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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Accelerated optimization of pure metal and ligand compositions for light-driven hydrogen production

Photocatalytic hydrogen production is a promising alternative to traditional hydrogen production. To implement photocatalytic hydrogen production the development of efficient, sustainable, and stable catalysts is necessary, and overcoming the current challenges surrounding high dimensional search spaces requires both computational and experimental efforts. Utilizing photo driven processes, stable colloidal metal catalysts can be formed in situ for efficient hydrogen production from water. When considering colloidal catalysts, stability is typically a concern solved through the addition of supports or ligands. In this work, poly(ethylene glycol) methyl ether thiol acts as a stabilizing ligand eliminating the need for catalyst supports while providing stable and active nanoparticle catalysts for more than 45 hours of reaction time and illumination. These systems utilize molecular photosensitizers, water reduction catalysts, stabilizing ligands, water, a sacrificial reductant, and organic solvents, posing new challenges pertaining to the optimization of multi-variable systems. Design of experiments (DOE) is applied to accelerate the understanding of variable interactions and is used as a tool to rapidly optimize the compositions of Au, Cu, Ni, and Fe containing systems. Through a collaboration leveraging computation and experimentation (both high throughput and characterizations), optimized performance peaks were obtained for each of these metals alongside distinct mapping of expected activity associated with photosensitizer, metal, and ligand concentration variations. With the highly digitized workflow, this study allowed for comparative generalizations to be made regarding photo driven hydrogen production for all four metals.

08 HYDROGEN↗
DOE OSTI2021

Aqueous TiO 2 Nanoparticles React by Proton-Coupled Electron Transfer

Redox reactions of aqueous colloidal TiO 2 4 nm nanoparticles (NPs) have been examined, including both citratecapped and uncapped NPs (c-TiO 2 and uc-TiO 2 ). Photoreduction gave stable blue colloidal c-TiO 2 R NPs with 10–60 electrons per particle. Equilibration of these reduced NPs with soluble redox reagents such as methylviologen (MV 2+ ) provided measurements of the colloid reduction potential as a function of pH. The potentials of c-TiO 2 from pH 2–9 varied linearly with pH, with a slope of –60 ± 5 mV/pH. Estimates of the potential at pH 12 were consistent with extrapolating that line to high pH. The reduction potentials did not correlate with the zeta potentials (ζ) or the surface charge of the NPs across this pH range. Similar reduction potentials were observed for c- and uc-TiO 2 at low pH even though they have quite different ζ potentials. These results show that the common surface-charging explanation of the pH dependence is not tenable in these systems. Oxidation of reduced c-TiO 2 R with the electron-transfer oxidant potassium triiodide (KI 3 ) occurred with a significant drop in pH, showing that protons were released when the electrons were removed from the NPs. Smaller pH drops were observed for the proton-coupled electron transfer (PCET) reagents O 2 (air) and 4-MeO-TEMPO (4-methoxy-2,2,6,6-tetramethylpiperine-1-oxy radical). The difference in the number of protons released with KI 3 vs O 2 and 4-MeO-TEMPO was roughly one proton per electron removed. Thus, the thermodynamically preferred reactivity of these colloidal TiO 2 NPs is PCET over the pH 2–13 range studied. The measured redox potentials refer to the chemical process TiO 2 + H + + e – → TiO 2 ·e – ,H + ; and therefore they do not correspond with an electronic energy such as a conduction band edge or flat band potential. The 1e – /1H + stoichiometry means that the TiO 2 reduction potentials correspond to a TiO 2 –H bond dissociation free energy (BDFE), determined to be 49 ± 2 kcal mol –1 . The PCET description is consistent with the pH dependence of E(TiO 2 /TiO 2 ·e – ,H + ), the release of protons upon oxidation, the lack of correlation with ζ potentials, the similarity of capped and uncapped NPs, and the small change in the potential and BDFE from the first to the last electron/proton pair (H atom) removed. Furthermore, this behavior is suggested to be the norm for redox-active oxide/water interfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Particles Growing in Solutions: Depletion Forces and Instability of Homogeneous Particle Distribution

Crystallites, droplets and amorphous precipitates growing from supersaturated solution are surrounded by zones, which are depleted with respect to the molecules they are built of. If two such particles of colloidal size are separated by a distance comparable to their diameters, then the depletion within the gap between particles is deeper than that at the outer portion of the particles. This will cause depletion attraction between the particles should appear. It may cause particle coagulation and decay of the originally homogeneous particle distribution into a system of clouds within which the particle number density is higher, separated by the region of the lower number density. Stability criterion, Q = 4 pi R(exp 3)c/3 >> 1, was analytically found along with typical particle density distribution wavevector q = (Q/I)(exp 1/2)(a/R)(exp 1/4). Here, R and a are the particle and molecular radii, respectively, c is the average molecular number density in solution and I is the squared diffusion length covered by a molecule during a typical time characterizing decay of molecular concentration in solution due to consumption of the molecules by the growing particles.

