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All sources NASA NTRS DOE OSTI

DOE OSTI2022

Bioinspired and biomolecular catalysts for energy conversion and storage

Metalloenzymes are remarkable for facilitating challenging redox transformations with high efficiency and selectivity. In the area of alternative energy, scientists aim to capture these properties in bioinspired and engineered biomolecular catalysts for the efficient and fast production of fuels from low-energy feedstocks such as water and carbon dioxide. In this short review, efforts to mimic biological catalysts for proton reduction and carbon dioxide reduction are highlighted. Two important recurring themes are the importance of the microenvironment of the catalyst active site and the key role of proton delivery to the active site in achieving desired reactivity. As a result, perspectives on ongoing and future challenges are also provided.

14 SOLAR ENERGY↗

DOE OSTI2022

Lignin-based jet fuel and its blending effect with conventional jet fuel

Sustainable aviation fuels (SAFs) must demonstrate specific physical and chemical properties as well as material compatibility (i.e., seal swell) to be used as an aviation turbine fuel. Several alternative jet fuels incorporated in ASTM D7566 are comprised mainly of n/iso-alkanes and can only be blended up to 50 vol% due to material compatibility and density issues. Prior work illustrated the ability of cycloalkanes to replace aromatics’s role in material compatibility. Here, we report the first archival documentation of a feedstock and chemical process to yield a product composition able to complement existing SAF ASTM D7566 annexes. A lignin-based jet fuel (LJF) blend components is generated and composed of mostly C7-C18 mono, di, and tri-cycloalkanes. The neat LJF was blended with conventional jet fuel at 10 vol% (LJF blend) to simulate an ASTM “Fast Track” evaluation process. Fuel properties that are critical to engine operability (ATSM D4054 Tier 3 & 4) were either predicted or experimental tested based on the volume availability. All LJF blend’s critical properties fall within the experience range of conventional jet fuel, with o-ring swelling exceeding the typical range of conventional fuels. Here, these results in total support the potential use of this LJF pathway to complement other SAF pathways and achieve 100% drop-in SAF.

09 BIOMASS FUELS↗

DOE OSTI2021

Guidelines for performing lignin-first biorefining

With these guidelines, we aim to unite the lignin-first biorefining research field around best practices for performing or reporting feedstock analysis, reactor design, catalyst performance, and product yields.

09 BIOMASS FUELS↗

DOE OSTI2023

Disruption of p -coumaroyl-CoA:monolignol transferases in rice drastically alters lignin composition

Grasses are abundant feedstocks that can supply lignocellulosic biomass for production of cell-wall-derived chemicals. In grass cell walls, lignin is acylated with p-coumarate. These p-coumarate decorations arise from the incorporation of monolignol p-coumarate conjugates during lignification. A previous biochemical study identified a rice (Oryza sativa) BAHD acyltransferase (AT) with p-coumaroyl-CoA:monolignol transferase (PMT) activity in vitro. In this study, we determined that that enzyme, which we name OsPMT1 (also known as OsAT4), and the closely related OsPMT2 (OsAT3) harbor similar catalytic activity toward monolignols. We generated rice mutants deficient in either or both OsPMT1 and OsPMT2 by CRISPR/Cas9-mediated mutagenesis and subjected the mutants’ cell walls to analysis using chemical and nuclear magnetic resonance methods. Our results demonstrated that OsPMT1 and OsPMT2 both function in lignin p-coumaroylation in the major vegetative tissues of rice. Notably, lignin-bound p-coumarate units were undetectable in the ospmt1 ospmt2-2 double-knockout mutant. Further, in-depth structural analysis of purified lignins from the ospmt1 ospmt2-2 mutant compared with control lignins from wild-type rice revealed stark changes in polymer structures, including alterations in syringyl/guaiacyl aromatic unit ratios and inter-monomeric linkage patterns, and increased molecular weights. Furthermore, our results provide insights into lignin polymerization in grasses that will be useful for the optimization of bioengineering approaches for the effective use of biomass in biorefineries.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

Biochemical characterization of xyloglucan galactosyltransferases MUR3 and XLT2 from Spirodela polyrhiza

Glycosyltransferases (GTs) are the primary enzymes responsible for the biosynthesis of the complex polysaccharides in plant cell walls. Given the important role of GTs in plants, it is necessary to undertake their functional characterization to better understand plant cell wall synthesis pathways to develop improved feedstocks for efficient conversion into fuels and products to support the emerging bioeconomy. The GT47 family in plants represents a unique target for characterization due to the substantial diversity of donor and acceptor substrates observed within a single family. Here, we have carried out the biochemical characterization of MUR3 and XLT2 orthologs from the aquatic monocot Spirodela polyrhiza. Our findings support existing genetic and phylogenetic data classifying these enzymes as regio-specific galactosyltransferases involved in xyloglucan (XyG) sidechain biosynthesis. In addition, we have identified novel characteristics for both enzymes, such as in vitro arabinopyranosyltransferase activity and distinctiveness in xyloglucan reducing end specificity.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Variable Chain Length Carboxylic Acids as Modifiers to Enhance the Antiviral Efficacy of Sodium Dodecyl Sulfate.

