Magnitude and seasonal variation of N2O and CH4 emissions over a mixed agriculture-urban region

Inventory estimates of N2O and CH4 emissions disregard temporal and spatial variabilities, which hinders the search for effective local strategies to lower greenhouse gas emissions. We have quantified the emissions of N2O and CH4 in a mixed agriculture-urban region using two independent approaches, i.e., the vertical gradient method (VGM) and the radon-tracer method (RTM), compared the estimated annual fluxes with the EDGARv6.0 emissions, revealed the seasonal variations of the VGM fluxes, and inferred the sources that most likely cause the seasonal variations based on the footprint analysis even though our methods cannot attribute different sources. We show that the annual RTM estimates represented by the mode of lognormal fit for N2O and CH4 are 0.4 g m−2 yr−1 and 12 g m−2 yr−1, and the VGM estimates are 0.6 ± 0.3 g m−2 yr−1 and 13 ± 4 g m−2 yr−1, respectively. Furthermore, the average EDGARv6.0 emissions constrained by the VGM and the RTM footprints are 1.3 g m−2 yr−1 and 0.9 g m−2 yr−1 for N2O, and 21 g m−2 yr−1 and 18 g m−2 yr−1 for CH4. Compared to our estimated fluxes, EDGARv6.0 N2O and CH4 emissions are both overestimated; for N2O, it is mainly caused by an overestimation of the chemical industry's emission. Moreover, in contrast to EDGARv6.0′s nearly constant monthly emissions throughout the year, the VGM estimates of N2O and CH4 show seasonal variations with relatively high values from March to September, which is most likely caused by agricultural activities. Our study demonstrates that large nighttime vertical gradients of atmospheric N2O and CH4 mole fractions at a tall tower can be used to derive surface fluxes by the VGM; taken together with the RTM fluxes, both the annual means and the temporal variations of N2O and CH4 emissions can be constrained on a regional scale

Magnitude and seasonal variation of N2O and CH4 emissions over a mixed agriculture-urban region

Inventory estimates of N2O and CH4 emissions disregard temporal and spatial variabilities, which hinders the search for effective local strategies to lower greenhouse gas emissions. We have quantified the emissions of N2O and CH4 in a mixed agriculture-urban region using two independent approaches, i.e., the vertical gradient method (VGM) and the radon-tracer method (RTM), compared the estimated annual fluxes with the EDGARv6.0 emissions, revealed the seasonal variations of the VGM fluxes, and inferred the sources that most likely cause the seasonal variations based on the footprint analysis even though our methods cannot attribute different sources. We show that the annual RTM estimates represented by the mode of lognormal fit for N2O and CH4 are 0.4 g m−2 yr−1 and 12 g m−2 yr−1, and the VGM estimates are 0.6 ± 0.3 g m−2 yr−1 and 13 ± 4 g m−2 yr−1, respectively. Furthermore, the average EDGARv6.0 emissions constrained by the VGM and the RTM footprints are 1.3 g m−2 yr−1 and 0.9 g m−2 yr−1 for N2O, and 21 g m−2 yr−1 and 18 g m−2 yr−1 for CH4. Compared to our estimated fluxes, EDGARv6.0 N2O and CH4 emissions are both overestimated; for N2O, it is mainly caused by an overestimation of the chemical industry's emission. Moreover, in contrast to EDGARv6.0′s nearly constant monthly emissions throughout the year, the VGM estimates of N2O and CH4 show seasonal variations with relatively high values from March to September, which is most likely caused by agricultural activities. Our study demonstrates that large nighttime vertical gradients of atmospheric N2O and CH4 mole fractions at a tall tower can be used to derive surface fluxes by the VGM; taken together with the RTM fluxes, both the annual means and the temporal variations of N2O and CH4 emissions can be constrained on a regional scale

Ammonia emissions from a grazed field estimated by miniDOAS measurements and inverse dispersion modelling

