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All sources NASA NTRS DOE OSTI

DOE OSTI2018

Fermentation of dihydroxyacetone by engineered Escherichia coli and Klebsiella variicola to products

Methane can be converted to triose dihydroxyacetone (DHA) by chemical processes with formaldehyde as an intermediate. Carbon dioxide, a by-product of various industries including ethanol/butanol biorefineries, can also be converted to formaldehyde and then to DHA. DHA, upon entry into a cell and phosphorylation to DHA-3-phosphate, enters the glycolytic pathway and can be fermented to any one of several products. However, DHA is inhibitory to microbes due to its chemical interaction with cellular components. Fermentation of DHA to d -lactate by Escherichia coli strain TG113 was inefficient, and growth was inhibited by 30 g⋅L −1 DHA. An ATP-dependent DHA kinase from Klebsiella oxytoca (pDC117d) permitted growth of strain TG113 in a medium with 30 g⋅L −1 DHA, and in a fed-batch fermentation the d -lactate titer of TG113(pDC117d) was 580 ± 21 mM at a yield of 0.92 g⋅g −1 DHA fermented. Klebsiella variicola strain LW225, with a higher glucose flux than E. coli , produced 811 ± 26 mM d -lactic acid at an average volumetric productivity of 2.0 g −1 ⋅L −1 ⋅h −1 . Fermentation of DHA required a balance between transport of the triose and utilization by the microorganism. Using other engineered E. coli strains, we also fermented DHA to succinic acid and ethanol, demonstrating the potential of converting CH 4 and CO 2 to value-added chemicals and fuels by a combination of chemical/biological processes.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2019

Life Cycle Impact Assessment of Polylactic Acid (PLA) Produced from Sugarcane in Thailand

In this study we provide up-to-date cradle-to-gate information on the environmental footprint of polylactic acid (PLA) produced in Thailand at commercial scale, covering emerging topics such as water footprint and direct land use change. The enormous potential to further reduce the environmental impacts of PLA through improvements in feedstock production as well as in the PLA manufacturing process is also demonstrated. Life cycle assessment (LCA) is performed according to the ISO 14040/44 standard methodology. The 16 environmental impact categories from ILCD 2011 Midpoint + were considered for the hotspot analysis. As primary data actual industrial data were used for the sugar production, lactic acid production (Corbion) and PLA production (Total Corbion PLA), including various recently developed process insights. The agricultural feedstock production and the manufacturing process of PLA from sugar contributed most to the LCA impacts of PLA production. The sugarcane crop production particularly affected the environmental impact categories analyzed, including global warming potential (GWP), water, eutrophication, acidification, particulate matter and, inevitably, land use. However, when combined with the results of a sustainability risk assessment study, it becomes clear that land use and water-related impacts represent a low risk for the feedstock-sourcing area. The environmental impact categories of PLA manufacturing are mostly linked to energy and chemicals usage. Improvements in the environmental performance of PLA can be achieved through improvements in the sugarcane farming practices, higher efficiency bagasse boilers at the sugarmill, reduced usage of auxiliary chemicals and increased usage of renewable energy in the conversion process of sugar to PLA. From a cradle-to-gate perspective, considering the uptake of carbon dioxide in the PLA molecule, the GWP is 501 kg CO{sub 2} eq/ton PLA.

09 BIOMASS FUELS↗

DOE OSTI2021

Ad-apoptin inhibits glycolysis, migration and invasion in lung cancer cells targeting AMPK/mTOR signaling pathway

