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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Fuel Property-Informed Process Design for the Direct Catalytic Conversion of Cellulosics

The direct catalytic conversion of cellulosics (DC3) with supercritical methanol presents a promising pathway to completely solubilize woody biomass and produce >60% mass yield of C2-C6 oxygenates for light duty vehicle applications. Although the oxygenate composition can be tuned by modifying catalyst and process conditions, limited efforts to date have examined DC3 fuel properties for light duty fuel applications to iteratively inform conversion process design. In this work, we designed and evaluated multi-component surrogate bioblendstocks that represent major DC3 light oxygenates and refined catalyst formulations and distillation parameters to improve the resulting light duty fuel quality. Surrogate design for this novel fuel production pathway was based on a preliminary product slate that was systematically adjusted to determine impacts on fuel properties of interest including heating value, oxidative stability, and heat of vaporization, among others. The resulting predictions and measurements of these surrogates were then used to inform improvement of conversion process, and specifically, reformulation of the catalyst which resulted in production of a higher energy density fuel product primarily comprised of saturated alcohols. Fuel testing outcomes also informed downstream oxygenate separations requirements. This resulted in the production of a promising DC3 light-duty fuel blendstock with >15% greater energy density relative to ethanol, while maintaining high octane number and octane sensitivity.

BIOMASS FUELS↗
DOE OSTI2023

The Feasibility of Direct CO2 Conversion Technologies on Impacting Mid-Century Climate Goals

Recent IPCC modeling suggests that to limit global warming below 2 degrees C, "unprecedented" reductions in CO2 emissions will be required during the 2030-2050 time frame. The direct conversion of CO2 to fuels and chemicals using renewable electricity has garnered interest as one route to draw down emissions with the ability to synthesize products at a significantly lower carbon footprint than conventional methods. However, most direct CO2 conversion pathways are only in the early stages of development and face technical and market hurdles prior to scale-up, bringing into question what role they may play in influencing global CO2 emissions within this critical two-decade window. In this perspective, we highlight low-temperature electrolysis as a promising technology for direct CO2 conversion, including discussion on the products that could most impact global emission levels, and importantly, offer insight into the timeline, required advancements, and specific technical targets needed to successfully scale and deploy these technologies at the commercial level.

chemicals↗
DOE OSTI2025

Efficiency and Physical Limitations of Adiabatic Direct Energy Conversion in Axisymmetric Fields

We describe and analyze a new class of direct energy conversion schemes based on the adiabatic magnetic drift of charged particles in axisymmetric magnetic fields. The efficiency of conversion as well as the geometrical and dynamical limitations of the recoverable power are calculated. The geometries of these axisymmetric field configurations are suited for direct energy conversion in radiating advanced aneutronic reactors and in advanced divertors of deuterium-tritium tokamak reactors. The E × B configurations considered here do not suffer from the classical drawbacks and limitations of thermionic and magnetohydrodynamic high-temperature direct energy conversion devices.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2025

Mechanisms of direct and converse piezoelectricity in ferroelectric polymers

Within the linear regime of mechanical and electrical responses, it is commonly accepted that direct and converse piezoelectric coefficients should be the same. However, we observed a consistently higher converse d 31 (∼54 pm/V) than the direct d 31 (∼42 pC/N) for a quenched, stretched, annealed, and electrically poled poly(vinylidene fluoride-co-trifluorethylene) [P(VDF-TrFE)] 52/48 mol.% sample (abbreviated as coP-52/48QSAP). On the contrary, the direct and converse d 31 values were the same for coP-65/35QSAP and coP-55/45QSAP. Small-angle X-ray scattering results showed that coP-52/48QSAP had a higher amount of relaxor-like secondary crystals (SCs) in the oriented amorphous fraction (OAF) (SC OAF ) than coP-55/45QSAP and coP-65/35QSAP. To explain the experimental observation, we performed molecular dynamics (MD) simulation of the pure PVDF (without TrFE) to estimate direct and converse piezoelectricity for the PVDF OAF. Based on the MD simulation, the direct d 31 had a plateau value around 350 pC/N for the transverse (i.e., along the chain direction) strain up to 1 %, whereas the simulated converse d 31 could be lower (for electric field E < 0.8 MV/m), equal (for E = 0.8 MV/m), or higher (for E > 0.8 MV/m) than the direct d 31 , depending on the poling electric field. From the MD simulation, both mechano-electrostriction and electrostatic interaction were identified in the OAF as the driving force for enhanced piezoelectricity in ferroelectric PVDF. In conclusion, when ferroelectric domains were formed in the OAF by electric poling, the simulated converse d 31 became higher than the direct d 31 . Combining both experimental and MD simulation results, the higher converse d 31 than direct d 31 for coP-52/48QSAP was understood qualitatively.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Discovering Ni/Cu Single-Atom Alloy as a Highly Active and Selective Catalyst for Direct Methane Conversion to Ethylene: A First-Principles Kinetic Study