Ammonia (NH3) fluxes were estimated from a field being grazed by dairy cattle during spring by applying a backward Lagrangian stochastic model (bLS) model combined with horizontal concentration gradients measured across the field. Continuous concentration measurements at field boundaries were made by open-path miniDOAS (differential optical absorption spectroscopy) instruments while the cattle were present and for 6 subsequent days. The deposition of emitted NH3 to "clean" patches on the field was also simulated, allowing both "net" and "gross" emission estimates, where the dry deposition velocity (vd) was predicted by a canopy resistance (Rc) model developed from local NH3 flux and meteorological measurements. Estimated emissions peaked during grazing and decreased after the cattle had left the field, while control on emissions was observed from covariance with temperature, wind speed and humidity and wetness measurements made on the field, revealing a diurnal emission profile. Large concentration differences were observed between downwind receptors, due to spatially heterogeneous emission patterns. This was likely caused by uneven cattle distribution and a low grazing density, where "hotspots" of emissions would arise as the cattle grouped in certain areas, such as around the water trough. The spatial complexity was accounted for by separating the model source area into sub-sections and optimising individual source area coefficients to measured concentrations. The background concentration was the greatest source of uncertainty, and based on a sensitivity/uncertainty analysis the overall uncertainty associated with derived emission factors from this study is at least 30–40 %

Evaluating the use of an Unmanned Aerial Vehicle (UAV)-based active AirCore system to quantify methane emissions from dairy cows

Enteric fermentation and manure methane emissions from livestock are major anthropogenic greenhouse gas emissions. In general, direct measurements of farm-scale methane emissions are scarce due to the source complexity and the limitations of existing atmospheric sampling methods. Using an innovative UAV-based active AirCore system, we have performed accurate atmospheric measurements of CH4 mole fractions downwind of a dairy cow farm in the Netherlands on four individual days during the period from March 2017 to March 2019. The total CH4 emission rates from the farm were determined using the UAV-based mass balance approach to be 1.1-2.4 g/s. After subtracting estimated emission factors of manure onsite, we derived the enteric emission factors to be 0.20-0.51 kgCH4/AU/d (1 AU = 500 kg animal weight) of dairy cows. We show that the uncertainties of the estimates were dominated by the variabilities in the wind speed and the angle between the wind and the flight transect. Furthermore, nonsimultaneous sampling in the vertical direction of the plume is one of the main limiting factors to achieving accurate estimate of the CH4 emissions from the farm. In addition, a N2O tracer release experiment at the farm was performed when both a UAV and a mobile van were present to simultaneously sample the N2O tracer and the CH4 plumes from the farm, improving the source quantification with a correction factor of 1.04 and 1.22 for the inverse Gaussian approach and for the mass balance approach, respectively. The UAV-based active AirCore system is capable of providing useful estimates of CH4 emissions from dairy cow farms. The uncertainties of the estimates can be improved when combined with accurate measurements of local wind speed and direction or when combined with a tracer approach

Instrument development and application in studies and monitoring of ambient ammonia, Atmos

Abstract During recent years, it has become clear that ammonia is an important gas in relation to di!erent environmental issues, such as acidi"cation, eutrophication, human health and climate change (through particle formation). Therefore, there is a growing need to develop and apply instrumentation suitable for research into emission, dispersion, conversion and deposition of ammonia and ammonium. Recently, several instruments were developed suitable for measuring concentrations in ambient conditions even at very low levels, such as ammonia sensors suitable for monitoring and research, deposition measuring systems and aerosol samplers for on-line measurement of aerosol composition. These instruments have been tested and applied in a number of "eld studies. These studies include dry deposition measurements, ammonium nitrate studies in relation to the (in)direct aerosol e!ect, emission studies and policy evaluation with concentration and deposition monitoring data. The policy evaluation study showed that the measures to reduce ammonia emissions were not as successful as projected beforehand by statistical studies

Studying the spatial variability of methane flux with five eddy covariance towers of varying height

