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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Effective Biomass Fractionation through Oxygen-Enhanced Alkaline-Oxidative Pretreatment

The high recalcitrance of plant cell walls is an obstacle for effective chemical or biological conversion into renewable chemicals and transportation fuels. Here, we investigated the utilization of both oxygen (O 2 ) and hydrogen peroxide (H 2 O 2 ) as co-oxidants during alkalineoxidative pretreatment to improve biomass fractionation and increase enzymatic digestibility. The oxidative pretreatment of hybrid poplar was studied over a variety of conditions. Employing O 2 in addition to H 2 O 2 as a co-oxidant during the two-stage alkaline pre-extraction/coppercatalyzed alkaline hydrogen peroxide (Cu-AHP) pretreatment process resulted in a substantial improvement in delignification relative to using H 2 O 2 alone during the second-stage Cu-AHP pretreatment, leading to high overall sugar yields even at H 2 O 2 loadings as low as 2% (w/w of original biomass). The presence of H 2 O 2 , however, was both critical and synergistic. Performing analogous reactions in the absence of H 2 O 2 resulted in approximately 25% less delignification and a 30% decrease in sugar yields. The lignin isolated from this dual oxidant second stage had high aliphatic hydroxyl group content and reactivity to isocyanate, indicating that it is a promising substrate for the production of polyurethanes. To test the suitability of the isolated lignin as a source of aromatic monomers, the lignin was subjected to a sequential Bobbitt’s salt oxidation followed by formic-acid catalyzed depolymerization process. Monomer yields of approximately 17% (w/w) were obtained, and the difference in yields was not significant between lignin isolated from our Cu-AHP process with and without O 2 as a co-oxidant. Thus, the addition of O 2 did not lead to significant lignin crosslinking, a result consistent with the twodimensional heteronuclear single-quantum coherence (2D HSQC) NMR spectra of the isolated lignin.

09 BIOMASS FUELS↗
DOE OSTI2026

Evolution_and_engineering_of_pathways_for_aromatic_O-demethylation_in_Pseudomonas_putida_KT2440

Biological conversion of lignin from biomass offers a promising strategy for sustainable production of fuels and chemicals. However,aromatic compoundsderived from lignin commonly contain methoxy groups, andO-demethylation of these substrates is often a rate-limiting reaction that influences catabolic efficiency. Severalenzymefamilies catalyze aromaticO-demethylation, but they are rarely comparedin vivoto determine an optimal biocatalytic strategy. Here, two pathways for aromaticO-demethylation were compared inPseudomonas putidaKT2440. The native Rieske non-heme ironmonooxygenase(VanAB) and, separately, a heterologous tetrahydrofolate-dependentdemethylase(LigM) were constitutively expressed inP. putida, and the strains were optimized via adaptive laboratory evolution (ALE) withvanillateas a model substrate. All evolved strains displayed improved growth phenotypes, with the evolved strains harboring the native VanAB pathway exhibiting growth rates ∼1.8x faster than those harboring the heterologous LigM pathway.Enzyme kineticsandtranscriptomicsstudies investigated the contribution of selected mutations toward enhanced utilization of vanillate. The VanAB-overexpressing strains contained the most impactful mutations, including those in VanB, thereductasefor vanillateO-demethylase, PP_3494, a global regulator of vanillate catabolism, andfghA, involved in formaldehydedetoxification. These three mutations were combined into a single strain, which exhibited approximately 5x faster vanillate consumption than the wild-type strain in the first 8 h of cultivation. Overall, this study illuminates the details of vanillate catabolism in the context of two distinct enzymatic mechanisms,yielding a platform strain for efficientO-demethylation of lignin-related aromatic compounds to value-added products. This DOI contains supplementary material associated with the published manuscript.

CBI↗
NASA NTRS1972

An assessment of solar energy as a national energy resource

The applications are discussed of solar energy for thermal energy for buildings; chemical and biological conversion of organic materials to liquid, solid, and gaseous fuels; and the generation of electricity. It is concluded that if solar development programs are successful, building heating for public use is possible within 5 years, building cooling in 6 to 10 years, synthetic fuels from organic materials in 5 to 8 years, and electricity production in 10 to 15 years.