Non-toxic disinfectants composed of readily available commodity chemicals are needed for immediate response to the current COVID-19 pandemic. One such area is the active research field for food-grade sanitization. Combinations of levulinic acid, a five-carbon ketocarboxylic acid, and sodium dodecyl sulfate, have been frequently described for antibacterial use on food contact surfaces. Levulinic acid has been identified as a renewable feedstock but is not presently in commodity production. Other carboxylic acids, such as acetic acid, may be equally usable and food-safe. Acidic and buffered solutions were highly effective, yielding no countable surviving organisms. The high efficacy of each acid may suggest that carboxylic acid sanitizers in general have potential use against viruses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Rapid Characterization Tools for Process Optimization: Cooperative Research and Development (Final Report)

In this project Prenexus Health, Inc. (Prenexus) and NLR will develop rapid characterization tools to improve the Prenexus production process. First, we will develop a tool to predict the overall performance of the Prenexus manufacturing process converting high-fiber sugarcane to xylo-oligosaccharides (XOS) (both the overall process yield and the composition of the XOS product) using rapid characterization of the incoming feedstock and knowledge of key process parameters. This tool will dramatically increase Prenexus’ understanding of the overall process. Second, we will develop a tool to predict the concentration of soluble oligomeric and monomeric xylose and organic acids in multiple process streams at-line in the Prenexus process, enabling real-time process control of the conversion process.

09 BIOMASS FUELS↗

NASA NTRS2023

Analysis of the Solid Products from the OSCAR and the AOWG Trash Processing Systems

Two trash conversion systems that process space logistical trash for conversion into gases and liquids have minor solid product formation consisting of primarily high carbon ash, inorganic salts, and aluminum metal flakes. These solid products necessarily comprise part of the system output because the thermal degradation processes intentionally operate at temperatures below aluminum vaporization and do not convert all solid inorganics or carbon-based compounds into gaseous compounds (i.e., CO 2 or CH 4 ). The two systems included the Orbital Syngas/Commodity Augmentation Reactor (OSCAR) combustion system funded by the NASA Space Technology Mission Directorate (STMD) located at NASA’s Kennedy Space Center, and the Advanced Organic Waste Gasifier (AOWG) steam reforming system developed by Pioneer Astronautics in Lakewood, Colorado, and funded by the NASA Small Business Innovation Research (SBIR) Exploration Systems Development Mission Directorate (ESDMD). OSCAR residual solids were collected from suborbital flight and ground-based laboratory testing, while all AOWG samples were collected from ground testing. This report discusses the solid product characterization, including elemental analyses performed with scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS), and a surface chemistry performed with x-ray photoelectron spectroscopy (XPS). A particle size analysis was performed with sieves, followed by SEM analyses. These analyses were performed to elucidate what high value products can be extracted or utilized from the solid products for follow on infusion into chemical feedstocks, manufacturing additives, or in-situ construction-based material needs.

OSCAR↗

DOE OSTI2020

Woody Feedstocks 2019 State of Technology Report

The U.S. Department of Energy promotes production of advanced liquid transportation fuels from lignocellulosic biomass by funding fundamental and applied research that advances the state of technology (SOT). As part of its involvement with this overall mission, Idaho National Laboratory completes annual SOT reports for nth-plant biomass feedstock logistics. The purpose of the SOTs is to provide the status of feedstock supply system technology development for biomass to biofuels, based on actual data and experimental results relative to technical targets and cost goals from specific design cases. The 2019 Woody Feedstock SOT presents the State of Technology for feedstock supply to three individual thermochemical conversion pathways that utilize woody feedstocks: Indirect Liquefaction (IDL), Catalytic Fast Pyrolysis (CFP), and Algal-blend Hydrothermal liquefaction (AHTL). The 2019 reactor throat delivered feedstock costs were found to be $63.54/dry ton, $70.15/dry ton and $70.31/dry ton, respectively (2016$).

