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72 records · Page 4

All sources NASA NTRS DOE OSTI

DOE OSTI2021

Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes

Hierarchical self-assembly leading to organized supramolecular structures across multiple length scales has been of great recent interest. Earlier work from our laboratory reported the complexation of peptide amphiphile (PA) supramolecular polymers with oppositely charged polyelectrolytes into a single solid membrane at a macroscopic interface. We report here the formation of bulk gels with many internal interfaces between the covalent and supramolecular polymer components formed by the rapid chaotic mixing of solutions, one containing negatively charged PA nanofibers and the other the positively charged biopolymer chitosan. We found that formation of a contact layer at the interface of the solutions locks the formation of hydrogels with lamellar microstructure. The nanofiber morphology of the supramolecular polymer is essential to this process since gels do not form when solutions of supramolecular assemblies form spherical micelles. Here, we found that rheological properties of the gels can be tuned by changing the relative amounts of each component. Furthermore, both positively and negatively charged proteins are easily encapsulated within the contact layer of the gel, which provides an interesting biomedical function for these systems.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Persistent polyamorphism in the chiton tooth: From a new biomineral to inks for additive manufacturing

Engineering structures that bridge between elements with disparate mechanical properties are a significant challenge. Organisms reap synergy by creating complex shapes that are intricately graded. For instance, the wear-resistant cusp of the chiton radula tooth works in concert with progressively softer microarchitectural units as the mollusk grazes on and erodes rock. Herein, we focus on the stylus that connects the ultrahard and stiff tooth head to the flexible radula membrane. Using techniques that are especially suited to probe the rich chemistry of iron at high spatial resolution, in particular synchrotron Mössbauer and X-ray absorption spectroscopy, we find that the upper stylus of Cryptochiton stelleri is in fact a mineralized tissue. Remarkably, the inorganic phase is nano disperse santabarbaraite, an amorphous ferric hydroxyphosphate that has not been observed as a biomineral. The presence of two persistent polyamorphic phases, amorphous ferric phosphate and santabarbaraite, in close proximity, is a unique aspect that demonstrates the level of control over phase transformations in C. stelleri dentition. The stylus is a highly graded material in that its mineral content and mechanical properties vary by a factor of 3 to 8 over distances of a few hundred micrometers, seamlessly bridging between the soft radula and the hard tooth head. Furthermore, the use of amorphous phases that are low in iron and high in water content may be key to increasing the specific strength of the stylus. Finally, we show that we can distill these insights into design criteria for inks for additive manufacturing of highly tunable chitosan-based composites.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Driving macro-scale transformations in three-dimensional-printed biopolymers through controlled induction of molecular anisotropy at the nanoscale

Motivated by the need to harness the properties of renewable and biodegradable polymers for the design and manufacturing of multi-scale structures with complex geometries, we have employed our additive manufacturing platform that leverages molecular self-assembly for the production of metre-scale structures characterized by complex geometries and heterogeneous material composition. As a precursor material, we used chitosan, a chemically modified form of chitin, an abundant and sustainable structural polysaccharide. We demonstrate the ability to control concentration-dependent crystallization as well as the induction of the preferred orientation of the polymer chains through the combination of extrusion-based robotic fabrication and directional toolpathing. Anisotropy is demonstrated and assessed through high-resolution micro-X-ray diffraction in conjunction with finite element simulations. Using this approach, we can leverage controlled and user-defined small-scale propagation of residual stresses to induce large-scale folding of the resulting structures.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Antioxidant Activity, Microbiological Quality, and Acceptability of Spontaneously Fermented Shrimp Sausage (Litopenaeus vannamei)

