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At least 865 records · Page 48
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Screening of Lost Circulation Materials for Geothermal Applications: Experimental Study at High Temperature

Abstract This study presents a laboratory experimental research to determine the characteristics of lost circulation materials (LCMs) capable of addressing thermal degradation, providing bridging and sealing in geothermal conditions. Eleven different materials were tested: Walnut Fine, Walnut Medium, Sawdust, Altavert, Graphite Blend, Bentonite Chips, Micronized Cellulose (MICRO-C), Magma Fiber Fine, diatomaceous earth/amorphous silica powder (DEASP), Cotton Seed Hulls, and a Calcium Carbonate Blend. The filtration and sealing pressure of the LCMs were measured with HPHT equipment up to 149 °C (300 °F). Besides, the particle size distribution (PSD) of fine granular materials was measured. The results show that the performance of some LCM materials commonly used in geothermal operations is affected by high temperature. Characteristics such as shape and size made some materials more prone to thermal degradation. Also, it was found that the PSD of LCMs is a key factor in the effectiveness of bridging and sealing fractures. The results suggest that granular materials with a wide particle size distribution PSD are suitable for geothermal applications.

Energy & Fuels↗
DOE OSTI2025

Rheological Properties of Enzymatically Hydrolyzed Corn Stover Pretreated via Deacetylation and Mechanical Refining

Lignocellulosic biomass is a feedstock for fuels and chemicals that does not compete with food resources and has less contaminants than refuse-derived biomass feedstocks. To convert lignocellulosics to biofuels or value-added products, multiple processing steps are typically necessary. One method of producing biofuels from lignocellulosic biomass utilizes a deacetylation and mechanical refining pretreatment and an enzymatic hydrolysis reaction to produce fermentable sugars from cellulose and hemicellulose. The rheological properties of biomass, such as yield stress and plastic viscosity, change during enzymatic hydrolysis and alter the energy requirements for pumping and mixing, an important consideration for the design of processing equipment. The dynamic changes in rheological properties that occur in a corn stover feedstock undergoing enzymatic hydrolysis are characterized in this work, and the influence on pressure losses in piping systems is estimated. Two rheometer geometries were fabricated with stereolithography 3D printing to reduce wall slip and sample ejection. The slurries have complex rheological behaviors that include shear-thinning behavior. Shear stress ramps were performed on samples at 20 and 50 degrees C using the custom geometries, and the Herschel-Bulkley model was fit to the data. The dynamic nature of the rheological properties is correlated with changes in the average fiber length at various extents of reaction, and the influence of solids concentration on the observed rheology and piping pressure losses is discussed.

09 BIOMASS FUELS↗
DOE OSTI2021

Self-organization of nanoparticles and molecules in periodic Liesegang-type structures

Chemical organization in reaction-diffusion systems offers a strategy for the generation of materials with ordered morphologies and structural hierarchy. Periodic structures are formed by either molecules or nanoparticles. On the premise of new directing factors and materials, an emerging frontier is the design of systems in which the precipitation partners are nanoparticles and molecules. We show that solvent evaporation from a suspension of cellulose nanocrystals (CNCs) and L -(+)-tartaric acid [ L -(+)-TA] causes phase separation and precipitation, which, being coupled with a reaction/diffusion, results in rhythmic alternation of CNC-rich and L -(+)-TA–rich rings. The CNC-rich regions have a cholesteric structure, while the L -(+)-TA–rich bands are formed by radially aligned elongated bundles. The moving edge of the pattern propagates with a finite constant velocity, which enables control of periodicity by varying film preparation conditions. This work expands knowledge about self-organizing reaction-diffusion systems and offers a strategy for the design of self-organizing materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Protecting ice from melting under sunlight via radiative cooling

As ice plays a critical role in various aspects of life, from food preservation to ice sports and ecosystem, it is desirable to protect ice from melting, especially under sunlight. The fundamental reason for ice melt under sunlight is related to the imbalanced energy flows of the incoming sunlight and outgoing thermal radiation. Therefore, radiative cooling, which can balance the energy flows without energy consumption, offers a sustainable approach for ice protection. Here, we demonstrate that a hierarchically designed radiative cooling film based on abundant and eco-friendly cellulose acetate molecules versatilely provides effective and passive protection to various forms/scales of ice under sunlight. This work provides inspiration for developing an effective, scalable, and sustainable route for preserving ice and other critical elements of ecosystems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Water transport in reverse osmosis membranes is governed by pore flow, not a solution-diffusion mechanism