In this study, the spatial representativeness of eddy covariance (EC) methane (CH4) measurements was examined by comparing parallel CH4 fluxes from three short (6 m) towers separated by a few kilometres and from two higher levels (20 m and 60 m) at one location. The measurement campaign was held on an intensively managed grassland on peat soil in the Netherlands. The land use and land cover types are to a large degree homogeneous in the area. The CH4 fluxes exhibited significant variability between the sites on 30-min scale. The spatial coefficient of variation (CVspa) between the three short towers was 56% and it was of similar magnitude as the temporal variability, unlike for the other fluxes (friction velocity, sensible heat flux) for which the temporal variability was considerably larger than the spatial variability. The CVspa decreased with temporal averaging, although less than what could be expected for a purely random process (1/√N), and it was 14% for 26-day means of CH4 flux. This reflects the underlying heterogeneity of CH4 flux in the studied landscape at spatial scales ranging from 1 ha (flux footprint) to 10 km2 (area bounded by the short towers). This heterogeneity should be taken into account when interpreting and comparing EC measurements. On an annual scale, the flux spatial variability contributed up to 50% of the uncertainty in CH4 emissions. It was further tested whether EC flux measurements at higher levels could be used to acquire a more accurate estimate of the spatially integrated CH4 emissions. Contrarily to what was expected, flux intensity was found to both increase and decrease depending on measurement height. Using footprint modelling, 56% of the variation between 6 m and 60 m CH4 fluxes was attributed to emissions from local anthropogenic hotspots (farms). Furthermore, morning hours proved to be demanding for the tall tower EC where fluxes at 60 m were up to four-fold those at lower heights. These differences were connected with the onset of convective mixing during the morning period.Peer reviewe

Methane flux measurements on multiple scales in an agricultural landscape: linking tall tower flux measurements with short eddy covariance towers

Agricultural landscapes exhibit spatially and temporally complex methane (CH4) fluxes: emissions originate from strong point sources, such as ruminants and cowsheds, and from fertilisation of fields, which adds short-term peaks in the methane flux to the atmosphere [1]. Furthermore, in some locations, such as the study site, these sources are overlaid on a CH4 flux originating from underlying peaty soils and drainage ditches between the fields [2]. In order to account for all these different sources, the CH4 fluxes need to be monitored continuously with a system that integrates the fluxes over a large area, providing the effective flux of CH4 from the landscape (~1 km2) to the atmosphere. Traditionally eddy covariance (EC) method has been used to obtain the ecosystem scale (~ 1 ha) fluxes of various compounds. However, it is questionable whether EC fluxes at one location can capture the high variability of CH4 fluxes in an agricultural landscape. To test this, methane exchange was measured at three locations with short (6.5 m high) EC towers a few kilometres apart from each other and at two heights (20 m and 60 m) in one tall tower. Additionally, it is assessed whether the short tower fluxes can be upscaled to match the CH4 fluxes measured at the tall tower using footprint modelling. The measurement campaign was held between the 1st and 25th of July 2012 in the vicinity of the Cabauw Experimental Site for Atmospheric Research (CESAR) (51°58’12.00”N, 4°55’34.48”E), which is located in the Netherlands. The landscape is an intensively managed agricultural area, with soil consisting of peat, topped by an approximately 1 meter thick bed of clay. Tentative results show large variability in CH4 fluxes between the three short tower sites: cumulative CH4 fluxes over a 10-day-period range from 188 mg(CH4) m-2 to 306 mg(CH4) m-2. Tall tower CH4 fluxes from the same period summed up to 275 mg(CH4) m-2 (20 m height) and 430 mg(CH4) m-2 (60 m height). High fluxes at 60 m height could be explained by cowsheds within the footprint, whereas systems located closer to the ground did not detect the hotspot emissions from the cowsheds. The presentation will discuss CH4 flux variability in an agricultural landscape, issues related to upscaling flux measurements and the usability of EC CH4 flux measurements at tall towers for estimating landscape scale exchange of methane. [1] P.S. Kroon et al., 2007, Biogeosciences, 4, 715-728. [2] A.P. Schrier-Uijl et al., 2010, Plant Soil, 329, 509-520

Evaluating the performance of commonly used gas analysers for methane eddy covariance flux measurements: the InGOS inter-comparison field experiment