Donovan, P.↗
NASA NTRS1991

Planetary engineering

Assuming commercial fusion power, heavy lift vehicles and major advances in genetic engineering, the authors survey possible late-21st century methods of working major transformations in planetary environments. Much more Earthlike climates may be produced on Mars by generating low freezing point greenhouse gases from indigenous materials; on Venus by biological conversion of CO2 to graphite, by canceling the greenhouse effect with high-altitude absorbing fine particles, or by a sunshield at the first Lagrangian point; and on Titan by greenhouses and/or fusion warming. However, in our present state of ignorance we cannot guarantee a stable endstate or exclude unanticipated climatic feedbacks or other unintended consequences. Moreover, as the authors illustrate by several examples, many conceivable modes of planetary engineering are so wasteful of scarce solar system resources and so destructive of important scientific information as to raise profound ethical issues, even if they were economically feasible, which they are not. Global warming on Earth may lead to calls for mitigation by planetary engineering, e.g., emplacement and replenishment of anti-greenhouse layers at high altitudes, or sunshields in space. But here especially we must be concerned about precision, stability, and inadvertent side-effects. The safest and most cost-effective means of countering global warming - beyond, e.g., improved energy efficiency, CFC bans and alternative energy sources - is the continuing reforestation of approximately 2 times 107 sq km of the Earth's surface. This can be accomplished with present technology and probably at the least cost.

Pollack, James B.↗
NASA NTRS1993

Application of capillary fluid management techniques to the design of a phase separating microgravity bioreactor

Manned space missions require the development of compact, efficient, and reliable life support systems. A number of aqueous biological conversion processes are associated with bioregenerative life support systems. Vessels, or bioreactors, capable of supporting these processes in microgravity must be developed. An annular flow bioreactor has been conceived. It has the potential to incorporate containment, phase separation, gas exchange, and illumination into a single vessel. The bioreactor utilizes capillary fluid management techniques and is configured as a cylindrical tube in which a two-phase liquid-gas flow is maintained. Vanes placed around the inner perimeter enhance capillary forces and cause the liquid phase to attach and flow along the interior surface of the tube. No physical barrier is required to complete phase separation. It is shown analytically that liquid film thickness is limited only by vane geometry and that an annular flow bioreactor capable of managing 284 liters would occupy 0.7 cubic m, less than half the volume of a Spacelab experiment rack.

Finger, Barry W.↗
DOE OSTI2016

Hydrothermal Liquefaction of Wastewater Treatment Plant Solids

Feedstock cost is the greatest barrier to the commercial production of biofuels. The merits of any thermochemical or biological conversion process are constrained by their applicability to the lowest cost feedstocks. At PNNL, a recent resource assessment of wet waste feedstocks led to the identification of waste water treatment plant (WWTP) solids as a cost-negative source of biomass. WWTP solids disposal is a growing environmental concern [1, 2] and can account for up to half of WWTP operating costs. The high moisture content is well-suited for hydrothermal liquefaction (HTL), avoiding the costs and parasitic energy losses associated with drying the feedstock for incineration. The yield and quality of biocrude and upgraded biocrude from WWTP solids is comparable to that obtained from algae feedstocks but the feedstock cost is $500-1200 less per dry ton. A collaborative project was initiated and directed by the Water Environment & Reuse Foundation (WERF) and included feedstock identification, dewatering, shipping to PNNL, conversion to biocrude by HTL, and catalytic hydrothermal gasification of the aqueous byproduct. Additional testing at PNNL included biocrude upgrading by catalytic hydrotreatment, characterization of the hydrotreated product, and a preliminary techno-economic analysis (TEA) based on empirical results. This short article will cover HTL conversion and biocrude upgrading. The WERF project report with complete HTL results is now available through the WERF website [3]. The preliminary TEA is available as a PNNL report [4].

biocrude upgrading↗
DOE OSTI2020

Methods and systems for biological coal-to-biofuels and bioproducts

Methods and systems for the biological conversion of pretreated or solubilized coal or waste coal into biofuels. Coal (10) may be pretreated perhaps in a pretreatment reactor (13). Pretreated coal or even solubilized coal may be introduced into a processing reactor such as a bioreactor (16) containing a plurality of microorganisms (9) such as oleaginous microorganisms which can convert at least some of the pretreated or solubilized coal into lipids (19) or biomass (18), which then may be used directly or as a precursor for various products such as biofuels, feedstock, or the like.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2021

