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At least 109 records · Page 6

Process-oriented analysis of dominant sources of uncertainty in the land carbon sink

The observed global net land carbon sink is captured by current land models. All models agree that atmospheric CO 2 and nitrogen deposition driven gains in carbon stocks are partially offset by climate and land-use and land-cover change (LULCC) losses. However, there is a lack of consensus in the partitioning of the sink between vegetation and soil, where models do not even agree on the direction of change in carbon stocks over the past 60 years. This uncertainty is driven by plant productivity, allocation, and turnover response to atmospheric CO 2 (and to a smaller extent to LULCC), and the response of soil to LULCC (and to a lesser extent climate). Overall, differences in turnover explain ~70% of model spread in both vegetation and soil carbon changes. Further analysis of internal plant and soil (individual pools) cycling is needed to reduce uncertainty in the controlling processes behind the global land carbon sink.

54 ENVIRONMENTAL SCIENCES↗

Carbon Mineralization of Sulfate Wastes Containing Pb: Synchrotron Pb M3-Edge XANES Analysis of Simultaneous Heavy Metal and Carbon Sequestration

Sulfate wastes are produced in large quantities and contain toxic heavy metals such as lead (Pb), posing environmental risks. Because of favorable solubility differences, these wastes can be repurposed for engineered carbon dioxide (CO 2 ) sequestration. Understanding the fate and mobility of heavy metals during this process is important. This study focuses on Pb and the effect of zinc (Zn) on Pb in carbon mineralization. Synthesized gypsum was treated with a carbonate-rich solution at pH 11.5 to convert the sulfates to carbonates. Aqueous solutions and mineral solids were analyzed. Synchrotron-based micro-X-ray fluorescence and a novel application of Pb M3-edge X-ray absorption near-edge structure provided detailed insights into Pb distribution and mineral forms. Results showed significant reductions in aqueous Pb and Zn concentrations, indicating effective metal sequestration. Carbon mineralization transformed Pb from soluble anglesite (PbSO 4 ) into insoluble cerussite (PbCO 3 ) and hydrocerussite (Pb 3 (CO 3 ) 2 (OH) 2 ). Pb primarily precipitated onto calcium carbonate surfaces through surface-mediated precipitation reactions. While the presence of Zn modified crystallization dynamics, it did not impede Pb sequestration and potentially enhanced surface reactivity, facilitating greater Pb immobilization. These findings highlight carbon mineralization as a sustainable approach to immobilize toxic metals in sulfate wastes while advancing CO 2 sequestration efforts.

54 ENVIRONMENTAL SCIENCES↗

Insights from FEED studies for retrofitting existing fossil power plants with carbon capture technology

Recent United States Department of Energy (DOE) sponsored front-end engineering design (FEED) studies for retrofitting existing fossil-fueled power plants with state-of-the-art carbon capture technology contain previously overlooked real-world design considerations for near-term deployment of carbon capture. Insights from examining seven recently published FEED study reports are summarized in this paper. This includes a discussion of the design, performance, and cost implications associated with (1) location-specific considerations such as water availability, land availability, and accessibility; (2) host-plant-specific factors such as flue gas specifications, allowable degree of integration between the capture system and host plant, and operational mode; and (3) miscellaneous factors such as market conditions, permitting requirements, and business case incentives. In conclusion, this manuscript highlights (1) water availability as a key design and cost driver, with host plant steam extraction increasing capture system cooling water availability, (2) modularization and constructability impacts on the number of capture trains, (3) the impacts of host plant operational mode and capacity factor on the business case for installing capture, and (4) the merit of continued research, development, and demonstration efforts addressing steam extraction, host plant tie-in at the stack, solvent reclamation and air emissions control.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Pore-Scale Microenvironments Control Anthropogenic Carbon Mineralization Outcomes in Basalt

Thin sections and hand samples from 50 sidewall cores from the Wallula Basalt Pilot Demonstration, a basaltic carbon sequestration demonstration, provided the opportunity for the in-depth analysis of carbon mineralization induced by the injection of supercritical CO 2 . In this study, we used optical petrography and scanning electron microscopy to characterize the physical and chemical characteristics of the basalt components influenced by carbon mineralization reactions from all available hand samples and thin sections within the three CO 2 injection zones and caprock flow interiors. We found extensive carbonate mineralization, mostly in the form of nodules that were shown to be chemically zoned: Ca-dominant in the core regions and Ca-bearing Fe-dominant in the outer regions. Carbonate mineralization also took the form of fracture-filling carbonate cement, and acicular aragonite was also observed. Overall, we clarified the structural and paragenetic relationships between newly formed minerals, identifying a new fibro-palagonite-like, poorly crystalline silicate phase that grew on the carbonate nodules and pore-lining zeolites. Here we observed Fe-dominant carbonate precipitates surrounding acicular aragonite and rhombohedral Ca-carbonate cores, whereas previous studies of these zoned nodules did not observe these structures. A comprehensive accounting of the carbon mineralization products is vital to understand and predict the behavior of supercritical CO 2 in the subsurface given both the diversity of the host rock between and within injection zones, especially considering that the morphology and chemistry of the diverse precipitates are influenced by the pore-scale microenvironments of the basalt.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Position-specific carbon isotopes of Murchison amino acids elucidate extraterrestrial abiotic organic synthesis networks