Fermented shrimp sausages are prepared spontaneously with Litopenaeus vannamei as raw material. Shrimp is one of the marine sources with rich chitosan as bioactive compounds, antioxidants, vitamin E, and probiotic lactic acid bacteria (LAB) produced by fermentation processes. This study aimed to analyze the variations in antioxidant activity, vitamin E content, total LAB, total pathogenic bacteria, pH, and acceptability of shrimp sausage produced at different fermentation times. A completely randomized experimental design study was performed using four levels of exposure time, including control (0 days), 1, 2, and 3 days. The treatment was conducted spontaneously with 1.2% salt concentration, a drying temperature of 50°C for 3 h, and fermentation at 35°C. The evaluated parameters included the antioxidant activity measured with the radical 2,2-azino-bis (3-ethylbenzothiazoline-6-sulphonic acid) method, vitamin E levels by high-performance liquid chromatography, total LAB with total plate count, and Escherichia coli bacteria by the most probable number method. Salmonella sp. and Staphylococcus aureus were estimated by the identification method. A pH meter was used to assess acidity, and hedonic organoleptic testing was performed for taste, aroma, color, and texture. The results show significant differences in antioxidant activity, vitamin E, and shrimp sausage acceptability at varied fermentation times p ≤ 0.05 . However, the best formulation was obtained with the first-day fermented shrimp sausage, as shown by its bioactive content and the level of acceptability.

Afifah, Diana N.↗

DOE OSTI2022

Alaska Ocean Cluster (Final CTAP2.0 Report)

Sandia provided technical assistance to the Alaska Ocean Cluster to assess potential market opportunities regarding byproducts of crab in the greater Alaska region. Crab contains a wide variety of proteins, chitin, lipids, minerals, and pigments. Currently, only a small portion of these components are utilized, primarily proteins associated with crab meat. Sandia provided an assessment of the current market landscape and opportunities related to crab byproducts including market size and applications. Sandia subject matter experts conducted an analysis and provide the Alaska Ocean Cluster team with a report describing the state of research and market opportunities offered by Alaska crab byproducts. The final report focused on market opportunities regarding chitosan production, chitin extraction, as well as an overview of the key market players and applications.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2022

Enhancing organic matter removal, product recovery, and hydrogen generation from fermentation wastewater

Existing ethanol biorefineries produce billions of gallons of wastewater (stillage) that must be treated extensively prior to discharge or concentrated in an energy intense evaporation step to produce animal feed as a value-added bioproduct. Yeasts and filamentous fungi were screened for growth and reduction of soluble organic compounds, carbohydrates, and protein from stillage to identify species capable of rapidly concentrating organic compounds into readily separable biomass in an attempt to concentrate the product using a much more efficient centrifugation step. Yeasts amenable to production of biomass derived products including bio-oils (Yarrowia lipolytica and Rhodotorula pallida), chitosan (Aspergillus niger) and animal feed (Cyberlindnera jadinii) were identified as well as microbes capable of efficient production of small organic acids with applications as bioderived polymers including 3-hydroxypropionic acid (engineered A. niger) and lactic acid using a co-culture of Debaryomyces udenii and Lactobacillus pentosus. The filamentous fungus A. niger eliminated all specifically measured soluble organics (glycerol, acetate, lactate, ethanol, and citrate) in under 48 hours and reduced total soluble protein content by 46% and total carbohydrate content by 83% within 96 hours, the greatest reduction in organic content observed. During this process an A. niger strain engineered to produce 3-hydroxypropionic acid achieved a yield of 0.35 C-mol 3HP / C-mol non-protein organics consumed at an overall rate of 0.09 g/Lh in unmodified stillage without pH control. Stillage treated by the fodder yeast C. jadinii as well as stillage containing acetic or lactic acid was found to be most suitable for growth by electrogenic bacteria with applications in production of electricity or hydrogen from wastewater. This work establishes fungal and bacterial strains appropriate for biological treatment of stillage to produce biomass derived products, soluble commodity chemicals, energy, and treated water to reduce the energy intensity and improve the economics of ethanol biorefineries.

