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At least 883 records · Page 49

Sustainable Waste Tire Derived Carbon Material as a Potential Anode for Lithium-Ion Batteries

The rapidly growing automobile industry increases the accumulation of end-of-life tires each year throughout the world. Waste tires lead to increased environmental issues and lasting resource problems. Recycling hazardous wastes to produce value-added products is becoming essential for the sustainable progress of society. A patented sulfonation process followed by pyrolysis at 1100 °C in a nitrogen atmosphere was used to produce carbon material from these tires and utilized as an anode in lithium-ion batteries. The combustion of the volatiles released in waste tire pyrolysis produces lower fossil CO 2 emissions per unit of energy (136.51 gCO 2 /kW·h) compared to other conventional fossil fuels such as coal or fuel–oil, usually used in power generation. The strategy used in this research may be applied to other rechargeable batteries, supercapacitors, catalysts, and other electrochemical devices. The Raman vibrational spectra observed on these carbons show a graphitic carbon with significant disorder structure. Further, structural studies reveal a unique disordered carbon nanostructure with a higher interlayer distance of 4.5 Å compared to 3.43 Å in the commercial graphite. The carbon material derived from tires was used as an anode in lithium-ion batteries exhibited a reversible capacity of 360 mAh/g at C/3. However, the reversible capacity increased to 432 mAh/g at C/10 when this carbon particle was coated with a thin layer of carbon. In conclusion, a novel strategy of prelithiation applied for improving the first cycle efficiency to 94% is also presented.

25 ENERGY STORAGE↗

A Review of Clean Electricity Policies—From Countries to Utilities

Due to the heavy stress on environmental deterioration and the excessive consumption of fossil resources, the transition of global energy from fossil fuel energy to clean energy has significantly accelerated in recent years. The power industry and policymakers in almost all countries are focusing on clean energy development. Thanks to progressive clean energy policies, significant progress in clean energy integration and greenhouse gas reduction has been achieved around the world. However, due to the differences in economic structures, clean energy distributions, and development models, clean energy policy scope, focus, and coverage vary between different countries, states, and utilities. This paper aims at providing a policy review for readers to easily obtain clean energy policy information on various clean energies in the U.S. and some other countries. Firstly, this paper reviews and compares some countries’ clean energy policies on electricity. Then, taking the U.S. as an example, this paper introduces the clean energy policies of some representative states and utilities in the U.S in perspectives of renewable energies, electric vehicles, and energy storage.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Handling and Properties of Methanol as a Marine Fuel

Given the increasing concern around greenhouse gas emissions and the decline in the availability of fossil fuels, there is increasing global demand to develop alternate fuels for maritime transportation that are sustainable and which have lower greenhouse gas emissions. Methanol is one such alternative fuel that has garnered considerable attention given its potential to be produced by more sustainable processes and its more favorable greenhouse gas emission profile in comparison with current fossil fuels. Understanding the physical and chemical properties of methanol under a range of conditions is essential for its development as a marine fuel. In this study, we seek to define physical and chemical properties of different methanol samples to simulate real-world storage conditions as these data are lacking in the literature. Several methanol samples were evaluated: nearly pure methanol; International Organization for Standardization (ISO) marine methanol (MM) grades A, B, and C; and methanol plus higher alcohols. We first evaluated all methanol samples for impurities, acetic acid content, density, and distillation range. We then characterized the effects of water absorption and found that methanol can easily absorb unacceptable water content from humid air within hours, necessitating storage conditions that prevent this process. In eight-week aging experiments at 20 °C and 40 °C in ambient air, we did not observe significant oxidation for any of the methanol samples; however, we did observe increases in acid number. We assessed the impact of contamination of methanol with water, marine gas oil (MGO), and an MGO–biodiesel mixture on density, viscosity, distillation range, and lubricity. Finally, we show that MGO contamination of methanol results in a slight increase in sooting tendency. In aggregate, our results provide an in-depth analysis of physical and chemical properties of methanol as well as the impacts of storage conditions and impurities on the properties of fuel methanol.