The Murchison meteorite is a well-studied carbonaceous chondrite with relatively high concentrations of amino acids thought to be endogenous to the meteorite, in part because they are characterized by carbon isotope (δ 13 C) values higher than those typical of terrestrial amino acids. Past studies have proposed that extraterrestrial amino acids in the Murchison meteorite could have formed by Strecker synthesis (for α-amino acids), Michael addition (for β-amino acids), or reductive amination, but a lack of constraints have prevented confident discrimination among these possibilities, or assignment of specific formation pathways to each of several specific amino acids. Position-specific carbon isotope analysis differentiates amongst these mechanisms by relating molecular sites to isotopically distinct carbon sources and by constraining isotope effects associated with elementary chemical reactions. Prior measurements of the position-specific carbon isotopic composition of α-alanine from the Murchison CM chondrite demonstrated that alanine’s high δ 13 C VPDB value is attributable to the amine carbon (δ 13 C VPDB = +142 ± 20‰), consistent with Strecker synthesis drawing on 13 C-rich carbonyl groups in precursors (Chimiak et al., 2021). Here, we measured the δ 13 C composition of fragment ions generated by electron impact ionization of derivatized α-alanine, β-alanine, and aspartic acid from Murchison via gas chromatography-Fourier transform mass spectrometry. α-Alanine’s amine carbon yielded δ 13 C VPDB = +109 ± 21‰, which is consistent with the previously measured value and with formation from 13 C-rich precursors. β-Alanine’s amine carbon presents a lower δ 13 C VPDB = +33 ± 24‰, which supports formation from 13 C-rich precursors but potentially via a Michael addition mechanism rather than Strecker synthesis. Aspartic acid’s amine carbon has δ 13 C VPDB = -14 ± 5‰, suggesting synthesis from precursors distinct from those that generated the alanine isomers. Further, these measurements indicate that Murchison amino acids are a mixture of compounds made from different synthesis mechanisms, though some subsets likely drew on the same substrates; this conclusion highlights the complexity of extraterrestrial organic synthesis networks and the potential of emerging methods of isotope ratio analysis to elucidate the details of those networks.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Opportunities and Limitations of Nuclear Magnetic Resonance Spectroscopy in Astrobiology

For decades, Nuclear Magnetic Resonance (NMR) spectroscopy has been utilized as a powerful tool in various scientific disciplines, most prominently in chemistry, to determine molecular structures or monitor reactions. While well established in various fields, NMR applications in astrobiology are still unclear. This work aims to explore the potential of NMR in astrobiology, highlighting strengths but also weaknesses. We illustrate capabilities of NMR with two applications: (1) recently developed methods for position-specific carbon isotope analysis of complex organics; and (2) well-established tools for performing quantitative compositional analysis of complex organic mixtures. By utilizing samples relevant to astrobiology, specifically the amino acid valine and analogue mixtures of organics, we showcase that molecules retain a source dependent and distinct intramolecular carbon isotope fingerprint. We demonstrate that compositional sample analysis provides an independent and complementary line of evidence pointing towards the origin of a molecule or mixture. Together, these NMR tools have the potential to support life detection efforts, and aid in distinguishing between biotic and abiotic samples. Finally, we discuss sensitivity, detection limits, the portability of NMR, and propose how integration with mass-spectrometry techniques will be imperative to enable more targeted and comprehensive analyses relevant to astrobiology, including in-situ analysis but also sample return missions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Secondary porosity prediction in complex carbonate reefs using 3D CT scan image analysis and machine learning

Development and preservation of carbonate porosity and permeability are critical to characterizing reservoirs. However, secondary porosity, such as vugs and fractures, are difficult to identify and require collection of expensive wireline tools or core sampling. Wireline logs and cores have traditionally been used to identify the presence of secondary porosity but fail to quantify the contribution to total reservoir porosity. Additionally, advanced wireline logs and core are not readily available for most wells. Dual energy CT scans were collected on whole core from the A-1 Carbonate and Brown Niagaran formations drawn from six wells in northern Michigan. 3D analysis techniques were applied to identify and isolate secondary porosity features. A series of machine learning and data analytics techniques were applied to the dataset to predict secondary porosity features on basic wireline logs. The predictive model successfully predicted secondary porosity with high confidence.