Direct methane conversion to liquid fuels or value-added chemicals is a promising technology to utilize natural resources without resorting to further petroleum extraction. However, discovering efficient catalysts for this reaction is challenging due to either coke formation or unfavorable C-H bond activation. Herein, we design single-atom alloy (SAA) catalysts to simultaneously eliminate the above two bottlenecks based on mechanism-guided strategies: (1) the active single atom enables favorable C-H bond breaking and (2) the less reactive host metal facilitates C-C coupling and thus avoids strong binding of carbonaceous species. Employing electronic structure theory calculations, we screened the stability of multiple SAAs with 3d-5d transition metals atomically dispersed on a copper surface in terms of avoiding dopant aggregation and segregation. We then evaluated reactivities of the stable SAAs as catalysts for direct methane conversion to C2 products, including methane dehydrogenation and C-C coupling mechanisms. Combining selectivity analysis with kinetic modeling, we predicted that nickel dispersed on copper, i.e., Ni/Cu SAA, is a highly active and selective catalyst that can efficiently transform methane to ethylene. This work designs efficient SAA catalysts for direct methane activation and provides chemical insights into engineering compositions of SAAs to tune their catalytic performances.

Kothakonda, Manish↗
DOE OSTI2026

Decoupling plasma, catalyst, and gaseous mechanisms for non-oxidative methane conversion

Direct non-oxidative methane (CH 4 ) conversion to value-added hydrogen (H 2 ) and C 2 products remains hindered by fundamental catalytic scaling constraints and rapid surface deactivation at elevated temperatures. Plasma-enabled catalysis offers a promising route to overcome the thermodynamic and kinetic barriers of direct non-oxidative methane upgrading at mild conditions, yet control over C–C product selectivity and catalyst stability remains elusive. Here, we establish a unified mechanistic framework including Langmuir–Hinshelwood (L–H) and Langmuir–Rideal (L–R) mechanisms that disentangles the roles of plasma excitation (including vibrationally activated species and radicals), surface temperature (T sur ), and catalyst binding energy in steering CH 4 conversion to H 2 and C 2 hydrocarbons. Through a combination of density functional theory (DFT) informed microkinetic modeling, in situ and ex situ surface characterization, and product quantification under dielectric barrier discharge conditions, we show that vibrationally excited CH 4 lowers activation barriers selectively for dissociative chemisorption, enabling surface activation across a wide range of transition metal catalysts at low thermal energy input. We find that once CH 4 is dissociatively chemisorbed, the branching between C 2 H 2 , C 2 H 4 , and C 2 H 6 is governed by surface properties (carbon binding energy, T sur , etc), regardless of plasma excitation. The DFT informed microkinetic model decouples the effects of molecular activation from surface properties and indentifies operating windows that maximize target yields while suppressing carbon accumulation and subsequent catalytic inactivation. Experiments on polycrystalline Cu/Al 2 O 3 , Ni/Al 2 O 3 , and Pt/Al 2 O 3 validate these predictions, revealing catalyst-dependent branching toward ethane or ethylene and distinct deactivation profiles. We unify these trends into a generalized three-dimensional plasma-thermal-catalytic design space, from which reduced descriptors such as T vib /T sur in the limit of vibrationally excited L–H pathways emerge as predictive metrics. These results enable rational tuning of methane conversion pathways and unlock selective C 2 formation using earth-abundant metals under mild plasma conditions.

