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DOE OSTI2024

2D Metal/Graphene and 2D Metal/Graphene/Metal Systems for Electrocatalytic Conversion of CO 2 to Formic Acid

Efficiently transforming CO 2 into renewable energy sources is crucial for decarbonization efforts. Formic acid (HCOOH) holds great promise as a hydrogen storage compound due to its high hydrogen density, non-toxicity, and stability under ambient conditions. However, the electrochemical reduction of CO 2 (CO 2 RR) on conventional carbon black-supported metal catalysts faces challenges such as low stability through dissolution and agglomeration, as well as suffering from high overpotentials and the necessity to overcome the competitive hydrogen evolution reaction (HER). In this study, we modify the physical/chemical properties of metal surfaces by depositing metal monolayers on graphene (M/G) to create highly active and stable electrocatalysts. Strong covalent bonding between graphene and metal is induced by the hybridization of sp and d orbitals, especially the sharp $d_{z^2}$, $d_{yz}$, $d_{xz}$ orbitals of metals near the Fermi level, playing a decisive role. Moreover, charge polarization on graphene in M/G enables the deposition of another thin metallic film, forming metal/graphene/metal (M/G/M) structures. Finally, evaluating overpotentials required for CO 2 reduction to HCOOH, CO, and HER, we find that Pd/G, Pt/G/Ag, and Pt/G/Au exhibit excellent activity and selectivity toward HCOOH production. Our novel 2D hybrid catalyst design methodology may offer insights into enhanced electrochemical reactions through the electronic mixing of metal and other p-block elements.

2D Electrocatalysts↗

DOE OSTI2022

Carbon Intensities of Refining Products in Petroleum Refineries with Co-Processed Biofeedstocks

Petroleum refineries increasingly seek to generate fuels with lower carbon intensities (CIs; a measure of life cycle greenhouse gas [GHG] emissions per unit of energy of fuel; well-to-wheel [WTW]) to meet growing demand. Co-processing refers to a process that adds biomass-derived feedstocks to the fossil-based feedstocks of existing petroleum refinery process units. With the use of biofeedstocks, it is expected that co-processed fuels would have lower CIs than their petroleum counterparts without requiring changes in the existing infrastructure for producing, transporting, and using fuels. To quantify the GHG emissions reduction benefits of co-processing, this study uses a linear programming model to simulate petroleum refinery conditions with and without co-processing. The co-processing cases include three biofeedstocks (soy oil, tallow, and used cooking oil or UCO) used as 10 vol.% of the feedstock to a hydrotreater or hydrocracker since these lipid-based feedstocks have favorable properties to be treated in a hydrotreater or hydrocracker. In addition, we considered pyrolysis oil used as 10 vol.% of the feedstock to a fluid catalytic cracking (FCC) unit in the modeled refinery due to its higher oxygen content compared to other lipid-based feedstocks. Life cycle analysis (LCA) using two distinct approaches—process-level energy allocation and a refinery-level marginal approach—has been conducted for each case. The LCA results using process-level allocation show that there are no noticeable changes in emissions or energy use impacts at the facility level. The life cycle GHG emission reductions of co-processing cases are mainly related to the fraction of biogenic carbon embedded in each fuel product. For example, co-processed jet fuels (a mixture of fossil and biogenic fuels) made via hydrotreating or hydrocracking have higher biogenic carbon, which results in jet fuel CI reductions of 3.9%–8.6% compared to the CI of baseline petroleum jet fuels on a WTW basis. However, analysis of co-processed pyrolysis oil in an FCC shows that a higher fraction of biofeedstocks (29%) becomes process emissions (i.e., CO and CO 2 ), mainly due to the oxygenates in pyrolysis oil, and so it generates less renewable fuel than biofeedstocks co-processed via hydrotreating or hydrocracking. Using the refinery-level marginal approach, the changes in energy use and emissions of co-processing cases compared to the petroleum-only baseline case are allocated to the changes in fuel production (assuming renewable fuels). This approach generates the life cycle GHG emission values of co-processed renewable fuels, which are comparable to the CIs of standalone biofuel production pathways. However, as this approach relies on a rough assumption that product yields and emissions from co-processing units on fossil feedstocks remain the same with and without biofeedstock inputs, co-processing cases like FCC pyrolysis oil may generate quite skewed results.

