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DOE OSTI2023

The future of ship engines: Renewable fuels and enabling technologies for decarbonization

Shipping is one of the most efficient transportation modes for moving freight globally. International regulations concerning decarbonization and emission reduction goals drive rapid innovations to meet the 2030 and 2050 greenhouse gas reduction targets. The internal combustion engines used for marine vessels are among the most efficient energy conversion systems. Internal combustion engines dominate the propulsion system architectures for marine shipping, and current marine engines will continue to serve for several decades. However, to meet the aggressive goals of low-carbon-intensity shipping, there is an impetus for further efficiency improvement and achieving net zero greenhouse gas emissions. These factors drive the advancements in engine technologies, low-carbon fuels and fueling infrastructure, and emissions control systems. This editorial presents a perspective on the future of ship engines and the role of low-life cycle-carbon-fuels in decarbonizing the marine shipping sector. A selection of zero-carbon, net-zero carbon, and low-lifecycle-carbon-fuels are reviewed. This work focuses on the opportunities and challenges of displacing distillate fossil fuels for decarbonizing marine shipping. In conclusion, enabling technologies such as next-generation air handling, fuel injection systems, and advanced combustion modes are discussed in the context of their role in the future of low-CO 2 intensity shipping.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2026

Data for Impacts of Legacy and Contemporary Nitrogen Inputs on N2O and CO2 Emissions in Miscanthus and Maize Cultivated Soils

Nutrient inputs influence the sustainability of bioenergy crop production through contemporary (shortly after addition) and legacy effects (persisting over years) on microbial nitrogen (N) and carbon cycling, which contribute to greenhouse gas emissions. However, the relative importance of contemporary and legacy effects and how that could vary by crop functional types is poorly understood. Considering its rhizomatous roots and perennial growth, we hypothesized that Miscanthus × giganteu s ( M × g ) would be more sensitive to legacy N fertilization and the historical context of its environment than an annual crop like maize. To test this hypothesis, we examined the effects of legacy and contemporary N inputs on nitrous oxide (N2O) and carbon dioxide (CO2) emissions, as well as key N cycling genes in soils where M × g and maize were grown. A 150-day soil incubation experiment was conducted using soils from a long-term M × g and maize fertility experiment with three historic N fertilization rates (0, 112, and 336 kg N ha−1 year−1) and a contemporary amendment (60 mg N kg−1) with negative control (0 mg N kg−1). We observed significant increases in cumulative N2O emissions in M × g soils relative to maize soils, particularly at higher legacy fertilization rates, while contemporary N had no significant effect. Bacterial amoA gene abundance, which plays a significant role in nitrification in nutrient-rich soils, also increased with higher legacy fertilization rates in M × g soils but was unaffected by the contemporary N. In maize soils, legacy and contemporary N did not significantly affect N2O emissions, but cumulative CO2 emissions and amoA gene abundance significantly increased. The abundances of norB genes were not significantly influenced by either legacy fertilization or contemporary N amendments in either soil. Our findings demonstrate the greater importance of fertilization history over contemporary N in mediating soil N2O emissions, particularly for perennial bioenergy crops.

Carbon↗

DOE OSTI2023

Formation of hydrocarbons favored by high pressure at subduction zone conditions

Subduction zones enable carbon transport to the deep Earth. Inorganic and organic carbon in fluids released from the subducted slab are important in water-rock interactions. However, the potential role of reduced carbon species in fluids during subduction is still unclear. In particular, the pressure, temperature, and oxidation state conducive to the formation of fluid hydrocarbons are poorly understood. Here we focused on the role of pressure influencing the formation of hydrocarbons using diamond anvil cell experiments starting with 0.5 M Ca-acetate solutions over a broad range of pressures, from 1.6 to 4.6 GPa at temperatures of 300 and 350°C. Droplets of immiscible hydrocarbon fluid coexisting with aqueous carbonate or bicarbonate and crystals of calcite or aragonite were formed at peak pressure and temperature conditions in the experiments. Furthermore, greater quantities of hydrocarbons formed at higher pressure as revealed by measuring the in situ volume percent of the droplets. Measurement of the in situ Raman spectra of the co-existing aqueous solutions and analysis of the peak area ratios of acetate to HCO 3 – showed faster decrease at higher pressure, which indicated that the reactions forming hydrocarbons were accelerated by pressure. Compared to previous Na-acetate experiments at 300°C and 3.0 GPa, this study found hydrocarbons that were more methane-rich and had more propane and less isobutane. In experiments at 350°C, isobutane transformed to one or more aromatic hydrocarbons in an immiscible fluid. The air-dried aromatic hydrocarbons were measured using a UV laser, and show peaks of bitumen. Overall, our study supports the hypothesis that high pressures and high temperatures facilitate the possible occurrence of immiscible hydrocarbon fluids in the deep carbon cycle.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2021