09 BIOMASS FUELS↗

Resource demand growth and sustainability due to increased world consumption

The paper aims at continuing the discussion on sustainability and attempts to forecast the impossibility of the expanding consumption worldwide due to the planet’s limited resources. As the population of China, India and other developing countries continue to increase, they would also require more natural and financial resources to sustain their growth. We coarsely estimate the volumes of these resources (energy, food, freshwater) and the gross domestic product (GDP) that would need to be achieved to bring the population of India and China to the current levels of consumption in the United States. We also provide estimations for potentially needed immediate growth of the world resource consumption to meet this equality requirement. Given the tight historical correlation between GDP and energy consumption, the needed increase of GDP per capita in the developing world to the levels of the U.S. would deplete explored fossil fuel reserves in less than two decades. These estimates predict that the world economy would need to find a development model where growth would be achieved without heavy dependence on fossil fuels.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Admissible Powertrain Alternatives for Heavy-Duty Fleets: A Case Study on Resiliency and Efficiency

Heavy-duty vehicles dominate global freight movement and primarily rely on fossil-derived diesel fuel. However, fluctuations in crude oil prices and evolving emissions regulations have prompted interest in alternative powertrains to enhance fleet energy resiliency. This study paired real-world operational data from a large commercial fleet with high-fidelity vehicle models to evaluate the potential for replacing diesel internal combustion engine (ICE) trucks with alternative powertrain architectures. The baseline vehicle for this analysis is a diesel-powered ICE truck. Alternatives include ICE trucks fueled by bio- and renewable diesel, compressed natural gas (CNG) or hydrogen (H 2 ), as well as plug-in hybrid (PHEV), fuel cell electric (FCEV), and battery electric vehicles (BEV). While most alternative powertrains resulted in some payload capacity loss, the overall fleetwide impact was negligible due to underutilized payload capacity for the specific fleet considered in this study. For sleeper cab trucks, CNG-powered trucks achieved the highest replacement potential, covering 85% of the fleet. In contrast, H 2 and BEV architectures could replace fewer than 10% and 1% of trucks, respectively. Day cab trucks, with shorter daily routes, showed higher replacement potential: 98% for CNG, 78% for H 2 , and 34% for BEVs. However, achieving full fleet replacement would still require significant operational changes such as route reassignment and enroute refueling, along with considerable improvements to onboard energy storage capacity. Additionally, the higher total cost of ownership (TCO) for alternative powertrains remains a key challenge. This study also evaluated lifecycle impacts across various fuel sources, both fossil and bio-derived. Bio-derived synthetic diesel fuels emerged as a practical option for diesel displacement without disrupting operations. Conversely, H 2 and electrified powertrains provide limited lifecycle impacts under the current energy scenario. This analysis highlights the complexity of replacing diesel ICE trucks with admissible alternatives while balancing fleet resiliency, operational demands, and emissions goals. These results reflect a US-based fleet’s duty cycles, payloads, GVWR allowances, and an assumption of depot-only refueling/recharging. Applicability to other fleets and regions may differ based on differing routing practices or technical features such as battery swapping.

BEV↗

EARTH’S ROTATIONAL DECELERATION: DETERMINATION OF TIDAL FRICTION INDEPENDENT OF TIMESCALES

This paper determines Earth's rotational deceleration without relying on atomic or ephemeris timescales. Earth's rotation defines the civil time standard called Universal Time (UT). Our previous paper did not examine tidal friction in depth when analyzing the timescale divergence between UT and International Atomic Time (TAI). We examine all available paleontological fossils and deposits for the direct measurements of Earth's past rotation rates, because that record includes all contributing effects. We examine paleontological reports that date Earth's rotation rate using corals, bivalves, brachiopods, rhythmites, and stromatolites. Contributions that vary Earth's moment of inertia, such as continental plate drifts, coastline changes, ice age formations, and viscous glacial rebounds, are superimposed with the secular deceleration. The average deceleration of Earth's rotation rate from all available fossil data is found to be (5.969 ± 1.762) × 10{sup −7} rad yr{sup −2}. Our value is 99.8% of the total rotational deceleration determined by Christodoulidis et al., who used artificial satellite data, and our value is 96.6% of the expected tidal friction value obtained by Stephenson and Morrison. Taking the derivative of conserved angular momentum, the predicted lunar orbital deceleration caused by the average rotational deceleration corresponds closely to lunar models. When evaluating the significant time gaps between UT and TAI, Earth's rotational deceleration is a minor contributing factor. Also, the secular deceleration rate is necessary to correctly date ancient astronomical events. We strongly encourage that more ocean paleontological evidence be found to supplement the record to separate the many periodic variations embedded in these data.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

