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NASA NTRS1989

Non-noble electrocatalysts for alkaline fuel cells

Carbons activated with macrocyclics have attracted increasing attention as alternative electrocatalysts for oxygen reduction. Initial activity of these catalysts is good, but performance declines rapidly. Pyrolyzing the macrocyclic on the carbon support leads to enhanced stability and the catalysts retain good activity. The approach described is designed to develop bulk doped catalysts with similar structures to pyrolyzed macrocyclic catalysts. The transition metal and coordinated ligands are dispersed throughout the bulk of the conductive carbon skeleton. Two approaches to realizing this concept are being pursued, both involving the doping of carbon precursors. In one approach, the precursor is a solid phase carbon-containing ion-exchange resin. The precursor is doped with a transition metal and/or nitrogen, and the resulting mixture is pyrolyzed. In the other approach, the precursor is a gas-phase hydrocarbon. This is introduced with a transition metal species and nitrogen species into a reactor and pyrolyzed. Several studies have been conducted to determine if there is a synergistic effect between the transition metal and nitrogen and the effect of different methods of introducing the metal-nitrogen (M-N) coordination on performance. One approach was to introduce the metal and nitrogen separately, for example, by sequentially doping FeCl3 and NH4OH into the resin. Catalysts were prepared from an undoped ion-exchange resin, a resin doped only with N, a resin doped only with Fe, and a resin doped with both Fe and N. Introduction of nitrogen alone has no beneficial effect on the performance of the catalysts. The introduction of the Fe alone significantly improves the performance in both the high and low current density regions. When both Fe and N are introduced, the performance at lower current densities (catalytic activity) is increased beyond that of the Fe-doped carbon, but the performance at higher current densities is similar to the carbon containing only Fe. Catalysts prepared from resins-Fe(bipy)3SO4 precursors have performance that is only slightly less then CoTMPP adsorbed and pyroloyzed on Vulcan XC-72. Their performance is much better than carbons which have had the N and Fe introduced separately.

Sarangapani, S.↗

DOE OSTI2022

Efficient Electrochemical Reduction of CO 2 to Formate in Methanol Solutions by Mn‐Functionalized Electrodes in the Presence of Amines**

Carbon cloth electrode modified by covalently attaching a manganese organometallic catalyst is used as cathode for the electrochemical reduction of CO 2 in methanol solutions. Six different industrial amines are employed as co-catalyst in millimolar concentrations to deliver a series of new reactive system. While such absorbents were so far believed to provide a CO 2 reservoir and act as sacrificial proton source, we herein demonstrate that this role can be played by methanol, and that the adduct formed between CO 2 and the amine can act as an effector or inhibitor toward the catalyst, thereby enhancing or reducing the production of formate. Pentamethyldiethylentriamine (PMDETA), identified as the best effector in our series, converts CO 2 in wet methanolic solution into bisammonium bicarbonate. Computational studies revealed that this adduct is responsible for a barrierless transformation of CO 2 to formate by the reduced form of the Mn catalyst covalently bonded to the electrode surface. As a consequence, selectivity can be switched on demand from CO to formate anion, and in the case of (PMDETA) an impressive TON HCOO- of 2.8×10 4 can be reached. This new valuable knowledge on an integrated capture and utilization system paves the way toward more efficient transformation of CO 2 into liquid fuel.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2023

A Multi-Satellite Framework to Rapidly Evaluate Extreme Biosphere Cascades: The Western US 2021 Drought and Heatwave