Soil Moisture–Atmosphere Feedbacks Dominate Land Carbon Uptake Variability

Year-to-year changes in carbon uptake by terrestrial ecosystems play an essential role in determining atmospheric carbon dioxide concentrations. It remains uncertain to what extent temperature and water availability can explain these variations at the global scale. Here we use factorial climate model simulations and show that variability in soil moisture drives 90% of the inter-annual variability in global land carbon uptake, mainly through its impact on photosynthesis. We find that most of this ecosystem response occurs indirectly as soil moisture–atmosphere feedbacks amplify temperature and humidity anomalies, and enhance the direct effects of soil water stress. The strength of this feedback mechanism explains why coupled climate models indicate a dominant role of soil moisture which is not readily apparent in land surface model simulations and observational analyses. These findings highlight the need to account for feedbacks between soil and atmospheric dryness when estimating the carbon cycle’s response to climatic change globally, as well as when conducting field-scale investigations of the ecosystem response to droughts. Our results show that most of the global variability in modelled land carbon uptake is driven by temperature and vapour pressure deficit effects which are controlled by soil moisture.

Atmospheric dynamics↗

DOE OSTI2020

Global, Regional, and National Fossil-Fuel CO2 Emissions: 1751-2017

This data product is a time series of Carbon Dioxide (CO2) emissions from fossil fuel combustion and cement manufacture. Estimates of CO2 emissions are included for the globe and by nation back to 1751, and include emissions from solid fuel consumption, liquid fuel consumption, gas fuel consumption, cement production, and gas flaring. Per capita CO2 emissions and emissions from international trade (bunker fuels) are included as well; bunker fuels are not included in country totals, but are assigned to the country in which loading took place. Estimates are generated using the United Nations Energy Statistics database and the United States Geologic Survey’s cement statistics. Datasets produced from this group at Appalachian State University are located here, and are also located at https://energy.appstate.edu/research/work-areas/cdiac-appstate. Historic CDIAC data from Oak Ridge National Laboratory are located here: https://data.ess-dive.lbl.gov/view/doi:10.3334/CDIAC/00001_V2017. This dataset is the foundational dataset for the annual global carbon budget and other carbon cycle analyses that need relevant fossil fuel CO2 data. Within this data package are spreadsheets (.csv) of global and national estimates of CO2 emissions as well as text files of the ranking of each country’s total CO2 emissions and per capita for that year.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries

Silicon is a high-energy density anode material for lithium-ion batteries, but it possesses shortcomings such as poor electronic conductivity, interfacial instability and mechanical fracturing that hinder its battery cycling. Carbon coating has been an important strategy for stabilizing silicon anodes, but the effects of the silicon surface properties on carbon coating morphology and the consequent silicon cycling stability have not been clearly elucidated. Herein, we find that thermal oxidation of the silicon anodes followed by chemical vapor deposition of carbonaceous precursors leads to a well-ordered graphene coating, whereas disordered graphite coating is formed on the native silicon surface. Graphene-coated silicon exhibits superior cycling performance, retaining a discharge capacity of ~1300 mAh g -1 after 300 cycles, whereas the disordered graphite-coated silicon suffers continuous degradation, retaining only~600 mAh g -1 after 300 cycles. Cryogenic electron microscopy reveals the mechanism behind the difference in cycling stabilities; graphene coated silicon is able to withstand the large mechanical strains induced during extended cycling, whereas disordered graphite coating is ruptured, exposing silicon surfaces to the electrolyte, leading to extensive buildup of SEI and poor cycling performance. Characterization of the silicon surface reveals that thermal treatment yields an oxygen-rich surface layer, which is hypothesized to play a decisive role in dictating the carbon coating. This work highlights the effect of silicon surface properties on carbon coating microstructure, and presents thermal treatment as a facile avenue to attain graphene coating on silicon anodes.

