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

Preventing drift of oxygen isotopes of CO₂-in-air stored in glass sample flasks:new insights and recommendations

It is known that the oxygen isotope composition of CO2-in-air, when stored over longer time periods in glass sample flasks, tends to drift to more negative values while the carbon isotope composition remains stable. The exact mechanisms behind this drift were still unclear. New experimental results reveal that water already inside the flasks during sampling plays a major role in the drift of the oxygen isotopes. A drying method to remove any water sticking to the inner walls by evacuating the flasks for more than 72 h while heating to 60 °C significantly decreases drift of the oxygen isotopes. Moreover, flasks not dried with this method showed higher differences among drift rates of individual flasks. This is explained through the buildup of H2O molecules sticking to the inner walls. Humidity of the air samples in the flasks as well as surface characteristics will lead to differences among flasks. Results also show that permeability of water is higher through Viton O-ring flask seals than through polychlorotrifluoroethylene (PCTFE) shaft seals, and that the stability of flasks sealed with the latter is significantly better over time.</p

Preventing drift of oxygen isotopes of CO₂-in-air stored in glass sample flasks:new insights and recommendations

It is known that the oxygen isotope composition of CO2-in-air, when stored over longer time periods in glass sample flasks, tends to drift to more negative values while the carbon isotope composition remains stable. The exact mechanisms behind this drift were still unclear. New experimental results reveal that water already inside the flasks during sampling plays a major role in the drift of the oxygen isotopes. A drying method to remove any water sticking to the inner walls by evacuating the flasks for more than 72 h while heating to 60 °C significantly decreases drift of the oxygen isotopes. Moreover, flasks not dried with this method showed higher differences among drift rates of individual flasks. This is explained through the buildup of H2O molecules sticking to the inner walls. Humidity of the air samples in the flasks as well as surface characteristics will lead to differences among flasks. Results also show that permeability of water is higher through Viton O-ring flask seals than through polychlorotrifluoroethylene (PCTFE) shaft seals, and that the stability of flasks sealed with the latter is significantly better over time.</p

Preventing drift of oxygen isotopes of CO₂-in-air stored in glass sample flasks:new insights and recommendations

It is known that the oxygen isotope composition of CO2-in-air, when stored over longer time periods in glass sample flasks, tends to drift to more negative values while the carbon isotope composition remains stable. The exact mechanisms behind this drift were still unclear. New experimental results reveal that water already inside the flasks during sampling plays a major role in the drift of the oxygen isotopes. A drying method to remove any water sticking to the inner walls by evacuating the flasks for more than 72 h while heating to 60 °C significantly decreases drift of the oxygen isotopes. Moreover, flasks not dried with this method showed higher differences among drift rates of individual flasks. This is explained through the buildup of H2O molecules sticking to the inner walls. Humidity of the air samples in the flasks as well as surface characteristics will lead to differences among flasks. Results also show that permeability of water is higher through Viton O-ring flask seals than through polychlorotrifluoroethylene (PCTFE) shaft seals, and that the stability of flasks sealed with the latter is significantly better over time.</p