We quantify methane emissions in China and the contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. The inversion uses as a prior estimate the latest 2014 national sector-resolved anthropogenic emission inventory reported by the Chinese government to the United Nations Framework Convention on Climate Change (UNFCCC) and thus serves as a direct evaluation of that inventory. Emissions are optimized with a Gaussian mixture model (GMM) at up to resolution. The optimization is done analytically assuming log-normally distributed errors on prior emissions. Errors and information content on the optimized estimates are obtained directly from the analytical solution and also through a 36-member inversion ensemble. Our best estimate for total anthropogenic emissions in China is 65.0 (57.7–68.4) Tg a−1, where parentheses indicate the uncertainty range determined by the inversion ensemble. Contributions from individual sectors include 16.6 (15.6–17.6) Tg a−1 for coal, 2.3 (1.8–2.5) for oil, 0.29 (0.23–0.32) for gas, 17.8 (15.1–21.0) for livestock, 9.3 (8.2–9.9) for waste, 11.9 (10.7–12.7) for rice paddies, and 6.7 (5.8–7.1) for other sources. Our estimate is 21% higher than the Chinese inventory reported to the UNFCCC (53.6 Tg a−1), reflecting upward corrections to emissions from oil (+147 %), gas (+61 %), livestock (+37 %), waste (+41 %), and rice paddies (+34 %), but downward correction for coal (−15 %). It is also higher than previous inverse studies (43–62 Tg a−1) that used the much sparser GOSAT satellite observations and were conducted at coarser resolution. We are in particular better able to separate coal and rice emissions. Our higher livestock emissions are attributed largely to northern China where GOSAT has little sensitivity. Our higher waste emissions reflect at least in part a rapid growth in wastewater treatment in China. Underestimate of oil emissions in the UNFCCC report appears to reflect unaccounted-for super-emitting facilities. Gas emissions in China are mostly from distribution, in part because of low emission factors from production and in part because 42 % of the gas is imported. Our estimate of emissions per unit of domestic gas production indicates a low life-cycle loss rate of 1.7 % (1.3 %–1.9 %), which would imply net climate benefits from the current “coal-to-gas” energy transition in China. However, this small loss rate is somewhat misleading considering China's high gas imports, including from Turkmenistan where emission per unit of gas production is very high.
23 December 2021 in Geoscientific Model Development
We perform observing system simulation experiments (OSSEs) with the GEOS-Chem adjoint model to test how well methane emissions over North America can be resolved using measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and similar high-resolution satellite sensors. We focus analysis on the impacts of (i) spatial errors in the prior emissions and (ii) model transport errors. Along with a standard scale factor (SF) optimization we conduct a set of inversions using alternative formalisms that aim to overcome limitations in the SF-based approach that arise for missing sources. We show that 4D-Var analysis of the TROPOMI data can improve monthly emission estimates at 25 km even with a spatially biased prior or model transport errors (42 %–93 % domain-wide bias reduction; R increases from 0.51 up to 0.73). However, when both errors are present, no single inversion framework can successfully improve both the overall bias and spatial distribution of fluxes relative to the prior on the 25 km model grid. In that case, the ensemble-mean optimized fluxes have a domain-wide bias of 77 Gg d−1 (comparable to that in the prior), with spurious source adjustments compensating for the transport errors. Increasing observational coverage through longer-timeframe inversions does not significantly change this picture. An inversion formalism that optimizes emission enhancements rather than scale factors exhibits the best performance for identifying missing sources, while an approach combining a uniform background emission with the prior inventory yields the best performance in terms of overall spatial fidelity – even in the presence of model transport errors. However, the standard SF optimization outperforms both of these for the magnitude of the domain-wide flux. For the common scenario in which prior errors are non-random, approximate posterior error reduction calculations (derived via gradient-based randomization) for the inversions reflect the sensitivity to observations but have no spatial correlation with the actual emission improvements. This demonstrates that such information content analysis can be used for general observing system characterization but does not describe the spatial accuracy of the posterior emissions or of the actual emission improvements. Findings here highlight the need for careful evaluation of potential missing sources in prior emission datasets and for robust accounting of model transport errors in inverse analyses of the methane budget.
