Atmospheric Methane Research Articles

Composition of Methane Cycle Microbial Communities in the Upper Layers of Bottom Sediments of the Kara Sea

Composition of Methane Cycle Microbial Communities in the Upper Layers of Bottom Sediments of the Kara Sea

Evaluating the contribution of methanotrophy kinetics to uncertainty in the soil methane sink

The oxidation of atmospheric methane by soil microbes is an important natural sink for a potent greenhouse gas. However, estimates of the current and future soil methane sink are highly uncertain. Here we assessed the extent to which methanotrophy enzyme kinetics contribute to uncertainty in projections of the soil methane sink. We generated a comprehensive compilation of methanotrophy kinetic data from modern environments and assessed the patterns in kinetic parameters present in natural samples. Our compiled data enabled us to quantify the global soil methane sink through two idealized calculations comparing first-order and Michaelis–Menten models of kinetics. We show that these two kinetic models diverge only under high atmospheric CH4 scenarios, where first-order rate constants slightly overestimate the soil methane sink size, but produce similar predictions at modern atmospheric concentrations. Our compilation also shows that the kinetics of methanotrophy in natural soil samples is highly variable—both the V max (oxidation rate at saturation) and KM (half-saturation constant) in natural samples span over six orders of magnitude. However, accounting for the correlation we observe between V max and KM reduces the range of calculated uptake rates by as much as 96%. Additionally, our results indicate that variation in enzyme kinetics introduces a similar magnitude of variation in the calculated soil methane sink as temperature sensitivity. Systematic sampling of methanotroph kinetic parameters at multiple spatial scales should therefore be a key objective for closing the budget on the global soil methane sink.

The novel regulator HdrR controls the transcription of the heterodisulfide reductase operon hdrBCA in Methanosarcina barkeri.

Methanogenic archaea play a key role in the global carbon cycle because these microorganisms remineralize organic compounds in various anaerobic environments. The microorganism Methanosarcina barkeri is a metabolically versatile methanogen, which can utilize acetate, methanol, and H2/CO2 to synthesize methane. However, the regulatory mechanisms underlying methanogenesis for different substrates remain unknown. In this study, RNA-seq analysis was used to investigate M. barkeri growth and gene transcription under different substrate regimes. According to the results, M. barkeri showed the best growth under methanol, followed by H2/CO2 and acetate, and these findings corresponded well with the observed variations in genes transcription abundance for different substrates. In addition, we identified a novel regulator, MSBRM_RS03855 (designated as HdrR), which specifically activates the transcription of the heterodisulfide reductase hdrBCA operon in M. barkeri. HdrR was able to bind to the hdrBCA operon promoter to regulate transcription. Furthermore, the structural model analyses revealed a helix-turn-helix domain, which is likely involved in DNA binding. Taken together, HdrR serves as a model to reveal how certain regulatory factors control the expression of key enzymes in the methanogenic pathway.IMPORTANCEThe microorganism Methanosarcina barkeri has a pivotal role in the global carbon cycle and contributes to global temperature homeostasis. The consequences of biological methanogenesis are far-reaching, including impacts on atmospheric methane and CO2 concentrations, agriculture, energy production, waste treatment, and human health. As such, reducing methane emissions is crucial to meeting set climate goals. The methanogenic activity of certain microorganisms can be drastically reduced by inhibiting the transcription of the hdrBCA operon, which encodes heterodisulfide reductases. Here, we provide novel insight into the mechanisms regulating hdrBCA operon transcription in the model methanogen M. barkeri. The results clarified that HdrR serves as a regulator of heterodisulfide reductase hdrBCA operon transcription during methanogenesis, which expands our understanding of the unique regulatory mechanisms that govern methanogenesis. The findings presented in this study can further our understanding of how genetic regulation can effectively reduce the methane emissions caused by methanogens.