Ad-apoptin is a recombinant oncolytic adenovirus constructed by our laboratory that can express apoptin. It can selectively kill tumor cells without damaging normal cells. This study investigated the effects of Ad-apoptin on glycolysis, migration and invasion of non-small cell lung cancer. Cell viability and apoptosis were detected by CCK-8 and flow cytometry, respectively. Glycolysis was investigated by glucose consumption, lactic acid production and glycolytic key enzyme protein levels. Migration and invasion were evaluated via wound healing, transwell assays and epithelial-mesenchymal transition (EMT) protein levels. The interaction between apoptin and AMPK was detected by Co-IP. A nude mice tumor model was established to investigate the anti-cancer role of Ad-apoptin in vivo. The results showed that Ad-apoptin inhibits cell viability and induces apoptosis of A549 and NCI–H23 cells. Ad-apoptin can reduce the glucose uptake and lactic production in lung cancer cells, and reduce the expression of related glycolysis-limiting enzymes. At the same time, Ad-apoptin inhibited the migration and invasion of lung cancer. Immunoprecipitation showed that apoptin and AMPK could interact directly. Moreover, knockdown of AMPK significantly attenuated the inhibitory effect of Ad-apoptin on glycolysis, migration and invasion of A549 and NCI–H23 cells. Ad-apoptin can inhibit the growth of tumors in nude mice. Compared with the control group, Ad-apoptin had a significant inhibitory effect on AMPK knockdown tumors. The immunohistochemical results of tumor tissues were consistent with those in vitro. Collectively, Ad-apoptin targets AMPK and inhibits glycolysis, migration and invasion of lung cancer cells through the AMPK/mTOR signaling pathway. This suggests that Ad-apoptin may have therapeutic potential for lung cancer by targeting AMPK activation.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2016

PLA recycling by hydrolysis at high temperature

In this work the process of PLA hydrolysis at high temperature was studied, in order to evaluate the possibility of chemical recycling of this polymer bio-based. In particular, the possibility to obtain the monomer of lactic acid from PLA degradation was investigated. The results of some preliminary tests, performed in a laboratory batch reactor at high temperature, are presented: the experimental results show that the complete degradation of PLA can be obtained in relatively low reaction times.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1988

Dynamic cell culture system: a new cell cultivation instrument for biological experiments in space

The prototype of a miniaturized cell cultivation instrument for animal cell culture experiments aboard Spacelab is presented (Dynamic cell culture system: DCCS). The cell chamber is completely filled and has a working volume of 200 microliters. Medium exchange is achieved with a self-powered osmotic pump (flowrate 1 microliter h-1). The reservoir volume of culture medium is 230 microliters. The system is neither mechanically stirred nor equipped with sensors. Hamster kidney (Hak) cells growing on Cytodex 3 microcarriers were used to test the biological performance of the DCCS. Growth characteristics in the DCCS, as judged by maximal cell density, glucose consumption, lactic acid secretion and pH, were similar to those in cell culture tubes.

NASA Program Flight↗

DOE OSTI2021

Microalgae Conversion to Biofuels and Biochemical via Sequential Hydrothermal Liquefaction (SEQHTL) and Bioprocessing: 2020 State of Technology

A preliminary techno-economic analysis (TEA) was developed for the fiscal year 2020 state of technology (SOT) assessment to evaluate the benefits and risks for a large-scale microalga hydrothermal liquefaction (HTL) system based on most recent testing results. The focus of the study is directed toward the conversion system, which consists of five processes: two-stage sequential HTL (SEQHTL), biocrude upgrading to final fuels, bioprocessing for co-product generation, hydrogen generation, and steam cycle. In this system, algae biomass with corn stover supplement during the lower algae productivity seasons (winter, fall, and spring) to match the maximum algae seasonal production rate in summer is employed to maintain a constant plant capacity in all the seasons. Algae only (summer season) or algae/corn stover blended feedstock (other seasons) are sent to a two-stage SEQHTL process. In stage I, the carbohydrates in the feedstock are extracted and separated from the residual solid. The residual solid from stage I is further converted to biocrude in the SEQHTL stage II step. The biocrude is upgraded to final fuel products in an upgrading process. The extract stream from HTL stage I is sent to the bioprocessing section for co-product generation via fermentation of carbohydrate. Lactic acid (LA) is assumed to be the co-product based on current bioprocessing testing results.

