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DOE OSTI2022

In-situ thermal analysis of intermetallic and thermite projectiles in high velocity impact experiments

Particle fragmentation influences thermochemical energy conversion processes in different ways and is of significance in energy generation technologies. Different reactive material formulations trigger varied thermal response in extreme environments such as high velocity impact. Here we investigated optical thermal response of powder gun launched intermetallic (Al:Zr) and thermite (Al:MoO 3 ) projectiles using pyrometry and thermography. Projectiles were launched at 1250 m/s into an air-filled chamber and impacted a steel witness plate to create a dust explosion. The pyrometer was configured to measure temperatures directly at the point of impact, while the thermographic system measured temperatures throughout the explosion chamber. Results show that impact temperatures ranged between 3500 and 4000 K, but that the dynamics of energy conversion were different for the intermetallic and thermite projectiles. The intermetallic exhibited secondary reactions due to fragmented debris impacting the walls of the chamber. The thermite exhibited greater gas generation, propelling the debris field, and producing a more stochastic response with faster spreading and dissipation of thermal energy. Unique features such as microexplosions within fragmented particles were also analyzed. While both reactive materials produce similar temperatures, their mechanisms of energy conversion and release are different, indicating the potential of these materials for different ballistic applications.

42 ENGINEERING↗

DOE OSTI2022

The 2022 Plasma Roadmap: low temperature plasma science and technology

Abstract The 2022 Roadmap is the next update in the series of Plasma Roadmaps published by Journal of Physics D with the intent to identify important outstanding challenges in the field of low-temperature plasma (LTP) physics and technology. The format of the Roadmap is the same as the previous Roadmaps representing the visions of 41 leading experts representing 21 countries and five continents in the various sub-fields of LTP science and technology. In recognition of the evolution in the field, several new topics have been introduced or given more prominence. These new topics and emphasis highlight increased interests in plasma-enabled additive manufacturing, soft materials, electrification of chemical conversions, plasma propulsion, extreme plasma regimes, plasmas in hypersonics, data-driven plasma science and technology and the contribution of LTP to combat COVID-19. In the last few decades, LTP science and technology has made a tremendously positive impact on our society. It is our hope that this roadmap will help continue this excellent track record over the next 5–10 years.

plasma diagnostics↗

DOE OSTI2020

Performance and long-term stability of CO 2 conversion to formic acid using a three-compartment electrolyzer design

The electrochemical reduction of CO 2 to formate and formic acid has attracted a great amount of academic and commercial interest over the past five years. A number of experimental studies have generated data on the Faradaic performance and stability of various candidate catalyst materials in producing formate or formic acid. However, most of the data has been conducted at low current densities and over short time periods, typically hours to days. There is a critical need in providing long-term catalyst stability as well as electrolyzer-based operating data, which are needed for the commercial scale-up and operation of this technology, especially at high current densities. In this paper, the electrochemical CO 2 conversion to pure formic acid was conducted using a three-compartment design electrolyzer, demonstrating electrolyzer catalyst and performance stability for over 1000 h at current densities up to 200 mA cm -2 . Depending on the operation conditions, the electrolyzer directly produced a 6.03 to 12.92 wt% (1.3 to 2.8 M) formic acid product at Faradaic efficiencies ranging between 73.0 to 91.3%. Data on electrolyzer performance, including formic acid product generation rate, energy efficiency, and energy consumption are reported at three different current densities, 100, 200, and 250 mA cm -2 . Finally, a long term 1000 h electrolyzer stability run at 200 mA cm -2 is presented, providing information on the operating conditions required in obtaining stable electrolyzer performance. All the data will be extremely useful in the commercial scale-up of this technology.

