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At least 865 records · Page 48

All sources NASA NTRS DOE OSTI

DOE OSTI2024

Methane partial oxidation under periodic reaction conditions on Pt/Al 2 O 3

The increasing interest in utilizing methane, the primary component of natural gas, for chemical production has spurred research into methane partial oxidation (MPO) as an alternative to traditional steam methane reforming (SMR). MPO has lower energy requirements and potential for carbon capture, making it an attractive option for hydrogen production. Challenges remain, however, such as carbon deposition leading to degradation and achieving high hydrogen selectivity. Here, the impact of periodic reactor operation on MPO over a Pt/Al 2 O 3 catalyst was studied, primarily via varying reactor inlet compositions. Experiments were conducted using periodic operation strategies to assess the influence of changing reactant inlet concentrations on hydrogen formation during MPO. The results suggest that cycling between mixtures with low and high oxygen content can lead to transient hydrogen formation rates that surpass those achieved at steady state. Control experiments and density functional theory (DFT) calculations show that enhanced hydrogen formation can be attributed to the reaction between CO with hydroxyl groups at the metal and alumina support interface. Furthermore, this work underscores the critical role of surface coverages at the metal–support interface and suggests avenues for future exploration, including alternative support materials with higher OH mobility and changes in the cycling scheme to enhance catalyst performance under periodic conditions.

03 NATURAL GAS↗

DOE OSTI2023

Evaluation of Technologies for Destruction of LDR Organics in Hanford Tank Waste

Aqueous Hanford tank wastes contain soluble organics and some tanks contain small amounts (<100 mg/L) of organics that are regulated under the Land Disposal Restrictions (LDR) portions of the Resource Conservation and Recovery Act (RCRA). Most of these organics can be removed by evaporation, but some are not. Methods to destroy/remove organics that are regulated by the LDR section of the RCRA and that are not removed by evaporation may be needed if ambient temperature waste treatment processes are used to immobilize aqueous Hanford tank wastes. To identify viable and compatible organic removal or destruction pretreatment methods an evaluation was performed by a team of researchers. The team utilized a Systems Engineering Approach that examines all aspects of the technology, based on information available in the literature and the experience of the team members. That evaluation led to recommendations by the team to perform testing on technologies to determine efficacy in destroying organics in Hanford tank waste liquids. The primary technologies recommended are chemical oxidants, including permanganate, peroxymonosulfate or peroxydisulfate (PMS/PDS), hydrogen peroxide, and ozone. Ultraviolet light irradiation of the stream with a solid catalyst sorbent is also recommended for testing. A generalized description of the test program is also included.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Editorial: Deep-sea observation equipment and exploration technology

The increasing interest in deep-sea exploration is a crucial catalyst for driving advancements in deep-sea observation technology research. Numerous sophisticated sensors have been developed to facilitate comprehensive studies in deep-sea physics, chemistry, and geology. For example, cutting-edge small and compact seabed samplers are now employed on various platforms, such as Autonomous Underwater Vehicles (AUVs), Remotely Operated Vehicles (ROVs), and Human-Operated Vehicles (HOVs), enabling observation of the hadal zone. Additionally, Micro-electromechanical systems (MEMS) sensors are routinely utilized for ocean wave observation. This Research Topic aims to foster new insights into ocean exploration and observation technology, including ocean sensor technology, ocean observation platforms, and ocean observation reliability technology.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Facile hyperpolarization chemistry for molecular imaging and metabolic tracking of [1– 13 C]pyruvate in vivo

Hyperpolarization chemistry based on reversible exchange of parahydrogen, also known as Signal Amplification By Reversible Exchange (SABRE), is a particularly simple approach to attain high levels of nuclear spin hyperpolarization, which can enhance NMR and MRI signals by many orders of magnitude. SABRE has received significant attention in the scientific community since its inception because of its relative experimental simplicity and its broad applicability to a wide range of molecules, however, in vivo detection of molecular probes hyperpolarized by SABRE has remained elusive. Here we describe a first demonstration of SABRE-hyperpolarized contrast detected in vivo, specifically using hyperpolarized [1– 13 C]pyruvate. Biocompatible formulations of hyperpolarized [1– 13 C]pyruvate in, both, methanol-water, and ethanol-water mixtures followed by dilution with saline and catalyst filtration were prepared and injected into healthy Sprague Dawley and Wistar rats. Effective hyperpolarization-catalyst removal was performed with silica filters without major losses in hyperpolarization. Metabolic conversion of pyruvate to lactate, alanine, and bicarbonate was detected in vivo. Pyruvate-hydrate was also observed as a minor byproduct. Measurements were performed on the liver and kidney at 4.7 T via time-resolved spectroscopy and chemical-shift-resolved MRI. In addition, whole-body metabolic measurements were obtained using a cryogen-free 1.5 T MRI system, illustrating the utility of combining lower-cost MRI systems with simple, low-cost hyperpolarization chemistry to develop safe and scalable molecular imaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Bridging Structural and Chemical Insights: Integrating In Situ Electron Microscopy and X-ray Spectroscopy for Catalysis Research

