scholarly journals Inverse modelling of CF<sub>4</sub> and NF<sub>3</sub> emissions in East Asia

2018 ◽  
Vol 18 (18) ◽  
pp. 13305-13320 ◽  
Author(s):  
Tim Arnold ◽  
Alistair J. Manning ◽  
Jooil Kim ◽  
Shanlan Li ◽  
Helen Webster ◽  
...  

Abstract. Decadal trends in the atmospheric abundances of carbon tetrafluoride (CF4) and nitrogen trifluoride (NF3) have been well characterised and have provided a time series of global total emissions. Information on locations of emissions contributing to the global total, however, is currently poor. We use a unique set of measurements between 2008 and 2015 from the Gosan station, Jeju Island, South Korea (part of the Advanced Global Atmospheric Gases Experiment network), together with an atmospheric transport model, to make spatially disaggregated emission estimates of these gases in East Asia. Due to the poor availability of good prior information for this study, our emission estimates are largely influenced by the atmospheric measurements. Notably, we are able to highlight emission hotspots of NF3 and CF4 in South Korea due to the measurement location. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.3±2.7 and 0.36±0.11 Gg yr−1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6±0.07 Gg yr−1 in 2015, which equates to ∼1.6 % of the country's CO2 emissions. We also apply our method to calculate emissions of CHF3 (HFC-23) between 2008 and 2012, for which our results find good agreement with other studies and which helps support our choice in methodology for CF4 and NF3.

2018 ◽  
Author(s):  
Tim Arnold ◽  
Alistair Manning ◽  
Jooil Kim ◽  
Shanlan Li ◽  
Helen Webster ◽  
...  

Abstract. Well mixed abundances and decadal trends of carbon tetrafluoride (CF4) and nitrogen trifluoride (NF3) have been well characterised and have provided a time series of global total emissions. Information on locations of emissions contributing to the global total, however, is currently poor. We use a unique set of measurements between 2008 and 2015 from the Gosan station, Jeju Island, South Korea (part of the Advanced Global Atmospheric Gases Experiment network), together with an atmospheric transport model to make spatially disaggregated emission estimates of these gases in East Asia. Owing to the poor availability of good prior information for this study our results are strongly constrained by the atmospheric measurements. Notably, we are able to highlight emissions hotspots of NF3 and CF4 in South Korea, owing to the measurement location. We calculate emissions of CF4 to be quite constant between years 2008 and 2015 for both China and South Korea with 2015 emissions calculated at 4.33 ± 2.65 Gg yr−1 and 0.36 ± 0.11 Gg yr−1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6 ± 0.07 Gg yr−1 in 2015, which equates to ~ 1.6 % of the country's CO2 emissions. We also apply our method to calculate emissions of CHF3 (HFC-23) between 2008 and 2012, for which our results find good agreement with other studies and which helps support our choice in methodology for CF4 and NF3.


2020 ◽  
Author(s):  
Marine Remaud ◽  
Frédéric Chevallier ◽  
Philippe Peylin ◽  
Antoine Berchet ◽  
Fabienne Maignan

&lt;p&gt;Inverse systems that assimilate atmospheric carbon dioxide measurements (CO2) into a global atmospheric transport model, are commonly used together with anthropogenic emission inventories to infer net biospheric surface fluxes. However, when assimilating CO2 measurements only, the respiration fluxes cannot be disentangled from the gross primary production (GPP) fluxes, leaving few possibilities to interpret the inferred fluxes from a mechanistic point of view. Measurements of carbonyl sulfide (COS) may help to fill this gap: COS has similar diffusion pathway inside leaves&amp;#160;as CO2 but is not re-emitted into the atmosphere by the plant respiration. We explore here the benefit of assimilating both COS and CO2 measurements into the LMDz atmospheric transport model to constrain GPP and respiration fluxes separately. To this end, we develop an analytic inverse system based on the 14 Plant functional Type (PFTs) as defined in the ORCHIDEE land surface model. The vegetation uptake of COS is parameterized as a linear function of GPP and of the leaf relative uptake (LRU), which is the ratio of COS to CO2 deposition velocities in plants. A new parameterization of the atmosphere soil exchanges is also included. We use the system to optimize GPP and respiration fluxes separately at the seasonal scale over the globe. The results lead to a balanced COS global budget and a seasonality of the COS fluxes in better agreement with observations. We find a large sensitivity of the partition between the ocean emissions and the COS plant uptake to the LRU parameterizations.&lt;/p&gt;


2016 ◽  
Author(s):  
Dominik Schmithüsen ◽  
Scott Chambers ◽  
Bernd Fischer ◽  
Stefan Gilge ◽  
Juha Hatakka ◽  
...  

Abstract. A European-wide 222Radon/222Radon progeny comparison study has been conducted in order to determine correction factors that could be applied to existing atmospheric 222Radon data sets for quantitative use of this tracer in atmospheric transport model validation. Two compact and easy-to-transport Heidelberg Radon Monitors (HRM) were moved around to run for at least one month at each of the nine European measurement stations that were included in the comparison. Linear regressions between parallel data sets were calculated, yielding correction factors relative to the HRM ranging from 0.68 to 1.45. A calibration bias between ANSTO (Australian Nuclear Science and Technology Organisation) two-filter radon monitors and the HRM of ANSTO/HRM = 1.11 ± 0.05 was found. For continental stations, which use one-filter systems, preliminary 214Po/222Rn disequilibrium values were estimated to lie between 0.8 at mountain stations (e.g. Schauinsland) and 0.9 at non-mountain sites for sampling heights around 20 to 30 m above ground level. Respective corrections need to be applied to obtain a consistent European 222Radon data set for further applications.