10 SYNTHETIC FUELS↗

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 OSTI2024

Iron-sandstone synergy: Advancing in-situ hydrogen production from natural gas via electromagnetic heating

Here, to address the escalating demands for decarbonization in the petroleum industry, a carbon-zero technology, known as in-situ hydrogen (H 2 ) production via electromagnetic (EM)-assisted catalytic heating, has recently been proposed for generating and extracting clean H 2 directly from petroleum reservoirs. Although preliminary techno-economic analyses show significant potential of this emerging technology for clean and affordable hydrogen, the fundamentals of natural gas conversion to H 2 in the presence of reservoir rocks are poorly understood. In this study, we explore the synergy between sandstone and artificial iron-based catalysts in enhancing in-situ H 2 production from methane (CH 4 ) cracking under EM irradiation. The dynamic behaviors of sandstone under EM heating are comprehensively investigated, including its thermal behaviors, thermal runaway (TR) phenomenon, gas generation during TR, and energy consumption. We found that sandstone demonstrates an evident natural catalytic effect for promoting CH 4 conversion to H 2 , enabling H 2 production starting at about 394 °C. The natural catalytic role of iron minerals in sandstone is elucidated using various advanced characterization techniques. Remarkably, when adding iron catalysts into the sandstone, the highest H 2 concentration and CH 4 conversion reaches 91 mol.% and 80%, respectively, at a temperature of 666 °C, while they are 50 mol.% and 35%, respectively, for the sample consisting of iron catalysts and quartz at the same level of temperature. This result indicates a strong iron-sandstone synergy and a potential to stimulate H 2 production by leveraging this synergy. Throughout the experimental process, the generation of carbon oxides (CO and CO 2 ) is negligible. These findings pave a pathway towards future pilot for carbon-zero in-situ H 2 production from sandstone gas reservoirs.

03 NATURAL GAS↗

DOE OSTI2021

One-pot ethanol production under optimized pretreatment conditions using agave bagasse at high solids loading with low-cost biocompatible protic ionic liquid

Agave bagasse (AG) is a potential bioenergy feedstock due to its high biomass productivity, even in semiarid lands. In particular, ionic liquid (IL) pretreatment using aprotic ILs (AILs) has greatly reduced AG recalcitrance towards downstream processing by lowering lignin content and achieving high sugar yields. However, AIL's low biocompatibility towards enzymes and bacteria combined with the high initial cost has limited further development of this technology. In a wash-free one-pot (OP) ethanol conversion process, the evaluation of AG pretreatment with a biocompatible low-cost protic IL (PIL), 2-hydroxyethylammonium acetate ([2-HEA][OAc]) was achieved, where PIL pretreatment was followed by enzymatic saccharification, then ethanol fermentation in a single vessel. The pretreatment conditions were optimized using a central composite design to enable high sugar conversion at low PIL content. Under optimized pretreatment conditions (160 °C, 60% IL loading and 1.5 h), a yield of 132 kg of ethanol per Ton of untreated biomass was estimated using high solids loading (30% solids loading) under a PIL-OP scheme. High lignin removal (>50%), a decreased cellulose crystallinity, and high glucan conversion (>85%) were achieved with PIL-pretreated AG comparable to yields obtained in an AIL-AG pretreated sample using 1-ethyl-3-methyl-imidazolium acetate ([C 2 C 1 Im][OAc]). Here, these results using [2-HEA][OAc] demonstrate the potential of AG in an OP scheme with improved total ethanol yields paving the way towards a more feasible IL-based biorefinery.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Development of a 300 MWe Utility Scale Oxy-Fuel sCO2 Turbine

