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NASA NTRS1990

Advanced Composite Pistons

New concept involving improved configuration of reinforcing fibers and improved fabrication process proposed to improve thermal and mechanical properties of composite piston structures. Reduces amount of labor necessary to manufacture piston structures, with attendant reductions in costs. Single knitted-carbon-fiber sock used to form external surfaces of piston. Advantages include elimination of heavy dependence on inherently weak interlaminar properties of carbon-carbon; ease of automation to reduce fabrication costs; readily modifiable architecture to vary mechanical properties to desired values; and reduction in number of elements required to fabricate pistons. Advantage of piston structures lies in applications where light weight and high specific performance primary considerations.

Taylor, Allan H.↗

DOE OSTI2024

Aliphatic Amines from Waste Polyolefins by Tandem Pyrolysis, Hydroformylation, and Reductive Amination

Pyrolysis of waste plastics can produce a product mixture with a high concentration of olefins (>50 wt%). The olefins, as building blocks in the petroleum industry, are potential precursors for valuable commodity chemicals with higher values (>$2000 per ton). In this work, we produce aldehydes by hydroformylation of the olefins present in pyrolysis oil from colored post-consumer recycled high-density polyethylene (PCR-HDPE). The obtained aldehydes in the oil are then converted into aliphatic amines via reductive amination with a Ru/C catalyst. The aminated oil was characterized by multiple analytical chemistry techniques including elemental analysis, nuclear magnetic resonance spectroscopy, high-resolution liquid chromatography-mass spectrometry, and gas chromatography-mass spectrometry with a Polyarc flame ionization detector. The concentration of metals in the PCR-HDPE and oil changes during the tandem processes, showing limited effects of these elements (e.g., Al, Ca, Fe, Mg, Ti, Zn) on hydroformylation and reductive amination. Additionally, we demonstrated that reductive amination of aldehydes with varied carbon numbers and branching properties can be achieved in the presence of a complex mixture, including paraffins and aromatics. The results indicate that waste plastics have the potential to serve as a renewable source for mono and di aliphatic amines, thereby diminishing reliance on fossil feedstocks as the current primary amine source.

aliphatic amines↗

DOE OSTI2026

Polyketide synthase–like functionality acquired by plant fatty acid elongase

Fatty acid elongation typically proceeds through a four-step cycle of condensation, reduction, dehydration, and reduction for each two-carbon extension. Here, we describe a variation of this pathway in Orychophragmus limprichtianus, whose seed oil contains previously unknown C24-C28 keto-hydroxy fatty acids that account for ~25% of total fatty acids. These compounds are produced through an endoplasmic reticulum–localized discontinuous elongation process in which a 3-keto-hydroxy intermediate bypasses full reduction and is extended through a polyketide synthase–like mechanism. Transcriptomic and functional assays identified two divergent enzymes, a variant fatty acid elongase 1 (FAE1) and a low-activity 3-ketoacyl-CoA reductase (KCR1), as central to this process. Protein modeling and mutant analysis suggest that specific amino acid substitutions underlie altered KCR1 activity, enabling accumulation of keto intermediates. Our findings reveal unexpected flexibility in plant fatty acid elongation and provide innovative tools for engineering plants and microbes to produce renewable oils with tailored industrial functions.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2023

Comparisons of bpy and phen Ligand Backbones in Cr-Mediated (Co-)Electrocatalytic CO 2 Reduction

Due to the rise in atmospheric carbon dioxide (CO 2 ) concentrations, there is a need for the development of new strategies to enhance the selectivity and activity of the electrocatalytic conversion of CO 2 to value-added products. The incorporation of redox mediators (RMs) as co-catalysts to enhance the transfer of redox equivalents during catalysis has been gaining more attention in recent years across a variety of small molecule transformations. We have shown that using Cr-centered complexes with sulfone-based RMs leads to an enhancement of CO 2 reduction electrocatalysis under protic conditions via an inner-sphere mechanism. In these co-catalytic systems, an oxygen atom of the reduced RM binds to the Cr center to form a key intermediate stabilized by pancake bonding between the reduced aromatic components of the catalyst ligand backbone and the RM. This interaction facilitates the transfer of an electron and accesses a more kinetically favorable reaction pathway. Here, we show that expanding the aromatic character of the ligand backbone of the catalyst as well as the RM can cause a greater enhancement of co-electrocatalytic activity. These results suggest that further activity improvements can be achieved by focusing on the kinetic and thermodynamic parameters which control association between the catalyst and RM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2018