02 PETROLEUM↗

NASA NTRS2022

Employing Relaxed Smoothness Constraints on Imaginary Part of Refractive Index in AERONET Aerosol Retrieval Algorithm

In the Aerosol Robotic Network (AERONET) retrieval algorithm, smoothness constraints on the imaginary part of the refractive index provide control of retrieved spectral dependence of aerosol absorption by preventing the inversion code from fitting the noise in optical measurements and thus avoiding unrealistic oscillations of retrievals with wavelength. The history of implementation of the smoothness constraints in the AERONET retrieval algorithm is discussed. It is shown that the latest version of the smoothness constraints on the imaginary part of refractive index, termed standard and employed by Version 3 of the retrieval algorithm, should be modified to account for strong variability of light absorption by brown-carbon-containing aerosols in UV through mid-visible parts of the solar spectrum. In Version 3 strong spectral constraints were imposed at high values of the Ångström exponent (440–870 nm) since black carbon was assumed to be the primary absorber, while the constraints became increasingly relaxed as aerosol exponent deceased to allow for wavelength dependence of absorption for dust aerosols. The new version of the smoothness constraints on the imaginary part of the refractive index assigns different weights to different pairs of wavelengths, which are the same for all values of the Ångström exponent. For example, in the case of four-wavelength input, the weights assigned to short-wavelength pairs (440–675, 675–870 nm) are small so that smoothness constraints do not suppress natural spectral variability of the imaginary part of the refractive index. At longer wavelengths (870–1020 nm), however, the weight is 10 times higher to provide additional constraints on the imaginary part of refractive index retrievals of aerosols with a high Ångström exponent due to low sensitivity to aerosol absorption for longer channels at relatively low aerosol optical depths. The effect of applying the new version of smoothness constraints, termed relaxed, on retrievals of single-scattering albedo is analyzed for case studies of different aerosol types: black- and brown-carbon-containing fine mode aerosols, mineral dust coarse mode aerosols, and urban industrial fine mode aerosol. It is shown that for brown-carbon-containing aerosols employing the relaxed smoothness constraints resulted in significant reduction in retrieved single-scattering albedo and spectral residual errors (compared to standard) at the short wavelengths. For example, biomass burning smoke cases showed a reduction in single-scattering albedo and spectral residual error at 380 nm of ∼ 0.033 and ∼ 17 %, respectively, for the Rexburg site and ∼ 0.04 and ∼ 12.7 % for the Rimrock site, both AERONET sites in Idaho, USA. For a site with very high levels of black-carbon-containing aerosols (Mongu, Zambia), the effect of modification in the smoothness constraints was minor. For mineral dust aerosols at small Ångström exponent values (Mezaira site, UAE), the spectral constraint on the imaginary part of the refractive index was already relaxed in Version 3; therefore the new relaxed constraint results in minimal change. In the case of weakly absorbing urban industrial aerosols at the GSFC site, there are significant changes in retrieved single-scattering albedo using relaxed assumption, especially reductions at longer wavelengths: ∼ 0.016 and ∼ 0.02 at 875 and 1020 nm, respectively, for 440 nm aerosol optical depth (AOD) ∼ 0.3. The modification of smoothness constraints on the imaginary part of the refractive index has a minor effect on retrievals of other aerosol parameters such as the real part of the refractive index and parameters of the aerosol size distribution. The implementation of the relaxed smoothness constraints on the imaginary part of the refractive index in the next version of the AERONET inversion algorithm will produce significant impacts at some sites in short wavelength channels (380 and 440 nm) for some biomass burning smoke cases with significant brown carbon content and possibly in mid-visible channels (500 and 675 nm) to near-infrared channels (870 to 1020 nm) for some urban industrial aerosol types. However, most differences in single-scattering albedo retrievals between those applying the new relaxed constraint and the standard constraint will be within the uncertainty of the single-scattering albedo retrievals, depending on the level of aerosol optical depth, Ångström exponent, brown carbon content and wavelength.

