An improved divergence method has been developed to estimate annual methane (CH4) emissions from TROPOspheric Monitoring Instrument (TROPOMI) observations. It has been applied to the period of 2018 to 2021 over the Middle East, where the orography is complicated, and the mean mixing ratio of methane (XCH4) might be affected by albedos or aerosols over some locations. To adapt to extreme changes of terrain over mountains or coasts, winds are used with their divergent part removed. A temporal filter is introduced to identify highly variable emissions and to further exclude fake sources caused by retrieval artifacts. We compare our results to widely used bottom-up anthropogenic emission inventories: Emissions Database for Global Atmospheric Research (EDGAR), Community Emissions Data System (CEDS), and Global Fuel Exploitation Inventory (GFEI) over several regions representing various types of sources. The NOx emissions are from EDGAR and Daily Emissions Constrained by Satellite Observations (DECSO), and the industrial heat sources identified by Visible Infrared Imaging Radiometer Suite (VIIRS) are further used to better understand our resulting methane emissions. Our results indicate possibly large underestimations of methane emissions in metropolises like Tehran (up to 50 %) and Isfahan (up to 70 %) in Iran. The derived annual methane emissions from oil/gas production near the Caspian Sea in Turkmenistan are comparable to GFEI but more than 2 times higher than EDGAR and CEDS in 2019. Large discrepancies in the distribution of methane sources in Riyadh and its surrounding areas are found between EDGAR, CEDS, GFEI, and our emissions. The methane emission from oil/gas production to the east of Riyadh seems to be largely overestimated by EDGAR and CEDS, while our estimates as well as GFEI and DECSO NOx indicate much lower emissions from industrial activities. On the other hand, regions like Iran, Iraq, and Oman are dominated by sources from oil and gas exploitation that probably include more irregular releases of methane, with the result that our estimates, which include only invariable sources, are lower than the bottom-up emission inventories.@en

We present a new divergence method to estimated methane (CH₄) emissions from satellite observed mean mixing ratio of methane (XCH₄) by deriving the regional enhancement of XCH₄ in the Planetary Boundary Layer (PBL). The applicability is proven by comparing the estimated emissions with its known emission inventory from a 3-month GEOS-Chem simulation. When applied to TROPOspheric Monitoring Instrument observations, sources from well-known oil/gas production areas, livestock farms and wetlands in Texas become clearly visible in the emission maps. The calculated yearly averaged total CH₄ emission over the Permian Basin is 3.06 (2.82, 3.78) Tg a⁻¹ for 2019, which is consistent with previous studies and double that of EDGAR v4.3.2 for 2012. Sensitivity tests on PBL heights, on the derived regional background and on wind speeds suggest our divergence method is quite robust. It is also a fast and simple method to estimate the CH₄ emissions globally.

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Chemical transport models together with emission inventories are widely used to simulate NO2 concentrations over China, but validation of the simulations with in situ measurements has been extremely limited. Here we use ground measurements obtained from the air quality monitoring network recently developed by the Ministry of Environmental Protection of China to validate modeling surface NO2 concentrations from the CHIMERE regional chemical transport model driven by the satellite-derived DECSO and the bottom-up MIX emission inventories. We applied a correction factor to the observations to account for the interferences of other oxidized nitrogen compounds (NOz), based on the modeled ratio of NO2 to NOz. The model accurately reproduces the spatial variability in NO2 from in situ measurements, with a spatial correlation coefficient of over 0.7 for simulations based on both inventories. A negative and positive bias is found for the simulation with the DECSO (slope= 0.74 and 0.64 for the daily mean and daytime only) and the MIX (slope= 1.3 and 1.1) inventories, respectively, suggesting an underestimation and overestimation of NOx emissions from corresponding inventories. The bias between observed and modeled concentrations is reduced, with the slope dropping from 1.3 to 1.0 when the spatial distribution of NOx emissions in the DECSO inventory is applied as the spatial proxy for the MIX inventory, which suggests an improvement of the distribution of emissions between urban and suburban or rural areas in the DECSO inventory compared to that used in the bottom-up inventory. A rough estimate indicates that the observed concentrations, from sites predominantly placed in the populated urban areas, may be 10-40 % higher than the corresponding model grid cell mean. This reduces the estimate of the negative bias of the DECSO-based simulation to the range of -30 to 0 % on average and more firmly establishes that the MIX inventory is biased high over major cities. The performance of the model is comparable over seasons, with a slightly worse spatial correlation in summer due to the difficulties in resolving the more active NOx photochemistry and larger concentration gradients in summer by the model. In addition, the model well captures the daytime diurnal cycle but shows more significant disagreement between simulations and measurements during nighttime, which likely produces a positive model bias of about 15 % in the daily mean concentrations. This is most likely related to the uncertainty in vertical mixing in the model at night.

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