09 BIOMASS FUELS↗

DOE OSTI2017

Improving the circular economy via hydrothermal processing of high-density waste plastics

Highlights: • High-density plastics are susceptible to supercritical hydrothermal processing. • Plastics convert into their monomers and value-added chemical compounds. • Nearly 100% conversion of PC into synthetic crude oil. • Degradation of PET and PBT yields high quantity of their monomer terephtalic acid. • Hydrothermal processing is a prospective technology for unrecyclable waste plastics. - Abstract: Rising environmental concerns on climate changes are causing an increasing attention on circular economies. The plastic economy, in particular, is in focus due to the accelerating consumption of plastics, mainly derived from virgin feedstock, combined with the lack of plastic recycling strategies. This work presents a novel outlook on the potential of using supercritical hydrothermal processing of waste plastic fractions for tertiary recycling. The study investigates hydrothermal processing of nine different, high-density types of plastics into original resin monomers and other value-added chemical compounds. The outlook presents conversion yields, carbon balances, and chemical details on the products obtained. It is found that all the investigated resins are prone to hydrothermal treatment, and that high yields of monomers and high value compounds (up to nearly 100%), suitable for chemicals and fuels applications, can be obtained. For instance, for polycarbonate, styrene-butadiene, poly(lactic acid), poly(ethylene terephthalate), and poly(butylene terephthalate), original monomeric compounds can be reclaimed for manufacturing new resins. The promising results presented demonstrate that hydrothermal processing of high-density plastics is a prospective technology for increasing the circularity of the plastic economy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

PGC1α regulates mitochondrial oxidative phosphorylation involved in cisplatin resistance in ovarian cancer cells via nucleo-mitochondrial transcriptional feedback

Mitochondria play an important role in effective cell energy production and cell survival under stress conditions, such as treatment with chemotherapeutic drugs. Mitochondrial biogenesis is increased in ovarian cancer tissues, which is accompanied by alteration of mitochondrial energy metabolism, structure, and dynamics. These factors are involved in tumorigenesis and apoptosis resistance, highlighting the role of mitochondria in resisting cisplatin toxicity. Cisplatin-resistant ovarian cancer cells are dependent on mitochondrial OXPHOS for energy supply, and intracellular PGC1α-mediated mitochondrial biogenesis levels are increased in this cell line, indicating the important role of mitochondrial oxidative phosphorylation in cisplatin resistance. As PGC1α is a key molecule for integrating and coordinating nuclear DNA and mitochondrial DNA transcriptional machinery, an investigation into the regulatory mechanism PGC1α in mitochondrial energy metabolism via transcription may provide new clues for solving chemotherapy resistance. In the present study, it was demonstrated that inhibiting the expression of PGC1α decreased nuclear and mitochondrial DNA transcription factor expression, leading to increased lactic acid production and decreased cellular oxygen consumption and mitochondrial oxidative phosphorylation. Furthermore, mitochondrial stress-induced ROS production, as a feedback signal from mitochondria to the cell nucleus, increased PGC1α expression in SKOV3/DDP cells, which was involved in mitochondrial oxidative phosphorylation regulation. Collectively, the present study provides evidence that PGC1α-mediated nuclear and mitochondrial transcription feedback regulates energy metabolism and is involved in ovarian cancer cells escaping apoptosis during cisplatin treatment.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2014

Fabrication of micro-hollow fiber by electrospinning process in near-critical carbon dioxide