THE EATING HABITS OF MILKY WAY-MASS HALOS: DESTROYED DWARF SATELLITES AND THE METALLICITY DISTRIBUTION OF ACCRETED STARS

We study the mass spectrum of destroyed dwarfs that contribute to the accreted stellar mass of Milky Way (MW)-mass (M{sub vir} ∼ 10{sup 12.1} M{sub ⊙}) halos using a suite of 45 zoom-in dissipationless simulations. Empirical models are employed to relate (peak) subhalo mass to dwarf stellar mass, and we use constraints from z = 0 observations and hydrodynamical simulations to estimate the metallicity distribution of the accreted stellar material. The dominant contributors to the accreted stellar mass are relatively massive dwarfs with M{sub star} ∼ 10{sup 8}–10{sup 10}M{sub ⊙}. Halos with more quiescent accretion histories tend to have lower mass progenitors (10{sup 8}–10{sup 9} M{sub ⊙}), and lower overall accreted stellar masses. Ultra-faint mass (M{sub star} < 10{sup 5} M{sub ⊙}) dwarfs contribute a negligible amount (≪1%) to the accreted stellar mass and, despite having low average metallicities, supply a small fraction (∼2%–5%) of the very metal-poor stars with [Fe/H] < −2. Dwarfs with masses 10{sup 5} < M{sub star}/M{sub ⊙} < 10{sup 8} provide a substantial amount of the very metal-poor stellar material (∼40%–80%), and even relatively metal-rich dwarfs with M{sub star} > 10{sup 8} M{sub ⊙} can contribute a considerable fraction (∼20%–60%) of metal-poor stars if their metallicity distributions have significant metal-poor tails. Finally, we find that the generic assumption of a quiescent assembly history for the MW halo seems to be in tension with the mass spectrum of its surviving dwarfs. We suggest that the MW could be a “transient fossil”; a quiescent halo with a recent accretion event(s) that disguises the preceding formation history of the halo.

79 ASTRONOMY AND ASTROPHYSICS↗

THE ACS LCID PROJECT. XI. ON THE EARLY TIME RESOLUTION OF SFHs OF LOCAL GROUP DWARF GALAXIES: COMPARING THE EFFECTS OF REIONIZATION IN MODELS WITH OBSERVATIONS

The analysis of the early star formation history (SFH) of nearby galaxies, obtained from their resolved stellar populations, is relevant as a test for cosmological models. However, the early time resolution of observationally derived SFHs is limited by several factors. Thus, direct comparison of observationally derived SFHs with those derived from theoretical models of galaxy formation is potentially biased. Here we investigate and quantify this effect. For this purpose, we analyze the duration of the early star formation activity in a sample of four Local Group dwarf galaxies and test whether they are consistent with being true fossils of the pre-reionization era; i.e., if the quenching of their star formation occurred before cosmic reionization by UV photons was completed. Two classical dSph (Cetus and Tucana) and two dTrans (LGS-3 and Phoenix) isolated galaxies with total stellar masses between 1.3×10{sup 6} and 7.2×10{sup 6} M{sub ⊙} have been studied. Accounting for time resolution effects, the SFHs peak as much as 1.25 Gyr earlier than the optimal solutions. Thus, this effect is important for a proper comparison of model and observed SFHs. It is also shown that none of the analyzed galaxies can be considered a true fossil of the pre-reionization era, although it is possible that the outer regions of Cetus and Tucana are consistent with quenching by reionization.