BETO 2021 Peer Review - Cell Free and Immobilization Technologies (CFIT)

Today, several key factors negatively impact the production of fuels and chemicals from renewable sources. Common hindrances in the biological production of biochemicals are: (1) end-product or intermediate toxicity to the microbial biocatalyst, (2) the diversion of carbon to biomass formation, and (3) co-production of undesired byproducts. A particularly attractive alternative is to eliminate the biocatalyst entirely and instead operate the desired metabolic pathways in isolation, thus circumventing the roadblocks of biological toxicity, lower yields, and lack of specificity. However, cell-free enzyme systems still suffer from low productivities owing in part to the effects of free diffusion of intermediates, lack of long term enzyme stability, cofactor cost or inefficient recycling rates, and finally, the cost of enzyme production/purification. This project represents a new effort to propose innovative and cost competitive routes to producing biochemicals from a variety of feedstocks using cell free approaches. These routes will help reduce the current risk and cost associated with classical cell free production. Cell free technologies show promise for application to the production of toxic/inhibitory products or products difficult to separate from microbial growth media and can help reduce the production barriers in multiple areas of biological conversion of feedstocks to biochemicals.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2022

Performance Advantaged Thermosets from Bioderived Amines: Benefits in Manufacturing, Performance, and End-of-Life

Biomass derived monomers can offer unique functionality, often in the forms of heteroatoms, that is not easily accessible by routine petrochemical routes. Importantly, many of these monomers offer the potential to replace the petrochemical monomers used in the manufacture of thermosets to enable expanded functionality and performance. In the present work, we leverage amine containing monomers that can be obtained via biological conversions in both epoxy and benzoxazine thermosets. These monomers have a wide degree of functionality available to them that augment the material properties. In the case of benzoxazines, monomers that contain both an amine and carboxylic acid are used and the presence of the carboxylic acid leads to an acceleration in cure kinetics and a dramatic reduction in cure temperature. For the epoxy thermosets, multifunctional amine monomers are used as a hardener and the properties of the resultant materials are found to scale with the spacing and identity between reactive centers. The amines can be further modified and reacted to produce a mixed network of triazines and epoxy-amines that enables the end-of-life degradation of these materials. Importantly, subsequent process analysis reveals that the use of bioderived amines can present dramatic reductions in both supply chain energy and GHG emissions while possessing a cost similar to their petrochemical counterparts. Overall, this work demonstrates the robust potential to use bioderived amines for performance advantaged properties.

bioderived monomers↗
DOE OSTI2023

Cell Free and Immobilization Technologies (CFIT)