Electrospinning is a simple technique that has gained much attention because of its capability and feasibility in the fabrication of large quantities of fibers from polymer with diameters ranging in nano-microscale. These fibers provided high surface area to volume ratios, and it was of considerable interest for many applications, such as nanoparticle carriers in controlled release, scaffolds in tissue engineering, wound dressings, military wear with chemical and biological toxin-resistance, nanofibrous membranes or filters, and electronic sensors. Recently there has been a great deal of progress in the potential applications of hollow fibers in microfluids, photonics, and energy storage. In this work, electrospinning was conducted under high-pressure carbon dioxide (CO{sub 2}) to reduce the viscosity of polymer solution. The experiments were conducted at 313 K and ∼8.0 MPa. Polymer solution containing 5 wt% polymers which prepared in dichloromethane (DCM) with polyvinylpyrrolidone (PVP) to poly-L-lactic acid (PLLA) ratio 80:20 was used as a feed solution. The applied voltage was 15 kV and the distance of nozzle and collector was 8 cm. The morphology and structure of the fibers produced were observed using scanning electron microscopy (SEM). Under pressurized CO{sub 2}, PVP electrospun was produced without bead formation with diameter ranges of 608.50 - 7943.19 nm. These behaviors hold the potential to considerably improve devolatilization electrospinning processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Exploiting chitosan to improve the interface of nanocellulose reinforced polymer composites

Cellulose nanofibrils (CNFs) have been widely used as a nanofiller for polymer composite reinforcement due to their excellent mechanical properties. However, CNF is produced in water and needs to be dried prior to use in composite materials. The presence of hydroxyl groups on the surface of CNF creates strong hydrogen bonding that makes it difficult and costly to dry. Additionally, the hydrophilicity at the fiber surface results in agglomeration of CNFs within many polymer matrices. In this study, chitosan (CS) was co-precipitated with CNF to produce a dual-bonding filler for use in poly (lactic acid) (PLA) composites. CS promotes improved interfacial interaction within the polymer matrix by forming strong hydrogen bonds with the CNF and potential covalent bonds with the PLA. Finally, the results confirmed that the addition of a small amount of CS significantly improved the mechanical properties compared to PLA + CNF composites and neat PLA. The detailed study of the PLA + CNF/CS composites reveals the synergetic effect of the hydrogen and covalent bonding mechanism for PLA reinforcement.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2019

Abiotic Hydrolysis and Compostability of Blends Based on Cassava Starch and Biodegradable Polymers

When associated with polymer blends, starch may improve the biodegradability and compostability of other materials. The objectives of this work were to evaluate the abiotic hydrolysis and the composting process of films obtained from polymer blends between thermoplastic starch (TPS) and three other biodegradable polymers: poly[(butylene adipate)- co -(terephthalate)] (PBAT), poly(lactic acid) (PLA) and polyvinyl alcohol (PVA). PVA/TPS stood out as the most homogeneous blend and the one that showed the highest weight loss, with 46.21% of its initial weight remaining after abiotic hydrolysis tests. On the other hand, PBAT/TPS and PLA/TPS underwent more drastic and rapid degradation during composting in contrast to PVA/TPS. They became very fragmented after 21 days of composting, while the PVA/TPS was visually modified but remained unbroken until day 70. No blend sample exerted negative effects on the quality of the compost.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Atomic and molecular layer deposition for surface modification

Atomic and molecular layer deposition (ALD and MLD, respectively) techniques are based on repeated cycles of gas–solid surface reactions. A partial monolayer of atoms or molecules is deposited to the surface during a single deposition cycle, enabling tailored film composition in principle down to molecular resolution on ideal surfaces. Typically ALD/MLD has been used for applications where uniform and pinhole free thin film is a necessity even on 3D surfaces. However, thin – even non-uniform – atomic and molecular deposited layers can also be used to tailor the surface characteristics of different non-ideal substrates. For example, print quality of inkjet printing on polymer films and penetration of water into porous nonwovens can be adjusted with low-temperature deposited metal oxide. In addition, adhesion of extrusion coated biopolymer to inorganic oxides can be improved with a hybrid layer based on lactic acid. - Graphical abstract: Print quality of a polylactide film surface modified with atomic layer deposition prior to inkjet printing (360 dpi) with an aqueous ink. Number of printed dots illustrated as a function of 0, 5, 15 and 25 deposition cycles of trimethylaluminum and water. - Highlights: • ALD/MLD can be used to adjust surface characteristics of films and fiber materials. • Hydrophobicity after few deposition cycles of Al{sub 2}O{sub 3} due to e.g. complex formation. • Same effect on cellulosic fabrics observed with low temperature deposited TiO{sub 2}. • Different film growth and oxidation potential with different precursors. • Hybrid layer on inorganic layer can be used to improve adhesion of polymer melt.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Formulation of Green Particulate Composites from PLA and PBS Matrix and Wastes Deriving from the Coffee Production