The increasing frequency and intensity of climate extremes and complex ecosystem responses motivate the need for integrated observational studies at low-latency to determine biosphere responses and carbon-climate feedbacks. Here, we develop a satellite-based rapid attribution workflow and demonstrate its use at a 1–2-month latency to attribute drivers of the carbon cycle feedbacks during the 2020-2021 Western US drought and heatwave. In the first half of 2021, concurrent negative photosynthesis anomalies and large positive column CO 2 anomalies were detected with satellites. Using a simple atmospheric mass balance approach, we estimate a surface carbon efflux anomaly of 132 TgC in June 2021, a magnitude corroborated 28 independently with a dynamic global vegetation model. Integrated satellite observations of hydrologic processes, representing the soil-plant-atmosphere continuum (SPAC), show that these surface carbon flux anomalies are largely due to substantial reductions in photosynthesis because of a spatially widespread moisture-deficit propagation through the SPAC between 2020 and 2021. A causal model indicates deep soil moisture stores partially drove photosynthesis, maintaining its values in 2020 and driving its declines throughout 2021. The causal model also suggests legacy effects may have amplified photosynthesis deficits in 2021 beyond the direct effects of environmental forcing. The integrated, observation framework presented here provides a valuable first assessment of a biosphere extreme response and an independent testbed for improving drought propagation and mechanisms in models. The rapid identification of extreme carbon anomalies and hotspots can also aid mitigation and adaptation decisions.

Causal model↗

DOE OSTI2020

Unexpected mechanism for glucose-primed soil organic carbon mineralization under an anaerobic–aerobic transition

Redox reactions are important for cycling of carbon (C) in soils frequently subject to fluctuations in redox conditions, such as wetland soils, which contribute around one third of the global terrestrial C reservoir. Priming effects (PE), induction of changes in C mineralization due to additions of energy-rich organic carbon (OC) substrates, have been largely ignored during redox transitions in current modelling and experimental efforts for evaluating C cycles. In this study, we investigated the effects of glucose input on the mineralization of soil OC during an anaerobic-aerobic transition. Substantially more soil OC was mineralized under aerobic conditions in samples that received glucose under preceding anaerobic conditions compared to controls that did not receive glucose and to samples that received glucose under aerobic-only conditions. Our results reveal a novel PE by which glucose indirectly primes the mineralization of soil OC by increasing the reductive release of iron oxide-associated OC under anaerobic conditions, followed by a dramatic positive PE when aerobic conditions are reestablished. Inclusion of this novel indirect priming mechanism is crucial for accurately predicting the contribution of atmospheric greenhouse gases from soils experiencing redox fluctuations (e.g.,wetlands).

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2006

Adaptive Engine Technologies for Aviation CO2 Emissions Reduction

Adaptive turbine engine technologies are assessed for their potential to reduce carbon dioxide emissions from commercial air transports.Technologies including inlet, fan, and compressor flow control, compressor stall control, blade clearance control, combustion control, active bearings and enabling technologies such as active materials and wireless sensors are discussed. The method of systems assessment is described, including strengths and weaknesses of the approach. Performance benefit estimates are presented for each technology, with a summary of potential emissions reduction possible from the development of new, adaptively controlled engine components.

Mercer, Carolyn R.↗

DOE OSTI2020

Microbial sulfate reduction and organic sulfur formation in sinking marine particles

Climate change is driving an expansion of marine oxygen-deficient zones, which may alter the global cycles of carbon, sulfur, nitrogen, and trace metals. Currently, however, we lack a full mechanistic understanding of how oxygen deficiency affects organic carbon cycling and burial. In this work, we show that cryptic microbial sulfate reduction occurs in sinking particles from the eastern tropical North Pacific oxygen-deficient zone and that some microbially produced sulfide reacts rapidly to form organic sulfur that is resistant to acid hydrolysis. Particle-hosted sulfurization could enhance carbon preservation in sediments underlying oxygen-deficient water columns and serve as a stabilizing feedback between expanding anoxic zones and atmospheric carbon dioxide. A similar mechanism may help explain more-extreme instances of organic carbon preservation associated with marine anoxia in Earth history.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

Phase transformation and electrochemical charge storage properties of vanadium oxide/carbon composite electrodes synthesized via integration with dopamine