09 BIOMASS FUELS↗

DOE OSTI2024

Development of a New Aggregation Method to Remove Nanoplastics from the Ocean: Proof of Concept Using Mussel Exposure Tests

The overproduction and mismanagement of plastics has led to the accumulation of these materials in the environment, particularly in the marine ecosystem. Once in the environment, plastics break down and can acquire microscopic or even nanoscopic sizes. Given their sizes, microplastics (MPs) and nanoplastics (NPs) are hard to detect and remove from the aquatic environment, eventually interacting with marine organisms. This research mainly aimed to achieve the aggregation of micro- and nanoplastics (MNPs) to ease their removal from the marine environment. To this end, the size and stability of polystyrene (PS) MNPs were measured in synthetic seawater with the different components of the technology (ionic liquid and chitosan). The MPs were purchased in their plain form, while the NPs displayed amines on their surface (PS NP-NH2). The results showed that this technology promoted a significant aggregation of the PS NP-NH2, whereas, for the PS MPs, no conclusive results were found, indicating that the surface charge plays an essential role in the MNP aggregation process. Moreover, to investigate the toxicological potential of MNPs, a mussel species (M. galloprovincialis) was exposed to different concentrations of MPs and NPs, separately, with and without the technology. In this context, mussels were sampled after 7, 14, and 21 days of exposure, and the gills and digestive glands were collected for analysis of oxidative stress biomarkers and histological observations. In general, the results indicate that MNPs trigger the production of reactive oxygen species (ROS) in mussels and induce oxidative stress, making gills the most affected organ. Yet, when the technology was applied in moderate concentrations, NPs showed adverse effects in mussels. The histological analysis showed no evidence of MNPs in the gill’s tissues.

Cid-Samamed, Antonio (ORCID:0000000205073394)↗

DOE OSTI2025

A Sensitive Electrochemical Cholinesterase-Inhibiting Biosensor for Organophosphorus Pesticides Based on Ti 3 C 2 TX MXene Quantum Dots

Organophosphorus pesticides (OPs) pose significant environmental and health risks due to their widespread use and toxicity, primarily by inhibiting acetylcholinesterase. Traditional detection methods are often slow and costly, highlighting the urgent need for advanced, sensitive, and accessible technologies. This study developed a highly sensitive electrochemical cholinesterase-inhibiting biosensor for OP pesticides, utilizing Ti 3 C 2 T x MXene Quantum Dots (MQDs), which was synthesized via a hydrothermal method. The biosensor’s performance was characterized using electrochemical impedance spectroscopy, differential pulse voltammetry (DPV), and cyclic voltammetry. DPV proved to be the optimal technique, exhibiting an ultralow detection limit of 1 × 10 −17 M and a wide linear range (10 −14 –10 −8 M) for chlorpyrifos (a model OP) with an estimated inhibition constant of 62 nM. The biosensor demonstrated high selectivity for OPs (chlorpyrifos, acephate, glyphosate) over a non-target pyrethroid (permethrin), confirmed by distinct electrochemical signatures and compared to in vitro cholinergic activity assays in bean beetle homogenates. The enhanced performance is attributed to the high surface-to-volume ratio, quantum confinement effects, and superior conductivity of the MQDs, as well as the robust enzyme immobilization facilitated by glutaraldehyde cross-linking and a chitosan matrix. This work presents a promising platform for rapid, sensitive, and selective detection of OP pesticides, with potential applications in environmental monitoring and public health protection.

Chemistry↗

DOE OSTI2021

Direct Mercury Detection in Landfill Leachate Using a Novel AuNP-Biopolymer Carbon Screen-Printed Electrode Sensor

A novel Au nanoparticle (AuNP)-biopolymer coated carbon screen-printed electrode (SPE) sensor was developed through the co-electrodeposition of Au and chitosan for mercury (Hg) ion detection. This new sensor showed successful Hg2+ detection in landfill leachate using square wave anodic stripping voltammetry (SWASV) with an optimized condition: a deposition potential of −0.6 V, deposition time of 200 s, amplitude of 25 mV, frequency of 60 Hz, and square wave step voltage of 4 mV. A noticeable peak was observed at +0.58 V associated with the stripping current of the Hg ion. The sensor exhibited a good sensitivity of ~0.09 μA/μg (~0.02 μA/nM) and a linear response over the concentration range of 10 to 100 ppb (50–500 nM). The limit of detection (LOD) was 1.69 ppb, which is significantly lower than the safety limit defined by the United States Environmental Protection Agency (USEPA). The sensor had an excellent selective response to Hg2+ in landfill leachate against other interfering cations (e.g., Zn2+, Pb2+, Cd2+, and Cu2+). Fifteen successive measurements with a stable peak current and a lower relative standard deviation (RSD = 5.1%) were recorded continuously using the AuNP-biopolymer-coated carbon SPE sensor, which showed excellent stability, sensitivity and reproducibility and consistent performance in detecting the Hg2+ ion. It also exhibited a good reliability and performance in measuring heavy metals in landfill leachate.