Design and Development of Advanced Air-Cathodes for Li-Air Battery

NASA's future missions demand high energy density batteries. Current state-of-the-art lithium-ion batteries (LIBs) reach the specific energy capacity limits (<250 Wh/kg), thus new electrochemical storage technologies are needed to meet NASA's future mission requirement of >400 Wh/kg. Battery chemistries with higher theoretical energy densities in particular, Li-metal based battery chemistries such as Li-air, are being actively pursued, but there remains a number of issues to be solved. Development of advanced and optimized air cathodes will be crucial for improving capacity retention and cycle life of Li-air battery. The microstructure of carbon substrates and the catalytic oxygen reduction of the air-cathode play critical roles in the electrochemical performance in Li-air batteries. With the development and proper design of air cathodes, the energy efficiency and energy density can be enhanced significantly. In this presentation, the results of advanced permeable air cathodes design with different substrates such as 2D carbon paper or carbon cloth, vs 3D graphene or metal foam, different high surface area carbon materials and incorporation with catalysts on oxygen reduction reactions, different porosity controlling of air cathode as well the additives in electrolyte will be presented. The cycling and rate capability performance of these air-cathodes in the Li-air cells will be discussed as well.

Wu, James J.↗

DOE OSTI2022

Modeling Isothermal Reduction of Iron Ore Pellet Using Finite Element Analysis Method: Experiments & Validation

Iron ore pellet reduction experiments were performed with pure hydrogen (H2) and mixtures with carbon monoxide (CO) at different ratios. For direct reduction processes that switch dynamically between reformed natural gas and hydrogen as the reductant, it is important to understand the effects of the transition on the oxide reduction kinetics to optimize the residence time of iron ore pellets in a shaft reactor. Hence, the reduction rates were studied by varying experimental parameters such as the temperature (800, 850 & 900 °C), reactant gas flow rate (100, 150 & 200 cm3/min), pellet size and composition of the reactant gas mixture. The rate of reduction was observed to increase with an increase in temperature and reactant gas flow rate, but it decreased with an increase in pellet size. SEM greyscale analysis was performed to analyze the porosity and phase composition of partially reduced pellets. The porosity of the pellets was observed to increase from 0.3 for unreacted pellet to 0.42 for a completely reduced pellet. Energy-dispersive X-ray spectroscopy (EDAX) analysis was performed to identify the phases observed in the SEM images. The fraction of iron phase was observed to increase from the shell region of the pellet to the core region with an increase in the degree of reduction. A 2D-axisymmetric numerical model was developed on COMSOL Multiphysics, and it was validated using the conversion (X) vs. time curves obtained from each experiment. The model was able to accurately predict the total time needed for the complete conversion of a single iron ore pellet for multiple experiments. Effects of changes in the porosity and tortuosity of the pellet on the model were also studied and the rate of reduction was observed to be sensitive to changes in both porosity and tortuosity. The SEM analysis and the model results show that tortuosity is higher for pellets reduced with H2 than for pellets reduced with H2-CO gas mixtures.

08 HYDROGEN↗

DOE OSTI2020

A spatial emergent constraint on the sensitivity of soil carbon turnover to global warming

Carbon cycle feedbacks represent large uncertainties in climate change projections, and the response of soil carbon to climate change contributes the greatest uncertainty to this. Future changes in soil carbon depend on changes in litter and root inputs from plants and especially on reductions in the turnover time of soil carbon (τ s ) with warming. An approximation to the latter term for the top one metre of soil (ΔC s,τ ) can be diagnosed from projections made with the CMIP6 and CMIP5 Earth System Models (ESMs), and is found to span a large range even at 2 °C of global warming (-196 ± 117 PgC). Here, we present a constraint on ΔC s,τ , which makes use of current heterotrophic respiration and the spatial variability of τs inferred from observations. This spatial emergent constraint allows us to halve the uncertainty in ΔC s,τ at 2 °C to -232 ± 52 PgC.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Iron as a driver of organic carbon fate in permafrost regions