Aliaksandr Siniuk↗

DOE OSTI2025

Redox poise in R. rubrum phototrophic growth drives large-scale changes in macromolecular pathways

During photoheterotrophic growth on organic substrates, purple nonsulfur photosynthetic bacteria like Rhodospirillum rubrum can acquire electrons by multiple means, including oxidation of organic substrates, oxidation of inorganic electron donors (e.g., H 2 ), and by reverse electron flow from the photosynthetic electron transport chain. These electrons are stored as reduced electron-carrying cofactors (e.g., NAD(P)H and ferredoxin). The overall ratio of oxidized to reduced cofactors (e.g., NAD(P)+:NAD(P)H), or ’redox poise’, is difficult to understand or predict, as are the cellular processes for dissipating these reducing equivalents. Using physics-based models that capture mass action kinetics consistent with the thermodynamics of reactions and pathways, a range of redox conditions for heterophototrophic growth are evaluated, from conditions in which the NADP+/NADPH levels approach thermodynamic equilibrium to conditions in which the NADP+/NADPH ratio is far above the typical physiological values. Modeling predictions together with experimental measurements indicate that the redox poise of the cell results in large-scale changes in the activity of biosynthetic pathways and, thus, changes in cell macromolecule levels (DNA, RNA, proteins, and fatty acids). Furthermore, modeling predictions indicate that during phototrophic growth, reverse electron flow from the quinone pool is a minor contributor to the production of reduced cofactors (e.g., NAD(P)H) compared to other oxidative processes (H 2 and carbon substrate oxidation). Instead, the quinone pool primarily operates to aid ATP production. The high level of ATP, in turn, drives reduction processes even when NADPH levels are relatively low compared to NADP+ by coupling ATP hydrolysis to the reductive processes. The model, in agreement with experimental measurements of macromolecule ratios of cells growing on different carbon substrates, indicates that the dynamics of nucleotide versus lipid and protein production is likely a significant mechanism of balancing oxidation and reduction in the cell.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Redox Poise during Rhodospirillum rubrum Phototrophic Growth Drives Large-scale Changes in Macromolecular Synthesis Pathways

During photoheterotrophic growth on organic substrates, purple nonsulfur photosynthetic bacteria like Rhodospirillum rubrum can acquire electrons by multiple means, including oxidation of organic substrates, oxidation of inorganic electron donors (e.g., H2), and by reverse electron flow from the photosynthetic electron transport chain. These electrons are stored as reduced electron-carrying cofactors (e.g., NAD(P)H and ferredoxin). The overall ratio of oxidized to reduced cofactors (e.g., NAD(P)+:NAD(P)H), or ’redox poise’, is difficult to understand or predict, as are the cellular processes for dissipating these reducing equivalents. Using physics-based models that capture mass action kinetics consistent with the thermodynamics of reactions and pathways, a range of redox conditions for heterophototrophic growth are evaluated, from conditions in which the NADP+/NADPH levels approach thermodynamic equilibrium to conditions in which the NADP+/NADPH ratio is far above the typical physiological values. Modeling predictions together with experimental measurements indicate that the redox poise of the cell results in large-scale changes in the activity of biosynthetic pathways and, thus, changes in cell macromolecule levels (DNA, RNA, proteins, and fatty acids). Furthermore, modeling predictions indicate that during phototrophic growth, reverse electron flow from the quinone pool is a minor contributor to the production of reduced cofactors (e.g., NAD(P)H) compared to other oxidative processes (H2 and carbon substrate oxidation). Instead, the quinone pool primarily operates to aid ATP production. The high level of ATP, in turn, drives reduction processes even when NADPH levels are relatively low compared to NADP+ by coupling ATP hydrolysis to the reductive processes. The model, in agreement with experimental measurements of macromolecule ratios of cells growing on different carbon substrates, indicates that the dynamics of nucleotide versus lipid and protein production is likely a significant mechanism of balancing oxidation and reduction in the cell.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Chemical and Electrochemical O 2 Reduction on Earth-Abundant M-N-C Catalysts and Implications for Mediated Electrolysis

