Inferring European fossil fuel CO 2 emissions using TROPOMI NO 2 data and sector-based NO x  : CO 2 emission ratios

IF 5.7 1区 地球科学 Q1 ENVIRONMENTAL SCIENCES
Chlöe N. Schooling,Liang Feng,Ingrid Super,Paul I. Palmer
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Abstract

Accurate monitoring of fossil fuel CO 2  (ffCO 2 ) emissions is essential for tracking climate mitigation, yet natural carbon-cycle fluxes often obscure human-induced signals in atmospheric observations. This study presents a proof-of-concept satellite-driven data assimilation framework that uses nitrogen oxides (NO x  = NO + NO 2 ) – short-lived trace gases co-emitted with CO 2 –, to estimate ffCO 2 emissions. We estimate European NO x emissions for 2021 by assimilating TROPOMI NO 2 observations into an Ensemble Kalman Filter (EnKF) framework, optimised within the GEOS-Chem atmospheric transport model. We use a computationally efficient offline treatment of NO x chemistry, enabling large-ensemble inversions while retaining sensitivity to changes in photochemistry. Assimilating these data leads to a systematic reduction in the state vector uncertainty, with the mean uncertainty in total ffCO 2 emissions over Europe decreasing from 5.6 % in the prior to 3.3 % in the posterior. As well as overall improvement in model agreement with observations that corresponds to an annual correlation increase, Δ r =0.12, derived from the correlation of all daily model–observation pairs across all grid cells in the European domain. By leveraging sector-specific NO x  : CO 2 emission ratios, we translate our posterior NO x flux estimates into corresponding ffCO 2 estimates that capture enhanced seasonal variability. Our inferred ffCO 2 emissions exhibit elevated values in autumn and winter, spatially concentrated over major source regions and consistent with surface temperature variability. The inferred posterior adjustments include substantial increases in national emissions in several regions (20 %–91 % in national annual combustion CO 2 ), highlighting both the sensitivity of the method and the need for further validation and multi-species observational constraints. Independent evaluation against in situ measurements confirms significant improvements in mean error statistics in some regions. And updated national posterior ffCO 2 emissions show improved agreement with EDGAR across five high emitting European countries. This study demonstrates the potential of ensemble data assimilation and reduced-complexity chemistry to provide a first-order constraint on European ffCO 2 estimates, establishing a vital foundation for future joint NO 2 –CO 2 inversion systems.
利用TROPOMI NO . 2数据和基于部门的NO . x: CO . 2排放比推断欧洲化石燃料CO . 2排放量
精确监测化石燃料二氧化碳(ffCO 2)排放对于跟踪气候减缓至关重要,但在大气观测中,自然碳循环通量往往掩盖了人为引起的信号。本研究提出了一个概念验证卫星驱动的数据同化框架,该框架使用氮氧化物(NO x = NO + NO 2)——与CO 2共同排放的短寿命微量气体——来估算ffCO 2的排放量。我们通过将TROPOMI NO 2观测数据吸收到一个集成卡尔曼滤波(EnKF)框架中,并在GEOS-Chem大气输送模型中进行优化,估计了欧洲2021年的nox排放量。我们使用了一种计算效率高的NO x化学离线处理方法,在保持对光化学变化的敏感性的同时,实现了大集合反转。吸收这些数据导致状态向量不确定性的系统性降低,欧洲ffCO 2总排放量的平均不确定性从之前的5.6%下降到后验的3.3%。模型与观测值的一致性总体上有所改善,对应于年度相关性增加,Δ r =0.12,来自欧洲地区所有网格单元中所有每日模型-观测对的相关性。通过利用特定部门的nox: co2排放比,我们将我们的后验nox通量估计值转化为相应的ffco2估计值,从而捕捉到增强的季节变异性。我们推断的ffCO 2排放量在秋季和冬季呈上升趋势,空间上集中在主要源区,与地表温度变化一致。推断的后验调整包括几个地区的全国排放量大幅增加(全国年燃烧CO 2的20% - 91%),突出了该方法的敏感性以及进一步验证和多物种观测约束的必要性。根据现场测量结果进行的独立评估证实,在某些地区,平均误差统计数据有了显著改善。最新的国家后验ffCO 2排放量显示,五个高排放的欧洲国家与EDGAR的一致性有所提高。该研究证明了集成数据同化和降低复杂性化学的潜力,为欧洲ffCO 2估计提供了一级约束,为未来的no2 -CO 2联合反演系统奠定了重要基础。
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来源期刊
Atmospheric Chemistry and Physics
Atmospheric Chemistry and Physics 地学-气象与大气科学
CiteScore
10.70
自引率
20.60%
发文量
702
审稿时长
6 months
期刊介绍: Atmospheric Chemistry and Physics (ACP) is a not-for-profit international scientific journal dedicated to the publication and public discussion of high-quality studies investigating the Earth''s atmosphere and the underlying chemical and physical processes. It covers the altitude range from the land and ocean surface up to the turbopause, including the troposphere, stratosphere, and mesosphere. The main subject areas comprise atmospheric modelling, field measurements, remote sensing, and laboratory studies of gases, aerosols, clouds and precipitation, isotopes, radiation, dynamics, biosphere interactions, and hydrosphere interactions. The journal scope is focused on studies with general implications for atmospheric science rather than investigations that are primarily of local or technical interest.
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