Iron (Fe) and its biogeochemical interactions with organic carbon (OC) exert critical controls over carbon storage and water quality across Arctic and sub-Arctic landscapes. Permafrost thaw affects Fe–organic carbon interactions by exposing thawed material and driving shifts in hydrologic regimes. Here we propose a conceptual framework describing how Fe–OC interactions respond to permafrost thaw and the implications for global carbon cycling. The framework builds on current understanding of hydrologically driven processes that are altered by permafrost thaw, including microbial Fe reduction that influences OC decomposition and carbon emissions; Fe cycling through redox transformations and sulfide oxidation; dissolution and reprecipitation of Fe–OC assemblages; and Fe export to river networks. We put forward four testable hypotheses—on topics from Fe supply to its role in soil OC storage and transfer to rivers—to advance understanding of the coupled environmental controls on pore-scale reactions (that is, microscale reactions at mineral–water–microorganism interfaces) that are central to global Fe–OC cycling. Our framework highlights how soil-profile- and landscape-scale processes, such as hydrologic connectivity and redox dynamics, regulate pore-scale Fe–OC reactions.

Herndon, Elizabeth [ORNL] (ORCID:0000000291945493)↗

DOE OSTI2023

The Coastal Carbon Library and Atlas: Open source soil data and tools supporting blue carbon research and policy

Abstract Quantifying carbon fluxes into and out of coastal soils is critical to meeting greenhouse gas reduction and coastal resiliency goals. Numerous ‘blue carbon’ studies have generated, or benefitted from, synthetic datasets. However, the community those efforts inspired does not have a centralized, standardized database of disaggregated data used to estimate carbon stocks and fluxes. In this paper, we describe a data structure designed to standardize data reporting, maximize reuse, and maintain a chain of credit from synthesis to original source. We introduce version 1.0.0. of the Coastal Carbon Library, a global database of 6723 soil profiles representing blue carbon‐storing systems including marshes, mangroves, tidal freshwater forests, and seagrasses. We also present the Coastal Carbon Atlas, an R‐shiny application that can be used to visualize, query, and download portions of the Coastal Carbon Library. The majority (4815) of entries in the database can be used for carbon stock assessments without the need for interpolating missing soil variables, 533 are available for estimating carbon burial rate, and 326 are useful for fitting dynamic soil formation models. Organic matter density significantly varied by habitat with tidal freshwater forests having the highest density, and seagrasses having the lowest. Future work could involve expansion of the synthesis to include more deep stock assessments, increasing the representation of data outside of the U.S., and increasing the amount of data available for mangroves and seagrasses, especially carbon burial rate data. We present proposed best practices for blue carbon data including an emphasis on disaggregation, data publication, dataset documentation, and use of standardized vocabulary and templates whenever appropriate. To conclude, the Coastal Carbon Library and Atlas serve as a general example of a grassroots F.A.I.R. (Findable, Accessible, Interoperable, and Reusable) data effort demonstrating how data producers can coordinate to develop tools relevant to policy and decision‐making.

Holmquist, James R.↗

NASA NTRS1984

Preparation and evaluation of advanced catalysts for phosphoric acid fuel cells

The platinum electrocatalysts were characterized for their crystallite sizes and the degree of dispersion on the carbon supports. One application of these electrocatalysts was for anodic oxidation of hydrogen in hot phosphoric acid fuel cells, coupled with the influence of low concentrations of carbon monoxide in the fuel gas stream. In a similar way, these platinum on carbon electrocatalysts were evaluated for oxygen reduction in hot phosphoric acid. Binary noble metal alloys were prepared for anodic oxidation of hydrogen and noble metal-refractory metal mixtures were prepared for oxygen reduction. An exemplar alloy of platinum and palladium (50/50 atom %) was discovered for anodic oxidation of hydrogen in the presence of carbon monoxide, and patent disclosures were submitted. For the cathode, platinum-vanadium alloys were prepared showing improved performance over pure platinum. Preliminary experiments on electrocatalyst utilization in electrode structures showed low utilization of the noble metal when the electrocatalyst loading exceeded one weight percent on the carbon.