09 BIOMASS FUELS↗

DOE OSTI2020

Woody Feedstocks 2020 State of Technology Report

The U.S. Department of Energy promotes production of advanced liquid transportation fuels from lignocellulosic biomass by funding fundamental and applied research that advances the state of technology (SOT). As part of its involvement with this overall mission, Idaho National Laboratory completes annual SOT reports for nth-plant biomass feedstock logistics. The purpose of the SOTs is to provide the status of feedstock supply system technology development for biomass to biofuels, based on actual data and experimental results relative to technical targets and cost goals from specific design cases. The 2020 Woody Feedstock SOT is separated into three separate pathways that utilize woody feedstocks: indirect liquefaction (IDL), catalytic fast pyrolysis (CFP), and algal-blend hydrothermal liquefaction (AHTL).

09 BIOMASS FUELS↗

DOE OSTI2021

Woody Feedstocks 2021 State of Technology Report

09 BIOMASS FUELS↗

DOE OSTI2024

Performance Testing of a Moving-Bed Gasifier Using Coal, Biomass, and Waste Plastic Blends with Washed and Unwashed Legacy Coals and Other Waste Fuels to Generate White Hydrogen

The objective of this effort, primarily funded by the United States Department of Energy (DOE), and led by the Electric Power Research Institute, Inc. (EPRI), with support by Hamilton Maurer International (HMI) and Sotacarbo S.p.A. (Sotacarbo), has been to qualify coal, biomass, and plastic waste blends based on performance testing of selected fuel pellet compositions in a pilot-scale updraft moving-bed (UDMB) gasifier. The testing provided relevant data to advance the commercial-scale design of the moving-bed gasifier to be able to successfully use these feedstocks to produce hydrogen. In particular, the effects of waste plastics on feedstock development (i.e., blending and pelletizing) and the resulting products (i.e., syngas compositions, organic condensate production, and ash characteristics) are the focus. The gasifier used for testing is HMI’s moving-bed gasifier, which has been proven capable of gasifying nearly all coal ranks. It has also shown the ability in prior testing work to gasify wood chips (biomass). However, mixtures of these fuels with plastic wastes have not been prepared and gasified together. The three feedstocks were densified and pelletized by California Pellet Mill (CPM) to meet the feedstock size required by Sotacarbo’s 30mm ID UDMB gasifier, under contract to HMI. The technical tasks and results from this two-year research project included: (1) Feed Procurement and Preparation: Nine different tri-fuel pellets were prepared from varying compositions of fresh mined PRB coal, corn stover biomass, and car fluff waste plastics. Tri-fuel pellets were produced by CPM and shipped to Sotacarbo’s test facility in Carbonia, Sardinia, Italy. (2) Test Plan Development: A test plan was created to define the test runs to be performed. The test plan detailed the different UDMB gasification tests to be performed in Sotacarbo’s 12-inch ID pilot scale gasifier, the process monitoring instrumentation used, and the extractive samples recovered for analysis of the total gasification process mass and energy balance. (3) Gasifier Testing: Nine different gasification runs were performed in the pilot-scale gasifier at Sotacarbo using nine different fuel feedstock compositions generated from varying mixtures of PRB coal, biomass, and plastic wastes. The testing generated performance data on gasification reaction efficiency and performance, yielding relevant data for models used to scale up the gasifier design. This task also included work to refurbish and reassemble the pilot gasifier at Sotacarbo and perform a baseline 100% PRB coal run. (4) Data Analysis and Reporting: Review of the data, determination of figures of merit, and interpretation of the results are reported in the project’s final report, published in March 2024. The results show that all tri-fuel pellets gasified well and maintained structural integrity throughout the gasification process. The syngas generated can be shifted to hydrogen by using commercial syngas shifting technologies. (5) High Fidelity computational fluid dynamics (CFD) Simulation: The National Energy Technology Laboratory (NETL) team performed CFD simulations of the UDMB gasifier for two of the tri-fuel pellets gasified in Sotacarbo’s pilot scale gasifier. The kinetic mechanisms for the pyrolysis of each constituent, PRB coal, corn stover biomass, and waste plastics are based on thermogravimetric analysis performed by Sotacarbo. The gasification model was validated by comparing the predicted syngas composition at the exit of the gasifier with the measured syngas composition. In addition, the reactor’s measured internal temperature profile agreed well with the predicted internal reactor temperature profile. These results validate that the model can be used to predict the performance of the updraft moving bed gasifier for different feedstocks and operating conditions. This paper summarizes the results of the completed work in which the pelletizing procedure was validated to ensure the viability of the tri-fuel pellets for the gasification runs performed at Sotacarbo’s 30 mm UDMB gasifier. The gasification performance data from this series of nine runs will enable modeling of a full-scale HMI industrial scale gasifier supporting both combined heat and power, and Hydrogen production from coal (both fresh mined and legacy) combined with various biomass and waste plastics. Additionally, plans and progress on a follow-up project, being executed by the same project team, will be presented. In this project, a total of twenty (20) different feedstocks are being prepared from varying compositions of biomass (both woody biomass and corn stover) with a mixture of legacy coal waste, plastic waste, and refuse-derived fuel (RDF). The testing will provide information on gasification reaction efficiency/performance, yielding relevant data for models used to scale up the gasifier design to 50 megawatt electric (MWe) (equivalent hydrogen production). Tests will also be performed on a bench-scale fluidized-bed gasifier for comparison purposes. The results of this testing will be used to specify the range of feedstock blends that can be successfully gasified as well as quantify gasifier outputs based on specific blends.