Environmental transmission electron microscopy probes the local structure, composition, and chemistry of materials under gas environments, while ambient-pressure X-ray photoelectron spectroscopy provides ensemble chemical and electronic structure information in gaseous conditions. Both techniques utilize similar differential pumping schemes to mitigate electron scattering by the gas phase, allowing for unique opportunities to correlate gas–surface interactions across comparable pressure ranges. Their integration has advanced the understanding of various catalytic reactions, including the water–gas-shift reaction, CO oxidation, and surface passivation dynamics. In conclusion, this Mini-Review discusses their methodological advancements, challenges, and potential for further integration with other in situ techniques to address complex catalytic phenomena and guide catalyst design.

36 MATERIALS SCIENCE↗

DOE OSTI2020

How Rh surface breaks CO 2 molecules under ambient pressure

Utilization of carbon dioxide (CO 2 ) molecules leads to increased interest in the sustainable synthesis of methane (CH 4 ) or methanol (CH 3 OH). The representative reaction intermediate consisting of a carbonyl or formate group determines yields of the fuel source during catalytic reactions. However, their selective initial surface reaction processes have been assumed without a fundamental understanding at the molecular level. Here, we report direct observations of spontaneous CO 2 dissociation over the model rhodium (Rh) catalyst at 0.1 mbar CO 2 . The linear geometry of CO 2 gas molecules turns into a chemically active bent-structure at the interface, which allows non-uniform charge transfers between chemisorbed CO 2 and surface Rh atoms. By combining scanning tunneling microscopy, X-ray photoelectron spectroscopy at near-ambient pressure, and computational calculations, we reveal strong evidence for chemical bond cleavage of O-CO* with ordered intermediates structure formation of (2 × 2)-CO on an atomically flat Rh(111) surface at room temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

In-situ analysis of hydrazine decomposition products

A gas analyzer utilizing a nondispersive infrared (NDIR) detection system was used to monitor the ammonia and water vapor content of the products of a previously unused hydrazine gas generator. This provided an in-situ measurement of the generator's efficiency difficult to obtain by other means. The analyzer was easily installed in both the calibration and hydrazine systems, required no maintenance other than periodic zero adjustments, and performed well for extended periods in the operating range tested. The catalyst bed operated smoothly and repeatably during the 28 hr of testing. No major transients were observed on startup or during steady state operation. The amount of ammonia in the output stream of the gas generator was found to be a strong function of temperature at catalyst bed temperatures below 450 C. At temperatures above this, the efficiency remained nearly constant. On startup the gas generator efficiency was found to decrease with time until a steady state value was attained. Elevated catalyst bed temperatures in the periods before steady state operation was found to be responsible for this phenomenon.

Curran, Francis M.↗

NASA NTRS1987

In-situ analysis of hydrazine decomposition products

Curran, Francis M.↗

DOE OSTI2026

Interfacial Charge Transfer Pathways in Photoelectrochemical H 2 Evolution by a Single-Component Molecular Catalyst on a Conductive Metal Oxide

Dye-sensitized photoelectrosynthesis cells traditionally combine a photosensitizing dye to harvest light and a catalyst to generate chemical fuels on a semiconductor. Here, in this work, a photoactive catalyst capable of both light absorption and fuel formation, [Cp*Ir(4,4′-Y 2 -bpy)Cl][Cl] (Cp* = pentamethylcyclopentadienyl, bpy = 2,2′-bipyridine, Y = CH 2 PO 3 H 2 ), is anchored to a mesoporous tin-doped indium oxide (ITO) electrode and facilitates photoelectrochemical H 2 evolution in water without the need for additional photosensitizers or sacrificial reductants. Spectroelectrochemistry indicates a single-site H 2 evolution mechanism involving charge injection to ITO, in contrast to the bimetallic mechanism observed in solution. Cyclic voltammetry and variable-potential chronoamperometry under illumination probe competing pathways via interfacial electron transfer between the Ir hydride excited state and the conductive ITO electrode. A Marcus theory framework provides reorganization energies for competing interfacial electron transfer pathways from potential-dependent quantum yield measurements. The light-driven H 2 evolution catalysis on conducting oxide proceeds with high Faradaic efficiency and current densities comparable to photoelectrodes utilizing p-type semiconductors. By uncovering the principal electron transfer pathways that govern photocatalytic efficiency, this study establishes design principles for hybrid molecular photoelectrocatalysts.