The performance of eight fast-response methane (CH4) gas analysers suitable for eddy covariance flux measurements were tested at a grassland site near the Cabauw tall tower (Netherlands) during June 2012. The instruments were positioned close to each other in order to minimise the effect of varying turbulent conditions. The moderate CH4 fluxes observed at the location, of the order of 25 nmol m−2 s−1, provided a suitable signal for testing the instruments' performance. Generally, all analysers tested were able to quantify the concentration fluctuations at the frequency range relevant for turbulent exchange and were able to deliver high-quality data. The tested cavity ringdown spectrometer (CRDS) instruments from Picarro, models G2311-f and G1301-f, were superior to other CH4 analysers with respect to instrumental noise. As an open-path instrument susceptible to the effects of rain, the LI-COR LI-7700 achieved lower data coverage and also required larger density corrections; however, the system is especially useful for remote sites that are restricted in power availability. In this study the open-path LI-7700 results were compromised due to a data acquisition problem in our data-logging setup. Some of the older closed-path analysers tested do not measure H2O concentrations alongside CH4 (i.e. FMA1 and DLT-100 by Los Gatos Research) and this complicates data processing since the required corrections for dilution and spectroscopic interactions have to be based on external information. To overcome this issue, we used H2O mole fractions measured by other gas analysers, adjusted them with different methods and then applied them to correct the CH4 fluxes. Following this procedure we estimated a bias of the order of 0.1 g (CH4) m−2 (8% of the measured mean flux) in the processed and corrected CH4 fluxes on a monthly scale due to missing H2O concentration measurements. Finally, cumulative CH4 fluxes over 14 days from three closed-path gas analysers, G2311-f (Picarro Inc.), FGGA (Los Gatos Research) and FMA2 (Los Gatos Research), which were measuring H2O concentrations in addition to CH4, agreed within 3% (355–367 mg (CH4) m−2) and were not clearly different from each other, whereas the other instruments derived total fluxes which showed small but distinct differences (±10%, 330–399 mg (CH4) m−2).Peer reviewe

Quantifying nitrogen fluxes and their influence on the greenhouse gas balance: recent findings of the NitroEurope Integrated Project

The generation of reactive nitrogen (Nr) by human activities to stimulate agricultural productivity and the unintended formation of Nr in combustion processes both have major impacts on the global environment. Effects of excess Nr include the deterioration of air quality, water quality, soil quality and a decline in biodiversity. One of the most controversial impacts of nitrogen, however, is on the greenhouse gas balance. While recent papers have highlighted a possible benefit of nitrogen in enhancing rates of carbon sequestration, there remain many trade-offs between nitrogen and greenhouse gas exchange. The result is that the net effect of Nr on the global radiative balance has yet to be fully quantified. To better understand these relationships requires intense measurement and modelling of Nr fluxes at various temporal and spatial scales in order to make the link between different nitrogen forms and their fate in the environment. It is essential to measure fluxes for a wide range of ecosystems considering the biosphere-atmosphere exchange of the Nr components and greenhouse gases, as well as the fixation of di-nitrogen and its creation by denitrification. Long-term observations are needed for representative ecosystems, together with results from experiments addressing the responses of the key nitrogen and greenhouse gas fluxes to different global change drivers. The NitroEurope Integrated Project (in short NEU IP), funded under the 6th Framework Programme of the European Commission, has developed and applied a strategy for quantifying these different terms on multiple scales. With the project nearing completion, this presentation reports selected preliminary findings. It highlights the first estimates of Nr inputs and net green-house gas exchange for a series of 13 flux ‘supersites’, complemented by the emerging results of Nr concentrations and related N inputs at a network of 58 ‘inferential sites’, which extend the European representativity of the results. In addition, new low cost methods to measure nitrogen fluxes will be reported, which have been extensively tested at those sites. Results from this 3-tier flux network are underpinned by emerging findings from an extensive network of manipulation sites. A combination of modelling at plot, landscape and European scales is used to upscale the results. Finally the talk will illustrate how nitrogen mitigation techniques are being considered at the European scale, including an estimation of the scale of costs involved in simultaneously mitigating nitrous oxide, ammonia and nitrate losse