Quantifying fossil fuel methane emissions using observations of atmospheric ethane and an uncertain emission ratio

We present a method for estimating fossil fuel methane emissions using observations of methane and ethane, accounting for uncertainty in their emission ratio. The ethane:methane emission ratio is incorporated as a variable parameter in a Bayesian model, with its own prior distribution and uncertainty. We find that using an emission ratio distribution mitigates bias from using a fixed, potentially incorrect emission ratio and that uncertainty in this ratio is propagated into posterior estimates of emissions. A synthetic data test is used to show the impact of assuming an incorrect ethane:methane emission ratio and demonstrate how our variable parameter model can better quantify overall uncertainty. We also use this method to estimate UK methane emissions from high-frequency observations of methane and ethane from the UK Deriving Emissions linked to Climate Change (DECC) network. Using the joint methane-ethane inverse model, we estimate annual mean UK methane emissions of approximately 0.27 (95 % uncertainty interval 0.26–0.29) Tg per year from fossil fuel sources and 2.06 (1.99–2.15) Tg per year from non-fossil fuel sources, during the period 2015–2019. Uncertainties in UK fossil fuel emissions estimates are reduced on average by 15 %, and up to 35 %, when incorporating ethane into the inverse model, in comparison to results from the methane-only inversion.

Boreal forest fire CO and CH₄ emission factors derived from tower observations in Alaska during the extreme fire season of 2015

Recent increases in boreal forest burned area, which have been linked with climate warming, highlight the need to better understand the composition of wildfire emissions and their atmospheric impacts. Here we quantified emission factors for CO and CH4 from a massive regional fire complex in interior Alaska during the summer of 2015 using continuous high-resolution trace gas observations from the Carbon in Arctic Reservoirs Vulnerability Experiment (CRV) tower in Fox, Alaska. Averaged over the 2015 fire season, the mean CO / CO2 emission ratio was 0.142 ± 0.051, and the mean CO emission factor was 127 ± 40 g kg−1 dry biomass burned. The CO / CO2 emission ratio was about 39 % higher than the mean of previous estimates derived from aircraft sampling of wildfires from boreal North America. The mean CH4 / CO2 emission ratio was 0.010 ± 0.004, and the CH4 emission factor was 5.3 ± 1.8 g kg−1 dry biomass burned, which are consistent with the mean of previous reports. CO and CH4 emission ratios varied in synchrony, with higher CH4 emission factors observed during periods with lower modified combustion efficiency (MCE). By coupling a fire emissions inventory with an atmospheric model, we identified at least 34 individual fires that contributed to trace gas variations measured at the CRV tower, representing a sample size that is nearly the same as the total number of boreal fires measured in all previous field campaigns. The model also indicated that typical mean transit times between trace gas emission within a fire perimeter and tower measurement were 1–3 d, indicating that the time series sampled combustion across day and night burning phases. The high CO emission ratio estimates reported here provide evidence for a prominent role of smoldering combustion and illustrate the importance of continuously sampling fires across time-varying environmental conditions that are representative of a fire season.

Quantifying methane emissions from fossil fuel sources using a Bayesian inverse model and observations of ethane with an uncertain emissions ratio

<p>Methane is an important greenhouse gas with a range of anthropogenic sources, including livestock farming and fossil fuel production. It is important that methane emissions can be correctly attributed to their source, to aid climate change policy and emissions mitigation efforts. For source attribution, many ‘top-down’ models of atmospheric methane use spatial maps of sources from emissions inventory data coupled with an atmospheric transport model. However, this can cause difficulties if sources are co-located or if there is uncertainty in the sources’ spatial distributions.</p><p>To help with this issue and reduce overall uncertainty in estimates of methane emissions, recent methods have used observations of a secondary trace gas and its correlation with methane to infer methane emissions from a target sector. Most previous work has assumed a fixed emissions ratio between the two gases, which often does not reflect the true range of possible emission ratios. In this work, measurements of atmospheric ethane and its emissions ratio relative to methane are used to infer emissions of methane from fossil fuel sources. Instead of assuming a fixed emission ratio, our method allows for uncertainty in the emission ratio to be statistically propagated through the inverse model and incorporated into the sectoral estimates of methane emissions. We further demonstrate the inaccuracies that can result in an assessment of fossil fuel methane emissions if this uncertainty is not considered.</p><p>We present this novel method for modelling sectoral methane emissions with examples from a synthetic data experiment and give results from a case study of UK methane emissions. Methane and ethane observations from a tall tower network across the UK were used with this model to produce monthly estimates of UK fossil fuel methane emissions with improved uncertainty characterisation.</p>

