Project description:Methane emissions from lakes and reservoirs are a major natural source in the global budget of atmospheric CH4. A large fraction of these emissions are due to diffusive transport of CH4 from surface waters to the atmosphere. It was suggested recently that CH4 production in the oxic surface waters is required to compensate for diffusive CH4 emissions from lakes. In contrast, we demonstrate here that typical diffusive CH4-fluxes from sediments in shallow water zones, Fsed,S, suffice to explain CH4 emissions to the atmosphere. Our analysis is based on the combination of an exceptional data set on surface concentrations of CH4 with a mass balance model of CH4 that is focused on the surface mixed layer and considers CH4-fluxes from sediments, lateral transport, gas exchange with the atmosphere, and includes temperature dependencies of sediment fluxes and gas exchange. Fsed,S not only explains observed surface CH4 concentrations but also concentration differences between shallow and open water zones, and the seasonal variability of emissions and lateral concentration distributions. Hence, our results support the hypothesis that diffusive fluxes from shallow sediments and not oxic methanogenesis are the main source of the CH4 in the surface waters and the CH4 emitted from lakes and reservoirs.
Project description:Methyl bromide (CH3Br) and methyl chloride (CH3Cl) are major carriers of atmospheric bromine and chlorine, respectively, which can catalyze stratospheric ozone depletion. However, in our current understanding, there are missing sources associated with these two species. Here we investigate the effect of copper(II) on CH3Br and CH3Cl production from soil, seawater and model organic compounds: catechol (benzene-1,2-diol) and guaiacol (2-methoxyphenol). We show that copper sulfate (CuSO4) enhances CH3Br and CH3Cl production from soil and seawater, and it may be further amplified in conjunction with hydrogen peroxide (H2O2) or solar radiation. This represents an abiotic production pathway of CH3Br and CH3Cl perturbed by anthropogenic application of copper(II)-based chemicals. Hence, we suggest that the widespread application of copper(II) pesticides in agriculture and the discharge of anthropogenic copper(II) to the oceans may account for part of the missing sources of CH3Br and CH3Cl, and thereby contribute to stratospheric halogen load.
Project description:Emissions of microbially produced methane (CH4) from lake sediments are a major source of this potent greenhouse gas to the atmosphere. The rates of CH4 production and emission are believed to be influenced by electron acceptor distributions and organic carbon contents, which in turn are affected by anthropogenic inputs of nutrients leading to eutrophication. Here, we investigate how eutrophication influences the abundance and community structure of CH4 producing Archaea and methanogenesis pathways across time-resolved sedimentary records of five Swiss lakes with well-characterized trophic histories. Despite higher CH4 concentrations which suggest higher methanogenic activity in sediments of eutrophic lakes, abundances of methanogens were highest in oligotrophic lake sediments. Moreover, while the methanogenic community composition differed significantly at the lowest taxonomic levels (OTU), depending on whether sediment layers had been deposited under oligotrophic or eutrophic conditions, it showed no clear trend in relation to in situ distributions of electron acceptors. Remarkably, even though methanogenesis from CO2-reduction was the dominant pathway in all sediments based on carbon isotope fractionation values, taxonomic identities, and genomes of resident methanogens, CO2-reduction with hydrogen (H2) was thermodynamically unfavorable based on measured reactant and product concentrations. Instead, strong correlations between genomic abundances of CO2-reducing methanogens and anaerobic bacteria with potential for extracellular electron transfer suggest that methanogenic CO2-reduction in lake sediments is largely powered by direct electron transfer from syntrophic bacteria without involvement of H2 as an electron shuttle.
Project description:Coal mining is a major source of global anthropogenic methane (CH4) emissions contributing to climate change. The volume of coal traded has reached new heights in recent years, however, existing studies have ignored the impact of CH4 emissions induced by coal trade. This study investigates the spatiotemporal evolution of global coal trade-related CH4 emissions from 1990 to 2021. Global coal trade-related CH4 emissions increased 3.5 times from around 1.4 Tg to 6.1 Tg during this period. Examining past global coal trade activities reveals the extraordinary growth and prominence of the Asia-Pacific region. Australia, Indonesia, and Russia dominated trade-related CH4 emissions, accounting for 80.4% in 2021. Hub economies have the potential to drive significant mitigation of trade-related CH4 emissions through energy consumption transitions, the deployment of emissions mitigation technologies, and changes in trade structure. Our findings shed light on identifying trade-induced emissions hotspots and managing coal-related CH4 to mitigate climate change.
Project description:Wetland methane (CH4) emissions ([Formula: see text]) are important in global carbon budgets and climate change assessments. Currently, [Formula: see text] projections rely on prescribed static temperature sensitivity that varies among biogeochemical models. Meta-analyses have proposed a consistent [Formula: see text] temperature dependence across spatial scales for use in models; however, site-level studies demonstrate that [Formula: see text] are often controlled by factors beyond temperature. Here, we evaluate the relationship between [Formula: see text] and temperature using observations from the FLUXNET-CH4 database. Measurements collected across the globe show substantial seasonal hysteresis between [Formula: see text] and temperature, suggesting larger [Formula: see text] sensitivity to temperature later in the frost-free season (about 77% of site-years). Results derived from a machine-learning model and several regression models highlight the importance of representing the large spatial and temporal variability within site-years and ecosystem types. Mechanistic advancements in biogeochemical model parameterization and detailed measurements in factors modulating CH4 production are thus needed to improve global CH4 budget assessments.