Abstract Chemically preintercalated dopamine (DOPA) molecules were used as both a reducing agent and a carbon precursor to prepare δ‐V 2 O 5 · n H 2 O/C, H 2 V 3 O 8 /C, VO 2 (B)/C, and V 2 O 3 /C nanocomposites via hydrothermal treatment or hydrothermal treatment followed by annealing under Ar flow. We found that the phase composition and morphology of the produced composites are influenced by the DOPA:V 2 O 5 ratio used to synthesize (DOPA) x V 2 O 5 precursors through DOPA diffusion into the interlayer region of the δ‐V 2 O 5 · n H 2 O framework. The increase of DOPA concentration in the reaction mixture led to a more pronounced reduction of vanadium and a higher fraction of carbon in the composites’ structure, as evidenced by X‐ray photoelectron spectroscopy and Raman spectroscopy measurements. The electrochemical charge storage properties of the synthesized nanocomposites were evaluated in Li‐ion cells with nonaqueous electrolytes. δ‐V 2 O 5 · n H 2 O/C, H 2 V 3 O 8 /C, VO 2 (B)/C, and V 2 O 3 /C electrodes delivered high initial capacities of 214, 252, 279, and 637 mAh g –1 , respectively. The insights provided by this investigation open up the possibility of creating new nanocomposite oxide/carbon electrodes for a variety of applications, such as energy storage, sensing, and electrochromic devices.

Materials Science↗

DOE OSTI2020

Controlled Reduction of Graphene Oxide Using Sulfuric Acid

Sulfuric acid under different concentrations and with the addition of SO 3 (fuming sulfuric acid) was studied as a reducing agent for the production of reduced graphene oxide (RGO). Three concentrations of sulfuric acid (1.5, 5, and 12 M), as well as 12 M with 30% SO 3 , were used. The reduction of graphene oxide increased with H 2 SO 4 concentration as observed by Fourier-transformed infrared spectroscopy and X-ray photoelectron spectroscopy. It was observed that GO lost primarily epoxide functional groups from 40.4 to 9.7% and obtaining 69.8% carbon when using 12 M H 2 SO 4 , without leaving sulfur doping. Additionally, the appearance of hexagonal domain structures observed in transmission electron microscopy and analyzed by selected area electron diffraction patterns confirmed the improvement in graphitization. Although the addition of SO 3 in H 2 SO 4 improved the GO reduction with 74% carbon, as measured by XPS, the use of SO 3 introduced sulfur doping of 1.3%. RGO produced with sulfuric acid was compared with a sample obtained via ultraviolet (UV) irradiation, a very common reduction route, by observing that the RGO produced with sulfuric acid had a higher C/O ratio than the material reduced by UV irradiation. This work showed that sulfuric acid can be used as a single-step reducing agent for RGO without sulfur contamination.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Environmental life-cycle analysis of hydrogen technology pathways in the United States

Hydrogen is a zero-carbon energy carrier with potential to decarbonize industrial and transportation sectors, but its life-cycle greenhouse gas (GHG) emissions depend on its energy supply chain and carbon management measures (e.g., carbon capture and storage). Global support for clean hydrogen production and use has recently intensified. In the United States, Congress passed several laws that incentivize the production and use of renewable and low-carbon hydrogen, such as the Bipartisan Infrastructure Law (BIL) in 2021 and the Inflation Reduction Act (IRA) in 2022, which provides tax credits of up to $3/kg depending on the carbon intensity of the produced hydrogen. A comprehensive life-cycle accounting of GHG emissions associated with hydrogen production is needed to determine the carbon intensity of hydrogen throughout its value chain. In the United States, Argonne’s R&D GREET ® (Greenhouse Gases, Regulated emissions, and Energy use in Technologies) model has been widely used for hydrogen carbon intensity calculations. This paper describes the major hydrogen technology pathways considered in the United States and provides data sources and carbon intensity results for each of the hydrogen production and delivery pathways using consistent system boundaries and most recent technology performance and supply chain data.