A Red Fluorescent Protein-Based Probe for Detection of Intracellular Reactive Sulfane Sulfur

Reactive sulfane sulfur, including persulfide and polysulfide, is a type of regular cellular component, playing an antioxidant role. Its function may be organelle-dependent; however, the shortage of probes for detecting organellar reactive sulfane sulfur has hindered further investigation. Herein, we reported a red fluorescent protein (mCherry)-based probe for specifically detecting intracellular reactive sulfane sulfur. By mutating two amino acid residues of mCherry (A150 and S151) to cysteine residues, we constructed a mCherry mutant, which reacted with reactive sulfane sulfur to form an intramolecular –Sn– bond (n ≥ 3). The bond largely decreased the intensity of 610 nm emission (excitation at 587 nm) and slightly increased the intensity of 466 nm emission (excitation at 406 nm). The 466/610 nm emission ratio was used to indicate the relative abundance of reactive sulfane sulfur. We then expressed this mutant in the cytoplasm and mitochondria of Saccharomyces cerevisiae. The 466/610 nm emission ratio revealed that mitochondria had a higher level of reactive sulfane sulfur than cytoplasm. Thus, the mCherry mutant can be used as a specific probe for detecting reactive sulfane sulfur in vivo.

Quantifying burning efficiency in megacities using the NO₂∕CO ratio from the Tropospheric Monitoring Instrument (TROPOMI)

This study investigates the use of co-located nitrogen dioxide (NO2) and carbon monoxide (CO) retrievals from the TROPOMI satellite to improve the quantification of burning efficiency and emission factors (EFs) over the megacities of Tehran, Mexico City, Cairo, Riyadh, Lahore, and Los Angeles. Efficient combustion is characterized by high NOx (NO+NO2) and low CO emissions, making the NO2∕CO ratio a useful proxy for combustion efficiency (CE). The local enhancement of CO and NO2 above megacities is well captured by TROPOMI at short averaging times compared with previous satellite missions. In this study, the upwind background and plume rotation methods are used to investigate the accuracy of satellite-derived ΔNO2∕ΔCO ratios. The column enhancement ratios derived using these two methods vary by 5 % to 20 % across the selected megacities. TROPOMI-derived column enhancement ratios are compared with emission ratios from the EDGAR v4.3.2 (Emission Database for Global Atmospheric Research v4.3.2) and the MACCity (Monitoring Atmospheric Chemistry and Climate and CityZen) 2018 emission inventories. TROPOMI correlates strongly (r=0.85 and 0.7) with EDGAR and MACCity, showing the highest emission ratio for Riyadh and lowest emission ratio for Lahore. However, inventory-derived emission ratios are 60 % to 85 % higher than TROPOMI column enhancement ratios across the six megacities. The short lifetime of NO2 and the different vertical sensitivity of TROPOMI NO2 and CO explain most of this difference. We present a method to translate TROPOMI-retrieved column enhancement ratios into corresponding emission ratios, thereby accounting for these influences. Except for Los Angeles and Lahore, TROPOMI-derived emission ratios are close (within 10 % to 25 %) to MACCity values. For EDGAR, however, emission ratios are ∼65 % higher for Cairo and 35 % higher for Riyadh. For Los Angeles, EDGAR and MACCity are a factor of 2 and 3 higher than TROPOMI respectively. The air quality monitoring networks in Los Angeles and Mexico City are used to validate the use of TROPOMI. For Mexico City and Los Angeles, these measurements are consistent with TROPOMI-derived emission ratios, demonstrating the potential of TROPOMI with respect to monitoring burning efficiency.