We performed nonequilibrium molecular dynamics (NEMD) simulations and solvent permeation experiments to unravel the mechanism of water transport in reverse osmosis (RO) membranes. The NEMD simulations reveal that water transport is driven by a pressure gradient within the membranes, not by a water concentration gradient, in marked contrast to the classic solution-diffusion model. We further show that water molecules travel as clusters through a network of pores that are transiently connected. Permeation experiments with water and organic solvents using polyamide and cellulose triacetate RO membranes showed that solvent permeance depends on the membrane pore size, kinetic diameter of solvent molecules, and solvent viscosity. This observation is not consistent with the solution-diffusion model, where permeance depends on the solvent solubility. Motivated by these observations, we demonstrate that the solution-friction model, in which transport is driven by a pressure gradient, can describe water and solvent transport in RO membranes.

42 ENGINEERING↗
DOE OSTI2024

Atomistic, macromolecular model of the Populus secondary cell wall informed by solid-state NMR

Plant secondary cell walls (SCWs) are composed of a heterogeneous interplay of three major biopolymers: cellulose, hemicelluloses, and lignin. Details regarding specific intermolecular interactions and higher-order architecture of the SCW superstructure remain ambiguous. Here, we use solid-state nuclear magnetic resonance (ssNMR) measurements to infer refined details about the structural configuration, intermolecular interactions, and relative proximity of all three major biopolymers within air-dried Populus wood. To enhance the utility of these findings and enable evaluation of hypotheses in a physics-based environment in silico, the NMR observables are articulated into an atomistic, macromolecular model for biopolymer assemblies within the plant SCW. Through molecular dynamics simulation, we quantitatively evaluate several variations of atomistic models to determine structural details that are corroborated by ssNMR measurements.

09 BIOMASS FUELS↗
DOE OSTI2024

Three-dimensional printing of wood

Natural wood has served as a foundational material for buildings, furniture, and architectural structures for millennia, typically shaped through subtractive manufacturing techniques. However, this process often generates substantial wood waste, leading to material inefficiency and increased production costs. A potential opportunity arises if complex wood structures can be created through additive processes. Here, we demonstrate an additive-free, water-based ink made of lignin and cellulose, the primary building blocks of natural wood, that can be used to three-dimensional (3D) print architecturally designed wood structures via direct ink writing. The resulting printed structures, after heat treatment, closely resemble the visual, textural, olfactory, and macro-anisotropic properties, including mechanical properties, of natural wood. Our results pave the way for 3D-printed wooden construction with a sustainable pathway to upcycle/recycle natural wood.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Oil-impregnated densified wood veneer with high electrical insulation enabled by nanosized oil channels

Growing energy demands and renewable integration are stressing the aging power grid infrastructure. Lignocellulosic oil-impregnated paper is widely used in power transformers but suffers from critical limitations, such as low dielectric strength, mechanical strength, and thermal conductivity, causing premature transformer failures. Here, we demonstrate a superior electrically insulating oil-impregnated paper design using the naturally anisotropic structure of densified wood veneer to achieve nanosized channels of oil that efficiently disrupt electrical breakdown pathways. The developed oil-impregnated densified wood (ODW) creates aligned cellulose fibers with 166 ± 87–nanometer oil nanochannels, achieving record dielectric strength of 105 kilovolts per millimeter. The structure also delivers a mechanical strength of up to 384 megapascals and a thermal conductivity of 0.33 watts per meter per kelvin, enabling enhanced longevity upon thermal aging tests. The ODW could replace conventional transformer insulation to enhance power transformer performance and improve lifetime. Moreover, its anisotropic oil-filled nanochannel design offers a general strategy for hybrid dielectrics in medium- and high-voltage applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Co-expression of a β-d-xylosidase from Thermotoga maritima and a Family 10 xylanase from A. cellulolyticus significantly improves the xylan degrading activity of the Caldicellulosiruptor bescii exoproteome