Hwang, Jae-Hoon (ORCID:0000000220100864)↗

DOE OSTI2023

Electrospun PVA Fibers for Drug Delivery: A Review

Innovation in biomedical science is always a field of interest for researchers. Drug delivery, being one of the key areas of biomedical science, has gained considerable significance. The utilization of simple yet effective techniques such as electrospinning has undergone significant development in the field of drug delivery. Various polymers such as PEG (polyethylene glycol), PLGA (Poly(lactic-co-glycolic acid)), PLA(Polylactic acid), and PCA (poly(methacrylate citric acid)) have been utilized to prepare electrospinning-based drug delivery systems (DDSs). Polyvinyl alcohol (PVA) has recently gained attention because of its biocompatibility, biodegradability, non-toxicity, and ideal mechanical properties as these are the key factors in developing DDSs. Moreover, it has shown promising results in developing DDSs individually and when combined with natural and synthetic polymers such as chitosan and polycaprolactone (PCL). Considering the outstanding properties of PVA, the aim of this review paper was therefore to summarize these recent advances by highlighting the potential of electrospun PVA for drug delivery systems.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1992

Progress report

The NASA funding allowed Clark Atlanta University (CAU) to establish a High Performance Polymers And Ceramics (HiPPAC) Research Center. The HiPPAC Center is consolidating and expanding the existing polymer and ceramic research capabilities at CAU through the development of interdepartmental and interinstitutional research in: (1) polymer synthesis; (2) polymer characterization and properties; (3) polymer processing; (4) polymer-based ceramic synthesis; and (5) ceramic characterization and properties. This Center has developed strong interactions between scientists and materials scientists of CAU and their counterparts from sister institutions in the Atlanta University Center (AUC) and the Georgia Institute of Technology. As a component of the center, we have started to develop strong collaborations with scientists from other universities and the HBCU's, national and federal agency laboratories, and the private sector during this first year. During this first year we have refined the focus of the research in the HiPPAC Center to three areas with seven working groups that will start programmatic activities on January 1, 1993, as follows: (1) nonlinear optical properties of chitosan derivatives; (2) polymeric electronic materials; (3) nondestructive characterization and prediction of polyimide performance; (4) solution processing of high-performance materials; (5) processable polyimides for composite applications; (6) sol-gel based ceramic materials processing; and (7) synthetic based processing of pre-ceramic polymers.

Abhiraman, A.↗

NASA NTRS2009

Using Volcanic Ash to Remove Dissolved Uranium and Lead

Experiments have shown that significant fractions of uranium, lead, and possibly other toxic and/or radioactive substances can be removed from an aqueous solution by simply exposing the solution, at ambient temperature, to a treatment medium that includes weathered volcanic ash from Pu'u Nene, which is a cinder cone on the Island of Hawaii. Heretofore, this specific volcanic ash has been used for an entirely different purpose: simulating the spectral properties of Martian soil. The treatment medium can consist of the volcanic ash alone or in combination with chitosan, which is a natural polymer that can be produced from seafood waste or easily extracted from fungi, some bacteria, and some algae. The medium is harmless to plants and animals and, because of the abundance and natural origin of its ingredient( s), is inexpensive. The medium can be used in a variety of ways and settings: it can be incorporated into water-filtration systems; placed in contact or mixed with water-containing solids (e.g., soils and sludges); immersed in bodies of water (e.g., reservoirs, lakes, rivers, or wells); or placed in and around nuclear power plants, mines, and farm fields.