02 PETROLEUM↗

Carbon footprint prediction considering the evolution of alternative fuels and cargo: A case study of Yangtze river ships

For reducing carbon emissions in the shipping sector, application of alternative low-carbon and zero-carbon fuels is the consensus. However, requirements of economic development cannot be ignored while focusing on emission reduction. Cargo development is an important prerequisite. Considering the cargo growth as a novelty, a method to calculate the annual carbon emissions of different alternative fuel-powered ships in different cargo growth prospects and power scenarios is proposed. With respect to the time dimension, the relationship between alternative fuels, cargo, and carbon reduction is revealed. The Yangtze River bulk carrier case was studied and the life cycle carbon emission analysis of diesel, LNG hybrid, LNG, hydrogen, methanol, and ammonia were carried out. The annual carbon curves of the high, steady, and low cargo growth prospects were obtained for different scenarios of the power system structure. The results show that LNG hybrid, LNG and methanol fuels are currently the suitable choices. Their life cycle carbon emissions were reduced by 31.5–38.1% compared with those of diesel power. The carbon emissions of green hydrogen and green ammonia were reduced by 78.8% and 91.3%, respectively, compared with those of hydrogen and ammonia. The carbon reduction results of green fuels in their initial application were explored which are at 0.6–10.8%. In addition, there is a balanced annual growth rate, whose annual carbon curve will be steady under its corresponding scenario of power system structure, which could help the ship owners plan their future.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Embodied carbon in the U.S. manufacturing and trade

On average, one quarter of the global carbon footprint is embodied in traded goods. These emissions are a growing issue for global efforts to decarbonize the world economy. Embodied emissions in trade are not accounted for by existing greenhouse gas accounting systems. For example, countries only report their domestic carbon emissions (also known as production-based or territorial accounting) to the Intergovernmental Panel on Climate Change (IPCC). If the embodied carbon in trade were accounted for and reported, the promising climate trends depicted by many countries would be negated or reversed. For example, many achievements of reducing emissions by developed countries under the Kyoto Protocol would actually appear as emissions outsourced to developing countries. Like many other developed countries, the United States is a net importer of embodied greenhouse gas (GHG) emissions in trade. The goal of this study was to calculate the carbon footprint of various sectors of the U.S. economy using the latest available data and based on that, estimate the embodied carbon in certain manufacturing sector products imported and exported by the U.S. First, we conducted an input-output analysis to calculate the carbon footprint of 401 aggregate level sectors of the U.S. economy. After that, for a selected number of manufacturing subsectors /products(hereafter referred to as products),we collected their trade(import/export) data and combined that with their computed carbon footprint to estimate the embodied carbon in import and export of these products for the U.S. While we conducted the carbon footprint analysis for sectors covering the entire U.S. economy (401 sectors), we only conducted the embodied carbon in trade analysis for a few products within specific aggregate level manufacturing sectors,such as computer and electronic product manufacturing (NAICS 334), transport equipment manufacturing (NAICS 336), machinery manufacturing (NAICS 333), and chemical manufacturing (NAICS 325). It is possible to do the detailed embodied carbon analysis for all other products within the various aggregate level manufacturing sectors of the U.S. economy, but given the scope of this study and space constraint of this report, we only present the results for a few products. The results of our analysis for the selected products show the embodied carbon in trade for each product by country and also show the rankings of countries in terms of top importers and exporters of embodied carbon in trade with the U.S. Our results show that in majority of cases, the U.S. is a net importer of embodied carbon in trade. Unless consumption-based accounting is used, the U.S. and other net embodied carbon importing countries may continue to outsource their emissions to meet their climate change mitigation targets under the Paris Agreement, as observed previously with the Kyoto Protocol. Some countries reported reductions that exceeded their Kyoto targets, however, the changes in emissions embodied in imports were comparable to or larger than changes in domestic emissions. Traded emissions undermined emissions reductions in the Kyoto Protocol, and threaten to continue to do so for the Paris Agreement. New climate policies such as California’s Buy Clean act, EU’s proposed border carbon tax adjustment, as well as efforts in the private sector can help address the embodied carbon in traded products.