08 HYDROGEN↗

NASA NTRS1993

Production of O2 on the Moon: A lab-top demonstration of ilmenite reduction with hydrogen

Estimates of the costs of transporting materials from Earth to the Moon are around $25,000 per pound. Therefore, it is imperative that we learn to utilize the resources on the Moon to partially offset these 'astronomical' expenses. The production of oxygen on the Moon utilizing indigenous materials is crucial to the establishment and development of an autonomous lunar colony. Besides obvious biologic needs, this lunar liquid oxygen (LLOX) could result in tremendous cost savings on fuel for effective transportation systems, particularly with its export to low-Earth orbit. Over 20 different process concepts were proposed and evaluated for the production of oxygen from lunar materials. Simplicity, low energy, easily attainable feedstock, and low resupply mass are the keywords for the process(es) which will ultimately be selected for the initial production of oxygen on the Moon. One of these schemes, which has received considerable study to date, is the hydrogen reduction of ilmenite. In fact, Carbotek, Inc. (Houston, TX) patented an ilmenite, hydrogen-reduction technique involving a three-stage, fluidized-bed process for the production of LLOX. A lab-top demonstration unit of the basic concepts of this oxygen generation process that was constructed by our group at the University of Tennessee is explained. It utilizes many of the principles which must be addressed in designing an effective production plant for operation on the Moon.

Taylor, Lawrence A.↗

DOE OSTI2022

Impact of storage and blending of algae and forest product residue on fuel blendstock production

Seasonal impacts on the production of algae biomass require blending with other feedstocks such as wood to maintain consistent annual conversion capacity. Idaho National Laboratory (INL) has developed a long-term storage strategy for algae biomass using ensiling, or anaerobic wet storage, that was tested for blends of algae and wood to stabilize the feedstock supply for processing to fuels. Additionally, blending biomass (algae and wood) leverages existing biomass storage approaches commonly used by the feed and forage industry. Earlier research also has demonstrated positive results that indicate ensiling is more effective and economical in normalizing biomass feedstock supply prior to conversions such as HTL (hydrothermal liquefaction) than preserving biomass by drying. By assessing impacts beginning with upstream logistic operations and proceeding through each conversion step, this work focuses on conversion of ensiled and blended biomass to fungible liquid transportation fuel blendstocks. This is accomplished by conversion of the blended biomass (62% Chlorella sp. blended with 38% loblolly pine forest product residues [FPR]) to bio-crude through HTL and subsequent upgrading through HT (hydrotreating) with a commercial refinery catalyst analogous to a refinery process to produce hydrocarbon fuel. In this work, results indicate that carbon retention and quality are preserved in both the bio-crude and upgraded fuel from the ensiled blend, indicating the potential of this approach for managing seasonal variations in algae biomass productivity.

09 BIOMASS FUELS↗

DOE OSTI2026

Higher Wood Density Lowers Feedstock Cost and Has Minimal Impact on Biomass Conversion to Biofuels

Poplar and other woody feedstocks have the potential to provide up to 200 million tons of biomass per year that can be converted to liquid fuels. Most forestry strategies that aim to increase biomass productivity per hectare rely on short rotation plantations of fast-growing varieties. The improvement of the wood density as a key trait itself has largely been overlooked. We evaluated natural variation in wood density across a population of genetically diverse Populus trichocarpa trees grown in a common garden. Wood density varies greatly within this population but is heritable; higher wood density was not systematically associated with reduced growth, challenging assumptions of a trade-off between wood density and biomass accumulation. Furthermore, denser wood led to significant improvements throughout the supply chain including lowering biomass production and transportation costs. Higher density did not correlate with changes in biomass composition. Density did not impact bioconversion in the two feedstock-to-fuel pipelines tested (pretreatment by ionic liquids and fermentation to bisabolene or soaking in aqueous ammonia and fermentation to ethanol) on a representative subset of poplars. These findings highlight wood density as a promising breeding target for accelerating the development of high-yielding, conversion-efficient bioenergy crops and as an avenue for increasing landuse efficiency and reducing biomass transportation cost.