catalyst inactivation↗
DOE OSTI2022

A Very High Temperature Lead Cooled Microreactor Concept using Advanced Materials and Thermophotovoltaics Direct Energy Conversion Technology

Recently, significant advances have been made in designing high-temperature capable nuclear fuels. In parallel, important advances have occurred in design of nanophotonic structures (coatings) with ability to shape the frequencies of light being emitted from hot surfaces. In this project, we bring these materials advances together into a design for a new direct conversion nuclear powered system with high thermodynamic efficiency, inherent safety, and unprecedented reduction in size and weight relative to current designs. The concept involves using the heat generated from nuclear fission to raise the temperature of a selective thermal emitter to >800°C. The selective emitter shifts the normal broad brand emissions of light from its hot surface into the correct near- and mid-IR bands that produce electricity with inexpensive photovoltaic cells. We have designed a new annular flow Lead Fast Reactor (LFR) that minimizes overall reactor/power conversion footprint. The results indicate that the overall microreactor/power-system design offers a 2X reduction in size over existing technology that is based on the sCO 2 reverse compression Brayton cycle. Additionally, the only moving part in our design is a circulation pump to cool the PVT panels.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2024

Microwave-Assisted Conversion of 1,6-Hexanediol into Polycarbonate

The conversion of carbon dioxide into higher value chemicals is a viable way to support sustainability and net-zero economy goals. Of the different CO2 conversion routes, direct conversion offers a simplified process, lower reaction temperatures, and thus low energy input. Alcohols can be directly combined with CO2 to produce polycarbonates, e.g., DMC (dimethyl carbonate) formation from methanol and CO2. Recently CO2 and 1,6-hexanediol were shown to convert into poly(hexamethylene carbonate)diol using an atmospheric flow based process in single step. For these conversions, CeO2-based catalysts are widely used due to the abundance of oxygen vacancies that are believed to be the active sites for this reaction. Microwave (MW) heating is a unique approach that can provide selective volume-based heating and enhanced reaction rates and/or selectivities. For the current work, CO2 and diol conversion into polymers were investigated on different CeO2 catalysts under microwave heating and the performance was compared against conventional heating. The reaction products were analyzed using infrared spectroscopy (IR) and nuclear magnetic resonance (NMR) spectroscopy. Preliminary results showed microwaves irradiation produced faster rates of polycarbonate production as evidenced by IR data.

Kanitkar, Swarom↗
DOE OSTI2023

Direct catalytic conversion of alcohols to olefins of higher carbon number with reduced ethylene production

A catalyst composition for converting an alcohol to olefins, the catalyst composition comprising the following components: (a) a support (e.g., particles) comprising silicon and oxygen; (b) at least one of copper and silver residing on and/or incorporated into said support; and (c) at least one lanthanide element residing on and/or incorporated into said support. The catalyst may also further include component (d), which is zinc. Also described herein is a method for converting an alcohol to one or more olefinic compounds (an olefin fraction) by contacting the alcohol with a catalyst at a temperature of at least 100° C. and up to 500° C. to result in direct conversion of the alcohol to an olefin fraction containing one or more olefinic compounds containing at least three carbon atoms; wherein ethylene and propylene are produced in a minor proportion of the olefin fraction, and butenes and higher olefins are produced in major proportion.