catalysts↗

DOE OSTI2024

Modeling scale-up of particle coating by atomic layer deposition

Atomic layer deposition (ALD) is a promising technique to functionalize particle surfaces for energy applications including energy storage, catalysis, and decarbonization. In this work, we present a set of models of ALD particle coating to explore the transition from lab scale to manufacturing. Our models encompass the main particle coating manufacturing approaches including rotary bed, fluidized bed, and continuously vibrating reactors. These models provide key metrics, such as throughput and precursor utilization, required to evaluate the scalability of ALD manufacturing approaches and their feasibility in the context of energy applications. Our results show that designs that force the precursor to flow through fluidized particles transition faster to a transport-limited regime where throughput is maximized. They also exhibit higher precursor utilization. In the context of continuous processes, our models indicate that it is possible to achieve self-extinguishing processes with almost 100% precursor utilization. A comparison with past experimental results of ALD in fluidized bed reactors shows excellent qualitative and quantitative agreement.

25 ENERGY STORAGE↗

NASA NTRS2004

Automatic Control of Arc Process for Making Carbon Nanotubes

An automatic-control system has been devised for a process in which carbon nanotubes are produced in an arc between a catalyst-filled carbon anode and a graphite cathode. The control system includes a motor-driven screw that adjusts the distance between the electrodes. The system also includes a bridge circuit that puts out a voltage proportional to the difference between (1) the actual value of potential drop across the arc and (2) a reference value between 38 and 40 V (corresponding to a current of about 100 A) at which the yield of carbon nanotubes is maximized. Utilizing the fact that the potential drop across the arc increases with the interelectrode gap, the output of the bridge circuit is fed to a motor-control circuit that causes the motor to move the anode toward or away from the cathode if the actual potential drop is more or less, respectively, than the reference potential. Thus, the system regulates the interelectrode gap to maintain the optimum potential drop. The system also includes circuitry that records the potential drop across the arc and the relative position of the anode holder as function of time.

Scott, Carl D.↗

DOE OSTI2026

Upcycling Real‐World Post‐Consumer Polyolefins Plastics Into Light Olefins Via Microwave‐Assisted Processing

The rapid accumulation of plastic waste, particularly post-consumer polyolefins (POs) pose severe environmental and economic challenges worldwide. Recycling of post-consumer POs remains inefficient due to difficulties in separating mixed plastics, complex additives compositions, and high processing costs, resulting in recycling rates of less than 9%. To address these critical issues, this study utilized an innovative microwave-assisted catalytic upcycling approach for the efficient upcycling of complex post-consumer POs mixtures into valuable light olefins. Using the microwave-assisted catalytic upcycling approach, gas yields reached up to 80 wt.% from post-consumer POs mixtures, accompanied by a high selectivity (>70 wt.%) toward valuable light olefins. The upcycling of POs under microwave conditions is fully invested, including additives in real-word plastics, mixtures of different POs, reusability of catalyst, and more. The microwave-assisted catalytic upcycling approach offers an efficient, scalable, and cost-effective solution for upcycling post-consumer plastic mixtures, thereby advancing the principles of a circular economy.

42 ENGINEERING↗

DOE OSTI2023

Protection against Chemical Warfare Agents and Biological Threats Using Metal–Organic Frameworks as Active Layers