Caldicellulosiruptor species are hyperthermophilic, Gram-positive, anaerobes and the most thermophilic cellulolytic bacteria so far described. They have been engineered to convert switchgrass to ethanol without pretreatment and represent a promising platform for the production of fuels, chemicals and materials from plant biomass. Xylooligomers such as xylobiose and xylotriose that result from the breakdown of plant biomass more strongly inhibit cellulase activity than do glucose or cellobiose. High concentrations of xylobiose and xylotriose, are present in C. bescii fermentations after 90 h incubation and removal or breakdown of these types of xylooligomers is crucial to achieve high conversion of plant biomass to product. In previous studies the addition of exogenous β-d-xylosidase substantially improved the performance of glucanases and xylanases in vitro. β-d-Xylosidases are, in fact, essential enzymes in commercial preparations for efficient deconstruction of plant biomass. In addition, the combination of xylanase and β-d-xylosidase is known to exhibit synergistic action on xylan degradation. In spite of its ability to grow efficiently on xylan substrates, no extracellular β-d-xylosidase was identified in the C. bescii genome. Here we report that the co-expression of a thermal stable β-d-xylosidase from Thermotoga maritima and a xylanase from Acidothermus cellulolyticus in a C. bescii strain containing the A. cellulolyticus E1 endoglucanase significantly increased the activity of the exoproteome as well as growth on xylan substrates. The combination of these enzymes also resulted in increased growth on crystalline cellulose in the presence of exogeneous xylan.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Tracing Carbon Metabolism with Stable Isotope Metabolomics Reveals the Legacy of Diverse Carbon Sources in Soil

Tracking the metabolic activity of whole soil communities can improve our understanding of the transformation and fate of carbon in soils. For this work, we used stable isotope metabolomics to trace 13 C from nine labeled carbon sources into the water-soluble metabolite pool of an agricultural soil over time. Soil was amended with a mixture of all nine sources, with one source isotopically labeled in each treatment. We compared changes in the 13 C enrichment of metabolites with respect to carbon source and time over a 48-day incubation and contrasted differences between soluble sources (glucose, xylose, amino acids, etc.) and insoluble sources (cellulose and palmitic acid). Whole soil metabolite profiles varied singularly by time, while the composition of 13 C-labeled metabolites differed primarily by carbon source (R 2 = 0.68) rather than time (R 2 = 0.07), with source-specific differences persisting throughout incubations. The 13 C labeling of metabolites from insoluble carbon sources occurred slower than that from soluble sources but yielded a higher average atom percent (atom%) 13 C in metabolite markers of biomass (amino acids and nucleic acids). The 13 C enrichment of metabolite markers of biomass stabilized between 5 and 15 atom% 13 C by the end of incubations. Temporal patterns in the 13 C enrichment of tricarboxylic acid cycle intermediates, nucleobases (uracil and thymine), and by-products of DNA salvage (allantoin) closely tracked microbial activity. Our results demonstrate that metabolite production in soils is driven by the carbon source supplied to the community and that the fate of carbon in metabolites do not generally converge over time as a result of ongoing microbial processing and recycling.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Eight Metagenome-Assembled Genomes Provide Evidence for Microbial Adaptation in 20,000- to 1,000,000-Year-Old Siberian Permafrost

Permafrost microbes may be metabolically active in microscopic layers of liquid brines, even in ancient soil. Metagenomics can help discern whether permafrost microbes show adaptations to this environment. Thirty-three metagenome-assembled genomes (MAGs) were obtained from six depths (3.5 m to 20 m) of freshly cored permafrost from the Siberian Kolyma-Indigirka Lowland region. These soils have been continuously frozen for ~20,000 to 1,000,000 years. Eight of these MAGs were ≥80% complete with <10% contamination and were taxonomically identified as Aminicenantes, Atribacteria, Chloroflexi, and Actinobacteria within bacteria and Thermoprofundales within archaea. MAGs from these taxa have been obtained previously from nonpermafrost environments and have been suggested to show adaptations to long-term energy starvation, but they have never been explored in ancient permafrost. The permafrost MAGs had greater proportions in the Clusters of Orthologous Groups (COGs) categories of energy production and conversion and carbohydrate transport and metabolism than did their nonpermafrost counterparts. They also contained genes for trehalose synthesis, thymine metabolism, mevalonate biosynthesis, and cellulose degradation, which were less prevalent in nonpermafrost genomes. Furthermore, many of these genes are involved in membrane stabilization and osmotic stress responses, consistent with adaptation to the anoxic, high-ionic-strength, cold environments of permafrost brine films. Our results suggest that this ancient permafrost contains DNA of high enough quality to assemble MAGs from microorganisms with adaptations to survive long-term freezing in this extreme environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Biochemical and Regulatory Analyses of Xylanolytic Regulons in Caldicellulosiruptor bescii Reveal Genus-Wide Features of Hemicellulose Utilization