25 ENERGY STORAGE↗

DOE OSTI2023

Genomes to ecosystem function: Targeting critical knowledge gaps in methanogenesis and translation to updated global biogeochemical models

Natural freshwater temperate wetland systems currently represent the largest natural source of atmospheric methane, but are relatively understudied using systems biology tools (e.g. meta-omics) compared to other high producing methane systems (e.g. peat, tropical, or reconstructed wetlands). Using field investigations at the NOAA operated sentinel site on Lake Erie, methane producing activities and responses to geochemical conditions will be determined along seasonal and spatial gradients (Objective 1). Here, a combination of high-throughput activity and gas measurements, combined with high-resolution systems biology and analytical methods, will provide in depth knowledge of the microbiological, chemical, and physical constraints on methane production in wetlands. Using laboratory microcosms, the formation of anoxic microsites and their capacity to facilitate methane production in wetland soils will be simulated (Objective 2). This objective will validate the findings from the field investigations, offering a more controlled environment for teasing out the role of different yet interrelated variables. Lastly, these field and laboratory data will be used for multi-scale, process-level evaluation of an ecosystem biogeochemical model that accommodates these newly identified processes and parameterizes representation of these processes along relevant environmental gradients (Objective 3).This research will identify multiple interacting geochemical, ecological, and metabolic constraints that are poorly understood, oversimplified, or missing in global biogeochemical methane models. This proposal targets the role of oxygen limitation on methane processes in soil domains, to improve reactive transport models of microbial carbon cycling across terrestrial-aquatic soils and generate data on nutrient cycling activities in Great Lake wetlands. This information could provide new insights into the microbial controllers of Lake Erie eutrophication.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Myriad Mapping of nanoscale minerals reveals calcium carbonate hemihydrate in forming nacre and coral biominerals

Abstract Calcium carbonate (CaCO 3 ) is abundant on Earth, is a major component of marine biominerals and thus of sedimentary and metamorphic rocks and it plays a major role in the global carbon cycle by storing atmospheric CO 2 into solid biominerals. Six crystalline polymorphs of CaCO 3 are known—3 anhydrous: calcite, aragonite, vaterite, and 3 hydrated: ikaite (CaCO 3 ·6H 2 O), monohydrocalcite (CaCO 3 ·1H 2 O, MHC), and calcium carbonate hemihydrate (CaCO 3 ·½H 2 O, CCHH). CCHH was recently discovered and characterized, but exclusively as a synthetic material, not as a naturally occurring mineral. Here, analyzing 200 million spectra with Myriad Mapping (MM) of nanoscale mineral phases, we find CCHH and MHC, along with amorphous precursors, on freshly deposited coral skeleton and nacre surfaces, but not on sea urchin spines. Thus, biomineralization pathways are more complex and diverse than previously understood, opening new questions on isotopes and climate. Crystalline precursors are more accessible than amorphous ones to other spectroscopies and diffraction, in natural and bio-inspired materials.

58 GEOSCIENCES↗

DOE OSTI2025

Diel variation in CO 2 flux is substantial in many lakes

Lakes play a significant role in the global carbon cycle, acting as sources and sinks of carbon dioxide (CO 2 ). In situ measurements of CO 2 flux (FCO 2 ) from lakes have generally been collected during daylight, despite indications of significant diel variability. This introduces bias when scaling up to whole-lake annual aquatic carbon budgets. We conducted an international sampling program to ascertain the extent of diel variation in FCO 2 across lakes. We sampled 21 lakes over 41 campaigns and measured FCO 2 at 4-h intervals over a full diel cycle. Rates of FCO 2 ranged from −3.16 to 4.39 mmol m −2 h −1 . Integrated over a day, FCO 2 ranged from −381.68 to 878.49 mg C m −2 d −1 (mean = 76.54) across campaigns. We identified three characteristic diel patterns in FCO 2 related to trophic status and show that for half of the campaigns, daily flux estimates were biased by > 50% if based on a single (daytime) measurement.