A 300 MWe direct-fired supercritical carbon dioxide (sCO2) oxy-fuel turbine is being developed that will burn natural gas-fired, coal syngas and even hydrogen mixtures capable of 1,150ºC turbine inlet temperature at 300 bar. This design will significantly improve the state-of-the-art for thermal efficiency and results in a high-pressure stream of CO2 with 98%+ carbon capture, making the power plant near emission-free and more efficient than Natural Gas Combined Cycle (NGCC) plants with carbon capture. This power plant will be capable of burning coal through gasification and cleanup of the synthesis gas (syngas). sCO2 power cycles are a transformational technology for the energy industry, providing higher efficiency heat source energy conversion for conventional and alternative energy sources. This novel cycle significantly reduces capital costs because of smaller equipment footprints, design modularity, and allows for rapid cyclic load and source following to balance solar and wind energy power swings. Oxy-fuel sCO2 cycles take these advantages even further, utilizing higher firing temperatures, improved efficiency, and simpler carbon capture strategies. This turbine will require cooled turbine nozzles and blades as well as advanced thermal management systems to accommodate these high temperatures. The cooled blade heat transfer correlations required new test programs at higher Reynolds number than air-breathing gas turbines for impingement, serpentine, and pin-fin regions. Novel blade optimization was performed to maximize aerodynamic efficiency, while minimizing cooling flows. A turbine layout was generated utilizing individual combustor cans with cooled liners feeding into a 6-stage axial flow turbine with cooled stator nozzles and turbine blades. The case design and thermal management preliminary design will be described.

Moore, Jeffrey↗

DOE OSTI2021

Semiconductor quantum dots: Technological progress and future challenges

In quantum-confined semiconductor nanostructures, electrons exhibit distinctive behavior compared with that in bulk solids. This enables the design of materials with tunable chemical, physical, electrical, and optical properties. Zero-dimensional semiconductor quantum dots (QDs) offer strong light absorption and bright narrowband emission across the visible and infrared wavelengths and have been engineered to exhibit optical gain and lasing. These properties are of interest for imaging, solar energy harvesting, displays, and communications. Here, we offer an overview of advances in the synthesis and understanding of QD nanomaterials, with a focus on colloidal QDs, and discuss their prospects in technologies such as displays and lighting, lasers, sensing, electronics, solar energy conversion, photocatalysis, and quantum information.

García de Arquer, F. Pelayo↗

DOE OSTI2022

Performance Targets for Perovskite Photovoltaic Research, Development, and Demonstration Programs

On October 15, 2021, the U.S. Department of Energy Solar Energy Technologies Office (SETO) released the Performance Targets for Perovskite Photovoltaic Research, Development, and Demonstration Programs Request for Information (RFI) for public response and comment. The RFI sought feedback from industry, academia, research laboratories, government agencies, and other stakeholders on efficiency, stability and replicability performance targets for perovskite (PVSK) photovoltaic devices that could be utilized to align community efforts, ensure relevance of potential future funding programs, and accelerate technical and commercial development and de-risking of perovskite technologies. The RFI included the following proposed target matrix for power conversion efficiency (PCE), area, stability, and sample sizes, and included questions on relevance, completeness, and challenges.

14 SOLAR ENERGY↗

DOE OSTI2022

Wall plug efficiency analysis of a compact SRF industrial accelerator [Poster]

Superconducting radiofrequency cavities offer extremely high (>90%) RF-to-beam energy conversion efficiency. Recent breakthroughs in the Nb 3 Sn SRF cavity technology, successful demonstration of the conduction cooling technique, and the availability of high cooling capacity cryocoolers has made possible the use of SRF for industrial particle accelerators. However, the overall wall plug-to-beam efficiency of such an SRF accelerator can be limited by the wall plug-to-RF power efficiency of the RF source powering this accelerator. The present study quantifies the wall plug-to-beam efficiency of a conduction-cooled SRF accelerator considering several different choices of the RF power source. The study concludes that the wall plug efficiency of the accelerator is indeed limited by that of the power source.

43 PARTICLE ACCELERATORS↗

DOE OSTI2022

Wall plug efficiency analysis of a compact SRF industrial accelerator [Poster]

43 PARTICLE ACCELERATORS↗

DOE OSTI2023

Metal complexes and methods of making the same

Disclosed herein are embodiments of metal complexes and methods of making the same. The disclosed method embodiments provide a one-step approach to making metal complexes, such as complexes comprising lanthanide metals, rare earth metals, transition metals, main group metals, and/or actinide metals that can be used various applications, such as in separations technology, catalysis (e.g., catalysts for pharmaceutical synthesis and/or catalysts for biomass conversion), nuclear chemistry, LED phosphors, scintillator materials, magnetic materials, and nuclear fuels.