McKay, David S.↗

NASA NTRSDate not supplied

Experimental Observations of Mechanisms of Pattern Formation During Freeze Casting

Empirically, many different materials compositions have been freeze cast over the years. Few have been analyzed to better understand the mechanisms by which the ice crystal growth drives structure formation, particularly the substructures on the cell walls. Collating substructural features, for example, ridges, bridges, and “jellyfish-like” substructures, found on the cell walls of freeze-cast ceramics (platelets versus particles), fibrillated biopolymers (collagen, nanocellulose), and "smooth" biopolymers (chitosan, trehalose), we capture the ice crystal growth process and analyze it both in situ in 2D and "post-mortem" in 3D to gain insights into anisotropic ice crystal growth and other self-assembly mechanisms. Combining these experimental observations with 3D Phase-field simulations of structure formation in ice-templated materials, detailed in a companion presentation, it becomes possible to gain fundamental science insights and to obtain the desired structure-property-processing correlations not only at the more traditional macroscopic, but also at the meso- and microscopic scales.

Kaiyang Yin↗

NASA NTRSDate not supplied

Experimental Observations of Mechanisms of Pattern Formation During Freeze Casting

Kaiyan Yin↗

DOE OSTI2023

Biodegradable transient battery built on core-double-shell zinc microparticle networks

A transient or biodegradable battery is provided having a filament structure that limits the speed of reaction allowing for a longer duration of battery power with a controlled current limit. In one embodiment, the filament may be constructed of zinc microparticles or nanoparticles having a thin outer insulation whereby a chemical reaction at the center core results in the progressive disintegration of the insulation revealing more core material. In one embodiment, microparticles or nanoparticles are coated with outer layers of chitosan and Al2O3 nanofilms, respectively, with designable discharge current and battery lifespan by controlling the exposed cross-sectional area of the zinc microparticle center core and the length of the filament, respectively. This novel structure of biodegradable battery provides improved control of battery life and power output, providing a promising solution to power transient medical implants.

Wang, Xudong↗

DOE OSTI2022

Characterizing Electron Flow through Catechol‐Graphene Composite Hydrogels

Abstract Electronic materials that allow the controlled flow of electrons in aqueous media are required for emerging applications that require biocompatibility, safety, and/or sustainability. Here, a composite hydrogel film composed of graphene and catechol is electrofabricated, and that this composite offers synergistic properties is reported. Graphene confers metal‐like conductivity and enables charge‐storage through an electrical double layer mechanism. Catechol confers redox‐activity and enables charge‐storage through a redox mechanism. Importantly, there are two functional populations of catechols: conducting‐catechols (presumably in intimate contact with graphene) allow direct electron‐transfer; and non‐conducting‐catechols (presumably physically separated from graphene) require diffusible mediators to enable electron‐transfer. Using a variety of spectroelectrochemical measurements, that the capacity of the composite for charge‐storage increases in proportion to the extent by which the catechol‐groups can undergo redox‐state switching is demonstrated. To illustrate the broad relevance of this work, how the redox‐state switching can be related to both the charge storage of energy materials and the memory of molecular electronic materials is discussed. The authors believe this work is significant because it demonstrates that: conducting and redox‐active components enable distinctly different mechanisms for charge‐storage and electron‐transfer; these components act synergistically; and mediators provide unique opportunities to extend the capabilities of electronic materials.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Electrophoretic Deposition as a Versatile Low-Cost Tool to Construct a Synthetic Polymeric Solid-Electrolyte Interphase on Silicon Anodes: A Model System Investigation

Not Available

25 ENERGY STORAGE↗

DOE OSTI2021

A protein scaffold enables hydrogen evolution for a Ni-bisdiphosphine complex

We find that an artificial metalloenzyme acting as a functional biomimic of hydrogenase enzymes was activated by assembly via covalent attachment of the molecular complex, [Ni(PN glycine P) 2 ] 2- , within a structured protein scaffold. Electrocatalytic H2 production was observed from pH 3.0 to 10.0 for the artificial enzyme, while no electrocatalytic activity was observed for similar [Ni(PNP) 2 ] 2+ systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