Stonehart, P.↗

NASA NTRS2003

Method for the control of NOx emissions in long-range space travel

The wheat straw, an inedible biomass that can be continuously produced in a space vehicle has been used to produce activated carbon for effective control of NOx emissions from the incineration of wastes. The optimal carbonization temperature of wheat straw was found to be around 600 degrees C when a burnoff of 67% was observed. The BET surface area of the activated carbon produced from the wheat straw reached as high as 300 m2/g. The presence of oxygen in flue gas is essential for effective adsorption of NO by activated carbon. On the contrary, water vapor inhibits the adsorption efficiency of NO. Consequently, water vapor in flue gas should be removed by drying agents before adsorption to ensure high NO adsorption efficiency. All of the NO in the flue gas was removed for more than 2 h by the activated carbons when 10% oxygen was present and the ratio of carbon weight to the flue gas flow rate (W/F) was 30 g min/L, with a contact time of 10.2 s. All of NO was reduced to N2 by the activated carbon at 450 degrees C with a W/F ratio of 15 g min/L and a contact time of 5.1 s. Reduction of the adsorbed NO also regenerated the activated carbon, and the regenerated activated carbon exhibited an improved NO adsorption efficiency. However, the reduction of the adsorbed NO resulted in a loss of carbon which was determined to be about 0.99% of the activated carbon per cycle of regeneration. The sufficiency of the amount of wheat straw in providing the activated carbon based on a six-person crew, such as the mission planned for Mars, has been determined. This novel approach for the control of NOx emissions is sustainable in a closed system such as the case in space travel. It is simple to operate and is functional under microgravity environment.

NASA Discipline Life Support Systems↗

DOE OSTI2025

Nickel Enhances InPd-Catalyzed Nitrate Reduction Activity and N 2 Selectivity

Palladium–indium (PdIn) is a well-established bimetallic composition for reductively degrading nitrate anions, one of the most ubiquitous contaminants in the groundwater. However, the scarcity and the variable price of these rare-earth and platinum group critical metals may hinder their use for water treatment. Nickel (Ni), a nonprecious metal in the same element group as Pd, could partially replace and lower Pd usage if the resulting trimetallic composition is sufficiently catalytically active. Herein, we report the synthesis and nitrate reduction catalysis of activated carbon-supported “In-on-Pd-on-Ni” catalysts (InPdNi/AC). While bimetallic InPd/AC (0.05 wt % In, 1.3 wt % Pd) was expectedly active, trimetallic InPdNi/AC containing the same In amount, much less Pd (0.1 wt %), and 1 wt % Ni was >17 more active (k cat ≈ 20 vs 349 L min –1 g surface metal –1 ). X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations showed that Pd gained electron density from Ni, correlating to the increased nitrate reduction activity. Ammonium byproduct selectivity for InPdNi/AC (18% at 50% nitrate conversion) was lower compared to that of InPd/AC (48%), suggestive of the higher surface coverage of NO or its greater reactivity with NO 2 – , which led to more N 2 . Accounting for the catalyst precursor, manufacturing costs, and spent metal recovery, we calculated that Ni incorporation lowered the net catalyst cost significantly (from $\$$1028/kg to $\$$170/kg). The trimetallic composition lowered, by ∼26 times, the catalyst cost of a stirred tank reactor sized to the same treatment capacity as that for the bimetallic case. In conclusion, the results demonstrate that the partial replacement of the precious metal with an earth-abundant one leads to a higher efficiency and lower cost denitrification catalyst, via a material strategy that should be beneficial for other clean-water catalytic systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

The Significance of the 'Insignificant': Non-covalent Interactions in CO 2 Reduction Reactions with 3C-TM (TM=Sc-Zn) Single-Atom Catalysts