09 BIOMASS FUELS↗

DOE OSTI2022

Synthesis of Hydrophilic Derivative Surfactants From Algae-Derived Unsaponifiable Lipids

In the context of decarbonizing the economy, the utilization of biologically sourced feedstocks to produce replacements for petroleum-derived materials is becoming more urgent. Improving renewable biomass production and utilization is imperative for commercializing future biorefineries. Algae-derived biomass is a particularly promising feedstock thanks to its attractive oil content and composition; specifically, the high-value products in the unsaponifiable lipids have not been included in a conversion process. Here we demonstrate surfactant synthesis from a complex oil fraction as the hydrophobic donor moieties, yielding products that are similar to commercially available surfactants such as the linear alkyl benzene sulfonates. Unsaponifiable lipids extracted from algae were derivatized to non-ionic surfactants using a green chemical synthesis route based on a double esterification with succinic acid and polyethylene glycol. The in-depth molecular and structural surfactant characterization is included and indicates that the resulting properties fall between those of pure cholesterol and phytol used as surrogates for the reaction synthesis demonstration. This is the first demonstration of an effective and potentially high-value synthesis of functional surfactants with properties that can be tailored based on the relative composition of the resulting hydrocarbon alcohol components in the mixture. This novel green chemistry synthesis approach provides a route to high-value product synthesis from algae.

09 BIOMASS FUELS↗

DOE OSTI2025

Techno-economic analysis of synthetic fuel production from existing nuclear power plants across the United States

Abstract Low carbon synfuel can reduce dependence on fossil fuels like diesel and jet fuel, and, with large-scale cost-effective production, contribute to global transportation sector decarbonization, Simultaneously, nuclear power plants are struggling economically due to falling wholesale electricity prices. Converting existing nuclear plants for synfuel production could preserve these low-carbon assets and enable large-scale synfuel production, yet no comprehensive technoeconomic analysis exists. This study evaluates the potential of integrating synthetic fuel production with five US nuclear plants, considering electricity and fuel markets and carbon dioxide source access. Such integration could enhance nuclear plant profitability by up to $792 million and offer a 10% return on investment over 20 years. The hydrogen production tax credit from the 2022 Inflation Reduction Act is crucial, comprising 75% of revenues on average. Carbon feedstock transportation has the highest cost at 35%, followed closely by synfuel production capital costs. Incentive policies are thus key for the decarbonization of the transportation sector and the economic importance of the geographic location of Integrated Energy Systems.

Garrouste, Marisol (ORCID:0000000168388644)↗

DOE OSTI2024

Supported Platinum Nanoparticles Catalyzed Carbon–Carbon Bond Cleavage of Polyolefins: Role of the Oxide Support Acidity

Supported platinum nanoparticle catalysts are known to convert polyolefins to high-quality liquid hydrocarbons using hydrogen under relatively mild conditions. To date, few studies using platinum grafted onto various metal oxide (M x O y ) supports have been undertaken to understand the role of the acidity of the oxide support in the carbon-carbon bond cleavage of polyethylene under consistent catalytic conditions. Specifically, two Pt/M x O y catalysts (M x O y = SrTiO 3 and SiO 2 -Al 2 O 3 ; Al = 3.0 wt %, target Pt loading 2 wt % Pt similar to 1.5 nm), under identical catalytic polyethylene hydrogenolysis conditions (T = 300 degree celsius, P(H 2 ) = 170 psi, t = 24 h; M w = similar to 3,800 g/mol, M n = similar to 1,100 g/mol, D = 3.45, N branch/100C = 1.0), yielded a narrow distribution of hydrocarbons with molecular weights in the range of lubricants (M w = < 600 g/mol; M n < 400 g/mol; D = 1.5). While Pt/SrTiO 3 formed saturated hydrocarbons with negligible branching, Pt/SiO 2 -Al 2 O 3 formed partially unsaturated hydrocarbons (<1 mol % alkenes and similar to 4 mol % alkyl aromatics) with increased branch density (N branch/100C = 5.5). Further investigations suggest evidence for a competitive hydrocracking mechanism occurring alongside hydrogenolysis, stemming from the increased acidity of Pt/SiO 2 -Al 2 O 3 compared to Pt/SrTiO 3 . Additionally, the products of these polymer deconstruction reactions were found to be independent of the polyethylene feedstock, allowing the potential to upcycle polyethylenes with various properties into a value-added product.

36 MATERIALS SCIENCE↗