Today, several key factors negatively impact the production of fuels and chemicals from renewable sources. Common hindrances in the biological production of biochemicals are: (1) end-product or intermediate toxicity to the microbial biocatalyst, (2) the diversion of carbon to biomass formation, and (3) co-production of undesired byproducts. A particularly attractive alternative is to eliminate the biocatalyst entirely and instead operate the desired metabolic pathways in isolation, thus circumventing the roadblocks of biological toxicity, lower yields, and lack of specificity. However, cell-free enzyme systems still suffer from low productivities owing in part to the effects of free diffusion of intermediates, lack of long term enzyme stability, cofactor cost or inefficient recycling rates, and finally, the cost of enzyme production/purification. This project represents a new effort to propose innovative and cost competitive routes to producing biochemicals from a variety of feedstocks using cell free approaches. These routes will help reduce the current risk and cost associated with classical cell free production. Cell free technologies show promise for application to the production of toxic/inhibitory products or products difficult to separate from microbial growth media and can help reduce the production barriers in multiple areas of biological conversion of feedstocks to biochemicals. More specifically, we are developing new technologies and routes that could be used to produce high value biochemicals such as 2,3 BDO and terpenes (among many others) from biomass derived C5/C6 sugars or lignin but also from waste byproducts such as glycerol. This project will lead to significant innovation and also lead to new concepts and rational design of pathways and enzymes. Within this project, we will develop new metabolic enzyme cascades that will represent natural or artificial combinations of enzymes to produce the desired biochemicals from a variety of feedstocks. We are also developing basic design principals for constructing synthetic metabolons, using fusion proteins and synthetic protein scaffolds, to promote substrate channeling and stability while conserving peak activity. Additionally, our efforts include a techno economic analysis (TEA) of cell free approaches to provide the sensitivities of the process to enzyme loading, activity, pH, reactor volumes, cofactor recycling rates. Finally, we are focusing on further increasing stability, operating lifetime and efficiency of the pathway enzymes by immobilization on support surfaces. We are also focus on immobilizing pathway enzymes or combinations of enzymes on several different conducting polymers and evaluate the effect on stability and operating lifetime. As more combinations become available we will conduct a more systematic study of the means of immobilizing these enzymes. This preliminary work will enable the in-depth study of cofactor recycling at these interfaces using mediators for electron transfer. Taken together, these approaches will enable process intensification, continuous operation, lower capital and separations costs and end-product flexibility, and thus has the potential to contribute significantly to BETO's goals of cost competitive biofuels and bioproducts. To date we have demonstrated 1) the conversion of pyruvate to 2,3 BDO (4 enzymes with cofactor recycling, no additional cofactors needed) at >100g/L (>3g/L/h) using our enzyme tethering approach, 2) Generated mutants of a key redox enzyme with >180- fold improvement in NADH utilization over WT to >85% of NADPH utilization. 3) Produced mevalonate at >10g/L from glucose, limonene at >10g/L from mevalonate and more than >5g/L from glucose with crude enzyme preparations and complete cofactor recycling. 4) successfully generated fully active cross-linked aggregates (CLEAs) of NOX, a cofactor-regenerating water-forming oxidase that is key to our process with increased stability 5) Engineered and identified enzymes able to use the biomimetic cofactor NMN and synthesized new synthetic cofactors.

biocatalysis↗
DOE OSTI2024

Adaptive Laboratory Evolution for Enhanced Performance of Cupriavidus Necator on Formic Acid

The threat of global warming, driven by rising carbon emissions, highlights the need to decarbonize our economy. This requires innovative solutions for managing carbon waste and its effective utilization. One promising method for CO2 capture and sequestration is the electrochemical reduction of CO2 to formic acid, a soluble C1 molecule that can be used to store carbon and energy, and as a feedstock for biological conversion. Cupriavidus necator H16, a soil bacterium capable of consuming and growing on formic acid as its sole carbon and energy source, is well positioned to upgrade CO2-derived formic acid into platform chemicals and fuel precursors. To improve the performance of C. necator on formic acid, adaptive laboratory evolution (ALE), a proven tool for improving microbial fitness, has been conducted using continuous pH-stat bioreactors. The system works on the basis that consumption of formic acid raises the pH and triggers the addition of more formic acid to maintain the pH (in this case 6.7), such that formic acid is provided at the same rate as it is consumed. This system has been coupled with level control to achieve continuous fermentation where cells acquiring mutations that improve growth on formic acid become more abundant in the population, from which they can be isolated and characterized. During developmental experiments it was discovered that formic acid accumulated to inhibitory levels. It was determined that the nitrogen source, ammonium hydroxide, must be tailored to the carbon consumption to avoid formic acid accumulation. The ALE ran in three lineages for approximately 3000 hours and more than 500 generations. Evolved isolates obtained from each lineage demonstrated an increase in growth rate in conjunction with improve formate utilization compared to the parental strain when evaluated in pH-stat bioreactors. The isolates with improved performance were then subjected to whole genome sequencing to identify potentially causative mutations. Mutations in several key genes across different lineages have been found and will be evaluated individually and in combination to identify those that improve growth on formic acid. Incorporating these mutations into production strains has the potential to greatly improve formic acid conversion and further industrial decarbonization.

adaptive laboratory evolution↗
DOE OSTI2023

Meta-analysis of biogas upgrading to renewable natural gas through biological CO 2 conversion