M-N-C catalysts, incorporating non-precious-metal ions (e.g. M = Fe, Co) within a nitrogen-doped carbon support, have been the focus of broad interest for electrochemical O 2 reduction and aerobic oxidation reactions. The present study explores the mechanistic relationship between the O 2 reduction mechanism under electrochemical and chemical conditions. In this work, chemical O 2 reduction is investigated via the aerobic oxidation of a hydroquinone, in which the O–H bonds supply the protons and electrons needed for O 2 reduction to water. Mechanistic studies have been conducted to elucidate whether the M-N-C catalyst couples two independent half-reactions (IHR), similar to electrode-mediated processes, or mediates a direct inner-sphere reaction (ISR) between O 2 and the organic molecule. Kinetic data support the latter ISR pathway. This conclusion is reinforced by rate/potential correlations that reveal significantly different Tafel slopes, implicating different mechanisms for chemical and electrochemical O 2 reduction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Converting Carbon Dioxide into Carbon Nanotubes by Reacting with Ethane

In this study, the urgency to mitigate environmental impacts from anthropogenic CO 2 emissions has propelled extensive research efforts on CO 2 reduction. The current work reports a novel approach involving transforming CO 2 and ethane into carbon nanotubes (CNTs) using earth-abundant metals (Fe, Co, Ni) at 750 °C. This route facilitates long-term carbon storage via generating high-value CNTs and produces valuable syngas with adjustable H 2 /CO ratios as byproducts. Without CO 2 , direct pyrolysis of ethane undergoes rapid deactivation. The participation of CO 2 not only enhances the durability of the catalyst, but also contributes about 30 % of the CNTs production, presenting a viable solution to CO 2 challenges. The CNT morphology depends on the catalyst used. Co- and Ni-based catalysts produce CNT with a 20 nm diameter and micrometer length, whereas Fe-based catalysts yield bamboo-like structures. This work represents a pioneering effort in utilizing CO 2 and ethane for CNT production with potential environmental and economic benefits.

09 BIOMASS FUELS↗

DOE OSTI2024

A deep decarbonization framework for the United States economy – a sector, sub-sector, and end-use based approach

Achieving the United States' target of net-zero greenhouse gas emissions by 2050 will require technological transformations and energy sector mitigation. To understand the role of dynamically evolving technologies, identify synergies and dissonance and the effect of allocating limited low-carbon biomass resources in decarbonizing the U.S. economy, we developed the Decarbonization Scenario Analysis Model. A Life Cycle Assessment based approach is implemented considering the U.S. economy as the functional unit, to estimate greenhouse gas mitigation potential for projected energy demand based on several sector-level and cross-sectoral decarbonization pathways. Direct and supply-chain emissions are accounted, resulting from changes in patterns of energy generation and consumption, technology breakthroughs, and reductions in fugitive emissions over time at the granularity of economic sectors, sub-sectors, and end-use. Decarbonization strategies are implemented over a reference case developed using Energy Information Administration (EIA AEO) projection of economic activities for 2020–2050. Based on the considered scenarios, 80–90% economy-wide decarbonization relative to the 2020 reference case is projected. Electrification, low-carbon fuels, and reduction of fugitive emissions play the most significant role to decarbonization. The majority of the remaining emissions are accounted to the supply-chain and end-use emissions from natural gas and diesel fossil-based fuels in heavy duty transportation and heavy industries, highlighting the need for developing low-carbon and carbon-negative alternatives to mitigate those fossil-based carbon emissions.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

NASA NTRS2011

Effects of Absorbing Aerosols on Accelerated Melting of Snowpack in the Tibetan-Himalayas Region

The impacts of absorbing aerosol on melting of snowpack in the Hindu-Kush-Tibetan-Himalayas (HKTH) region are studied using NASA satellite and GEOS-5 GCM. Results from GCM experiments shows that a 8-10% in the rate of melting of snowpack over the western Himalayas and Tibetan Plateau can be attributed to the aerosol elevated-heat-pump (EHP) feedback effect (Lau et al. 2008), initiated by the absorption of solar radiation by absorbing aerosols accumulated over the Indo-Gangetic Plain and Himalayas foothills. On the other hand, deposition of black carbon on snow surface was estimated to give rise to a reduction in snow surface albedo of 2 - 5%, and an increased annual runoff of 9-24%. From case studies using satellite observations and re-analysis data, we find consistent signals of possible impacts of dust and black carbon aerosol in blackening snow surface, in accelerating spring melting of snowpack in the HKHT, and consequentially in influencing shifts in long-term Asian summer monsoon rainfall pattern.