Kiplinger, Jaqueline↗

DOE OSTI2023

Downregulation of barley ferulate 5-hydroxylase dramatically alters straw lignin structure without impact on mechanical properties

Barley is a major cereal crop for temperate climates, and a diploid genetic model for polyploid wheat. Cereal straw biomass is an attractive source of feedstock for green technologies but lignin, a key determinant of feedstock recalcitrance, complicates bio-conversion processes. However, manipulating lignin content to improve the conversion process could negatively affect agronomic traits. An alternative approach is to manipulate lignin composition which influences the physical and chemical properties of straw. This study validates the function of a barley ferulate 5-hydroxylase gene and demonstrates that its downregulation using the RNA-interference approach substantially impacts lignin composition. We identified five barley genes having putative ferulate 5-hydroxylase activity. Downregulation of HvF5H1 substantially reduced the lignin syringyl/guaiacyl (S/G) ratio in straw while the lignin content, straw mechanical properties, plant growth habit, and grain characteristics all remained unaffected. Metabolic profiling revealed significant changes in the abundance of 173 features in the HvF5H1-RNAi lines. The drastic changes in the lignin polymer of transgenic lines highlight the plasticity of barley lignification processes and the associated potential for manipulating and improving lignocellulosic biomass as a feedstock for green technologies. On the other hand, our results highlight some differences between the lignin biosynthetic pathway in barley, a temperate climate grass, and the warm climate grass, rice, and underscore potential diversity in the lignin biosynthetic pathways in grasses.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Biotic degradation of acetonitrile. Limitations, controls and conversion rates

This document has been prepared to support Washington River Protection Solutions (WRPS) in their evaluation of technologies to remediate organic compounds in the Liquid Effluent Retention Facility (LERF)/Effluent Treatment Facility (ETF) during direct feed low activity waste (DFLAW) operations at Hanford. This report summarizes the results of a review of the available literature describing aerobic and anaerobic biological treatment of acetonitrile and proposes a test matrix to evaluate microbial degradation rates of acetonitrile. Numerous studies describe acetonitrile degradation by pure culture strains of bacteria, fungi, and yeast; however, the purpose of this review was to provide estimations of degradation under conditions that more closely approximate the Liquid Effluent Retention Facility (LERF) basins at the Hanford Site. To this end, documented limitations, controls, and conversion rates are summarized for mixed and natural microbial communities being maintained or operated as a biological treatment for wastewater processing. Based on the literature evaluation, the inherent capacity and rates of microbial degradation of acetonitrile are sufficiently high that if applied in the LERF basins, acetonitrile removal would be achieved. To be clear, though, published studies have not been conducted under conditions that approximate or that could be directly related to the LERF basins. Thus, a focused test matrix the encompasses LERF relevant conditions to specifically measure microbial degradation of acetonitrile is proposed and the results would provide the strong technical justification for use of this low-cost efficient biological process at LERF during DFLAW operations and beyond.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Effect of H 2 O on the ethylene glycol/alkali dismantling of bagasse for high-value conversion

Using a high-boiling alcohol system to dismantle main components of biomass is a feasible technology. Reducing dismantle operating costs and improving dismantle efficiency are essential for promoting the green, economical, and sustainable development of biomass refining. Therefore, based on the low cost and chemical properties of H 2 O at high temperature, the effects of different H 2 O dosages in NaOH-catalyzed ethylene glycol (HBAA) system on the dismantling efficiency of bagasse, surface lignin coverage, recovered-lignin activity and enzymatic hydrolysis efficiency were investigated. Compared with the HBAA dismantling system without H 2 O, the HBAA system with 60% w/v H 2 O can obviously increase the removal rates of lignin and hemicellulose, while recovering up to 99% of cellulose and significantly declining surface lignin coverage, thus enhancing the enzymatic hydrolysis efficiency. Additionally, the results of density functional theory calculations and 2D HSQC NMR analysis prove that the synergy between H 2 O and ethylene glycol can promote the esterification reaction occurrence at the α-C carbon cation in β-O-4 structure of lignin, thereby protecting the β-O-4 aromatic ether bond. Simultaneously, when the H 2 O dosage increase from 0% to 60%, the enzymatic yield increases from 84.51% to 93.74% with an enzyme load of 10 FPU/g. Based on experimental results, this study conducted a techno-economic analysis of bagasse dismantling for ethanol and co-production of lignin, achieving a minimum ethanol selling price of $\$$1.07 per kg. Here, in this study, a green and economical solution for dismantling the main components of bagasse is developed, which is important for the high-value conversion of bagasse.