Biogas upgrading through CO 2 conversion by hydrogenotrophic methanogenesis is receiving an increasing attention worldwide because of the demand for renewable natural gas. Herein, a holistic and statistical study of the operation conditions, driving forces, performances, and potential implementation of biogas upgrading via biological CO 2 conversion was conducted. Based on a systematic review and meta-analysis of 46 existing publications that were selected from 1475 papers, we have compiled a global dataset of CO 2 bioconversion biogas upgrading, encompassing 308 study cases. Subsequently, we employed a rigorous analytical framework incorporating data processing and mixed effects linear regression analysis to examine the dataset. This analysis revealed a significant positive relationship between the H 2 :CO 2 ratio and the methane percentage in the upgraded biogas when using the study as a random effect. Furthermore, we performed meta-analysis on observations taken when the ratio was close to 4:1 and found that ex situ reactors (91.93% [88.11%, 95.75%]) can perform better than in situ reactors (84.74% [80.69%, 88.80%]). No evidence of differential performance was found based on the present dataset between different temperature regimes or operation modes. Furthermore, those findings establish a database that will contribute to a deeper understanding of the biogas upgrading via biological CO 2 conversion.

Biogas upgrading↗
DOE OSTI2022

Synthetic Microbial Consortium for Biological Breakdown and Conversion of Lignin

The plant polymer lignin is the most abundant renewable source of aromatics on the planet and conversion of it to valuable fuels and chemicals is critical to the economic viability of a lignocellulosic biofuels industry and to meeting the DOE’s 2022 goal of $\$2.50$/gallon mean biofuel selling price. Presently, there is no efficient way of converting lignin into valuable commodities. Current biological approaches require mixtures of expensive ligninolytic enzymes and engineered microbes. This project was aimed at circumventing these problems by discovering commensal relationships among fungi and bacteria involved in biological lignin utilization and using this knowledge to engineer microbial communities capable of converting lignin into renewable fuels and chemicals. Essentially, we aimed to learn from, mimic and improve on nature. We discovered fungi that synergistically work together to degrade lignin, engineered fungal systems to increase expression of the required enzymes and engineered organisms to produce products such as biodegradable plastics precursors.

09 BIOMASS FUELS↗
DOE OSTI2025

Characterization of Coal Seam Produced Water from the Appalachian Basin: Geochemistry, Microbiology, and Biocatalyst Development for Biological CO 2 Conversion

To enhance domestic energy repositories, it is necessary to develop carbon utilization technologies to repurpose unused carbon sources, and/or enhance the economic viability and carbon conversion efficiency of current technologies. To this end we have developed a biocatalyst, enriched from coal seam produced water, to convert gaseous and liquid C1 compounds (e.g. CO 2 , bicarbonate, formate, and/or methanol) into acetate, a C2 organic acid with a projected global market size of $\$$32.4 billion USD by 2030.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2024

Machine learning-aided inverse design for biogas upgrading through biological CO 2 conversion

The biogas upgrading process through bioconversion of CO 2 to CH 4 by hydrogenotrophic methanogens is an attractive strategy for energy decarbonation. Many studies have optimized operational parameters to improve key performance indicators such as CH 4 % and H 2 utilization efficiency. However, inconsistent laboratory conditions make it challenging to compare results. Existing models for analyzing operating conditions can only assess the impact of individual conditions and lack the ability to simultaneously optimize multiple conditions. To address this, two XGBoost models were built with R 2 of 0.779 and 0.903 with data collected from literatures and were embedded into multi-objective partitive swarm optimization algorithm to optimal operating conditions. Predictions were compared with experimental validations under optimized conditions, revealing an 8.50% and 2.95% relative error in CH 4 % and H 2 conversion rate, respectively. This approach streamlines biogas upgrading processes, offering a data-driven solution to enhance efficiency and consistency in the pursuit of sustainable methane production.