79 ASTRONOMY AND ASTROPHYSICS↗

Chandra and JVLA Observations of HST Frontier Fields Cluster MACS J0717.5+3745

To investigate the relationship between thermal and non-thermal components in merger galaxy clusters, we present deep JVLA and Chandra observations of the HST Frontier Fields cluster MACS J0717.5+3745. The Chandra image shows a complex merger event, with at least four components belonging to different merging subclusters. Northwest of the cluster, ∼0.7 Mpc from the center, there is a ram-pressure-stripped core that appears to have traversed the densest parts of the cluster after entering the intracluster medium (ICM) from the direction of a galaxy filament to the southeast. We detect a density discontinuity north-northeast of this core, which we speculate is associated with a cold front. Our radio images reveal new details for the complex radio relic and radio halo in this cluster. In addition, we discover several new filamentary radio sources with sizes of 100–300 kpc. A few of these seem to be connected to the main radio relic, while others are either embedded within the radio halo or projected onto it. A narrow-angled-tailed (NAT) radio galaxy, a cluster member, is located at the center of the radio relic. The steep spectrum tails of this active galactic nucleus lead into the large radio relic where the radio spectrum flattens again. This morphological connection between the NAT radio galaxy and relic provides evidence for re-acceleration (revival) of fossil electrons. The presence of hot ≳20 keV ICM gas detected by Chandra near the relic location provides additional support for this re-acceleration scenario.

79 ASTRONOMY AND ASTROPHYSICS↗

Deep Very Large Array Observations of the Merging Cluster CIZA J2242.8+5301: Continuum and Spectral Imaging

Despite the progress that has been made in understanding radio relics, there are still open questions regarding the underlying particle acceleration mechanisms. In this paper, we present deep 1–4 GHz Very Large Array (VLA) observations of CIZA J2242.8+5301 ( z = 0.1921), a double radio relic cluster characterized by small projection on the plane of the sky. Our VLA observations reveal, for the first time, the complex morphology of the diffuse sources and the filamentary structure of the northern relic. Additionally, we discover new, faint, diffuse radio emission extending north of the main northern relic. Our Mach number estimates for the northern and southern relics, based on the radio spectral index map obtained using the VLA observations and existing LOw Frequency ARray (LOFAR) and Giant Metrewave Radio Telescope data, are consistent with previous radio and X-ray studies ( and ). However, color–color diagrams and models suggest a flatter injection spectral index than the one obtained from the spectral index map, indicating that projection effects might be not entirely negligible. The southern relic consists of five "arms." Embedded in it, we find a tailed radio galaxy that seems to be connected to the relic. A spectral index flattening, where the radio tail connects to the relic, is also measured. We propose that the southern relic may trace AGN fossil electrons that are reaccelerated by a shock, with an estimated strength of . High-resolution mapping of other tailed radio galaxies also supports a scenario where AGN fossil electrons are revived by the merger event and could be related to the formation of some diffuse cluster radio emission.

79 ASTRONOMY AND ASTROPHYSICS↗

Creating Accurate Methane Emission Inventories through Data-Driven Airborne Survey Strategies

Because natural gas emits less carbon than other fossil fuels, it holds promise as a green energy transition fuel. However, the overall carbon footprint of natural gas is significantly elevated by methane emissions that occur during its production and transmission (Cusworth et al. 2022). Methane “super-emitters,” while comprising only about 1% of sites, are responsible for the majority of oil- and gas-sourced methane emissions, making their detection and mitigation critical in reducing the climate impact of natural gas and in meeting national and global sustainability goals (Sherwin et al. 2024). Yet, despite advancements in detection, significant uncertainties remain regarding the size, frequency, and duration distributions of methane emissions (e.g., Frankenberg et al. 2016, Cusworth et al. 2022, Chen, Sherwin et al. 2022, Conrad et al. 2023, Johnson et al. 2023, Sherwin et al. 2024) underscoring the need for comprehensive emissions inventories segmented by basin across the US. Airborne surveys are well-suited for collecting data to build these comprehensive, basin-level inventories because they allow for extensive spatial coverage, and have the spatial resolution, and the sensitivity to pinpoint individual methane sources. As remote sensing technologies enable rapid basin-scale surveys, it is imperative to establish scientifically and statistically robust standards to generate reliable and actionable emissions inventories. Recent work has shown that differences in airborne sampling strategies, detection technologies, and analysis can lead to large differences between survey conclusions if not correctly accounted for (Chen et al. 2024). This elevates the importance of incorporating proper sampling and analysis techniques when designing a methane emissions monitoring campaign to produce accurate results and facilitate cross-study comparisons. In this paper, we describe a survey strategy designed using the latest conclusions from the literature to align results from different aerial surveys. We identify several sampling and analysis principles, including large sample sizes, balanced sampling across oil and gas production, careful survey area definition, and a unified protocol for analysis, to be vital to producing an unbiased estimate of basin-scale emissions. We present results from a Department of Energy-funded project that deployed this survey strategy in two understudied oil and gas- producing regions in the United States: the Haynesville Basin in Texas and Louisiana, and the Woodford Shale in the Anadarko Basin in Oklahoma.