Economics of enhanced methane oxidation relative to carbon dioxide removal

Mitigating short-term global warming is imperative, and a key strategy involves reducing atmospheric methane (CH4) due to its high radiative forcing and short lifespan. This objective can be achieved through methods such as oxidising methane at its source or implementing enhanced oxidation techniques to reduce atmospheric CH4 concentrations. In this study, we use a range of metrics to analyse both the impact and value of enhanced CH4 oxidation relative to carbon dioxide (CO2) removal on global temperature. We apply these metrics to a select group of model studies of thermal-catalytic, photocatalytic, biological and capture-based oxidation processes under different greenhouse gas (GHG) concentrations. Using a target cost of €220-1000/tCO2 for CO2 removal, our findings indicate that metrics valuing enhanced oxidation techniques based on their contribution to mitigating the long-term level of warming show these techniques are uncompetitive with CO2 removal. However, when using metrics that value enhanced oxidation of CH4 based on its impact on the immediate rate of warming, photocatalytic methods may be competitive with CO2 removal, whereas biofiltration, thermal-catalytic oxidation and capture-based units remain uncompetitive. We conclude that if the policy goal is to target the immediate rate of warming, it may be more valuable to incentivise CO2 removal and enhanced oxidation of methane under separate GHG targets.

Distinct structure, assembly, and gene expression of microplankton in two Arctic estuaries with varied terrestrial inputs

The Laptev Sea is a major Marginal Sea in the Western Arctic Ocean. The Arctic amplification brought by global warming influences the hydrological properties of rivers passing through the permafrost zone, which would alter the biological community structure at continental margin. In this study, the structure, assembly, and gene expression of planktonic microbial communities in two estuaries (Protoka Ularovskaya River Estuary, PURE; Lena River Estuary, LRE) of Laptev Sea were examined to investigate the environmental effects of polar rivers. PURE and LRE exhibited distinct environmental characteristics: low temperature and high salinity for PURE, and high temperature and low salinity for LRE, influenced by runoff size. Salinity more closely influenced microbial communities in LRE, with freshwater species playing a significant role in community composition. The findings revealed differences between two estuaries in community composition and diversity. Prokaryotes and microeukaryotes had shown different assembly patterns in response to habitat changes caused by terrestrial freshwater input. Furthermore, compared with the PURE, the co-occurrence and inter-domain network of the LRE, which was more affected by terrestrial input, was more complex and stable. Functional gene prediction revealed a higher gene expression of methane metabolism in LRE than in PURE, particularly those related to methane oxidation, and this conclusion could help better explore the impact of global warming on the methane cycle in the Arctic Marginal Seas. This study explored the increased freshwater runoffs under the background of global warming dramatically affect Arctic microplankton communities from community structure, assembly and gene expression aspects.

Active anaerobic methane oxidation in the groundwater table fluctuation zone of rice paddies

Rice paddies are globally important sources of methane emissions and also active regions for methane consumption. However, the impact of fluctuating groundwater levels on methane cycling has received limited attention. In this study, we delved into the activity and microbial mechanisms underlying anaerobic oxidation of methane (AOM) in paddy fields. A comprehensive approach was employed, including 13C stable isotope assays, inhibition experiments, real-time quantitative reverse transcription PCR, metagenomic sequencing, and binning technology. Geochemical profiles revealed the abundant coexistence of both methane and electron acceptors in the groundwater table fluctuation (GTF) zone, at a depth of 40–60 cm. Notably, the GTF zone exhibited the highest rate of AOM, potentially linked to the reduction of iron oxides and nitrate. Within this zone, Candidatus Methanoperedens (belonging to the ANME-2d group) dominated the Archaea population, accounting for a remarkable 85.4 %. Furthermore, our results from inhibition experiments, RT-qPCR, and metagenome-assembled genome (MAG) analysis highlighted the active role of Ca. Methanoperedens GTF50 in the GTF zone. This microorganism could independently mediate AOM process through the intriguing “reverse methanogenesis” pathway. Considering the similarity in geochemical conditions across different paddy fields, it is likely that Ca. Methanoperedens-mediated AOM is prevalent in the GTF zones.

Physiological basis for atmospheric methane oxidation and methanotrophic growth on air

Atmospheric methane oxidizing bacteria (atmMOB) constitute the sole biological sink for atmospheric methane. Still, the physiological basis allowing atmMOB to grow on air is not well understood. Here we assess the ability and strategies of seven methanotrophic species to grow with air as sole energy, carbon, and nitrogen source. Four species, including three outside the canonical atmMOB group USCα, enduringly oxidized atmospheric methane, carbon monoxide, and hydrogen during 12 months of growth on air. These four species exhibited distinct substrate preferences implying the existence of multiple metabolic strategies to grow on air. The estimated energy yields of the atmMOB were substantially lower than previously assumed necessary for cellular maintenance in atmMOB and other aerobic microorganisms. Moreover, the atmMOB also covered their nitrogen requirements from air. During growth on air, the atmMOB decreased investments in biosynthesis while increasing investments in trace gas oxidation. Furthermore, we confirm that a high apparent specific affinity for methane is a key characteristic of atmMOB. Our work shows that atmMOB grow on the trace concentrations of methane, carbon monoxide, and hydrogen present in air and outlines the metabolic strategies that enable atmMOB to mitigate greenhouse gases.