Elgowainy, Amgad↗

DOE OSTI2020

Empirical Evidence for the Potential Climate Benefits of Decarbonizing Light Vehicle Transport in the U.S. with Bioenergy from Purpose-Grown Biomass with and without BECCS

Climate mitigation scenarios limiting global temperature increases to 1.5 °C rely on decarbonizing vehicle transport with bioenergy production plus carbon capture and storage (BECCS), but climate impacts for producing different bioenergy feedstocks have not been directly compared experimentally or for ethanol vs electric light-duty vehicles. A field experiment at two Midwest U.S. sites on contrasting soils revealed that feedstock yields of seven potential bioenergy cropping systems varied substantially within sites but little between. Bioenergy produced per hectare reflected yields: miscanthus > poplar > switchgrass > native grasses ≈ maize stover (residue) > restored prairie ≈ early successional. Greenhouse gas emission intensities for ethanol vehicles ranged from 20 to -179 g CO 2 e MJ –1 : maize stover $\gg$ miscanthus ≈ switchgrass ≈ native grasses ≈ poplar > early successional ≥ restored prairie; direct climate benefits ranged from ~80% (stover) to 290% (restored prairie) reductions in CO 2 e compared to petroleum and were similar for electric vehicles. With carbon capture and storage (CCS), reductions in emission intensities ranged from 204% (stover) to 416% (restored prairie) for ethanol vehicles and from 329 to 558% for electric vehicles, declining 27 and 15%, respectively, once soil carbon equilibrates within several decades of establishment. Extrapolation based on expected U.S. transportation energy use suggests that, once CCS potential is maximized with CO 2 pipeline infrastructure, negative emissions from bioenergy with CCS for light-duty electric vehicles could capture >900 Tg CO 2 e year –1 in the U.S. In the future, as other renewable electricity sources become more important, electricity production from biomass would offset less fossil fuel electricity, and the advantage of electric over ethanol vehicles would decrease proportionately.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Novel candidate taxa contribute to key metabolic processes in Fennoscandian Shield deep groundwaters

The continental deep biosphere contains a vast reservoir of microorganisms, although a large proportion of its diversity remains both uncultured and undescribed. In this study, the metabolic potential (metagenomes) and activity (metatranscriptomes) of the microbial communities in Fennoscandian Shield deep subsurface groundwaters were characterized with a focus on novel taxa. DNA sequencing generated 1270 de-replicated metagenome-assembled genomes and single-amplified genomes, containing 7 novel classes, 34 orders, and 72 families. The majority of novel taxa were affiliated with Patescibacteria, whereas among novel archaea taxa, Thermoproteota and Nanoarchaeota representatives dominated. Metatranscriptomes revealed that 30 of the 112 novel taxa at the class, order, and family levels were active in at least one investigated groundwater sample, implying that novel taxa represent a partially active but hitherto uncharacterized deep biosphere component. The novel taxa genomes coded for carbon fixation predominantly via the Wood–Ljungdahl pathway, nitrogen fixation, sulfur plus hydrogen oxidation, and fermentative pathways, including acetogenesis. These metabolic processes contributed significantly to the total community’s capacity, with up to 9.9% of fermentation, 6.4% of the Wood–Ljungdahl pathway, 6.8% of sulfur plus 8.6% of hydrogen oxidation, and energy conservation via nitrate (4.4%) and sulfate (6.0%) reduction. Key novel taxa included the UBA9089 phylum, with representatives having a prominent role in carbon fixation, nitrate and sulfate reduction, and organic and inorganic electron donor oxidation. These data provided insights into deep biosphere microbial diversity and their contribution to nutrient and energy cycling in this ecosystem.

Candidatus↗

DOE OSTI2020

Low cost textile-grade carbon-fiber epoxy composites for automotive and wind energy applications

Carbon fiber reinforced polymer composites are highly desirable for automotive and wind energy applications due to advantages associated with weight reduction, high stiffness and strength, durability, and recyclability. The high cost of carbon fiber has been a limiting factor in its widespread adoption in non-aerospace applications. A low cost (estimated < $11 per kg) wide tow (450-600k) carbon fiber derived from textile grade polyacrylonitirile precursor, and hence called Textile Grade Carbon Fiber (TCF) is introduced in this paper. Fundamental aspects of the TCF are discussed along with a detailed characterization of its mechanical properties. Two manufacturing processes relevant to automotive and wind energy applications are considered, namely-compression molding and resin infusion. Furthermore, at various stages the TCF has been compared to commercial non-aerospace 50k carbon fiber composite. Detailed physical and mechanical properties including tensile, flexural, compression, and interlaminar shear properties are reported and compared to non-aerospace carbon fiber composite. The results provide a means for designers and end-users in the automotive and wind energy sector to consider different forms of economical non-aerospace carbon fibers.