Particulate composites based on poly(lactic acid) and poly(butylene succinate) biopolymers have been formulated. Silver skin, the by-product derived from the roasting of coffee beans, has been used as a filler up to a 30 wt% of loading. The microstructure, crystallinity, thermal stability, mechanical properties and water absorption of the derived composites have been investigated. Data so far collected underline that a trade-off of the mechanical properties can be obtained by adding the filler, while the overall amount of crystallinity remains constant. Up to the highest filler content, moisture uptake follows a Fichian behaviour while the value of the contact angle is slightly increased by modification. Thus, silver skin, which actually is used for fuel or soil fertilization, finds here a different environmentally friendly valorization into the field of biocomposites.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Biopolymer foams - Relationship between material characteristics and foaming behavior of cellulose based foams

Biopolymers are becoming increasingly important to both industry and consumers. With regard to waste management, CO{sub 2} balance and the conservation of petrochemical resources, increasing efforts are being made to replace standard plastics with bio-based polymers. Nowadays biopolymers can be built for example of cellulose, lactic acid, starch, lignin or bio mass. The paper will present material properties of selected cellulose based polymers (cellulose propionate [CP], cellulose acetate butyrate [CAB]) and corresponding processing conditions for particle foams as well as characterization of produced parts. Special focus is given to the raw material properties by analyzing thermal behavior (differential scanning calorimetry), melt strength (Rheotens test) and molecular weight distribution (gel-permeation chromatography). These results will be correlated with the foaming behavior in a continuous extrusion process with physical blowing agents and underwater pelletizer. Process set-up regarding particle foam technology, including extrusion foaming and pre-foaming, will be shown. The characteristics of the resulting foam beads will be analyzed regarding part density, cell morphology and geometry. The molded parts will be tested on thermal conductivity as well as compression behavior (E-modulus, compression strength)

36 MATERIALS SCIENCE↗

DOE OSTI2016

Potentiodynamic studies of Ni-P-TiO{sub 2} nano-composited coating on the mild steel deposited by electroless plating method

Now a days, corrosion studies are important for reducing the wastage of metals. The importance of corrosion studies is two folds i.e. first is economic, including the reduction of material losses resulting from the wasting away or sudden failure of materials and second is conservation Electroless process is an autocatalytic reduction method in which metallic ions are reduced in the solution. Nanocomposite coatings of Ni-P-TiO{sub 2} on mild steel are deposited by varying volume of TiO{sub 2} nano-powder by electroless method from Ni-P plating bath containing Nickel Sulphate as a source of nickel ions, sodium hypophosphite as the reducing agent, lactic acid as a complexing agents and TiO{sub 2} nano powder. Electroless Ni-P-TiO{sub 2} coating have been widely used in the chemical process industries, mechanical industries, electronic industries and chloroalkali industries due to their excellent corrosion with mechanical properties. In the present work, deposition of Ni-P alloy coating and Ni-P-TiO{sub 2} nanocomposited coatings were done on the mild steel and corrosion properties were studied with Potentio-dynamic polarization measurements method in 3.5 wt% sodium chloride solution. It showed in the experiments that Ni-P-TiO{sub 2} nanocomposited coating has better corrosion resistance as comparedthan Ni-P alloy coating. Morphological studies were done by field emission scanning electron microscopy (FESEM), energy–dispersive analysis of X-ray (EDAX) and X-ray diffraction (XRD). These studies confirmed the deposition of Ni-P alloy coating and Ni-P-TiO{sub 2} nanocomposited coating.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Comparative genomics of Fructobacillus spp. and Leuconostoc spp. reveals niche-specific evolution of Fructobacillus spp.