Chernov, A. A.↗
DOE OSTI2026

Colloidal Synthesis of Palladium Nanocluster‐Decorated Cs 3 Sb 2 Cl 9 Perovskite Heterostructural Nanorods for Enhanced CO 2 Photoreduction

Developing efficient and sustainable photocatalysts for CO 2 reduction remains a significant challenge, particularly with environmentally benign materials. Here, in this study, we report the first one-step synthesis of metal–lead-free perovskite heterostructural nanocrystals by decorating Cs 3 Sb 2 Cl 9 perovskite nanorods with size-controlled Pd nanoclusters via a one-step hot-injection method. The resulting Pd-Cs 3 Sb 2 Cl 9 heteronanorods (HNRs) exhibit strong interfacial electronic coupling, enhanced charge separation, and excellent colloidal stability. Transient absorption spectroscopy and DFT calculations reveal a built-in electric field that drives directional electron transfer from the perovskite host to the Pd domains. Under UV irradiation, the Pd-Cs 3 Sb 2 Cl 9 HNRs demonstrate excellent CO 2 photoreduction activity with high CH 4 selectivity, achieving a record apparent quantum yield (AQY) of 2.62% among halide perovskite nanocrystal-based systems with a large electronic yield of 689.3 ± 12.2 µmol·g cat −1 . In situ spectroscopic monitoring and Gibbs free energy analysis further unveil a Pd-facilitated reaction pathway involving stabilization of key intermediates. This work introduces a new class of lead-free perovskite-based heterostructures through a facile one-step synthesis strategy and offers a new design principle for next-generation photocatalysts for solar fuel production.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2020

Introduction to special issue: Colloidal quantum dots

The quantum confinement effect has driven the development and exploration of colloidal semiconductor nanocrystals over approximately the past three decades. These semiconductor nanostructures are typically synthesized as stable colloidal dispersions in solution-phase chemical batch reactions at relatively low temperatures. Researchers have developed a wide range of reaction conditions to produce a variety of shapes, compositions, and structures with well-controlled sizes and low polydispersities. The shape can be controlled to produce confinement in one, two, or all three spatial dimensions, the latter defining a “quantum dot.” Combining two or more semiconductors within the various nanostructures produces additional optical and electronic degrees of freedom. These mixed compositional nanostructures have properties not accessible in bulk semiconductor systems. Further, researchers have fabricated novel nanoheterostructures, such as “dot-in-rods,” quantum wells, core/shell structures, giant-core/shell tetrapods where the core is one material and the arm is another, Janus structures that consist of spherical structures with well-defined internal heterostructures, nano-dumbbells, hollow-core structures, and many other novel and interesting structures. The structural variations are seemingly only limited by the creativity of the various researchers engaged in these endeavors.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Toward High Efficiency Water Processed Organic Photovoltaics: Controlling the Nanoparticle Morphology with Surface Energies

Here efficient organic photovoltaic devices fabricated from water-based colloidal dispersions with donor:acceptor composite nanoparticles achieving up to 9.98% power conversion efficiency (PCE) are reported. This high efficiency for water processed organic solar cells is attributed to morphology control by surface energy matching between the donor and the acceptor materials. Indeed, due to a low interfacial energy between donor and the acceptor, no large phase separation occurs during the nanoparticle formation process as well as upon thermal annealing. Indeed, synchrotron-based scanning transmission X-ray microscopy reveals that the internal morphology of composite nanoparticles is intermixed as well as the active layer morphology after thermal treatment. The PCE of this system reaches 85% that of devices prepared from chlorinated solvent. The gap between water-based inks and organic solvent-based inks gets narrower, which is promising for the development of eco-friendly processing and fabrication of organic photovoltaics.