03 NATURAL GAS↗

Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations

We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from -0.58 to -0.02 Wm -2 , with a mean of -0.27 Wm -2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of -0.35 Wm -2 . Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.

54 ENVIRONMENTAL SCIENCES↗

Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010

Four different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) frequently used in 3-D models are evaluated using a 0-D box model representing the Los Angeles metropolitan region during the California Research at the Nexus of Air Quality and Climate Change (CalNex) 2010 campaign. We constrain the model predictions with measurements from several platforms and compare predictions with particle- and gas-phase observations from the CalNex Pasadena ground site. That site provides a unique opportunity to study aerosol formation close to anthropogenic emission sources with limited recirculation. The model SOA that formed only from the oxidation of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. The Community Multiscale Air Quality (WRF-CMAQ) model (version 5.0.1) provides excellent predictions of secondary inorganic particle species but underestimates the observed SOA mass by a factor of 25 when an older VOC-only parameterization is used, which is consistent with many previous model–measurement comparisons for pre-2007 anthropogenic SOA modules in urban areas. Including SOA from primary semi-volatile and intermediate-volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model–measurement agreement for mass concentration. The results from the three parameterizations show large differences (e.g., a factor of 3 in SOA mass) and are not well constrained, underscoring the current uncertainties in this area. Our results strongly suggest that other precursors besides VOCs, such as P-S/IVOCs, are needed to explain the observed SOA concentrations in Pasadena. All the recent parameterizations overpredict urban SOA formation at long photochemical ages (≈ 3 days) compared to observations from multiple sites, which can lead to problems in regional and especially global modeling. However, reducing IVOC emissions by one-half in the model to better match recent IVOC measurements improves SOA predictions at these long photochemical ages. Among the explicitly modeled VOCs, the precursor compounds that contribute the greatest SOA mass are methylbenzenes. Measured polycyclic aromatic hydrocarbons (naphthalenes) contribute 0.7% of the modeled SOA mass. The amounts of SOA mass from diesel vehicles, gasoline vehicles, and cooking emissions are estimated to be 16–27, 35–61, and 19–35%, respectively, depending on the parameterization used, which is consistent with the observed fossil fraction of urban SOA, 71(±3) %. The relative contribution of each source is uncertain by almost a factor of 2 depending on the parameterization used. In-basin biogenic VOCs are predicted to contribute only a few percent to SOA. A regional SOA background of approximately 2.1 μg m −3 is also present due to the long-distance transport of highly aged OA, likely with a substantial contribution from regional biogenic SOA. The percentage of SOA from diesel vehicle emissions is the same, within the estimated uncertainty, as reported in previous work that analyzed the weekly cycles in OA concentrations (Bahreini et al., 2012; Hayes et al., 2013). However, the modeling work presented here suggests a strong anthropogenic source of modern carbon in SOA, due to cooking emissions, which was not accounted for in those previous studies and which is higher on weekends. Lastly, this work adapts a simple two-parameter model to predict SOA concentration and O/C from urban emissions. This model successfully predicts SOA concentration, and the optimal parameter combination is very similar to that found for Mexico City. This approach provides a computationally inexpensive method for predicting urban SOA in global and climate models. We estimate pollution SOA to account for 26 Tg yr −1 of SOA globally, or 17% of global SOA, one-third of which is likely to be non-fossil.