Opinion: A research roadmap for exploring atmospheric methane removal via iron salt aerosol

Abstract. The escalating climate crisis requires rapid action to reduce the concentrations of atmospheric greenhouse gases and lower global surface temperatures. Methane will play a critical role in near-term warming due to its high radiative forcing and short atmospheric lifetime. Methane emissions have accelerated in recent years, and there is significant risk and uncertainty associated with the future growth in natural emissions. The largest natural sink of methane occurs through oxidation reactions with atmospheric hydroxyl and chlorine radicals. Enhanced atmospheric oxidation could be a potential approach to remove atmospheric methane. One method proposes the addition of iron salt aerosol (ISA) to the atmosphere, mimicking a natural process proposed to occur when mineral dust mixes with chloride from sea spray to form iron chlorides, which are photolyzed by sunlight to produce chlorine radicals. Under the right conditions, lofting ISA into the atmosphere could potentially reduce atmospheric methane concentrations and lower global surface temperatures. Recognizing that potential atmospheric methane removal must only be considered an additive measure – in addition to, not replacing, crucial anthropogenic greenhouse gas emission reductions and carbon dioxide removal – roadmaps can be a valuable tool to organize and streamline interdisciplinary and multifaceted research to efficiently move towards understanding whether an approach may be viable and socially acceptable or if it is nonviable and further research should be deprioritized. Here we present a 5-year research roadmap to explore whether ISA enhancement of the chlorine radical sink could be a viable and socially acceptable atmospheric methane removal approach.

Interpreting the Seasonality of Atmospheric Methane

AbstractSurface and satellite observations of atmospheric methane show smooth seasonal behavior in the Southern Hemisphere driven by loss from the hydroxyl (OH) radical. However, observations in the Northern Hemisphere show a sharp mid‐summer increase that is asymmetric with the Southern Hemisphere and not captured by the default configuration of the GEOS‐Chem chemical transport model. Using an ensemble of 22 OH model estimates and 24 wetland emission inventories in GEOS‐Chem, we show that the magnitude, latitudinal distribution, and seasonality of Northern Hemisphere wetland emissions are critical for reproducing the observed seasonality of methane in that hemisphere, with the interhemispheric OH ratio playing a lesser role. Reproducing the observed seasonality requires a wetland emission inventory with ∼80 Tg a−1 poleward of 10°N including significant emissions in South Asia, and an August peak in boreal emissions persisting into autumn. In our 24‐member wetland emission ensemble, only the LPJ‐wsl MERRA‐2 inventory has these attributes.

Anurans and their contribution to agriculture: a review

Anurans and their contribution to agriculture: a review

Holed up, but thriving: Impact of multitrophic cryoconite communities on glacier elemental cycles

Cryoconite holes (water and sediment-filled depressions), found on glacier surfaces worldwide, serve as reservoirs of microbes, carbon, trace elements, and nutrients, transferring these components downstream via glacier hydrological networks. Through targeted amplicon sequencing of carbon and nitrogen cycling genes, coupled with functional inference-based methods, we explore the functional diversity of these mini-ecosystems within Antarctica and the Himalayas. These regions showcase distinct environmental gradients and experience varying rates of environmental change influenced by global climatic shifts. Analysis revealed a diverse array of photosynthetic microorganisms, including Stramenopiles, Cyanobacteria, Rhizobiales, Burkholderiales, and photosynthetic purple sulfur Proteobacteria. Functional inference highlighted the high potential for carbohydrate, amino acid, and lipid metabolism in the Himalayan region, where organic carbon concentrations surpassed those in Antarctica by up to 2 orders of magnitude. Nitrogen cycling processes, including fixation, nitrification, and denitrification, are evident, with Antarctic cryoconite exhibiting a pronounced capacity for nitrogen fixation, potentially compensating for the limited nitrate concentrations in this region. Processes associated with the respiration of elemental sulfur and inorganic sulfur compounds such as sulfate, sulfite, thiosulfate, and sulfide suggest the presence of a complete sulfur cycle. The Himalayan region exhibits a higher potential for sulfur cycling, likely due to the abundant sulfate ions and sulfur-bearing minerals in this region. The capability for complete iron cycling through iron oxidation and reduction reactions was also predicted. Methanogenic archaea that produce methane during organic matter decomposition and methanotrophic bacteria that utilize methane as carbon and energy sources co-exist in the cryoconite, suggesting that these niches support the complete cycling of methane. Additionally, the presence of various microfauna suggests the existence of a complex food web. Collectively, these results indicate that cryoconite holes are self-sustaining ecosystems that drive elemental cycles on glaciers and potentially control carbon, nitrogen, sulfur, and iron exports downstream.