Li, Zhenglong↗
DOE OSTI2022

Catlas: an automated framework for catalyst discovery demonstrated for direct syngas conversion

Catalyst discovery is paramount to support access to energy and key chemical feedstocks in a post fossil fuel era. Exhaustive computational searches of large material design spaces using ab initio methods like density functional theory (DFT) are infeasible. We seek to explore large design spaces at relatively low computational cost by leveraging large, generalized, graph-based machine learning (ML) models, which are pretrained and therefore require no upfront data collection or training. We present Catlas, a framework that distributes and automates the generation of adsorbate-surface configurations and ML inference of DFT energies to achieve this goal. Catlas is open source, making ML assisted catalyst screenings easy and available to all. To demonstrate its efficacy, we use Catlas to explore catalyst candidates for the direct conversion of syngas to multi-carbon oxygenates. For this case study, we explore 947 stable/metastable binary, transition metal intermetallics as possible catalyst candidates. On this subset of materials, we are able to predict the adsorption energy of key descriptors, *CO and *OH, with good accuracy (0.16, 0.14 eV MAE, respectively). Using the projected selectivity towards C 2+ oxygenates from an existing microkinetic model, we identified 144 candidate materials. For 10 promising candidates, DFT calculations reveal a good correlation with our assessment using ML. Finally, among the top elemental combinations were Pt–Ti, Pd–V, Ni–Nb, and Ti–Zn, all of which appear unexplored experimentally.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Review of Direct Neutron Conversion and Detection Processes

Commercial and laboratory neutron detection systems use indirect neutron response of materials like pressurized helium-3 (via nuclear reaction 3He(n, p)3H) to measure and count neutrons emanating from a source. Recently a host of semiconductors, especially a ternary semiconductor of lithium indium diselenide (6LiInSe2) and a quaternary alloy of enriched lithium-6, indium, phosphorous, and selenium (6LiInP2Se6), have shown promising neutron counting possibilities by directly converting neutrons into charge-carrying elements within the body of the semiconductor. These semiconductors have high thermal neutron capture cross sections, suitable energy bandgaps (~2.0 electron volts) for room-temperature operations, and a favorable electronic band structure for efficient electron charge transport. The article examines the semiconductor properties of these compounds in terms of their neutron counting capabilities and possible ways to extract neutron energy information from them. Lithium-6 and boron-10 (with thermal neutron absorption cross sections of 938 ± 6 and 3855 ± 26 barns, respectively) produce charged particles to be measured via indirect neutron interactions. The efficiency of indirect conversion neutron detectors is limited because of the inefficiencies in conversion mechanism. In case of direct conversion, the neutrons create charged particles in a single material for neutron capture and charge collection, increasing detection efficiency. Unlike 3He proportional counters, which provide no neutron energy information, the semiconductors can be used as neutron energy spectrometer. Fully resolved neutron energy by 6LiInP2Se6 from a plutonium-beryllium source has been reported in the literature. We will discuss the influence of these multilayered semiconductors’ crystallographic structures and growth techniques on neutron energy determination.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2021

Isolated copper–tin atomic interfaces tuning electrocatalytic CO 2 conversion

Direct experimental observations of the interface structure can provide vital insights into heterogeneous catalysis. Examples of interface design based on single atom and surface science are, however, extremely rare. Here, we report Cu–Sn single-atom surface alloys, where isolated Sn sites with high surface densities (up to 8%) are anchored on the Cu host, for efficient electrocatalytic CO 2 reduction. The unique geometric and electronic structure of the Cu–Sn surface alloys (Cu 97 Sn 3 and Cu 99 Sn 1 ) enables distinct catalytic selectivity from pure Cu 100 and Cu 70 Sn 30 bulk alloy. The Cu 97 Sn 3 catalyst achieves a CO Faradaic efficiency of 98% at a tiny overpotential of 30 mV in an alkaline flow cell, where a high CO current density of 100 mA cm –2 is obtained at an overpotential of 340 mV. Density functional theory simulation reveals that it is not only the elemental composition that dictates the electrocatalytic reactivity of Cu–Sn alloys; the local coordination environment of atomically dispersed, isolated Cu–Sn bonding plays the most critical role.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Center for direct catalytic conversion of biomass to biofuels (Final Technical Report)