Lau, William K. M.↗

DOE OSTI2022

Annual carbon sequestration and loss rates under altered hydrology and fire regimes in southeastern USA pocosin peatlands

Peatlands drained for agriculture or forestry are susceptible to the rapid release of greenhouse gases (GHGs) through enhanced microbial decomposition and increased frequency of deep peat fires. We present evidence that rewetting drained subtropical wooded peatlands (STWPs) along the southeastern USA coast, primarily pocosin bogs, could prevent significant carbon (C) losses. To quantify GHG emissions and storage from drained and rewetted pocosin we used eddy covariance techniques, the first such estimates that have been applied to this major bog type, on a private drained (PD) site supplemented by static chamber measurements at PD and Pocosin Lakes National Wildlife Refuge. Net ecosystem exchange measurements showed that the loss was 21.2 Mg CO2 ha –1 year –1 (1 Mg = 10 6 g) in the drained pocosin. Under a rewetted scenario, where the annual mean water table depth (WTD) decreased from 60 to 30 cm, the C loss was projected to fall to 2 Mg CO 2 ha –1 year –1 , a 94% reduction. If the WTD was 20 cm, the peatlands became a net carbon sink (–3.3 Mg CO2 ha –1 year –1 ). Hence, net C reductions could reach 24.5 Mg CO 2 ha –1 year –1 , and when scaled up to the 4000 ha PD site nearly 100,000 Mg CO 2 year –1 of creditable C could be amassed. We conservatively estimate among the 0.75 million ha of southeastern STWPs, between 450 and 770 km 2 could be rewet, reducing annual GHG emissions by 0.96–1.6 Tg (1 Tg = 10 12 g) of CO 2 , through suppressed microbial decomposition and 1.7–2.8 Tg via fire prevention, respectively. Despite covering <0.01% of US land area, rewetting drained pocosin can potentially provide 2.4% of the annual CO 2 nationwide reduction target of 0.18 Pg (1 Pg = 10 15 g). Finally, suggesting pocosin restoration can contribute disproportionately to the US goal of achieving net-zero emission by 2050.

58 GEOSCIENCES↗

DOE OSTI2025

Hot Hydrogen Exposure of U x Zr 1-x C y Nuclear Fuel: The Effect of Additional Carbon

Nuclear thermal propulsion (NTP) using hydrogen as propellant in a solid-state fission reactor to reach temperatures of up to 3000K can achieve significantly higher specific impulse than chemical propulsion. A promising fuel that is again considered for NTP is U x Zr 1-x C y . To reduce the overall mass loss as well as the uranium fuel loss, a range of experiments using additional carbon in hot hydrogen (2600 K, 6 SLPM flow rate) were performed for up to 5-6 h. Both a CH 4 addition (0.1 and 0.2 vol%) in the hydrogen stream and the use of sacrificial graphite pieces upstream of the samples were tested, with sample compositions from 5 at% UC to 30 at% UC. The results showed a strong reduction of mass loss, up to a factor of 3, as well as a reduction of surface uranium losses in the presence of additional carbon in the atmosphere. Even with additional carbon in the atmosphere, material with 30 at% UC was not stable, but material with 20 at% UC was stable for up to 6h. The sample surfaces showed texturing after processing, possibly by grain growth on the surface. This led to a separation into grains with high uranium content close to the (100)-orientation, and with low uranium content in grains close to the (111)-orientation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Supplementing biofuel mandates with a carbon mitigation policy can lead to water quality co-benefits