Reducing Methane Emissions with Humic Acid–Iron Complex in Rice Cultivation: Impact on Greenhouse Gas Emissions and Rice Yield

Methane emissions from flooded rice paddies are a major source of atmospheric methane and represent a significant greenhouse gas with high climate-forcing potential due to anthropogenic activities globally. For sustainable agriculture, it is necessary to find effective methods for mitigating greenhouse gas emissions without reducing crop productivity. We investigated mechanisms to reduce methane emissions during rice cultivation by applying rice straw, rice husk biochar, humic acid, and a humic acid–iron complex, assessing greenhouse gases and rice yield over a single season. The results demonstrated that the treatment plots with rice straw and the humic acid–iron complex significantly reduced methane emissions (563 ± 113.9 kg ha−1) by 34.4% compared to plots treated with rice straw alone (859 ± 126.4 kg ha−1). Rice yield was not compromised compared to the control group treated with only NPK fertilizer, and growth in terms of plant height and tiller number was enhanced in the plots treated with rice straw and the humic acid–iron complex. Conversely, the plots treated solely with rice husk biochar and humic acid did not show a methane reduction effect when compared to the NPK treatment. The humic acid–iron complex has demonstrated potential as a methane mitigation agent with practical applicability in the field, warranting further long-term studies to validate its effectiveness.

Unraveling the dynamics of atmospheric methane: the impact of anthropogenic and natural emissions

The reduction in methane concentration is crucial for achieving the goals of the Paris agreement. However, its annual growth rate is unstable, and understanding the reasons for changes in methane growth is essential for climate policy-making. Currently, there is considerable uncertainty regarding its attribution. Here, we utilize multi-source data and optimal fingerprinting methods to detect the contributions of several key drivers to the methane trend and interannual variability. We find that the methane growth trend is primarily influenced by anthropogenic emissions, while interannual variability is predominantly determined by wetland and biomass burning emissions. This result underscores the central role of anthropogenic emissions in methane dynamics, providing confidence in the effectiveness of human efforts to control methane atmospheric concentrations through emission reductions. It also helps alleviate concerns about the recent surge in atmospheric methane concentration, as it may be a short-term peak caused by increased wetland emissions rather than a long-term change.

Extraction, purification, and clumped isotope analysis of methane (Δ13CDH3 and Δ12CD2H2) from sources and the atmosphere

Abstract. Measurements of the clumped isotope anomalies (Δ13CDH3 and Δ12CD2H2) of methane have shown potential for constraining methane sources and sinks. At Utrecht University, we use the Thermo Scientific Ultra high-resolution isotope-ratio mass spectrometer to measure the clumped isotopic composition of methane emitted from various sources and directly from the atmosphere. We have developed an extraction system with three sections for extracting and purifying methane from high (> 1 %), medium (0.1 % to 1 %), and low-concentration (< 0.1 %) samples, including atmospheric air (∼ 2 ppm = 0.0002 %). Depending on the methane concentration, a quantity of sample gas is processed that delivers 3 ± 1 mL of pure methane, which is the quantity typically needed for one clumped isotope measurement. For atmospheric air with a methane mole fraction of 2 ppm, we currently process up to 1100 L of air. The analysis is performed on pure methane, using a dual-inlet setup. The complete measurement time for all isotope signatures is about 20 h for one sample. The mean internal precision values of sample measurements are 0.3 ± 0.1 ‰ for Δ13CDH3 and 2.4 ± 0.8 ‰ for Δ12CD2H2. The long-term reproducibility, obtained from repeated measurements of a constant target gas, over almost 3 years, is around 0.15 ‰ for Δ13CDH3 and 1.2 ‰ for Δ12CD2H2. The measured clumping anomalies are calibrated via the Δ13CDH3 and Δ12CD2H2 values of the reference CH4 used for the dual-inlet measurements. These were determined through isotope equilibration experiments at temperatures between 50 and 450 °C. We describe in detail the optimized sampling, extraction, purification, and measurement technique followed in our laboratory to measure the clumping anomalies of methane precisely and accurately. This paper highlights the extraction and one of the first global measurements of the clumping anomalies of atmospheric methane.