25 January 2021 in Atmospheric Chemistry and Physics
We apply airborne measurements across three seasons (summer, winter and spring 2017–2018) in a multi-inversion framework to quantify methane emissions from the US Corn Belt and Upper Midwest, a key agricultural and wetland source region. Combing our seasonal results with prior fall values we find that wetlands are the largest regional methane source (32 %, 20 [16–23] Gg/d), while livestock (enteric/manure; 25 %, 15 [14–17] Gg/d) are the largest anthropogenic source. Natural gas/petroleum, waste/landfills, and coal mines collectively make up the remainder. Optimized fluxes improve model agreement with independent datasets within and beyond the study timeframe. Inversions reveal coherent and seasonally dependent spatial errors in the WetCHARTs ensemble mean wetland emissions, with an underestimate for the Prairie Pothole region but an overestimate for Great Lakes coastal wetlands. Wetland extent and emission temperature dependence have the largest influence on prediction accuracy; better representation of coupled soil temperature–hydrology effects is therefore needed. Our optimized regional livestock emissions agree well with the Gridded EPA estimates during spring (to within 7 %) but are ∼ 25 % higher during summer and winter. Spatial analysis further shows good top-down and bottom-up agreement for beef facilities (with mainly enteric emissions) but larger (∼ 30 %) seasonal discrepancies for dairies and hog farms (with > 40 % manure emissions). Findings thus support bottom-up enteric emission estimates but suggest errors for manure; we propose that the latter reflects inadequate treatment of management factors including field application. Overall, our results confirm the importance of intensive animal agriculture for regional methane emissions, implying substantial mitigation opportunities through improved management.
The atmospheric methane (CH 4 ) growth rate surged after 2019, peaking at 16.2 parts per billion per year (ppb year −1 ) in 2020 before declining to 8.6 ppb year −1 in 2023. Using multiple atmospheric inversions constrained by observation- and model-based prescribed hydroxyl radical (OH) fields and CH 4 atmospheric data, we show that a drop of OH radicals in 2020–2021, followed by recovery in 2022–2023, accounted for 83% of year-on-year variations in the CH 4 growth rate, the rest being explained by wetland and inland water emissions, which increased between 2019 and 2020–2022 [+8.6 ± 2.6 teragrams of CH 4 per year (TgCH 4 year −1 )] and then decreased between 2022 and 2023 (−9.9 ± 3.3 TgCH 4 year −1 ). Most emission changes from 2019 to 2023 occurred in northern tropical wetlands in Africa and Asia, whereas South American wetlands emissions declined and Arctic emissions increased after 2019.
Carbon monoxide (CO) is an ozone precursor, oxidant sink, and widely used pollution tracer. The importance of anthropogenic versus other CO sources in the US is uncertain. Here, we interpret extensive airborne measurements with an atmospheric model to constrain US fossil and nonfossil CO sources. Measurements reveal a low bias in the simulated CO background and a 30% overestimate of US fossil CO emissions in the 2016 National Emissions Inventory. After optimization we apply the model for source partitioning. During summer, regional fossil sources account for just 9%–16% of the sampled boundary layer CO, and 32%–38% of the North American enhancement—complicating use of CO as a fossil fuel tracer. The remainder predominantly reflects biogenic hydrocarbon oxidation plus fires. Fossil sources account for less domain‐wide spatial variability at this time than nonfossil and background contributions. The regional fossil contribution rises in other seasons, and drives ambient variability downwind of urban areas.
The US Corn Belt is a global hotspot of atmospheric ammonia (NH3), a gas known to adversely impact the environment and human health. We combine hourly tall tower (100 m) measurements and bi‐weekly, spatially distributed, ground‐based observations from the Ammonia Monitoring Network with the US National Emissions Inventory (NEI) and WRF‐Chem simulations to constrain NH3 emissions from April to September 2017–2019. We show that: (1) NH3 emissions peaked from May to July and were 1.6–1.7 times the annual NEI average; (2) average growing season NH3 emissions from agricultural lands were remarkably similar across years (3.27–3.64 nmol m−2 s−1), yet showed substantial episodic variability driven by meteorology and land management; (3) dry deposition was 40% of gross emissions from agricultural lands and exceeded 100% of gross emissions in natural lands. Our findings provide an important benchmark for evaluating future NH3 emissions and mitigation efforts.