With energy shortages and excessive CO 2 emissions driving climate change, converting CO 2 into high-value-added products offers a promising solution for carbon recycling. We investigate CO 2 reduction reactions (CO2RR) catalyzed by 10 single-atom catalysts (SACs), incorporating weak non-covalent interactions, specifically lone pair-π and H-π interactions. The SACs, consisting of transition metals coordinated by three carbon atoms in a defective graphene substrate (3C-TM, TM=Sc-Zn), leverage these interactions to influence the energy fluctuations of intermediates and the limiting potentials of CO 2 RR, without altering the overall reaction pathway. Further, our findings show that SACs based on early transition metals (Sc, Ti, V, Cr) can serve as catalysts for C 1 products, including HCOOH, HCHO, CH 3 OH, and CH 4 , while those based on Fe and Co are suitable for CO formation. Driving force analysis helps bridge theoretical results with experimental observations and propose a modified approach for assessing hydrogen evolution reactions (HER) competition. SACs based on Ni and Cu exhibit moderate HER tolerance, while early transition metals excel in selective CO 2 reduction. We also identify a linear scaling relationship between the free energies of *COOH and *CO. This study offers valuable insights for future experimental studies and large-scale computational screenings.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Data-driven simultaneous process optimization and adsorbent selection for vacuum pressure swing adsorption

Technologies for post-combustion carbon capture are essential for the reduction of greenhouse gas emissions to the atmosphere. However, they are still associated with high costs and energy consumption. Intensified processes for carbon capture have the potential to overcome these challenges due to their higher efficiency, lower capital cost, and increased operational flexibility. Here, this work investigates simultaneous optimization of process conditions and adsorbent selection for a modular Vacuum Pressure-Swing Adsorption system designed for CO 2 capture. Both surrogate-based Nonlinear Programming and Mixed-Integer Nonlinear Programming approaches are applied and compared in terms of computational efficiency and solution accuracy. Moreover, process performance results are examined by applying several data analytics techniques to gain insights into the material-process correlations. Data-driven classifiers and neural networks can accurately predict whether a material is likely to satisfy purity, recovery, and energy constraints when operated at optimal process conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

An Integrated Feasibility Study of Reservoir Thermal Energy Storage (RTES) in Portland, OR, USA

In regions with long cold overcast winters and sunny summers, Deep Direct-Use (DDU) can be coupled with Reservoir Thermal Energy Storage (RTES) technology to take advantage of pre-existing subsurface permeability to save summer heat for later use during cold seasons. Many aquifers worldwide are underlain by permeable regions (reservoirs) containing brackish or saline groundwater that has limited beneficial use due to poor water quality. We investigate the utility of these relatively deep, slow flowing reservoirs for RTES by conducting an integrated feasibility study in the Portland Basin, Oregon, USA, developing methods and obtaining results that can be widely applied to RTES systems elsewhere. As a case study, we have conducted an economic and social cost-benefit analysis for the Oregon Health and Science University (OHSU), a teaching hospital that is recognized as critical infrastructure in the Portland Metropolitan Area. Our investigation covers key factors that influence feasibility including 1) the geologic framework, 2) heat and fluid flow modeling, 3) capital and maintenance costs, 4) the regulatory framework, and 5) operational risks. By pairing a model of building seasonal heat demand with an integrated model of RTES resource supply, we determine that the most important factors that influence RTES efficacy in the study area are operational schedule, well spacing, the amount of summer heat stored (in our model, a function of solar array size), and longevity of the system. Generally, heat recovery efficiency increases as the reservoir and surrounding rocks warm, making RTES more economical with time. Selecting a base-case scenario, we estimate a levelized cost of heat (LCOH) to compare with other sources of heating available to OHSU and find that it is comparable to unsubsidized solar and nuclear, but more expensive than natural gas. Additional benefits of RTES include energy resiliency in the event that conventional energy supplies are disrupted (e.g., natural disaster) and a reduction in fossil fuel consumption resulting in a smaller carbon footprint. Key risks include reservoir heterogeneity and a possible reduction in permeability through time due to scaling (mineral precipitation). Lastly, a map of thermal energy storage capacity for the Portland Basin yields a total of 43,400 GWh, suggesting tremendous potential for RTES in the Portland Metropolitan Area.