Exogenous Carbon is Unlikely to be the Source of Methane Microseepage Emissions on Mars

A complete understanding of methane in the atmosphere of Mars requires information on putative sources. Organic carbon derived from meteoritic sources, such as interplanetary dust particles (IDPs), over geologic time is the best-defined source of organic carbon on the surface of Mars. Here we examine two different mechanisms for degrading this material to produce methane (1) Ultraviolet photolysis and (2) thermal decomposition. Neither of these mechanisms can produce sufficient methane under realistic assumptions to explain observed methane at Gale Crater, suggesting that IDPs are not the primary source material producing methane on Mars.

Deep understanding the formation of MnCoOx in-situ grown on foam nickel towards efficient lean methane catalytic oxidation

Methane is the second largest greenhouse gas in the world, with a stronger greenhouse effect than carbon dioxide. The efficient elimination of methane in the atmosphere has important engineering significance in slowing down global temperature rise, energy resource utilization, collaborative control of pollutants, and promoting technological innovation. In this work, a general hydrothermal synthesis method was introduced to in-situ construct four different morphologies of MnCoOx (including rod-, spherical-, filamentous- and bulk-shape) on foam nickel (NF). The synthesis of MnCoOx/NF with different morphologies was due to changes in NF pretreatment conditions and precipitants, which affected the nucleation and growth rates of MnCoOx, ultimately resulting in different morphologies. When the four different morphologies of MnCoOx/NF were used as catalysts for lean methane catalytic oxidation, MnCoOx/NF-r exhibited the best excellent catalytic activity, and the T90 occurred at 428 °C in space velocity of 48,000 mL g−1 h−1. Such an outstanding performance was attributed to the unique properties of the MnCoOx/NF-r including the larger surface area and more oxygen vacancies for providing more active sites and a higher oxygen migration rate, which was very beneficial for improving the catalytic oxidation performance of methane.

Using Different Spectroscopic Databases to Model the Transfer of Radiation in the Near-IR Range and Retrieve the Content of Methane in the Atmosphere

Using Different Spectroscopic Databases to Model the Transfer of Radiation in the Near-IR Range and Retrieve the Content of Methane in the Atmosphere

High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills

Abstract. We quantify 2019 annual mean methane emissions in the contiguous US (CONUS) at 0.25° × 0.3125° resolution by inverse analysis of atmospheric methane columns measured by the Tropospheric Monitoring Instrument (TROPOMI). A gridded version of the US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) serves as the basis for the prior estimate for the inversion. We optimize emissions and quantify observing system information content for an eight-member inversion ensemble through analytical minimization of a Bayesian cost function. We achieve high resolution with a reduced-rank characterization of the observing system that optimally preserves information content. Our optimal (posterior) estimate of anthropogenic emissions in CONUS is 30.9 (30.0–31.8) Tg a−1, where the values in parentheses give the spread of the ensemble. This is a 13 % increase from the 2023 GHGI estimate for CONUS in 2019. We find emissions for livestock of 10.4 (10.0–10.7) Tg a−1, for oil and gas of 10.4 (10.1–10.7) Tg a−1, for coal of 1.5 (1.2–1.9) Tg a−1, for landfills of 6.9 (6.4–7.5) Tg a−1, for wastewater of 0.6 (0.5–0.7), and for other anthropogenic sources of 1.1 (1.0–1.2) Tg a−1. The largest increase relative to the GHGI occurs for landfills (51 %), with smaller increases for oil and gas (12 %) and livestock (11 %). These three sectors are responsible for 89 % of posterior anthropogenic emissions in CONUS. The largest decrease (28 %) is for coal. We exploit the high resolution of our inversion to quantify emissions from 70 individual landfills, where we find emissions are on median 77 % larger than the values reported to the EPA's Greenhouse Gas Reporting Program (GHGRP), a key data source for the GHGI. We attribute this underestimate to overestimated recovery efficiencies at landfill gas facilities and to under-accounting of site-specific operational changes and leaks. We also quantify emissions for the 48 individual states in CONUS, which we compare to the GHGI's new state-level inventories and to independent state-produced inventories. Our posterior emissions are on average 27 % larger than the GHGI in the largest 10 methane-producing states, with the biggest upward adjustments in states with large oil and gas emissions, including Texas, New Mexico, Louisiana, and Oklahoma. We also calculate emissions for 95 geographically diverse urban areas in CONUS. Emissions for these urban areas total 6.0 (5.4–6.7) Tg a−1 and are on average 39 (27–52) % larger than a gridded version of the 2023 GHGI, which we attribute to underestimated landfill and gas distribution emissions.