54 ENVIRONMENTAL SCIENCES↗

Intensified Soil Moisture Extremes Decrease Soil Organic Carbon Decomposition: A Mechanistic Modeling Analysis

Earth system models have predicted that there will be more frequent and severe precipitation and drought events in terrestrial ecosystems. Microbially mediated decomposition of soil organic carbon (SOC) tends to increase as soils wet and decrease as soils dry. However, the long-term SOC change under intensified moisture extremes remains poorly known as it depends on the frequency and intensity of soil drying and wetting. In this study, we explored long-term SOC dynamics under scenarios of alternating drying-wetting cycles using the Microbial-ENzyme Decomposition model, a mechanistic microbial model. The model was parameterized with 11 years of observations from a temperate deciduous broadleaf forest site, showing satisfactory model performance in both model calibration (R 2 = 0.67) and validation (R 2 = 0.69) against heterotrophic respiration. We then used the model to simulate the long-term SOC dynamics under five scenarios of alternating drying-wetting cycles with different frequencies and severities over a period of 100 years. Results showed that the changes in active microbial biomass C and the corresponding turnover rates of SOC pools were more sensitive to soil drying than soil wetting. As a result, the cumulative soil carbon emission from microbial respiration decreased by 433.7 g C m -2 after the 100-year simulation in the highest frequency and intensity moisture scenario, but was not significantly affected by the lowest frequency and intensity scenario. This study emphasizes the nonlinear response of SOC decomposition to soil moisture changes, which causes decreased decomposition by microbes under drying that is, not compensated by increased decomposition under wetting conditions.

58 GEOSCIENCES↗

Market Analysis: Upcycling Natural Gas Into Solid Carbon Products

The purpose of this report is to execute a market analysis to determine the potential market opportunities for natural gas-derived high-value carbon products and their associated applications. Currently, associated gas is released through the process of either venting or flaring. Vented or flared natural gas is presently lost to the atmosphere, despite the fact that it represents a significant resource of both carbon and hydrogen—two products that could have significant value. Transforming some of this underutilized supply into high-cost products could contribute to realizing the full value of United States (U.S.) natural gas resources. The products analyzed in this report are carbon fiber, carbon nanotubes, synthetic graphite, and carbon black. The report also touches on the market opportunities for hydrogen, a by-product of the pyrolysis process.

03 NATURAL GAS↗

Spatially resolved nanostructural analysis of disordered phases in carbonated alkali-activated slag

Alkali-activated slag (AAS) is a promising low-CO 2 alternative cement consisting of several disordered phases of similar composition. Although their local atomic arrangements are known to influence macroscopic behavior, determination of structural changes in response to external stimuli remains a challenge. Here, X-ray diffraction-computed tomography (XRD-CT), pair distribution function-CT (PDF-CT), and nanoprobe X-ray fluorescence (nano-XRF) have been used to uncover how an increase of magnesium in AAS affects the atomic structure and spatial arrangement of phases after aggressive carbonation (100% dry CO 2 ), conditions experienced in applications such as oil and gas wells and geological storage of CO 2 . From PDF-CT it is found that a higher magnesium content decreases the average nanoscale crystallite size of disordered calcium carbonate. At the same time, higher magnesium content is correlated with a less decalcified C-(N)-A-S-H gel, as determined via analysis of Ca-Si atom-atom correlations from PDF-CT and Ca/Si ratios from nano-XRF. Finally, nano-XRF reveals that the disordered (i.e., amorphous) calcium carbonate is stabilized by the presence of silicates.

McCaslin, Eric R. [Princeton Univ., NJ (United Sta↗

Techno-Economic Analysis of an SOFC Hybrid Carbon Conversion Concept

This is a presentation prepared for the 2023 Hydrogen and Fuel Cell Seminar to take place in Long Beach, CA on February 7-9, 2023. The presentation highlights analysis recently conducted by NETL on the cost and performance associated with operating SOFC systems in a hybridized configuration with compressed air energy storage.