14 SOLAR ENERGY↗
DOE OSTI2021

Out of the Lab: 3D Printing on Non-Ideal Surfaces

In this work, coaxial direct ink writing is utilized to print sensitive or encapsulated materials onto heterogeneous and rough substrates. By enclosing the core fluid within a rigid ceramic shell, continuity is maintained even when printing on substrates traditionally considered challenging. This work presents the development of a coaxial ceramic direct ink writing system and investigates co-flow dynamics through microfluidic principles. A specially designed coaxial nozzle enables the co-extrusion of an alumina shell, with indium-tin-oxide inks serving as the core material. This approach allows the fabrication of core-shell ceramic structures suitable for future high-temperature applications on rough surfaces. The colloidal inks are tailored to achieve the necessary rheological properties and sintering performance. Additionally, flow simulations, guided by microfluidic co-flow principles, are employed to define the processing parameters for coaxial printing, ensuring precise control over the core-shell architectures. Physical modeling is further applied to study core deformation and eccentricity. These simulations are experimentally validated, supporting the successful deposition of coaxial ceramic features on heterogeneous, high-temperature ceramic substrates.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2023

Manipulation of self-organized multi-vortical states in active magnetic roller suspensions

Ensembles of active magnetic colloids demonstrate complex collective behavior and self-organization when driven out of equilibrium by external magnetic fields. The interplay between magnetic and hydrodynamic interactions often result in spontaneous self-assembly and the emergence of localized vortices in ensembles of ferromagnetic rollers. We report experimental and computational study of the self-organized multi-vortical state in ensembles of magnetic rollers under the imposed external confining potential realized by patterned substrates. We explore the behavior of the system on a substrate patterned with shallow wells ordered in a lattice with square symmetry and lattice spacing smaller than the wells’ diameter. Here we demonstrate, that ensembles of active magnetic rollers evolve in response to changes in the geometry of the confining lattice from a globally correlated state characterized by anti-ferromagnetic vortex ordering to a state with rapidly changing particle flows and self-organized vortical states with a lattice constant larger than one of the confining pattern. Our experimental observations are accompanied by numerical simulations based on phenomenological coarse grained particle dynamics coupled to Navier–Stokes hydrodynamics in shallow water approximation. The reported results provide insights into the collective behavior of active magnetic rollers under confinement and suggest strategies for the manipulation of collective dynamic states in active magnetic liquids.

36 MATERIALS SCIENCE↗
NASA NTRS2014

Protein Colloidal Aggregation Project

To investigate the pathways and kinetics of protein aggregation to allow accurate predictive modeling of the process and evaluation of potential inhibitors to prevalent diseases including cataract formation, chronic traumatic encephalopathy, Alzheimer's Disease, Parkinson's Disease and others.

Technology Portfolio System↗
DOE OSTI2024

Simulation of Particulate Transport for Delivery of Solid Amendments into the Subsurface: FY24 Status Report

For particulate-based amendments to be viable for field-scale remediation at the Hanford Site (e.g., 200 DV-1 Operable Unit), particles need to be delivered a sufficient radial distance from an injection well and retained at concentrations high enough for effective treatment. An accurate description of the particle radius of influence (ROI) is critical for developing an overall remediation strategy. However, field-scale particle simulations are currently limited due to insufficient simulation capabilities and a lack of experimental data to validate and parameterize particle transport models. To help build toward field-scale deployment, this fiscal year (FY) we have (1) developed a pre screening tool to estimate particle transport, (2) implemented particle transport models within PFLOTRAN, and (3) conducted preliminary estimations of particle ROI. While field-scale numerical simulations will ultimately be necessary before remedy design and field implementation, we have developed a pre-screening tool that offers valuable estimations of expected particle injectability and ROI in a 1-D system. The advantage of the tool is that it does not require extensive laboratory experiments and instead makes predictions based solely on routine laboratory measurements. This tool can assist in down-selection and decision-making by identifying which particle amendment systems are worth pursuing in future laboratory experiments, such as 1-D column tests and beyond. With any system, scaling up from the lab to the field presents challenges. Currently, there is no field data available for model calibration or validation. However, the theoretical particle models being developed herein are the best tools available to guide progress toward field deployment. To help bridge this gap and verify model predictions, larger-scale lab experiments are being proposed. To advance simulation capabilities, six particle transport models are being integrated into the reactive transport simulator PFLOTRAN. These include colloid filtration theory (CFT) and five additional particle transport models (M1-M5). Each model, from M1 to M5, progressively incorporates additional particle transport and retention processes. Ultimately, the simplest model capable of accurately describing 1-D column data will be selected and parameterized. During FY24, the CFT and M1 model have been fully implemented within PFLOTRAN. Using an existing 1 D column experiment, the two currently implemented particle transport models (CFT and M1), and associated parameters, were fit to this experiment. While simpler model formulations are helpful for estimations, these formulations could not fully describe particle transport and retention behavior in the previous 1-D column experiment. Thus, additional complexities will need to be considered, which will be accounted for in the M2-M5 model formulations. Additionally, because a viscous, shear thinning fluid was required to keep particles in suspension, considerations for flow will also need to also be accounted for. Therefore, a new immiscible two-phase flow mode is currently being implemented in PFLOTRAN. With some modifications, this new flow module could also support simulation of non-Newtonian liquid amendments, foams, and emulsions. We also estimated the expected ROI of solid amendments using 1-D simulations. The average predicted ROI was approximately 15 ft for micron-sized zero valent iron (mZVI) suspended in xanthan gum (XG). Using the pre screening tool and ROI estimates, additional amendment-delivery laboratory characterization and experiments are proposed. The results from additional experiments can be used to validate and parametrize particulate transport model formulations, which will ultimately provide predictive capabilities for field amendment-delivery systems.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS2019