Geogenic Phosphorus Enrichment in Groundwater due to Anaerobic Methane Oxidation-Coupled Fe(III) Oxide Reduction.

Accumulation of geogenic phosphorus (P) in groundwater is an emerging environmental concern, which is closely linked to coupled processes involving FeOOH and organic matter under methanogenic conditions. However, it remains unclear how P enrichment is associated with methane cycling, particularly the anaerobic methane oxidation (AMO). This study conducted a comprehensive investigation of carbon isotopes in dissolved inorganic carbon (DIC), CO2, and CH4, alongside Fe isotopes, microbial communities, and functions in quaternary aquifers of the central Yangtze River plain. The study found that P concentrations tended to increase with Fe(II) concentrations, δ56Fe, and δ13C-DIC, suggesting P accumulation due to the reductive dissolution of FeOOH under methanogenic conditions. The positive correlations of pmoA gene abundance versus δ13C-CH4 and Fe concentrations versus δ13C-CH4, and the prevalent presence of Candidatus_Methanoperedens, jointly demonstrated the potential significance of Fe(III)-mediated AMO process (Fe-AMO) alongside traditional methanogenesis. The increase of P concentration with δ13C-CH4 value, pmoA gene abundance, and Fe concentration suggested that the Fe-AMO process facilitated P enrichment in groundwater. Redundancy analysis confirmed this assertion, identifying P concentration as the primary determinant and the cooperative influence of Fe-AMO microorganisms such as Candidatus_Methanoperedens and Geobacter on P enrichment. Our work provided new insights into P dynamics in subsurface environments.

Cost modeling of photocatalytic decomposition of atmospheric methane and nitrous oxide

Abstract The photocatalytic decomposition of atmospheric methane (CH4) and nitrous oxide (N2O) could be valuable tools for mitigating climate change; however, to date, few photocatalyst deployment strategies have had their costs modeled. Here, we construct basic cost models of three photocatalytic CH4 and N2O decomposition systems: 1) a ground-based solar system with natural airflow over photocatalyst-painted rooftops, 2) a ground-based LED-lit system with fan-driven airflow, and 3) an aerosol-based solar system on solid particles dispersed in the atmosphere. Each model takes as inputs the photocatalyst’s apparent quantum yield (AQY; a measure of how efficiently photons drive a desired chemical reaction) and the local CH4 or N2O concentration. Each model calculates an overall rate of greenhouse gas drawdown and returns a levelized cost of greenhouse gas removal per equivalent ton of carbon dioxide (tCO2e). Based on prior studies of atmospheric carbon dioxide removal, we adopt $100/tCO2e as a target cost.

We estimate that painting rooftops with photocatalysts might meet the target cost for decomposition of >10ppm CH4 with catalyst AQYs >4%. If painting and cleaning costs were reduced by a factor of ~3 from our scenario, removal of ambient CH4 could meet the cost target with AQYs >1% and removal of ambient N2O could do so with AQYs >0.1%. 
Fan-driven systems with LED illumination appear to be very challenging, achieving removal costs <$100/tCO2e only for AQYs of >10% for CH4 and >1% for N2O. Dispersing photocatalytic aerosols in the troposphere could be cost-effective with AQYs of >0.4% for ambient CH4 or >0.04% for ambient N2O. However, the mass of aerosols required is large and their side effects and social acceptability are uncertain. We note that, for any system, AQYs on the order of 1% will likely be extremely challenging to achieve with such dilute reagents.