Biogas upgrading↗
DOE OSTI2019

Identifying and creating pathways to improve biological lignin valorization

Biological lignin valorization to fuels and value-added chemicals enables sustainable and economic biorefineries. Even though significant progress has been made, several major challenges arose due to high recalcitrance and heterogeneity of lignin, which needs to be addressed to improve lignin processing. This work demonstrates an overview of biological lignin conversion and its regulation from a metabolic engineering and systems biology viewpoint. Biological lignin valorization includes three stages: lignin depolymerization, aromatics degradation, and target product biosynthesis. Ligninolytic microorganisms have an extensive enzymatic toolbox to break down the lignin and convert heterogeneous lignin derivatives to central intermediates, such as protocatechuate or catechol, through a peripheral pathway. These intermediates undergo ring cleavage via the β-ketoadipate pathway and are ultimately transformed into metabolites by yielding acetyl-CoA for internal product biosynthesis, such as triacylglycerols, polyhydroxyalkanoates, etc. Bioprospecting will expand the knowledge base of ligninolytic microbial communities, strains, and enzymes to facilitate the understanding of aromatics metabolism. Systems biology analyses achieve an understanding of molecular and systems-level degradation mechanisms and metabolic pathways of lignin and aromatics. By identifying these mechanisms, synthetic biology provides promising approaches to create the lignin conversion pathways and engineer ligninolytic strains suitable as potential hosts for lignin conversion. Techno-economic analysis of biological lignin upgrading to coproducts in biorefineries will guide the implementation of lignin valorization by mitigating technical risk for scale-up and improving the profitability of biorefinery. Through improving the understanding of biological lignin valorization, it should be possible to create biological lignin valorization route to effectively produce value-added products from lignin.

09 BIOMASS FUELS↗
DOE OSTI2017

Base-Catalyzed Depolymerization of Solid Lignin-Rich Streams Enables Microbial Conversion

Lignin valorization offers significant potential to enhance the economic viability of lignocellulosic biorefineries. However, because of its heterogeneous and recalcitrant nature, conversion of lignin to value-added coproducts remains a considerable technical challenge. Here, we employ base-catalyzed depolymerization (BCD) using a process-relevant solid lignin stream produced via deacetylation, mechanical refining, and enzymatic hydrolysis to enable biological lignin conversion. BCD was conducted with the solid lignin substrate over a range of temperatures at two NaOH concentrations, and the results demonstrate that the lignin can be partially extracted and saponified at temperatures as low as 60 degrees C. At 120 °C and 2% NaOH, the high extent of lignin solubility was accompanied by a considerable decrease in the lignin average molecular weight and the release of lignin-derived monomers including hydroxycinnamic acids. BCD liquors were tested for microbial growth using seven aromatic-catabolizing bacteria and two yeasts. Three organisms (Pseudomonas putida KT2440, Rhodotorula mucilaginosa, and Corynebacterium glutamicum) tolerate high BCD liquor concentrations (up to 90% v/v) and rapidly consume the main lignin-derived monomers, resulting in lignin conversion of up to 15%. Furthermore, as a proof of concept, muconic acid production from a representative lignin BCD liquor was demonstrated with an engineered P. putida KT2440 strain. Our results highlight the potential for a mild lignin depolymerization process to enhance the microbial conversion of solid lignin-rich biorefinery streams.

09 BIOMASS FUELS↗
DOE OSTI2019

Opportunities and Challenges for Catalysis in Carbon Dioxide Utilization

The environmental and societal consequences of the increasing levels of carbon dioxide in our atmosphere are among the most significant challenges society currently faces. Carbon dioxide utilization, in which carbon dioxide is either used directly or converted into more valuable products, is likely to be one component of a broad strategy to reduce carbon dioxide emissions, a challenge that will require both technological and policy changes. Here, catalysis is crucial to the successful conversion of carbon dioxide into value-added products. Furthermore, we provide a review on chemical and biological systems for carbon dioxide conversion directed toward the readers of ACS Catalysis, which focuses on providing a general perspective on the field, rather than technical details. We discuss both challenges related to the conversion of carbon dioxide into specific products such as carbon monoxide, formic acid, methanol, methane, ethylene, fuels, carboxylic acids, and polymers as well as general challenges for the field. We also compare and contrast different methods for carbon dioxide conversion, for example homogeneous versus heterogeneous catalysis or photosynthetic versus nonphotosynthetic biological conversion, and highlight areas where one approach may have advantages over another. In a concluding section, we identify problems related to carbon dioxide conversion that will need to be addressed for technology to be both viable and reduce carbon dioxide emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