de Eyto, Elvira [Marine Institute, Mayo (Ireland)]↗

NASA NTRS2016

Drought Rapidly Diminishes the Large Net CO2 Uptake in 2011 Over Semi-Arid Australia

Each year, terrestrial ecosystems absorb more than a quarter of the anthropogenic carbon emissions, termed as land carbon sink. An exceptionally large land carbon sink anomaly was recorded in 2011, of which more than half was attributed to Australia. However, the persistence and spatially attribution of this carbon sink remain largely unknown. Here we conducted an observation-based study to characterize the Australian land carbon sink through the novel coupling of satellite retrievals of atmospheric CO2 and photosynthesis and in-situ flux tower measures. We show the 2010-11 carbon sink was primarily ascribed to savannas and grasslands. When all biomes were normalized by rainfall, shrublands however, were most efficient in absorbing carbon. We found the 2010-11 net CO2 uptake was highly transient with rapid dissipation through drought. The size of the 2010-11 carbon sink over Australia (0.97 Pg) was reduced to 0.48 Pg in 2011-12, and was nearly eliminated in 2012-13 (0.08 Pg). We further report evidence of an earlier 2000-01 large net CO2 uptake, demonstrating a repetitive nature of this land carbon sink. Given a significant increasing trend in extreme wet year precipitation over Australia, we suggest that carbon sink episodes will exert greater future impacts on global carbon cycle.

fluorescence↗

NASA NTRS2019

Thinner Bark Increases Sensitivity of Wetter Amazonian Tropical Forests to Fire

Understory fires represent an accelerating threat to Amazonian tropical forests and can, during drought, affect larger areas than deforestation itself. These fires kill trees at rates varying from < 10 to c. 90% depending on fire intensity, forest disturbance history and tree functional traits. Here, we examine variation in bark thickness across the Amazon. Bark can protect trees from fires, but it is often assumed to be consistently thin across tropical forests. Here, we show that investment in bark varies, with thicker bark in dry forests and thinner in wetter forests. We also show that thinner bark translated into higher fire-driven tree mortality in wetter forests, with between 0.67 and 5.86 gigatonnes CO2 lost in Amazon understory fires between 2001 and 2010. Trait-enabled global vegetation models that explicitly include variation in bark thickness are likely to improve the predictions of fire effects on carbon cycling in tropical forests.

Carbon cycle↗

NASA NTRS2019

Thinner Bark Increases Sensitivity of Wetter Amazonian Tropical Forests to Fire

Understory fires represent an accelerating threat to Amazonian tropical forests and can, during drought, affect larger areas than deforestation itself. These fires kill trees at rates varying from < 10 to c. 90% depending on fire intensity, forest disturbance history, and tree functional traits. Here, we examine variation in bark thickness across the Amazon. Bark can protect trees from fires, but it is often assumed to be consistently thin across tropical forests. Here, we show that investment in bark varies, with thicker bark in dry forests and thinner in wetter forests. We also show that thinner bark translated into higher fire-driven tree mortality in wetter forests, with between 0.67 to 5.86 gigatons CO2 lost in Amazon understory fires between 2001-2010. Trait-enabled global vegetation models that explicitly include variation in bark thickness are likely to improve the predictions of fire effects on carbon cycling in tropical forests.

Carbon cycle↗

DOE OSTI2023

Modeling strategies and data needs for representing coastal wetland vegetation in land surface models

Vegetated coastal ecosystems sequester carbon rapidly relative to terrestrial ecosystems. Coastal wetlands are poorly represented in land surface models, but work is underway to improve process-based, predictive modeling of these ecosystems. Here, in this work, we identify guiding questions, potential simulations, and data needs to make progress in improving representation of vegetation in terrestrial–aquatic interfaces, with a focus on coastal and estuarine ecosystems. We synthesize relevant plant traits and environmental controls on vegetation that influence carbon cycling in coastal ecosystems. We propose that models include separate plant functional types (PFTs) for mangroves, graminoid salt marshes, and succulent salt marshes to adequately represent the variation in aboveground and belowground productivity between common coastal wetland vegetation types. We also discuss the drivers and carbon storage consequences of shifts in dominant PFTs. We suggest several potential approaches to represent the diversity in vegetation tolerance and adaptations to fluctuations in salinity and water level, which drive key gradients in coastal wetland ecosystems. Finally, we discuss data needs for parameterizing and evaluating model implementations of coastal wetland vegetation types and function.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Widespread co‐occurrence of Sebacinales and arbuscular mycorrhizal fungi in switchgrass roots and soils has limited dependence on soil carbon or nutrients