The SARS-CoV-2 pandemic outbreak and the unfortunate misuse of toxic chemical warfare agents (CWAs) highlight the importance of developing functional materials to protect against these chemical and pathogen threats. Metal–organic frameworks (MOFs), which comprise a tunable class of crystalline porous materials built from inorganic nodes and organic linkers, have emerged as a class of heterogeneous catalysts capable of rapid detoxification of multiple classes of these harmful chemical or biological hazards. In particular, zirconium-based MOFs (Zr-MOFs) feature Lewis acidic nodes that serve as active sites for a wide range of catalytic reactions, including the hydrolysis of organophosphorus nerve agents within seconds in basic aqueous solutions. In addition, postsynthetic modification of Zr-MOFs enables the release of active species capable of reacting with and deactivating harmful pathogens. Despite this impressive performance, utilizing Zr- MOFs in powder form is not practical for application in masks or protective uniforms. To address this challenge, our team sought to develop MOF/fiber composite systems that could be adapted for use under realistic operating conditions to protect civilians, military personnel, and first responders from harmful pathogens and chemical warfare agents. Over the last several years, our group has designed and fabricated reactive and biocidal MOF/fiber composites that effectively capture and deactivate these toxic species. In this Account, we describe the evolution of these porous and reactive MOF/fiber composites and focus on key design challenges and considerations. First, we devised a scalable method for the integration of Zr-MOFs onto textile substrates using aqueous precursor solutions and without using pretreated textiles, highlighting the potential scalability of this method. Moving beyond standard textiles, we also developed a microbial synthesis strategy to prepare hierarchically porous MOF/bacterial cellulose nanofiber composite sponges that can both capture and detoxify nerve agents when exposed to contaminated gas flows. The mass loading of the MOF in the nanofibrous composite sponge is up to 90%, affording higher work capacities compared to those of textile-fiber-based composites with relatively lower MOF loadings. Next, we demonstrated that heterogeneous polymeric bases are suitable replacements for volatile liquid bases typically used in solution-phase reactions, and we showed that these composite systems are capable of effectively hydrolyzing nerve agents in the solid state by using only water that is present as humidity. Moreover, incorporating a reactive dye precursor into the composite affords a dual function sensing and detoxifying material that changes color from white to orange upon reaction with the byproduct following nerve agent hydrolysis, demonstrating the versatility of this platform for use in decontamination applications. We then created chlorine-loaded MOF/fiber composites that act as biocidal and reactive textiles that are capable of not only detoxifying sulfur-mustard-based chemical warfare agents and simulants but also deactivating both bacteria and the SARS-CoV-2 virus within minutes of exposure. Lastly, we synthesized a mixed-metal Ti/Zr-MOF coating on cotton fibers to afford a photoactive biocidal cloth that shows fast and broad-spectrum biocidal performance against viruses and Gram-positive and Gram-negative bacteria under visible light irradiation. Given the tunable, multifunctional nature of these MOF/fiber composites, we believe that this Account will offer new insights for the rational design and preparation of functional MOF/fiber composites and pave the way toward the development of next-generation reactive and protective textiles.

36 MATERIALS SCIENCE↗

DOE OSTI2024

One-Step Synthesis and Operando Electrochemical Impedance Spectroscopic Characterization of Heterostructured MoP–Mo 2 N Electrocatalysts for Stable Hydrogen Evolution Reaction

Here this study presents a novel synthesis of self-standing MoP and Mo 2 N heterostructured electrocatalysts with enhanced stability and catalytic performance. Facilitated by the controlled phase and interfacial microstructure, the seamless structures of these catalysts minimize internal resistivity and prevent local corrosion, contributing to increased stability. The chemical synthesis proceeds with etching step to activate the surface, followed by phosphor-nitriding in a chemical vapor deposition chamber to produce MoP-Mo 2 N@Mo heterostructured electrocatalysts. X-ray diffraction analyses confirm the presence of MoP, Mo 2 N, and Mo phases in the electrocatalyst. Morphology studies using scanning electron microscopy characterizes the hierarchical growth of structures, indicating successful formation of the heterostructure. X-ray photoelectron spectroscopy (XPS) analyses of the as-synthesized and post-catalytic activity samples reveal the chemical shift in terms of binding energy (BE) of Mo 3d XPS peak, especially after catalytic activity. The XPS BE shifts attributed to changes in oxidation state, electron transfer, and surface reconstruction during catalysis. Electrochemical evaluation of the catalysts demonstrates the superior performance of the MoP-Mo 2 N@Mo heterostructured catalyst in hydrogen evolution reactions (HER), with lower overpotentials and enhanced Tafel slopes. Stability tests reveal changes in double layer capacitance over time, suggesting surface reconstruction and increased active surface area during catalysis. Operando electrochemical impedance spectroscopy (EIS) further elucidates the dynamic changes in resistance and charge transfer during HER. Overall, comprehensive understanding of the synthesis, characterization, and electrochemical behavior of the developed MoP-Mo 2 N@Mo heterostructured electrocatalyst as presented in this paper highlights their potential utilization in sustainable energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2012