Lignocellulosic biomass has only one-third the energy density of crude oil and lacks petroleum’s versatility as a feedstock for fuels and chemicals. Since 2009, the Center for direct Catalytic Conversion of Biomass to Biofuels (C3Bio) has recognized the potential of chemical catalysis and fast-pyrolysis to overcome such limitations by transforming the main components of biomass (cellulose, xylan, and lignin) from grasses and trees directly to liquid hydrocarbons and aromatic co-products. In 2014, C3Bio proposed to develop critical systems-level understanding of how biomass structural complexity at molecular, nanoscale, and mesoscale levels impacts the yields and selectivities of desired products from catalytic and pyrolytic transformations. Our long-term goal was to gain unprecedented control of effective routing of carbon: we aimed to specify both the structures within, and the reaction products from, lignocellulosic biomass. Enabled by the EFRC high-risk, high-reward approach to grand challenge science, our interdisciplinary team of plant biologists, chemists, and chemical engineers disrupted the conventional paradigm of the cellulosic biorefinery into a new future of “no carbon left behind” - the full utilization of carbon from plant cell walls in energy-dense fuels.

09 BIOMASS FUELS↗
DOE OSTI2021

DOE Energy Frontier Research Centers Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio)

New capabilities to predict, design and control the chemistries of carbon could answer a global imperative to transition from fossil-based to sustainable transportation fuels. While the use of inexpensive hydrocarbons has been an unparalleled achievement and enabler of economic prosperity for many nations, singular dependence upon crude oil has given rise to systemic vulnerabilities in climate, energy, economic, and national security. Lignocellulosic biomass, a renewable and carbon-neutral resource, has the potential to displace an estimated annual equivalent of three billion barrels of oil in the U.S. alone (National Research Council 2009, U. S. Department of Energy, 2011). However, biomass has only one-third the energy density of crude oil (Agrawal and Singh 2009, Richard 2010) and lacks petroleum’s versatility as a feedstock for fuels and chemicals. These limitations keep biomass conversion below the efficiency level needed for strategic impact while the scientific challenge of routing carbon from one molecular context to another remains unmet. In 2009, the Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio) recognized the potential of chemical catalysis and fast pyrolysis to overcome such limitations by transforming the main components of biomass (cellulose, xylan, and lignin) from grasses and trees directly to liquid hydrocarbons and aromatic co-products. Enabled by the EFRC high-risk, high-reward approach to grand challenge science, C3Bio researchers have been key national players in disrupting the conventional paradigm of the cellulosic biorefinery into a new future of “no carbon left behind”—the full utilization of carbon from plant cell walls in energy-dense fuels (Fig. 1). We identified catalytic and fast-pyrolytic pathways that utilize cellulose, xylan and, most significantly, lignin. We developed catalytic processes that deoxygenate and transform monomers and isolated polymers into useful products and tested their use with intact biomass. We gained control of lignin synthesis within plants and initiated tailoring biomass to its end-use through the tools of plant molecular biology and genetic engineering. C3Bio breakthroughs have increased the energy density of biomass-derived substrates via catalytic and pyrolytic conversions into products such as benzoquinones, furfural and hydroxymethylfurfural, levoglucosan and levulinic acid, methoxypropylphenols and propylbenzene. Such advances in biomass conversion would not have been possible without simultaneous advances in analytical instrumentation and methodologies, and imaging technologies and applications. The legacy science developed by C3Bio enables design and control strategies for achieving a targeted product portfolio of fuel and chemical feedstocks from a diverse range of native and tailored biomass. Our research provides the knowledge base required for a bio-economy with product streams as diverse in functionality as those of the petrochemical industry. Coupling targeted computational modeling with experimentation, we achieved: (1) fundamental understanding of biopolymers and cell wall architecture assembly, (2) discovery of new chemistries that allow the development of highly selective pathways to fuels and desirable chemicals, and (3) an integrated systems-level understanding to control catalytic and pyrolytic pathways.