Advanced Colloids Experiment (Temperature Controlled) – ACE-T5

The attached will be presented at the JSC Science Symposium as a preview of the ACE-T5 flight experiment. The Principal Investigator (PI) for this experiment is Professor Ali Mohraz at the University of California - Irvine.Bijels (bicontinuous interfacially jammed emulsion gels) were discovered in 2007 at the University of Edinburgh. These materials feature a tubular, bicontinuous arrangement of two fluid phases separated by a monolayer of jammed colloidal particles at the interface.Because of their unique morphological characteristics, bijels hold significant promise as next-generation materials for energy and biotechnology applications. But in order to fully realize their potential, their physics and mechanical properties must be better understood. The mechanical properties and stability of bijels is mediated by an interplay between interfacial forces that impart elasticity to the system, and external stresses. Unfortunately, the interfacial forces are inherently coupled with density differences and cannot be studied systematically in the presence of gravity.

Mohraz, Ali↗
NASA NTRS2001

STS-102 Expedition 2 Increment and Science Briefing

Merri Sanchez, Expedition 2 Increment Manager, John Uri, Increment Scientist, and Lybrease Woodard, Lead Payload Operations Director, give an overview of the upcoming activities and objectives of the Expedition 2's (E2's) mission in this prelaunch press conference. Ms. Sanchez describes the crew rotation of Expedition 1 to E2, the timeline E2 will follow during their stay on the International Space Station (ISS), and the various flights going to the ISS and what each will bring to ISS. Mr. Uri gives details on the on-board experiments that will take place on the ISS in the fields of microgravity research, commercial, earth, life, and space sciences (such as radiation characterization, H-reflex, colloids formation and interaction, protein crystal growth, plant growth, fermentation in microgravity, etc.). He also gives details on the scientific facilities to be used (laboratory racks and equipment such as the human torso facsimile or 'phantom torso'). Ms. Woodard gives an overview of Marshall Flight Center's role in the mission. Computerized simulations show the installation of the Space Station Remote Manipulator System (SSRMS) onto the ISS and the installation of the airlock using SSRMS. Live footage shows the interior of the ISS, including crew living quarters, the Progress Module, and the Destiny Laboratory. The three then answer questions from the press.

Source record↗
NASA NTRS1998

Coulomb Crystallization of Charged Microspheres Levitated in a Gas Discharge Plasma

The technical topic of the project was the experimental observation of Coulomb crystallization of charged microspheres levitated in a gas discharge plasma. This suspension, sometimes termed a dusty plasma, is closely analogous to a colloidal suspension, except that it has a much faster time response, is more optically thin, and has no buoyancy forces to suspend the particles. The particles are levitated by electric fields. Through their collective Coulomb repulsions, the particles arrange themselves in a lattice with a crystalline symmetry, which undergoes an order-disorder phase transition analogous to melting when the effective temperature of the system is increased. Due to gravitational sedimentation, the particles form a thin layer in the laboratory, so that the experimental system is nearly 2D, whereas in future microgravity experiments they are expected to fill a larger volume and behave like a 3D solid or liquid. The particles are imaged using a video camera by illuminating them with a sheet of laser light. Because the suspension is optically thin, this imaging method will work as well in a 3D microgravity experiment as it does in a 2D laboratory system.

Goree, John↗
DOE OSTI2021

A Laboratory Assessment and Optimization of Nanoparticle-Stabilized CO2 Foams for Hydraulic Fracturing Applications

In this research, we have conducted a comprehensive assessment and optimization of aqueous CO2 foams for fracturing applications. The performance of CO2 foams is evaluated using three major matrices: foam stability, foam apparent viscosity, and leakoff. The response of these performance matrices to different internal factors and external conditions is evaluated. These factors and conditions include foam quality, nanoparticle concentration, salinity, shear rate, surfactant type and concentration, polymer concentration, and temperature. Before foam generation, the colloidal stability of the nanosilica dispersion is evaluated at different types of electrolytes and under high temperatures. With a good salinity resistance and thermal stability, the nanosilica is then used for the entire set of foam generation experiments. The foam configuration with optimized parameters is used for the leakoff test, which serves as a supplementary section to further demonstrate the advantages of the proposed foam system. Then the final commercialization section provides a general view of what should be considered to commercialize the research results. In general, it is found that the aqueous CO2 foam system has demonstrated a good potential to be used as a fracturing fluid. The design of the foam system needs to consider formations properties and formation fluid properties etc. to realize the optimal performance of the system on a laboratory scale.