Microbial deconstruction of lignocellulose for the production of biofuels and chemicals requires the hydrolysis of heterogeneous hemicelluloses to access the microcrystalline cellulose portion. This work extends previous in vivo and in vitro efforts to characterize hemicellulose utilization by integrating genomic reconstruction, transcriptomic data, operon structures, and biochemical characteristics of key enzymes to understand the deployment and functionality of hemicellulases by the extreme thermophile Caldicellulosiruptor bescii .

Biotechnology & Applied Microbiology↗
DOE OSTI2023

Comparative Genomic Analyses of Cellulolytic Machinery Reveal Two Nutritional Strategies of Marine Labyrinthulomycetes Protists

Labyrinthulomycetes are a group of ubiquitous and diverse unicellular Stramenopiles and have long been known for their vital role in ocean carbon cycling. However, their ecological function from the perspective of organic matter degradation remains poorly understood. This study reports high-quality genomes of two newly isolated Labyrinthulomycetes strains, namely, Botryochytrium sp. strain S-28 and Oblongichytrium sp. strain S-429, and provides molecular analysis of their ecological functions using comparative genomics and a biochemical assay. Our results suggest that Labyrinthulomycetes may occupy multiple ecological niches in marine ecosystems because of the significant differences in gene function among different genera. Certain strains could degrade wheat bran independently by secreting cellulase. The key glycoside hydrolase families (GH1, GH5, and GH9) related to cellulase and the functional domains of carbohydrate-active enzymes (CAZymes) were more enriched in their genomes. This group can actively participate in marine biochemical cycles as decomposers. In contrast, other strains that could not produce cellulase may thrive as “leftover scavengers” and act as a source of nutrients to the higher-trophic-level plankton. In addition, our findings emphasize the dual roles of endoglucanase, acting as both exo- and endoglucanases, in the process of cellulose degradation. Using genomic, biochemical, and phylogenetic analyses, our study provides a broader insight into the nutritional patterns and ecological functions of Labyrinthulomycetes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Vibrational Sum-Frequency Generation Hyperspectral Microscopy for Molecular Self-Assembled Systems

In this review, we discuss the recent developments and applications of vibrational sum-frequency generation (VSFG) microscopy. This hyperspectral imaging technique can resolve systems without inversion symmetry, such as surfaces, interfaces and noncentrosymmetric self-assembled materials, in the spatial, temporal, and spectral domains. We discuss two common VSFG microscopy geometries: wide-field and confocal point-scanning. We then introduce the principle of VSFG and the relationships between hyperspectral imaging with traditional spectroscopy, microscopy, and time-resolved measurements. We further highlight crucial applications of VSFG microscopy in self-assembled monolayers, cellulose in plants, collagen fibers, and lattice self-assembled biomimetic materials. In these systems, VSFG microscopy reveals relationships between physical properties that would otherwise be hidden without being spectrally, spatially, and temporally resolved. Lastly, we discuss the recent development of ultrafast transient VSFG microscopy, which can spatially measure the ultrafast vibrational dynamics of self-assembled materials. The review ends with an outlook on the technical challenges of and scientific potential for VSFG microscopy.