Societal Impact Statement This work addresses a novel group of Sebacinales mycorrhizal fungi being considered for development as inoculants in managed ecosystems because of their potential access to nutrients in soil organic matter. By comparing the diversity, distributions, and abundances of the Sebacinales with the more common arbuscular mycorrhizal fungi in switchgrass, a biofuel crop, we demonstrate that current suggestions for a Sebacinales revolution in agriculture should be tempered by their ecology. In particular, Sebacinales are rare compared to arbuscular mycorrhizal fungi, and are only weakly associated with soil carbon, suggesting that ideas about improved soil carbon cycling associated with Sebacinales need to be sufficiently studied across a range of environmental conditions prior to their consideration for broad‐spectrum soil inoculants. Summary Arbuscular mycorrhizal (AM) fungi are widespread and important root symbionts, but recent work suggests that Sebacinales fungi may play an equally important role in both plant success and ecosystem carbon and nutrient cycling based on their worldwide occurrence and putative access to organic matter. However, the ecological impacts of Sebacinales will depend on their abundance and distribution relative to AM fungi and environmental soil carbon and nutrient patterns, which remain unexplored. We characterized Glomeromycota and Sebacinales fungi in switchgrass ( Panicum virgatum L.) roots and soils across 14 sites with diverse soil conditions. We examined group richness differences, co‐occurrence patterns, and how the relative abundance of these fungi related to soil carbon, nutrient stoichiometry, and host size. Sebacinales were widespread, but less diverse, common, and abundant than Glomeromycota. Moreover, co‐occurrences were predominantly random, suggesting relatively few interactions between these groups. Sebacinales increased relative to Glomeromycota in soils with more carbon, but explanatory power was limited. Based on our findings, we suggest that Sebacinales are likely complementary to AM fungi in roots. Expectations that Sebacinales have large effects on soil carbon and nutrient cycling may need to be reconsidered, at least based on their limited abundances relative to AM fungi in switchgrass. This is an important consideration as Sebacinales are candidates for use as inoculants in managed ecosystems.

Lee, Marissa R.↗

DOE OSTI2023

Diminishing marginal effect in estimating the dissolved organic carbon export from a watershed

Dissolved organic carbon (DOC) can be initially moved from soils to inland waters with surface runoff, and then mineralized, buried, or eventually delivered to the coastal ocean. This land-to-ocean phase of the DOC flux must be accounted for to comprehensively understand the global carbon cycle. To estimate the terrestrial-aquatic DOC leaching, calculating the product of the riverine DOC concentration and the corresponding river discharge measured at the watershed outlet is a common method. However, it is challenging to frequently and exactly record riverine DOC concentrations, thus the relationship between DOC concentrations and discharges (C-Q relationship) are established and used to interpolate the time-series of DOC concentrations. We found that the widely used time-dependent and time-independent C-Q regression models are weak in representing their altered relationship when the discharge is extremely high, which was named as diminishing marginal effect. In this study, we evaluated the performance of two C-Q regression models and discussed possible reasons for the diminishing marginal effect. We suggest that repeated and long-term measurements of the DOC concentration are required to adequately analyze their relationships, especially during the early spring and seasons with heavy precipitations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Sustainability of soil organic carbon in consolidated gully land in China’s Loess Plateau