14 SOLAR ENERGY↗

DOE OSTI2022

Novel Co‐Catalytic Activities of Solid and Liquid Phase Catalysts in High‐Rate Li‐Air Batteries

Abstract Li‐air batteries are considered strong candidates for the next‐generation energy storage systems designed for electrical transportation. However, low cyclability and current rates are two major drawbacks that hinder them from further realization. These issues necessitate the discovery of novel materials to significantly enhance the redox process of discharge products. In this study, a novel catalytic system comprised of tin sulfide (SnS) nanoflakes as a solid catalyst and tin iodide (SnI 2 ) as a dual‐functional electrolyte additive is discovered. This system enables operating the battery at high current rates up to 10 000 mA g −1 (corresponding to 1 mA cm −2 ). The SnS catalyst shows outstanding catalytic activity for both oxygen reduction and evolution reactions compared to carbon, noble metals, and other transition metal dichalcogenides. It also exhibits good structural integrity at high rates. The computations indicate numerous possible oxygen reduction sites without oxygen dissociations on the SnS surface through solution mechanism that is likely responsible for the formation of Li 2 O 2 . The calculations also indicate that the role of the SnI 2 is not only reacting with the lithium anode to provide protection but reducing the charge potential by promoting catalytic decomposition of the Li 2 O 2 . This work provides new novel additives for designing high‐rate Li‐air batteries.

25 ENERGY STORAGE↗

DOE OSTI2026

Carbon nanodot precursors enable ultrahigh-loading copper single-atom catalysts for oxygen reduction reaction

Single-atom catalysts (SACs) have attracted significant attention in electrocatalysis due to their high metal utilization and tunable electronic structures; however, their practical implementation is often limited by poor atomic dispersion, low metal loadings (typically < 1 wt%), and insufficient anchoring of single metal atoms on catalyst supports. Herein, we report a simple and versatile strategy to synthesize copper single-atom catalysts (Cu-SACs) with ultrahigh metal loading using citric-acid-derived carbon nanodots as metal-capturing precursors. Through hydrothermal treatment followed by pyrolysis in the presence of urea, atomically dispersed copper atoms coordinated with nitrogen are incorporated into a carbon framework, achieving a Cu loading of up to 20 wt% while maintaining atomic dispersion. Notably, a significant fraction of the copper single atoms exists as Cu+–N2 coordination, which provides under-coordinated and catalytically active sites. The resulting Cu-SAC exhibits promising oxygen reduction reaction (ORR) activity in alkaline media, delivering a limiting current density comparable to that of commercial 20 wt% Pt/C with a predominant four-electron reduction pathway. Despite this high intrinsic activity, durability tests reveal gradual performance degradation under prolonged electrochemical operation, which is attributed to demetallation and aggregation of copper single atoms into metallic nanoparticles. These results demonstrate the potential of carbon nanodot-based platforms for synthesizing high-loading SACs, while underscoring the critical need to simultaneously control carbon porosity and metal–nitrogen coordination to enhance active-site accessibility and durability.

Sharma, Prakhar [University of Kentucky]↗

DOE OSTI2021

Novel technologies for emission reduction complement conservation agriculture to achieve negative emissions from row-crop production

Plants remove carbon dioxide from the atmosphere through photosynthesis. Because agriculture’s productivity is based on this process, a combination of technologies to reduce emissions and enhance soil carbon storage can allow this sector to achieve net negative emissions while maintaining high productivity. Unfortunately, current row-crop agricultural practice generates about 5% of greenhouse gas emissions in the United States and European Union. Here, to reduce these emissions, significant effort has been focused on changing farm management practices to maximize soil carbon. In contrast, the potential to reduce emissions has largely been neglected. Through a combination of innovations in digital agriculture, crop and microbial genetics, and electrification, we estimate that a 71% (1,744 kg CO 2 e/ha) reduction in greenhouse gas emissions from row crop agriculture is possible within the next 15 y. Importantly, emission reduction can lower the barrier to broad adoption by proceeding through multiple stages with meaningful improvements that gradually facilitate the transition to net negative practices. Emerging voluntary and regulatory ecosystems services markets will incentivize progress along this transition pathway and guide public and private investments toward technology development. In the difficult quest for net negative emissions, all tools, including emission reduction and soil carbon storage, must be developed to allow agriculture to maintain its critical societal function of provisioning society while, at the same time, generating environmental benefits.

54 ENVIRONMENTAL SCIENCES↗