54 ENVIRONMENTAL SCIENCES↗

Variability and quasi-decadal changes in the methane budget over the period 2000–2012

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH 4 ) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH 4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32]Tg CH 4 yr -1 higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13 CH 4 . However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH 4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH 4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13 CH 4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

58 GEOSCIENCES↗

Aerosols at the poles: an AeroCom Phase II multi-model evaluation

Abstract. Atmospheric aerosols from anthropogenic and natural sources reach the polar regions through long-range transport and affect the local radiation balance. Such transport is, however, poorly constrained in present-day global climate models, and few multi-model evaluations of polar anthropogenic aerosol radiative forcing exist. Here we compare the aerosol optical depth (AOD) at 550 nm from simulations with 16 global aerosol models from the AeroCom Phase II model intercomparison project with available observations at both poles. We show that the annual mean multi-model median is representative of the observations in Arctic, but that the intermodel spread is large. We also document the geographical distribution and seasonal cycle of the AOD for the individual aerosol species: black carbon (BC) from fossil fuel and biomass burning, sulfate, organic aerosols (OAs), dust, and sea-salt. For a subset of models that represent nitrate and secondary organic aerosols (SOAs), we document the role of these aerosols at high latitudes.The seasonal dependence of natural and anthropogenic aerosols differs with natural aerosols peaking in winter (sea-salt) and spring (dust), whereas AOD from anthropogenic aerosols peaks in late spring and summer. The models produce a median annual mean AOD of 0.07 in the Arctic (defined here as north of 60° N). The models also predict a noteworthy aerosol transport to the Antarctic (south of 70° S) with a resulting AOD varying between 0.01 and 0.02. The models have estimated the shortwave anthropogenic radiative forcing contributions to the direct aerosol effect (DAE) associated with BC and OA from fossil fuel and biofuel (FF), sulfate, SOAs, nitrate, and biomass burning from BC and OA emissions combined. The Arctic modelled annual mean DAE is slightly negative (−0.12 W m−2), dominated by a positive BC FF DAE in spring and a negative sulfate DAE in summer. The Antarctic DAE is governed by BC FF. We perform sensitivity experiments with one of the AeroCom models (GISS modelE) to investigate how regional emissions of BC and sulfate and the lifetime of BC influence the Arctic and Antarctic AOD. A doubling of emissions in eastern Asia results in a 33 % increase in Arctic AOD of BC. A doubling of the BC lifetime results in a 39 % increase in Arctic AOD of BC. However, these radical changes still fall within the AeroCom model range.

54 ENVIRONMENTAL SCIENCES↗

Detection and variability of combustion-derived vapor in an urban basin

Abstract. Water emitted during combustion may comprise a significant portion of ambient humidity (&gt; 10 %) in urban areas, where combustion emissions are strongly focused in space and time. Stable water vapor isotopes can be used to apportion measured humidity values between atmospherically transported and combustion-derived water vapor, as combustion-derived vapor possesses an unusually negative deuterium excess value (d-excess, d = δ 2 H − 8 δ 18 O). We investigated the relationship between the d-excess of atmospheric vapor, ambient CO 2 concentrations, and atmospheric stability across four winters in Salt Lake City, Utah. We found a robust inverse relationship between CO 2 excess above background and d-excess on sub-diurnal to seasonal timescales, which was most prominent during periods of strong atmospheric stability that occur during Salt Lake City winter. Using a Keeling-style mixing model approach, and assuming a molar ratio of H 2 O to CO 2 in emissions of 1.5, we estimated the d-excess of combustion-derived vapor in Salt Lake City to be −179 ± 17 ‰, consistent with the upper limit of theoretical estimates. Based on this estimate, we calculate that vapor from fossil fuel combustion often represents 5–10 % of total urban humidity, with a maximum estimate of 16.7 %, consistent with prior estimates for Salt Lake City. Moreover, our analysis highlights that changes in the observed d-excess during periods of high atmospheric stability cannot be explained without a vapor source possessing a strongly negative d-excess value. Further refinements in this humidity apportionment method, most notably empirical validation of the d-excess of combustion vapor or improvements in the estimation of the background d-excess value in the absence of combustion, can yield more certain estimates of the impacts of fossil fuel combustion on urban humidity and meteorology.