2019 ◽  
Author(s):  
Jinwoong Kim ◽  
Saroja Polavarapu ◽  
Douglas Chan ◽  
Michael Neish

Abstract. In this study, we present the development of a regional atmospheric transport model for greenhouse gas (GHG) simulation based on an operational weather forecast model and a chemical transport model at Environment and Climate Change Canada (ECCC), with the goal of improving our understanding of the high spatio-temporal resolution interaction between the atmosphere and surface GHG fluxes over Canada and the United States. The regional model uses 10 km × 10 km horizontal grid spacing and 80 vertical levels spanning the ground to 0.1 hPa. The lateral boundary conditions of meteorology and tracers are provided by the global transport model used for GHG simulation at ECCC. The performance of the regional model and added benefit of the regional model over our lower resolution global models is investigated in terms of modelled CO2 concentration and meteorological forecast quality for multiple seasons in 2015. We find that our regional model has the capability to simulate high spatial (horizontal and vertical) and temporal scales of atmospheric CO2 concentrations, based on comparisons to surface and aircraft observations. In addition, reduced bias and standard deviation of forecast error in boreal summer are obtained by the regional model. Better representation of model topography in the regional model reduces transport and representation errors significantly compared to the global model, especially in regions of complex topography, as revealed by the more precise and detailed structure of the CO2 diurnal cycle produced at observation sites and in model space. The new regional model will form the basis of a flux inversion system that estimates regional scale fluxes of GHGs over Canada.


2006 ◽  
Vol 6 ◽  
pp. 1041-1047 ◽  
Author(s):  
Raquel Nieto ◽  
Luis Gimeno

An advanced Lagrangian atmospheric transport model (FLEXTRAP) was used to identify the possible sources of middle-lived pollutants over the Iberian Peninsula. A period of 4 years, 2000—2003, was analyzed. Transatlantic transport is the main pathway of the air reaching the Iberian Peninsula in the studied range of 3—10 days; local sources are limited to 3 days of transport. The presence of North America as a source from days 6—10 of transport identifies this region as the main potential contributor to the middle-lived pollutants over the Iberian Peninsula.


2020 ◽  
Vol 13 (1) ◽  
pp. 269-295
Author(s):  
Jinwoong Kim ◽  
Saroja M. Polavarapu ◽  
Douglas Chan ◽  
Michael Neish

Abstract. In this study, we present the development of a regional atmospheric transport model for greenhouse gas (GHG) simulation based on an operational weather forecast model and a chemical transport model at Environment and Climate Change Canada (ECCC), with the goal of improving our understanding of the high-spatiotemporal-resolution interaction between the atmosphere and surface GHG fluxes over Canada and the United States. The regional model uses 10 km×10 km horizontal grid spacing and 80 vertical levels spanning the ground to 0.1 hPa. The lateral boundary conditions of meteorology and tracers are provided by the global transport model used for GHG simulation at ECCC. The performance of the regional model and added benefit of the regional model over our lower-resolution global models is investigated in terms of modelled CO2 concentration and meteorological forecast quality for multiple seasons in 2015. We find that our regional model has the capability to simulate the high spatial (horizontal and vertical) and temporal scales of atmospheric CO2 concentrations based on comparisons to surface and aircraft observations. In addition, the bias and standard deviation of forecast error in boreal summer are reduced by the regional model. Better representation of model topography in the regional model results in improved simulation of the CO2 diurnal cycle compared to the global model at Walnut Grove, California. The new regional model will form the basis of a flux inversion system that estimates regional-scale fluxes of GHGs over Canada.


2017 ◽  
Author(s):  
Yu Liu ◽  
Nicolas Gruber ◽  
Dominik Brunner

Abstract. The emission of CO2 from the burning of fossil fuel is a prime determinant of variations in atmospheric CO2. Here, we simulate this fossil fuel signal together with the natural and background components with a regional high-resolution atmospheric transport model for central and southern Europe considering separately the emissions from different sectors and countries on the basis of emission inventories and hourly emission time functions. The simulated variations in atmospheric CO2 agree very well with observation-based estimates, although the observed variance is slightly underestimated, particularly for the fossil fuel component. Despite relatively rapid atmospheric mixing, the simulated fossil fuel signal reveals distinct annual mean structures deep into the troposphere reflecting the spatially dense aggregation of most emissions. The fossil fuel signal accounts for more than half of the total (fossil fuel + biospheric + background) temporal variations in atmospheric CO2 in most areas of northern and western central Europe, with the largest variations occurring on diurnal timescales owing to the combination of diurnal variations in emissions and atmospheric mixing/transport out of the surface layer. Their co-variance leads to a fossil-fuel diurnal rectifier effect with a magnitude as large as 9 ppm compared to a case with time-constant emissions. The spatial pattern of CO2 from the different sectors largely reflects the distribution and relative magnitude of the corresponding emissions, with power plant emissions leaving the most distinguished mark. An exception is southern and western Europe, where the emissions from the transportation sector dominate the fossil fuel signal. Most of the fossil fuel CO2 remains within the country responsible for the emission, although in smaller countries, up to 80 % of the fossil fuel signal can come from abroad. A fossil fuel emission reduction of 30 % is clearly detectable for a surface-based observing system for atmospheric CO2, while it is beyond the edge of detectability for the current generation of satellites with the exception of a few hotspot sites. Changes in variability in atmospheric CO2 might open an additional door for the monitoring and verification of changes in fossil fuel emissions, primarily for surface based systems.


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