Chemistry↗
DOE OSTI2020

Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi 0.6 Mn 0.2 Co 0.2 O 2 Cathodes

In this work, we explore the influence of binder coverage and chemistry on the interfacial properties of the textured Ni-rich cathode LiNi 0.6 Mn 0.2 Co 0.2 O 2 . We find that the formation of the cathode/electrolyte interphase (CEI) composition varies significantly for cathodes coated with either poly(vinylene fluoride) (PVDF), carboxymethyl cellulose (CMC), or lithium polyacrylate (LiPAA) after cycling to high upper cutoff voltages (4.5 V vs Li/Li). The PVDF-coated samples had a thinner CEI and twice the relative concentration of LiF and Li 2 CO 3 to Li x PO y F z species in the CEI compared to the uncoated sample. This correlated with significantly lower interfacial impedance (285 vs ~1700 Ohm-cm 2 ) and improved capacity retention between cycles of the PVDF-coated samples compared to the other binder compositions and the uncoated sample. CMC-coated samples performed worst, with a CEI comprised of greater amounts of Li x PO y F z . In addition, we find the choice of binder results in the selective protection or promotion of electrolyte reactions at the (104) surface of the 622 cathode. This suggests that the choice of binder can impact the surface chemistry and performance of high voltage cathodes and supports an avenue for interest in multifunctional binders for stabilizing the CEI.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

raogroupuiuc/yl_variantcalling

NGS analysis for mutation analysis in Yarrowia lipolytica evolved strains. Yarrowia lipolytica, an oleaginous yeast, shows promise for industrial fermentation due to its robust acetyl-CoA flux and well-developed genetic engineering tools. However, its lack of an active xylose metabolism restricts the conversion of cellulosic sugars to valuable products. To address this, metabolic engineering, and adaptive laboratory evolution (ALE) were applied to the Y. lipolytica PO1f strain, resulting in an efficient xylose-assimilating strain (XEV). Whole-genome sequencing (WGS) of the XEV followed by reverse engineering revealed that the amplification of the heterologous oxidoreductase pathway and a mutation in the GTPase-activating protein gene (YALI0B12100g) might be the primary reasons for improved xylose assimilation in the XEV strain. When a sorghum hydrolysate was used, the XEV strain showed superior xylose consumption and lipid production compared to its parental strain (X123). This study advances our understanding of xylose metabolism in Y. lipolytica and proposes effective metabolic engineering strategies for optimizing lignocellulosic hydrolysates.

Deewan, Anshu↗
DOE OSTI2019

A two-phase substrate model for enzymatic hydrolysis of lignocellulose: application to batch and continuous reactors

Abstract Background Enzymatic hydrolysis continues to have a significant projected production cost for the biological conversion of biomass to fuels and chemicals, motivating research into improved enzyme and reactor technologies in order to reduce enzyme usage and equipment costs. However, technology development is stymied by a lack of accurate and computationally accessible enzymatic-hydrolysis reaction models. Enzymatic deconstruction of cellulosic materials is an exceedingly complex physico-chemical process. Models which elucidate specific mechanisms of deconstruction are often too computationally intensive to be accessible in process or multi-physics simulations, and empirical models are often too inflexible to be effectively applied outside of their batch contexts. In this paper, we employ a phenomenological modeling approach to represent rate slowdown due to substrate structure (implemented as two substrate phases) and feedback inhibition, and apply the model to a continuous reactor system. Results A phenomenological model was developed in order to predict glucose and solids concentrations in batch and continuous enzymatic-hydrolysis reactors from which liquor is continuously removed by ultrafiltration. A series of batch experiments were performed, varying initial conditions (solids, enzyme, and sugar concentrations), and best-fit model parameters were determined using constrained nonlinear least-squares methods. The model achieved a good fit for overall sugar yield and insoluble solids concentration, as well as for the reduced rate of sugar production over time. Additionally, without refitting model coefficients, good quantitative agreement was observed between results from continuous enzymatic-hydrolysis experiments and model predictions. Finally, the sensitivity of the model to its parameters is explored and discussed. Conclusions Although the phenomena represented by the model correspond to behaviors that emerge from clusters of mechanisms, and hence a set of model coefficients are unique to the substrate and the enzyme system, the model is efficient to solve and may be applied to novel reactor schema and implemented in computational fluid dynamics (CFD) simulations. Hence, this modeling approach finds the right balance between model complexity and computational efficiency. These capabilities have broad application to reactor design, scale-up, and process optimization.

09 BIOMASS FUELS↗