Biofuel mandates can impact the environment in multiple ways that may be positive or negative, including affecting life-cycle greenhouse gas (GHG) emissions by displacing fossil fuels, affecting soil carbon stocks due to accompanying land use change, and water quality due to changes in fertilizer requirements and the mix of crops used as feedstocks. To achieve desired environmental outcomes in the presence of a biofuel mandate, additional policy instruments must be adopted to supplement the mandate. We develop an integrated and spatially explicit ecosystem-economic modeling framework to analyze the cost-effectiveness of alternative policies to achieve desired targets for GHG emissions reduction from the agricultural and fuel sectors in the USA and nitrate leaching reduction in the Gulf of Mexico below the levels that would be achieved by a corn ethanol and/or a cellulosic ethanol mandate in the USA. We find that while a corn ethanol mandate lowers GHG emissions, it increases nitrate leaching due to the expansion of corn production; a cellulosic ethanol mandate lowers both GHG emissions and nitrate leaching relative to a corn ethanol mandate, but the additional carbon and nitrate prices are needed to achieve anticipated GHG reduction and nitrate reduction targets. We also find that accompanying a biofuel mandate with a GHG reduction target alone leads to substantial nitrate reduction co-benefits, but a nitrate reduction target alone is less effective in reducing GHG emissions. Combining a GHG standard with a nitrate standard can achieve GHG and nitrate reduction targets at lower carbon and nitrate prices as compared to implementing each of these policies independently. Furthermore, our findings show that disregarding policy co-benefits can overestimate the GHG and nitrate prices needed to achieve policy targets and higher policy costs.

09 BIOMASS FUELS↗

DOE OSTI2023

Influence of Spatial Dipole Pattern in Asian Aerosol Changes on East Asian Summer Monsoon

Since China implemented the Air Pollution Prevention and Control Action Plan in 2013, the aerosol emissions in East Asia have been greatly reduced, while emissions in South Asia have continued to increase. This has led to a dipole pattern of aerosol emissions between South Asia and East Asia. We report the East Asian summer monsoon (EASM) responses to the dipole changes in aerosol emissions during 2013–17 are investigated using the atmosphere model of Community Earth System Model version 2 (CESM2). We show that decreases in East Asian emissions alone lead to a positive aerosol effective radiative forcing (ERF) of 1.59 (±0.97) W m -2 over central-eastern China (25°–40°N, 105°–122.5°E), along with a 0.09 (±0.07)°C warming in summer during 2013–17. The warming intensified the land–sea thermal contrast and increased the rainfall by 0.32 (±0.16) mm day -1 . When considering both the emission reductions in East Asia and increases in South Asia, the ERF is increased to 3.39 (±0.89) W m -2 , along with an enhanced warming of 0.20 (±0.08)°C over central-eastern China, while the rainfall insignificant decreased by 0.07 (±0.16) mm day -1 . It is due to the westward shift of the strengthened western Pacific subtropical high, linked to the increase in black carbon in South Asia. Based on multiple EASM indices, the reductions in aerosol emissions from East Asia alone increased the EASM strength by almost 5%. Considering the effect of the westward shift of WPSH, the dipole changes in emissions together increased the EASM by 5%–15% during 2013–17, revealing an important role of South Asian aerosols in changing the East Asian climate.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Influence of Spatial Dipole Pattern in Asian Aerosol Changes on East Asian Summer Monsoon

Since China implemented the Air Pollution Prevention and Control Action Plan in 2013, the aerosol emissions in East Asia have been greatly reduced, while emissions in South Asia have continued to increase. This has led to a dipole pattern of aerosol emissions between South Asia and East Asia. Here, the East Asian summer monsoon (EASM) responses to the dipole changes in aerosol emissions during 2013–17 are investigated using the atmosphere model of Community Earth System Model version 2 (CESM2). We show that decreases in East Asian emissions alone lead to a positive aerosol effective radiative forcing (ERF) of 1.59 (±0.97) W m -2 over central-eastern China (25°–40°N, 105°–122.5°E), along with a 0.09 (±0.07)°C warming in summer during 2013–17. The warming intensified the land–sea thermal contrast and increased the rainfall by 0.32 (±0.16) mm day -1 . When considering both the emission reductions in East Asia and increases in South Asia, the ERF is increased to 3.39 (±0.89) W m -2 , along with an enhanced warming of 0.20 (±0.08)°C over central-eastern China, while the rainfall insignificant decreased by 0.07 (±0.16) mm day -1 . It is due to the westward shift of the strengthened western Pacific subtropical high, linked to the increase in black carbon in South Asia. Based on multiple EASM indices, the reductions in aerosol emissions from East Asia alone increased the EASM strength by almost 5%. Finally, considering the effect of the westward shift of WPSH, the dipole changes in emissions together increased the EASM by 5%–15% during 2013–17, revealing an important role of South Asian aerosols in changing the East Asian climate.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Seasonal Fluctuations in Iron Cycling in Thawing Permafrost Peatlands