54 ENVIRONMENTAL SCIENCES↗

Online characterization of primary and secondary emissions of particulate matter and acidic molecules from a modern fleet of city buses

The potential impact of transitioning from conventional fossil fuel to a non-fossil-fuel vehicle fleet was investigated by measuring primary emissions via extractive sampling of bus plumes and assessing secondary mass formation using the Gothenburg Potential Aerosol Mass (Go:PAM) reactor from 76 in-use transit buses. Online chemical characterization of gaseous and particulate emissions from these buses was conducted using chemical ionization mass spectrometry (CIMS) with acetate as the reagent ion, coupled with the Filter Inlet for Gases and AEROsols (FIGAERO). Acetate reagent ion chemistry selectively ionizes acidic compounds, including organic and inorganic acids, as well as nitrated and sulfated organics. A significant reduction (48 %–98 %) in fresh particle emissions was observed in buses utilizing compressed natural gas (CNG), biodiesels like rapeseed methyl ester (RME) and hydrotreated vegetable oil (HVO), and hybrid-electric HVO (HVO HEV ) compared to diesel (DSL). However, secondary particle formation from photooxidation of emissions was substantial across all the fuel types. The median ratio of particle mass emission factors of aged to fresh emissions increased in the following order: DSL buses at 4.0, HVO buses at 6.7, HVO HEV buses at 10.5, RME buses at 10.8, and CNG buses at 84. Of the compounds that can be identified by CIMS, fresh gaseous emissions from all Euro V/EEV (Enhanced Environmentally friendly Vehicle) buses, regardless of fuel type, were dominated by nitrogen-containing compounds such as nitrous acid (HONO), nitric acid (HNO 3 ), and isocyanic acid (HNCO), alongside small monoacids (C 1 –C 3 ). Notably, the emission of nitrogen-containing compounds was lower in Euro VI buses equipped with more advanced emission control technologies. Secondary gaseous organic acids correlated strongly with gaseous HNO 3 signals (R 2 =0.85–0.99) in Go:PAM, but their moderate to weak correlations with post-photooxidation secondary particle mass suggest that they are not reliable tracers of secondary organic aerosol formation from bus exhaust. Our study highlights that non-regulated compounds and secondary pollutant formation, not currently addressed in legislation, are crucial considerations in the evaluation of environmental impacts of future fuel and engine technology shifts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantification of regional net CO 2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements

Inverse model intercomparison projects (MIPs) provide a chance to assess the uncertainties in inversion estimates arising from various sources. However, accurately quantifying ensemble CO 2 flux errors remains challenging and often relies on the ensemble spread. This study proposes a method for quantifying the errors in regional net surface–atmosphere CO 2 flux estimates from models taken from the Orbiting Carbon Observatory-2 (OCO-2) v10 MIP by using independent airborne CO 2 measurements for the period 2015–2017. We first calculate the root mean square error (RMSE) between the ensemble mean of posterior CO 2 concentrations and airborne observations and then isolate the CO 2 concentration errors caused solely by the ensemble mean of posterior net fluxes by subtracting the observation, representation, and transport errors from seven regions. Our analysis reveals that the flux errors projected onto CO 2 space account for 55 %–85 % of the regional average RMSE over the 3 years, ranging from 0.88 to 1.91 ppm. In five regions, the error estimates based on observations exceed those computed from the ensemble spread of posterior fluxes by a factor of 1.33–1.93, implying an underestimation of the actual flux errors, while their magnitudes are comparable in two regions. The adjoint sensitivity analysis identifies that the underestimation of flux errors is prominent where the magnitudes of fossil fuel emissions exceed those of terrestrial-biosphere fluxes by a factor of 3–31 over the 3 years. This suggests the presence of systematic biases in the inversion estimates associated with errors in the prescribed fossil fuel emissions common to all models. Our study emphasizes the value of airborne measurements for quantifying regional errors in ensemble net CO 2 flux estimates.

54 ENVIRONMENTAL SCIENCES↗