Buchheit, Kyle L.↗

Cradle-to-Gate greenhouse gas emissions of the production of ethylene from U.S. Corn ethanol and comparison to fossil-derived ethylene production

Conventional ethylene production heavily depends on fossil-derived feedstocks via steam cracking, a very energy- and emission-intensive process. Researchers have been exploring alternatives to reduce CO 2 emissions including producing ethylene from biobased feedstocks. This paper evaluates the cradle-to-gate greenhouse gas (GHG) emissions of bioethylene produced from U.S. corn ethanol. The analysis includes different pathways for the dehydration of corn ethanol to ethylene and co-processing routes via fluid catalytic cracking (FCC) processes. For the FCC co-processing route carbon-14 analysis is used to determine bioethanol yields. A 127% reduction in life cycle GHG emissions of bioethylene is estimated compared to fossil-derived ethylene for the base case. Additional case studies are also discussed to understand the reduction of GHG emissions due to sustainable corn farming and renewable power use, biogenic carbon capture, and fuel switch with biofuels at the ethanol plant, and its impact on bioethylene GHG emissions.

carbon footprint↗

A bloom of a single bacterium shapes the microbiome during outdoor diatom cultivation collapse

Algae-dominated ecosystems are fundamentally influenced by their microbiome. We lack information on the identity and function of bacteria that specialize in consuming algal-derived dissolved organic matter in high algal density ecosystems such as outdoor algal ponds used for biofuel production. Here, we describe the metagenomic and metaproteomic signatures of a single bacterial strain that bloomed during a population-wide crash of the diatom, Phaeodactylum tricornutum, grown in outdoor ponds. 16S rRNA gene data indicated that a single Kordia sp. strain (family Flavobacteriaceae) contributed up to 93% of the bacterial community during P. tricornutum demise. Kordia sp. expressed proteins linked to microbial antagonism and biopolymer breakdown, which likely contributed to its dominance over other microbial taxa during diatom demise. Analysis of accompanying downstream microbiota (primarily of the Rhodobacteraceae family) provided evidence that cross-feeding may be a pathway supporting microbial diversity during diatom demise. In situ and laboratory data with a different strain suggested that Kordia was a primary degrader of biopolymers during algal demise, and co-occurring Rhodobacteraceae exploited degradation molecules for carbon. An analysis of 30 Rhodobacteraceae metagenome assembled genomes suggested that algal pond Rhodobacteraceae commonly harbored pathways to use diverse carbon and energy sources, including carbon monoxide, which may have contributed to the prevalence of this taxonomic group within the ponds. These observations further constrain the roles of functionally distinct heterotrophic bacteria in algal microbiomes, demonstrating how a single dominant bacterium, specialized in processing senescing or dead algal biomass, shapes the microbial community of outdoor algal biofuel ponds.

Kordia↗

Direct and Sensitive Electrochemical Evaluation of Pramipexole Using Graphitic Carbon Nitride (gCN) Sensor

Pramipexole (PMXL) belongs to the benzothiazole class of aromatic compounds and is used in treating Parkinson’s disease; however, overdosage leads to some abnormal effects that could trigger severe side effects. Therefore, it demands a sensitive analytical tool for trace level detection. In this work, we successfully developed an electrochemical sensor for the trace level detection of PMXL, using the voltammetric method. For the analysis, graphitic carbon nitride (gCN) was opted and synthesized by using a high-temperature thermal condensation method. The synthesized nanoparticles were employed for surface characterization, using transmission electron microscopy (TEM), X-ray diffraction (XRD), and atomic force microscopy (AFM) techniques. The electrochemical characterization of the material was evaluated by using the electrochemical impedance spectroscopy (EIS) technique to evaluate the solution–electrode interface property. The cyclic voltammetry (CV) behavior of PMXL displayed an anodic peak in the forward scan, indicating that PMXL underwent electrooxidation, and an enhanced detection peak with lower detection potential was achieved for gCN-modified carbon paste electrode (gCN·CPE). The influence of different parameters on the electrochemical behavior was analyzed, revealing the diffusion governing the electrode process with an equal number of hydronium ions and electron involvement. For the fabricated gCN·CPE, good linearity range was noticed from 0.05 to 500 µM, and a lower detection limit (L D ) of 0.012 µM was achieved for the selected concentration range (0.5 to 30 µM). Selectivity of the electrode in PMXL detection was investigated by conducting an interference study, while the tablet sample analysis demonstrates the sensitive and real-time application of the electrode. The good recovery values for the analysis illustrate the efficiency of the electrode for PMXL analysis.

36 MATERIALS SCIENCE↗

Offshore Geologic Carbon Storage Data Collection and Data Gaps Analysis

This is a TRS documenting the Offshore Geologic Carbon Storage Data Collection. It describes the Data Collection web application and its creation as well as an accompanying Data Gaps Assessment. We present an interactive data collection and data gaps analysis to aggregate, understand, and disseminate the data that are publicly available to support offshore GCS in the United States. This data collection and data gaps analysis can be leveraged by stakeholders to understand where GCS may be viable offshore, create GCS project analogs, and address challenges to GCS in offshore environments.

58 GEOSCIENCES↗