42 ENGINEERING↗

NASA NTRS2010

Microscopic Scale Simulation of the Ablation of Fibrous Materials

Ablation by oxidation of carbon-fiber preforms impregnated in carbonized phenolic matrix is modeled at microscopic scale. Direct numerical simulations show that the carbonized phenolic matrix ablates in volume leaving the carbon fibers exposed. This is due to the fact that the reactivity of carbonized phenolic is higher than the reactivity of carbon fibers. After the matrix is depleted, the fibers ablate showing progressive reduction of their diameter. The overall material recession occurs when the fibers are consumed. Two materials with the same carbon-fiber preform, density and chemical composition, but with different matrix distributions are studied. These studies show that at moderate temperatures (< 1000 K) the microstructure of the material influences its recession rate; a fact that is not captured by current models that are based on chemical composition only. Surprisingly, the response of these impregnated-fiber materials is weakly dependent on the microstructure at very high temperatures (e.g., Stardust peak heating conditions: 3360K).

Lachaud, Jean Romain↗

NASA NTRS2010

Microscopic Scale Simulation of the Ablation of Fibrous Materials

This slide presentation reviews the ablation by oxidation of carbon-fiber preforms impregnated in carbonized phenolic-formaldehyde matrix is modeled at microscopic scale. Direct numerical simulations show that the matrix ablates in volume leaving the carbon fibers exposed. This is due to the fact that the reactivity of carbonized phenolics is higher than the reactivity of carbon fibers. After the matrix is depleted, the fibers ablate showing progressive reduction of their diameter. The overall material recession occurs when the fibers are consumed. Two materials with the same carbon-fiber preform, density and chemical composition, but with different matrix distributions are studied. These studies show that at moderate temperatures (< 1000K) the microstructure of the material influences its recession rate; a fact that is not captured by current models that are based on chemical composition only. Surprisingly, the response of these impregnated-fiber materials is weakly dependent on the microstructure at very high temperatures (e.g., Stardust peak heating conditions: 3360K).

Lachaud, Jean↗

NASA NTRS1989

Stable carbon and sulfur isotopes as records of the early biosphere

The abundance ratios of the stable isotopes of light elements such as carbon and sulfur can differ between various naturally-occurring chemical compounds. If coexisting compounds have achieved mutual chemical and isotopic equilibrium, then the relative isotopic composition can record the conditions at which equilibrium was last maintained. If coexisting chemical compounds indeed formed simultaneously but had not achieved mutual equilibrium, then their relative isotopic compositions often reflect the conditions and mechanisms associated with the kinetically controlled reactions responsible for their production. In the context of Mars, the stable isotopic compositions of various minerals might record not only the earlier environmental conditions of the planet, but also whether or not the chemistry of life ever occurred there. Two major geochemical reservoirs occur in Earth's crust, both for carbon and sulfur. In rocks formed in low temperature sedimentary environments, the oxidized forms of these elements tend to be enriched in the isotope having the larger mass, relative to the reduced forms. In sediments where the organics and sulfides were formed by biological processes, these isotopic contrasts were caused by the processes of biological CO2 fixation and dissimilatory sulfate reduction. Such isotopic contrasts between oxidized and reduced forms of carbon and sulfur are permitted by thermodynamics at ambient temperatures. However, nonbiological chemical reactions associated with the production of organic matter and the reduction of organics and sulfides are extremely slow at ambient temperatures. Thus the synthesis of organics and sulfides under ambient conditions illustrates life's profound role as a chemical catalyst that has altered the chemistry of Earth's crust. Because the stable isotopes of carbon and sulfur can reflect their chemistry, they are useful probes of the Martian surface.