Massive gully land consolidation projects, launched in China’s Loess Plateau, aim to restore 2667 km 2 agricultural lands in total by consolidating 2026 highly eroded gullies. This effort represents a social engineering project where the economic development and livelihood of the farming families are closely tied to the ability of these emergent landscapes to provide agricultural services. Whether these ‘time zero’ landscapes have the resilience to provide a sustainable soil condition such as soil organic carbon (SOC) content remains unknown. By studying two watersheds, one of which is a control site, we show that the consolidated gully serves as an enhanced carbon sink, where the magnitude of SOC increase rate (1.0 gC/m 2 /year) is about twice that of the SOC decrease rate (-0.5 gC/m 2 /year) in the surrounding natural watershed. Over a 50-year co-evolution of landscape and SOC turnover, we find that the dominant mechanisms that determine the carbon cycling are different between the consolidated gully and natural watersheds. In natural watersheds, the flux of SOC transformation is mainly driven by the flux of SOC transport; but in the consolidated gully, the transport has little impact on the transformation. Furthermore, we find that extending the surface carbon residence time has the potential to efficiently enhance carbon sequestration from the atmosphere with a rate as high as 8 gC/m 2 /year compared to the current 0.4 gC/m 2 /year. The success for the completion of all gully consolidation would lead to as high as 26.67 GgC/year sequestrated into soils. This work, therefore, not only provides an assessment and guidance of the long-term sustainability of the ‘time zero’ landscapes but also a solution for sequestration CO 2 into soils.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2023

Remote Sensing of Dissolved Organic Carbon (DOC) Stocks, Fluxes and Transformations Along the Land-Ocean Aquatic Continuum: Advances, Challenges, and Opportunities

From stream headwaters to the deep ocean, dissolved organic carbon (DOC) is ubiquitous across the world’s aquatic systems, where it fulfills important biogeochemical and ecological functions. Importantly, DOC is a dynamic component of the carbon cycle and represents a global reservoir (mass of carbon) equivalent in size to the atmospheric CO 2 pool. The mobilization, transport, and transformations of DOC along the land-ocean aquatic continuum biogeochemically connect terrestrial landscapes, freshwater and marine ecosystems, and the atmosphere. As a result, DOC budgets are vulnerable to climate- and human-driven changes. Having the ability to quantify DOC stocks, fluxes, and transformations consistently and accurately in aquatic systems is therefore critical to our understanding of DOC’s functions in the environment and of their susceptibility to change. In recent years, optical techniques and synoptic earth observations have opened new doors to achieve this objective on a global scale. In this review, we explore how in situ measurements, earth observations, and the models they inform have facilitated the large-scale quantification of DOC stocks, fluxes, and transformations along the land-ocean aquatic continuum and how they have helped shape our current understanding of the global DOC cycle. The review also explores the limitations and challenges we still face today, and discusses how upcoming and future sensors are expected to provide new insights into our understanding of the global DOC cycle.

Dissolved organic carbon↗

DOE OSTI2021

Projecting Permafrost Thaw of Sub-Arctic Tundra With a Thermodynamic Model Calibrated to Site Measurements

Northern circumpolar permafrost thaw affects global carbon cycling, as large amounts of stored soil carbon becomes accessible to microbial breakdown under a warming climate. The magnitude of carbon release is linked to the extent of permafrost thaw, which is locally variable and controlled by soil thermodynamics. Soil thermodynamic properties, such as thermal diffusivity, govern the reactivity of the soil-atmosphere thermal gradient, and are controlled by soil composition and drainage. In order to project permafrost thaw for an Alaskan tundra experimental site, we used seven years of site data to calibrate a soil thermodynamic model using a data assimilation technique. The model reproduced seasonal and interannual temperature dynamics for shallow (5–40 cm) and deep soil layers (2–4 m), and simulations of seasonal thaw depth closely matched observed data. The model was then used to project permafrost thaw at the site to the year 2100 using climate forcing data for three future climate scenarios (RCP 4.5, 6.0, and 8.5). Minimal permafrost thawing occurred until mean annual air temperatures rose above the freezing point, after which we measured over a 1 m increase in thaw depth for every 1 °C rise in mean annual air temperature. Under no projected warming scenario was permafrost remaining in the upper 3 m of soil by 2100. We demonstrated an effective data assimilation method that optimizes parameterization of a soil thermodynamic model. The sensitivity of local permafrost to climate warming illustrates the vulnerability of sub-Arctic tundra ecosystems to significant and rapid soil thawing.

54 ENVIRONMENTAL SCIENCES↗