In permafrost peatlands, up to 20% of total organic carbon (OC) is bound to reactive iron (Fe) minerals in the active layer overlying intact permafrost, potentially protecting OC from microbial degradation and transformation into greenhouse gases (GHG) such as CO 2 and CH 4 . During the summer, shifts in runoff and soil moisture influence redox conditions and therefore the balance of Fe oxidation and reduction. Whether reactive iron minerals could act as a stable sink for carbon or whether they are continuously dissolved and reprecipitated during redox shifts remains unknown. We deployed bags of synthetic ferrihydrite (FH)-coated sand in the active layer along a permafrost thaw gradient in Stordalen mire (Abisko, Sweden) over the summer (June to September) to capture changes in redox conditions and quantify the formation and dissolution of reactive Fe(III) (oxyhydr)oxides. We found that the bags accumulated Fe(III) under constant oxic conditions in areas overlying intact permafrost over the full summer season. In contrast, in fully thawed areas, conditions were continuously anoxic, and by late summer, 50.4 ± 12.8% of the original Fe(III) (oxyhydr)oxides were lost via dissolution. Periodic redox shifts (from 0 to +300 mV) were observed over the summer season in the partially thawed areas. This resulted in the dissolution and loss of 47.2 ± 20.3% of initial Fe(III) (oxyhydr)oxides when conditions are wetter and more reduced, and new formation of Fe(III) minerals (33.7 ± 8.6% gain in comparison to initial Fe) in the late summer under more dry and oxic conditions, which also led to the sequestration of Fe-bound organic carbon. Our data suggest that there is seasonal turnover of iron minerals in partially thawed permafrost peatlands, but that a fraction of the Fe pool remains stable even under continuously anoxic conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Near-Net-Shape Hot Isostatic Press Manufacturing Modality for sCO2 CSP Capital Cost Reduction

Through this DOE funded 3.5-year research project, feasibility of fabricating supercritical carbon dioxide (sCO2) turbine components by powder metallurgy (PM) based near-net-shape (NNS) hot isostatic pressing (HIP) was demonstrated in a turbine nozzle ring, a turbine casing with Haynes 282 powder, and a bimetallic pipe with Haynes 282 and SS415 powder. As-HIP microstructure of various powders and HIP processing conditions was studied to downselect a condition for the prototype components. Tensile strength and low cycle fatigue (LCF) capability of PM HIP 282 was found to be superior to cast 282, despite a debit in creep stress capability that could be mitigated by component design modification. Near-Net-shape with minimal post machining was achieved by modeling the non-uniform shrinkage during HIP cycle and designing the HIP tooling to meet dimensional targets. The prototypes of turbine nozzle ring and bimetallic pipe were successful in achieving overall dimension, microstructure, and properties, despite dimensional tolerance affected by chemical milling rate. The prototype of a 1700lbs turbine casing was partially successful in achieving dimension, microstructure in as-HIP state, and providing consistent mechanical properties, however, cracking issue during post heat treatment required further investigation. The estimated manufacturing cost using NNS HIP was a ~50% reduction compared to forging with extensive machining, which translated into ~$100/kWe CAPEX cost reduction for concentrated solar power (CSP) power block.