Ethylene glycol↗

DOE OSTI2021

BETO 2021 Peer Review - Bio-Insecticides from Thermochemical Biomass Conversion

This work is developing a sustainable and inexpensive bioinsecticide that leverages the inherent chemical functionality created from thermochemical biomass conversion. The impact of this project lies at the intersection of energy and agricultural sustainability. Thermochemical conversion of biomass to fuels remains an attractive pathway, and bioinsecticides, isolated from a fraction of upgraded bio-oils, are a high-valued coproduct that can increase biorefinery profitability. Existing insecticide products are facing significant pressure from regulators and consumers due to negative health and environmental impacts. Bioinsecticides, produced through the deconstruction of biomass, can offer a safer more environmentally benign alternative due to the chemical homology with biologically degraded lignin. To enable thermochemical coproduction of bioinsecticides insecticidal activity must be competitive with existing products, separations of the bioinsecticide must be technically viable, and the overall process economics must be improved. Using vacuum distillation, we have separated a bioinsecticide active ingredient that has similar activity to current commercial products, and technoeconomic modeling has shown it can be produced at market competitive prices. This work has established a bioinsecticide fraction that is ready for further, more resource intensive development by addressing early technical, economic, and toxicological risks.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Predicting Trends in VOC Through Rapid, Multimodal Characterization of State-of-the-Art p-i-n Perovskite Devices

Perovskite photovoltaic technologies are approaching commercial deployment, yet single junction and tandem architectures both still have significant room to improve power conversion efficiency and stability. The ability to perform rapid screening of material quality after altering processing conditions is critical to accelerating the optimization and commercialization of perovskite-based technologies. Currently, researchers utilize a wide range of stand-alone metrology tools to isolate sources of power loss throughout a device stack, which can be slow and labor intensive. Here, we demonstrate the use of a multimodal metrology approach to rapidly determine the maximum achievable and predicted open circuit voltages of >100 perovskite devices during fabrication. Acquisition of these different data is facilitated by combining them into a single integrated measurement platform. We show that these data and automated analysis can be used to rapidly understand and ultimately predict quantitative trends in open circuit voltages of state-of-the-art device architectures. The data and automated analysis workflow presented provides a reliable approach to quickly identify absorber and charge transport layer combinations that can lead to improved open circuit voltages.

14 SOLAR ENERGY↗

DOE OSTI2023

DPE Techno-Economic Analyses

This National Energy Technology Laboratory (NETL) report presents the results of an extensive set of techno-economic analyses for several open-cycle coal fuel oxy-fired direct power extraction (DPE) concepts. These power cycles make use of a conducting plasma accelerated through a magnetic field to generate direct current directly without the need for moving parts. Similar to gas turbines, the efficiency of the power cycle increases with increasing working fluid temperature and typically, plasma temperatures are much higher than the inlet temperature of even the most advanced gas turbine available today, affording the opportunity for very high cycle efficiencies. Most of the study uses high-fidelity models to assess a coal-fueled oxy-combustion DPE system with an AUSC steam bottoming cycle. Two baseline configurations were explored, one with relatively conservative operating point parameters and another with relatively aggressive operating point parameters. Additional analysis on the high-fidelity models as well as reduced order models were performed to analyze the cost and performance potential more thoroughly for the baseline systems and to compare their performance to two alternate open-cycle DPE systems.

30 DIRECT ENERGY CONVERSION↗