09 BIOMASS FUELS↗
DOE OSTI2025

Engineering PdAu/CeO 2 Alloy/Oxide Interfaces for Selective Methane‐to‐Methanol Conversion with Water

The direct conversion of methane-to-methanol remains a critical challenge in methane valorization. In this study, we unveil the crucial role of PdAu/CeO 2 catalysts in enabling selective methane transformation under mild conditions, using only water as the sole oxidant. Through a combination of experimental techniques, including XPS and catalytic testing, alongside density functional theory (DFT) calculations, we demonstrate that a Pd 0.3 Au 0.7 /CeO 2 catalyst, which predominantly exposes isolated Pd atoms, achieves remarkable methanol selectivity (∼80%) at 500 K with a 1:1 methane-to-water ratio. While Pd/CeO 2 efficiently activates methane, its tendency for overreaction leads to complete methanol decomposition, thereby limiting selectivity. Alloying Pd with Au on ceria mitigates this over-reactivity, preventing methanol degradation while maintaining sufficient catalytic activity. The PdAu/CeO 2 composite exhibits a synergistic effect: Pd in contact with the ceria support facilitates methane activation and water dissociation, while Au fine-tunes reactivity to promote methanol formation. DFT calculations confirm that isolated Pd sites at the PdAu/CeO 2 interface play a key role in balancing activity and selectivity. This work underscores the importance of alloy/oxide interfaces in controlling selective methane conversion with water and offers valuable insights for designing highly efficient catalysts for methanol synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Direct Catalytic Conversion of Ethanol to C 5+ Ketones: Role of Pd–Zn Alloy on Catalytic Activity and Stability

Abstract Ethanol can be used as a platform molecule for synthesizing valuable chemicals and fuel precursors. Direct synthesis of C 5+ ketones, building blocks for lubricants and hydrocarbon fuels, from ethanol was achieved over a stable Pd‐promoted ZnO‐ZrO 2 catalyst. The sequence of reaction steps involved in the C 5+ ketone formation from ethanol was determined. The key reaction steps were found to be the in situ generation of the acetone intermediate and the cross‐aldol condensation between the reaction intermediates acetaldehyde and acetone. The formation of a Pd–Zn alloy in situ was identified to be the critical factor in maintaining high yield to the C 5+ ketones and the stability of the catalyst. A yield of >70 % to C 5+ ketones was achieved over a 0.1 % Pd‐ZnO‐ZrO 2 mixed oxide catalyst, and the catalyst was demonstrated to be stable beyond 2000 hours on stream without any catalyst deactivation.

Subramaniam, Senthil↗
DOE OSTI2020

Performance Criteria for Capture and/or Immobilization Technologies (Revision 1)