02 PETROLEUM↗
DOE OSTI2023

Soft matter roadmap

Soft materials are usually defined as materials made of mesoscopic entities, often self-organised, sensitive to thermal fluctuations and to weak perturbations. Archetypal examples are colloids, polymers, amphiphiles, liquid crystals, foams. The importance of soft materials in everyday commodity products, as well as in technological applications, is enormous, and controlling or improving their properties is the focus of many efforts. From a fundamental perspective, the possibility of manipulating soft material properties, by tuning interactions between constituents and by applying external perturbations, gives rise to an almost unlimited variety in physical properties. Together with the relative ease to observe and characterise them, this renders soft matter systems powerful model systems to investigate statistical physics phenomena, many of them relevant as well to hard condensed matter systems. Understanding the emerging properties from mesoscale constituents still poses enormous challenges, which have stimulated a wealth of new experimental approaches, including the synthesis of new systems with, e.g. tailored self-assembling properties, or novel experimental techniques in imaging, scattering or rheology. Theoretical and numerical methods, and coarse-grained models, have become central to predict physical properties of soft materials, while computational approaches that also use machine learning tools are playing a progressively major role in many investigations. This Roadmap intends to give a broad overview of recent and possible future activities in the field of soft materials, with experts covering various developments and challenges in material synthesis and characterisation, instrumental, simulation and theoretical methods as well as general concepts.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Electrolytic Coagulant Generation for Treating Flowback and Produced Water for Reuse

This research investigated a novel electrochemical process for producing a ferric iron coagulant for use in treating flowback and produced water (FPW) from hydraulic fracturing and oil production operations. The electrolytic coagulant generation (ECG) system uses an electrochemical cell to produce acid and base from oilfield brine solutions. The acid is used to dissolve scrap iron to provide a Fe 3+ coagulating agent, and the base is used to neutralize the treated water. The costs for generating the ferric iron coagulant were determined as a function of current density and feed water salinity. The process was shown to be effective for removing colloidal bentonite particles from brine solutions. Here, the process has several advantages over conventional electrocoagulation using iron anodes, including: the ability to treat anoxic waters, elimination of electrode fouling, lower cost for the coagulant, and the ability to deliver Fe 3+ doses greater than 1 mM, since it is not limited by the amount of dissolved oxygen required to oxidize ferrous to ferric iron.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Establishing a silica gel zone in well annulus and evaluating its performance in blocking vertical water flow

Wells are often constructed for monitoring purposes with relatively long screen lengths (e.g., >10 m). Vertical water flows can occur within the artificial or natural filterpack annulus that surrounds the screened interval, bypassing packer assemblies installed inside the wellbore. Attempts to isolate discrete vertical zones during groundwater sampling are unsuccessful when annular flow occurs and lead to remedy decisions based on biased or incorrect interpretations. Blocking vertical annular water flow and contaminant transport will help obtain more accurate concentrations of contaminants from sampling in targeted depth intervals. The application of silica gels formed from the injected colloidal silica CS suspensions is a novel approach to minimize or prevent movement of vertical movement of groundwater in the surrounding filterpack annulus. In this work, we tested the feasibility of injecting CS suspensions to target locations and developed a modified CS formulation that is injectable and prevents gravity sinking. We studied the distribution and penetration of silica gel at laboratory scale in mock well annulus with surrounding formations. We evaluated the performance of the silica gel in blocking vertical water flow in the annulus and in minimizing chemical transport through the gel zone. CS suspension formulations have been defined that are ready for injection, stay in target locations, and form gel within desired time frames. Injection of CS suspensions achieved uniform distribution in a well annulus filter pack, fully occupied the annulus pore space, and penetrated the formation surrounding the filter packer with a sufficient distance to create a hydraulic annular seal when the injection was applied at a sufficient rate. The depth of penetration into the formation was dependent on the permeability contrast between the filter pack and the surrounding formation. Silica gel that formed in the annulus blocked vertical water flow and stopped the chemical transport through the gel zone. In conclusion, this research reveals that using CS suspension injection and sequential gelation (CS-GEL) is a promising technology for blocking vertical water flow and chemical transport through the filter pack in targeted zones within the annulus of long-screened well systems.

Colloidal silica suspension↗