Project description:Large greenhouse gas emissions occur via the release of carbon dioxide (CO2) and methane (CH4) from the surface layer of lakes. Such emissions are modeled from the air-water gas concentration gradient and the gas transfer velocity (k). The links between k and the physical properties of the gas and water have led to the development of methods to convert k between gases through Schmidt number normalization. However, recent observations have found that such normalization of apparent k estimates from field measurements can yield different results for CH4 and CO2. We estimated k for CO2 and CH4 from measurements of concentration gradients and fluxes in four contrasting lakes and found consistently higher (on an average 1.7 times) normalized apparent k values for CO2 than CH4. From these results, we infer that several gas-specific factors, including chemical and biological processes within the water surface microlayer, can influence apparent k estimates. We highlight the importance of accurately measuring relevant air-water gas concentration gradients and considering gas-specific processes when estimating k.
Project description:Airborne measurements offer an effective way to quantify urban emissions of greenhouse gases (GHGs). However, it may be challenging due to the requirement of high measurement precision and sufficiently enhanced signals. We developed a new active AirCore system based on the previous unmanned aerial vehicle (UAV) version, which is capable of sampling atmospheric air for several hours aboard a lightweight aircraft for postflight simultaneous and continuous measurements of N2O, CH4, CO2, and CO. We performed 13 flights over the urban areas of Groningen, Utrecht, and Rotterdam and evaluated the aircraft-based AirCore measurements against in situ continuous CH4 measurements. One flight was selected for each of the three urban areas to quantify the emissions of N2O and CH4. Compared to the Dutch inventory, the estimated N2O emissions (364 ± 143 kg h-1) from the Rotterdam area are ∼3 times larger, whereas those for Groningen (95 ± 90 kg h-1) and Utrecht (32 ± 16 kg h-1) are not significantly different. The estimated CH4 emissions for all three urban areas (Groningen: 2534 ± 1774 kg CH4 hr-1, Utrecht: 1440 ± 628 kg CH4 hr-1, and Rotterdam: 2419 ± 922 kg CH4 hr-1) are not significantly different from the Dutch inventory. The innovative aircraft-based active AirCore sampling system provides a robust means of high-precision and continuous measurements of multiple gas species, which is useful for quantifying GHG emissions from urban areas.
Project description:Globally, rivers and streams are important sources of carbon dioxide and methane, with small rivers contributing disproportionately relative to their size. Previous research on greenhouse gas (GHG) emissions from surface water lacks mechanistic understanding of contributions from streambed sediments. We hypothesise that streambeds, as known biogeochemical hotspots, significantly contribute to the production of GHGs. With global climate change, there is a pressing need to understand how increasing streambed temperatures will affect current and future GHG production. Current global estimates assume linear relationships between temperature and GHG emissions from surface water. Here we show non-linearity and threshold responses of streambed GHG production to warming. We reveal that temperature sensitivity varies with substrate (of variable grain size), organic matter (OM) content and geological origin. Our results confirm that streambeds, with their non-linear response to projected warming, are integral to estimating freshwater ecosystem contributions to current and future global GHG emissions.
Project description:There are limited data for greenhouse gas (GHG) emissions from smallholder agricultural systems in tropical peatlands, with data for non-CO2 emissions from human-influenced tropical peatlands particularly scarce. The aim of this study was to quantify soil CH4 and N2 O fluxes from smallholder agricultural systems on tropical peatlands in Southeast Asia and assess their environmental controls. The study was carried out in four regions in Malaysia and Indonesia. CH4 and N2 O fluxes and environmental parameters were measured in cropland, oil palm plantation, tree plantation and forest. Annual CH4 emissions (in kg CH4 ha-1 year-1 ) were: 70.7 ± 29.5, 2.1 ± 1.2, 2.1 ± 0.6 and 6.2 ± 1.9 at the forest, tree plantation, oil palm and cropland land-use classes, respectively. Annual N2 O emissions (in kg N2 O ha-1 year-1 ) were: 6.5 ± 2.8, 3.2 ± 1.2, 21.9 ± 11.4 and 33.6 ± 7.3 in the same order as above, respectively. Annual CH4 emissions were strongly determined by water table depth (WTD) and increased exponentially when annual WTD was above -25 cm. In contrast, annual N2 O emissions were strongly correlated with mean total dissolved nitrogen (TDN) in soil water, following a sigmoidal relationship, up to an apparent threshold of 10 mg N L-1 beyond which TDN seemingly ceased to be limiting for N2 O production. The new emissions data for CH4 and N2 O presented here should help to develop more robust country level 'emission factors' for the quantification of national GHG inventory reporting. The impact of TDN on N2 O emissions suggests that soil nutrient status strongly impacts emissions, and therefore, policies which reduce N-fertilisation inputs might contribute to emissions mitigation from agricultural peat landscapes. However, the most important policy intervention for reducing emissions is one that reduces the conversion of peat swamp forest to agriculture on peatlands in the first place.