The capture and subsequent immobilization of regulated volatile radionuclides from the off-gas streams of a used nuclear fuel (UNF) reprocessing facility has been a topic of substantial research interest for the US Department of Energy and its international counterparts. Removal of specific radionuclides from the plant effluent streams before discharge to the environment is required to meet regulations set forth by the US Environmental Protection Agency. Upon removal, the radionuclides, as well as associated sorbents that cannot be regenerated in a cost-effective manner, are destined for conversion to a waste form. Research in separation and capture methodologies has included a wide range of technology types, and studies of waste forms are correspondingly diverse. In considering the future development and implementation of both sorbents and waste forms, it is necessary to identify benchmark measures of performance to objectively evaluate each sorbent system or waste form. Sets of performance criteria and associated metrics have been developed for sorbent and waste form evaluation. These criteria address physical, radiological, and chemical characteristics, technical practicality, technical maturity, cost, and, for sorbents, system performance. The criteria and metrics appear to be robust and should be applicable despite the eventual waste classification (as either high- or low-level waste). They are flexible enough to address both aqueous reprocessing and electrochemical reprocessing of UNF. These criteria sets can serve as tools to evaluate performance at multiple stages within the development process, and in this revision (Revision 1) they have been used to assess technologies relating to krypton/xenon separations and iodine capture from off-gas streams arising from UNF reprocessing. Assessment of krypton/xenon separations using engineered forms of two zeolite minerals (silver mordenite and hydrogen mordenite in a polyacrylonitrile-based binder [AgZ-PAN/HZ-PAN]) found that the zeolite-based separation is relatively advanced in its development, but several key issues require resolution. First, desorption processes for both krypton and xenon require refinement to provide an understanding of the product purity that can be achieved. Second, adsorption rate data is needed in order to calculate the bed depth required for effective separation. Finally, it is strongly recommended that a technical review of krypton/xenon separation by AgZ-PAN/HZ-PAN be performed to synergize available data and assess the cost savings and operational benefits that may be realized from implementation of this technology. Assessment of metal organic frameworks (MOFs) for their use in the separation of krypton/xenon found that the ideal separation would be performed using a single-column system with a MOF selective for krypton over xenon. A robust research effort should work to identify a krypton-selective MOF designed to operate at temperatures of approximately 0°C or higher, which could be preferred over cryogenic krypton/xenon capture for used fuel reprocessing off-gas streams. In the case of the CaSDB-MOF (the most well-understood xenon sorbent to date), two issues are judged of high importance. First, xenon breakthrough capacity for the CaSDB-MOF in prototypical conditions should be determined. Preliminary research indicates that breakthrough may be near immediate, presenting a substantial obstacle in separative system design. Second, development of desorption methodology should be performed to determine regeneration time, energy requirements, and the product stream composition. Silver-based sorbents (AgZ and AgAero) for use in iodine capture from the dissolver off-gas were evaluated against the established criteria. These sorbents are significantly better understood for this application as a result of research efforts over the past decade. The potential implementation of AgAero at a large scale is hindered by its physical degradation by components of the dissolver off-gas stream. Less is known about the adsorption of iodine by these sorbents from other off-gas streams in the plant. Initial experimental efforts have been closely coordinated in an effort to understand organic iodine (such as would be found in the vessel off-gas) adsorption by AgZ and AgAero. Future work should expand this experimental program, and analysis of other reprocessing facility off-gas streams such as the vitrification off-gas stream should be conducted to better understand other potential applications for iodine sorbents. A review of iodine waste form development shows that this area is diverse and that multiple promising waste forms have been identified for the immobilization of radioactive iodine. Efforts related to the direct conversion of iodine sorbents (including AgZ and AgAero) should be continued because of the advantages of direct conversion in a waste management strategy and other sorbents should continue to be advanced as merited.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

U-gas +Cool GTL™ - A New Integrated Process for Direct Biomass Conversion to Liquid Fuels

The U-Gas gasification technology, marketed by Sungas, is a proven fluid bed gasification technology for biomass conversion. U-Gas has been tested on a wide variety of biomass feeds including wood and waste streams. The U-Gas Technology has successfully converted wood for more than 20 years in a gasification plant in Skive Denmark at the 150t/d size. GTI has also recently developed the Cool GTL process for converting biogas to high quality gasoline, jet, and diesel fuels. The technoeconomics and LCA for the combination of the two technologies results an integrated optimized process, which will be discussed. The Cool GTL process is still in development and the development should be complete by 2023. Cool GTL converts high CO2 content feeds to synthesis gas with a 2-2.4/1 H2/CO ratio suitable for fuels synthesis. The process is based on a novel, highly stabile CO2/steam reforming catalyst. The 2.0-2.4/1 H2/CO synthesis gas ratio is always achieved, independently of feed CO2 content, by adjusting the amount of water added according to the amount of CO2 in the feed. The reformer catalyst has been tested for 500 hours and shows no measurable deactivation. The product from the reformer then goes directly to a low temperature slurry bed Fischer Tropsch reactor with an integrated finishing hydroisomerization reactor which makes hydrocarbon liquids from the synthesis gas. With this configuration no wax is produced. The technoeconomics and carbon intensity for the integration of UGas and the Cool GTL processes will be compared to other biomass conversion approaches. The use of electrolysis to boost H2 in the feed and increase liquid production will also be analyzed as a potential process improvement with sensitivities to the cost of electricity and the use of renewable electricity.

09 BIOMASS FUELS↗