Desmarais, David J.↗

NASA NTRS2009

Late Reduction Textures in Almahata Sitta Ureilite

The Almahata Sitta ureilite, derived from asteroid 2008 TC3, consists of many individual fragments recovered from the Nubian dessert strewn field [1]. Like most ureilites, it contains abundant carbon and exhibits examples of disequilibrium textures that record a late reduction event accompanied by rapid cooling (tens of degC/h) from high temperatures (1150-1300 C). Variations in Fe/Mg of silicate minerals are accompanied by variations in Fe/Mn, indicating loss of Fe into metal [2]. In coarser-grained fragments of Almahata Sitta, olivine exhibits irregular high mg# rims in contact with networks of interstitial metal 5- 20 microns in typical thickness. This is a common ureilite texture thought to be driven by the reaction of graphite to a CO gas phase and the concurrent reduction of FeO in olivine to Fe metal, with excess silica going primarily into pyroxene (2MgFeSiO4 + C approaches MgSiO4 + MgSiO3 + 2Fe + CO) [3, see also 4,5,6]. Other fragments of Almahata Sitta exhibit anomalous textures such as fine grain size, high porosity, and abundant graphite. Within these fragments pyroxene locally exhibits high-mg# rims in contact with metal and a discreet silica phase, suggesting that the reduction mechanism MgFeSi2O6 + C approaches MgSiO3 + Fe + SiO2 + CO. Metals in Almahata Sitta are particularly unaltered in comparison to ureilite finds. Variations in minor and trace element composition of this metal might partly result from localized dilution as iron is supplied by reduction of silicates.

Herrin, J. S.↗

DOE OSTI2024

Carbon Footprint Analysis of Floating PV Systems

This report, conducted by the Dutch research organization TNO, presents the first detailed life cycle inventory (LCI) analysis of operational floating photovoltaic (FPV) systems. The study, focusing on two operational systems in Western Europe, reveals that FPV systems on small inland water bodies can be a valuable complement to ground-mounted PV systems in terms of greenhouse gas emissions reduction. If PV module degradation is limited, these systems' carbon footprint is 3-4 times lower than the EU grid mix target for 2030. The report compares two FPV systems with different floater compositions (HDPE and steel/HDPE) to hypothetical ground-mounted systems, using comprehensive background data. The findings highlight the necessity for long-term monitoring and thorough environmental assessments. Josco Kester, a scientist at TNO, underscores the potential environmental benefits of these systems, which could enhance the adoption of renewable energy technologies.

14 SOLAR ENERGY↗

DOE OSTI2023

Low-carbon fuels for spark-ignited engines: A comparative study of compressed natural gas and liquefied petroleum gas on a CFR engine with exhaust gas recirculation

Decades of work on low-carbon fuels have established their potential for substantial emissions reductions; however, their adoption is still limited by infrastructure concerns and engine efficiency deficits. As infrastructures have begun to evolve, research on strategies that maximize engine efficiency through interactions with fuel properties must also now take center place. This paper compares the performance, emissions, and combustion characteristics of two forefront low-carbon fuels: compressed natural gas (CNG) and liquefied petroleum gas (LPG) in a cooperative fuel research (CFR) engine over a range of compression ratios and engine loads. The effects of exhaust gas recirculation (EGR), end-gas auto-ignition, and a novel combustion control tool, the combustion intensity metric (CIM), were also evaluated at different stoichiometric engine operating conditions. In comparison to LPG, CNG operation demonstrated an extended knock-free regime, allowing engine operation at higher engine loads and compression ratios, but LPG operation exhibited enhanced combustion characteristics with higher peak pressures and faster apparent heat release rates (AHRR). LPG operation achieved higher brake thermal efficiencies and lower equivalent CO 2 emissions compared to CNG operation at the tested engine loads and compression ratios. LPG demonstrated significantly higher EGR tolerance limits compared to CNG, with a maximum of 28% EGR rate, compared to 23% for CNG. This improved EGR dilution tolerance was responsible for a 90% reduction in NOx emissions for LPG compared to a maximum of 70% with CNG. EGR dilution also exhibited more effective knock mitigation potential with LPG, suppressing knock intensity values by up to 98% and transitioning the engine operation towards normal combustion from heavy knocking conditions. As a result, the CIM was found to decrease burn durations and improve the quality of combustion by controlling the desired fraction of end-gas auto-ignition.

33 ADVANCED PROPULSION SYSTEMS↗