 2 . These biospheric CO 2 estimates show that annual UK biospheric sources and sinks are roughly in balance. These annual mean estimates consistently indicate a greater net release of CO 2 than the prior estimates, which show much more pronounced uptake in summer months

The global methane budget 2000–2017

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30∘ N) compared to mid-latitudes (∼ 30 %, 30–60∘ N) and high northern latitudes (∼ 4 %, 60–90∘ N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4 yr−1 by 8 Tg CH4 yr−1, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning

Development and application of a system for the analysis of atmospheric, water and sediment nitrogen and carbon

Eutrophication and climate change, key environmental concerns, are both linked to the carbon and nitrogen cycles hence the improved understanding of these cycles is essential. Currently, there is no system that simultaneously measures the fluxes of the three key gas phase products of nitrogen and carbon cycling (CO2, CH4 and N2O) in submerged ecosystems with hourly time resolution. A “Lake-in-a-box” (mesocosm) was developed in the laboratory which allowed the monitoring of key components of the carbon and nitrogen cycles within the air, water and sediments. The approach is automated, simple and time efficient and novel in its ability to examine many different carbon and nitrogen compounds in all three physical component of the “lake”. Dramatic fluctuations in gaseous flux and the concentrations of overlying water and sedimentary carbon and nitrogen compounds were noted over a three week period. These were split into five distinct phases which were linked to changes in sedimentary N and C cycling. The results highlighted the important of links between the two cycles and supported recent studies showing that estuarine sediments can act as both a source and a sink of nitrogen

Increasing anthropogenic methane emissions arise equally from agricultural and fossil fuel sources

International audienc

Regional trends and drivers of the global methane budget.

The ongoing development of the Global Carbon Project (GCP) global methane (CH4 ) budget shows a continuation of increasing CH4 emissions and CH4 accumulation in the atmosphere during 2000-2017. Here, we decompose the global budget into 19 regions (18&nbsp;land and 1 oceanic) and five key source sectors to spatially attribute the observed global trends. A comparison of top-down (TD) (atmospheric and transport model-based) and bottom-up (BU) (inventory- and process model-based) CH4 emission estimates demonstrates robust temporal trends with CH4 emissions increasing in 16 of the 19 regions. Five regions-China, Southeast Asia, USA, South Asia, and Brazil-account for &gt;40% of the global total emissions (their anthropogenic and natural sources together totaling &gt;270&nbsp;Tg CH4 &nbsp;yr-1 in 2008-2017). Two of these regions, China and South Asia, emit predominantly anthropogenic emissions (&gt;75%) and together emit more than 25% of global anthropogenic emissions. China and the Middle East show the largest increases in total emission rates over the 2000 to 2017 period with regional emissions increasing by &gt;20%. In contrast, Europe and Korea and Japan show a steady decline in CH4 emission rates, with total emissions decreasing by ~10% between 2000 and 2017. Coal mining, waste (predominantly solid waste disposal) and livestock (especially enteric fermentation) are dominant drivers of observed emissions increases while declines appear driven by a combination of waste and fossil emission reductions. As such, together these sectors present the greatest risks of further increasing the atmospheric CH4 burden and the greatest opportunities for greenhouse gas abatement