In this study, Fructobacillus spp. in fructose-rich niches belong to the family Leuconostocaceae . They were originally classified as Leuconostoc spp., but were later grouped into a novel genus, Fructobacillus , based on their phylogenetic position, morphology and specific biochemical characteristics. The unique characters, so called fructophilic characteristics, had not been reported in the group of lactic acid bacteria, suggesting unique evolution at the genome level. Here we studied four draft genome sequences of Fructobacillus spp. and compared their metabolic properties against those of Leuconostoc spp. As a result, Fructobacillus species possess significantly less protein coding sequences in their small genomes. The number of genes was significantly smaller in carbohydrate transport and metabolism. Several other metabolic pathways, including TCA cycle, ubiquinone and other terpenoid-quinone biosynthesis and phosphotransferase systems, were characterized as discriminative pathways between the two genera. The adhE gene for bifunctional acetaldehyde/alcohol dehydrogenase, and genes for subunits of the pyruvate dehydrogenase complex were absent in Fructobacillus spp. The two genera also show different levels of GC contents, which are mainly due to the different GC contents at the third codon position. In conclusion, the present genome characteristics in Fructobacillus spp. suggest reductive evolution that took place to adapt to specific niches.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2018

Biodegradation in Soil of PLA/PBAT Blends Compatibilized with Chain Extender

This paper presents a study of biodegradation, in soil, of samples of poly(butylene adipate-co-terephthalate)(PBAT), poly(lactic acid) (PLA) and blends of these materials prepared in torque rheometer with the addition of a chain extender. Film samples of these materials were buried in soil under controlled laboratory conditions. The degraded samples were regularly taken from soil and analyzed by visual inspection, size exclusion chromatography, differential scanning calorimetry and infrared spectroscopy. Respirometry biodegradation tests were conducted to assess samples mineralization degree. Blends showed higher degree of crystallinity compared to pure polymers. Crystallinity degree enhanced during the biodegradation process in all samples, being able to causing the samples to degrade slowly. The study showed the great complexity of the biodegradation process of PLA and PBAT blends when compatibilized with a chain extender. The biodegradation rate showed different results depending on the characteristic applied to evaluate it: visual, molecular weight or mineralization. The chain extender had strong influence in PBAT and blends degradation, slowing the process as observed by the variation of molecular weight and carbonyl index. Blends showed an intermediate behavior compared to the original polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Aerobic oxidation of glycerol catalyzed by M salts of PMo 12 O 40 3- (M = K + , Zn 2+ , Cu 2+ , Al 3+ , Cr 3+ , Fe 3+ )

Glycerol is a co-product in the manufacture of biodiesel from vegetable oil and animal fat. A significant increase in biodiesel production results in adramatic overproduction of glycerol. The oxidation of glycerol to lactic acid (LA) by O 2 is considered to be a promising technology to increase the value of glycerol. Studies on the fundamental reaction mechanism vary for different catalytic systems. Here in this work we have chosen Keggin polyoxometalates (POMs) as an exemplary family of water-soluble hydrolytically and oxidatively-stable, fully-inorganic complexes with transition-metal and non-transition-metal counter-cations (M in the formula, MPMo 12 O 40 , where M = H + , K + , Zn 2+ , Cu 2+ , Al 3+ , Cr 3+ , Fe 3+ in appropriate number to counterbalance the 3- charge of PMo 12 O 40 3- ). Reactions involving hydrogen peroxide, an intermediate during glycerol oxidation, produce free radicals. A kinetic analysis reveals that the radical chain length under typical conditions is about 20–30. After minimal optimization, the yield of LA was 88% at glycerol conversion > 97% (1.0 M aqueous solution of glycerol, 4.0 mM of the Al salt of PMo 12 O 40 3- , henceforth “AlPMo”, 10 bar O 2 at 60 °C, reaction time 6.0 h).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