Compact, Lightweight Adsorber and Sabatier Reactor for CO2 Capture and Reduction for Consumable and Propellant Production

The utilization of CO2 to produce (or recycle) life support consumables, such as O2 and H2O, and to generate propellant fuels is an important aspect of NASA's concept for future, long duration planetary exploration. One potential approach is to capture and use CO2 from the Martian atmosphere to generate the consumables and propellant fuels. Precision Combustion, Inc. (PCI), with support from NASA, continues to develop its regenerable adsorber technology for capturing CO2 from gaseous atmospheres (for cabin atmosphere revitalization and in-situ resource utilization applications) and its Sabatier reactor for converting CO2 to methane and water. Both technologies are based on PCI's Microlith(R) substrates and have been demonstrated to reduce size, weight, and power consumption during CO2 capture and methanation process. For adsorber applications, the Microlith substrates offer a unique resistive heating capability that shows potential for short regeneration time and reduced power requirements compared to conventional systems. For the Sabatier applications, the combination of the Microlith substrates and durable catalyst coating permits efficient CO2 methanation that favors high reactant conversion, high selectivity, and durability. Results from performance testing at various operating conditions will be presented. An effort to optimize the Sabatier reactor and to develop a bench-top Sabatier Development Unit (SDU) will be discussed.

Junaedi, Christian↗

DOE OSTI2024

Impact of electrolyte solutions on carbon dioxide fixation in single chamber Al–CO 2 battery

Governments and research & development (R&D) organizations are actively initiating various programs and research strategies for CO 2 capture, its utilization, and integration with long duration energy storage from renewable sources worldwide. In line with the carbon capture goals, here we report a novel electrochemical Al-CO 2 battery cell, that can simultaneously capture CO 2 and convert it into value-added products, in addition to long-duration energy generation and storage. Here, this innovative approach employs cost-effective Al metal as an anode and an in-house synthesized Ni–Fe based bimetallic double hydroxide catalyst as the cathode, with meticulously optimized compositions and morphologies. We explore the impact of different aqueous electrolyte solutions compositions on the cell performance, demonstrating up to 10 h of stable long duration energy storage with a stable voltage profile. The cell exhibits low polarization even at high current densities of up to 12 mA cm -2 and maintains stable cycling over 500 h. Through Fourier-transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray Diffraction and X-ray photoelectron spectroscopy (XPS) analysis, we determined that the discharge product is either NaAlCO 3 (OH) 2 or KAlCO 3 (OH) 2 , distinct from the Al 2 (CO 3 ) 3 typically reported in conventional Al–CO 2 batteries.

25 ENERGY STORAGE↗

DOE OSTI2020

Ultrathin Porous Hydrocarbon Membranes Templated by Nanoparticle Assemblies

Porous polymer membranes are widely desired as catalyst supports, sensors, and active layers for separation membranes. We demonstrate that electron beam irradiation of freely suspended gold or Fe 3 O 4 nanoparticle (NP) monolayer sheets followed by wet chemical etching is a high-fidelity strategy to template two-dimensional (2D) porous crosslinked hydrocarbon membranes. This approach, which relies on secondary electrons generated by the NP cores, can further be used to transform three-dimensional (3D) terraced gold NP supercrystals into 3D porous hydrocarbon membranes. We utilize electron tomography to show how the number of NP layers (monolayer to pentalayer) controls attenuation and scattering of the primary e-beam, which in turn determines ligand crosslink density and 3D pore structure. Furthermore, electron tomography also reveals that many nanopores are vertically continuous due to preferential sintering of NPs. This work demonstrates new routes for the construction of functional nanoporous media.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2026

Controlled Acidity Gradients Enable CO 2 Reduction to Formic Acid (Not Formate) by Molecular Electrocatalysts

Neutral or basic conditions are commonly required for the selective electrochemical reduction of CO 2 , leading to the accumulation of carbonate salts and the generation of formate rather than formic acid. A generalizable strategy for obtaining formic acid (not formate) in the electroreduction of CO 2 with molecular catalysts is introduced, based on controlling acidity gradients using a dual-electrolyte cell with a proton-exchange membrane. This approach uses anodic water oxidation as the source of protons and electrons for CO 2 reduction to formic acid, while mitigating H 2 evolution near the cathode and avoiding carbonate formation. Mechanistic studies, including systems modeling, provide insight into the origin of the formic acid selectivity and guide the broader implementation of this strategy in molecular electrocatalysis for CO 2 utilization.

Alcohols↗