14 SOLAR ENERGY↗

DOE OSTI2020

In situ reductive dissolution to remove Iodine-129 from aquifer sediments

The use of an aqueous reductant (Na-dithionite) with pH buffer (K-carbonate, pH 12) was evaluated in this laboratory study as a potential remedial approach for removing Fe oxide associated iodine and enhancing pump-and-treat extraction from iodine-contaminated sediments in the unconfined aquifer in the 200 West Area of the Hanford site. X-ray fluorescence data of untreated sediment indicated that iodine was largely associated with Fe (i.e., incorporated into Fe oxides), however, XANES data was inconclusive as to valence state. During groundwater leaching, aqueous and adsorbed iodine was quickly released, then additional iodine was slowly released potentially from dissolution of one or more surface phases. The Na-dithionite treatment removed greater iodine mass (2.9x) at a faster rate (1 to 4 orders of magnitude) compared to leaching with groundwater alone. Iron extractions for untreated and treated sediments showed a decrease in Fe(III)-oxides, which likely released iodine to aqueous solution. Solid phase inorganic carbon and aqueous Ca and Mg analysis further confirmed that significant calcite dissolution did not occur in these experiments meaning these phases did not release significant iodine. Although it was expected that, after treatment, 127 I concentrations would eventually be lower than untreated sediments, leaching experiments showed continued, elevated iodine concentrations for treated samples over 750 hours. Stop flow events during 1-D column leaching suggested that some iodide precipitated within the first few pore volumes. In the survey of metals during leaching, some silver was detected which could have been solubilized by the elevated pH of initial Na-dithionite injection. Then, silver (or other metals) could have subsequently precipitated with iodide during the initial stop flow event forming a slowly dissolving source. Although significantly greater iodine is removed with treatment, the long-term leaching needs to be investigated further as it may limit dithionite treatment at the field scale.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Closing the Loop on Automotive Carbon Fiber Prepreg Manufacturing Scrap

The project demonstrated how to “close the loop” on carbon fiber by integrating industrial carbon fiber scrap into new functional components in an automotive lightweighting application. The project serves as a validation of discontinuous recycled carbon fiber in a commercial context, while generating comprehensive material data throughout the production chain. To this end, the project exhibited increasing complexity as material evaluation progressed from benchtop to commercial scale through full-scale part production, with key material properties thoroughly characterized throughout the process. Of particular focus was the form of the fiber that was fed into compounding, as recycled fiber has historically been problematic to feed at commercial-scale. Carbon fiber is energy-intensive to manufacture, so reuse of existing fiber material can reduce costs and increase sustainability. Additionally, by integrating recovered short fiber into a thermoplastic, regrind processes can be used to provide feedstock for later generations of product. While regrind plastics are not “infinitely recyclable”, reusing the manufacturing scrap over several generations of products can greatly increase material sustainability and lower the fractional embodied energy of each successive product. As such, this project supports the IACMI technical goals of (1) 25% lower carbon fiber-reinforced polymer (CFRP) cost, (2) 50% reduction in CFRP embodied energy, and (3) 80% composite recyclability into useful products. The initial stage of the project involved down selecting surface treatment (sizing) chemistries. Sizing evaluations were performed on Vartega’s chemically recycled intermediate modulus fiber along with standard modulus dry scrap which was oversized with sizing provided by Michelman. More dramatic improvements from sizing were found on the standard rather than the intermediate modulus fibers. The strength of the chemically recycled individual fibers were evaluated by Michelman and ORNL through single fiber testing and found to be comparable to similarly evaluated virgin fibers. UDRI’s mechanical testing on injection molded test specimens identified similar mechanical properties and fiber distribution relative to benchmark specimens. Additional surface chemistry tests and visualizations were performed by the Colorado School of Mines to confirm close conformance between the benchmark and recycled-fiber specimens. As the mechanical test results exceeded the 80% threshold established as the go/no-go(GNG), the project scale was increased to use commercial-scale equipment that would both better characterize the manufacturing utility of the target product format and allow qualitative assessment of a complex commercial part. An upscaled compounding evaluation was performed with a 27 mm twin-screw compounding extruding using oversized standard modulus fibers that were formatted to improve bulk solids transfer. The project team anticipated that milestone mechanical benchmarks could be achieved given the favorable performance of the sized standard modulus material identified in the initial micro-compounding trials. While the mechanical performance did meet the milestone target for that phase of the project, mechanical properties for this standard modulus-based compound were still less than those of the Ford specification. To compare the performance, the project team oversized intermediate modulus dry fibers and compounded them with the project resin at BASF using a 40 mm compounder. Test specimen mechanical performance exceeded the targets laid out in both the project milestone and the Ford specification. A series of prototype parts were successfully molded, albeit with instances of short shot components due to the high thermal conductivity of the carbon fiber compared to glass fiber for which the prototype tool was designed for. The project demonstrated that recycled carbon fiber is a viable option in fiber reinforced compound, providing greatly increased strength and modulus for applications that require them. The “agglomerated” format that facilitated effective bulk solids transfer of recovered fiber showed promise for industrial application.

36 MATERIALS SCIENCE↗