Network-Forming Liquids from Metal-Bis(acetamide) Frameworks with Low Melting Temperatures
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99 GENERAL AND MISCELLANEOUS↗
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Liquid Heterostructures: Generation of Liquid–Liquid Interfaces in Free-Flowing Liquid Sheets
Not Available
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Theoretical performance of liquid ammonia, hydrazine, and mixture of liquid ammonia and hydrazine as fuels with liquid oxygen bifluoride as oxidant for rocket engines III : liquid ammonia
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Huff, Vearl N↗
Critical Heat Flux of Liquid Hydrogen, Liquid Methane, and Liquid Oxygen: A Review of Available Data and Predictive Tools
Available experimental data dealing with critical heat flux (CHF) of liquid hydrogen (LH 2 ), liquid methane (LCH 4 ), and liquid oxygen (LO 2 ) in pool and flow boiling are compiled. The compiled data are compared with widely used correlations. Experimental pool boiling CHF data for the aforementioned cryogens are scarce. Based on only 25 data points found in five independent sources, the correlation of Sun and Lienhard (1970) is recommended for predicting the pool CHF of LH 2 . Only two experiments with useful CHF data for the pool boiling of LCH 4 could be found. Four different correlations including the correlation of Lurie and Noyes (1964) can predict the pool boiling CHF of LCH 4 within a factor of two for more than 70% of the data. Furthermore, based on the 19 data points taken from only two available sources, the correlation of Sun and Lienhard (1970) is recommended for the prediction of pool CHF of LO 2 . Flow boiling CHF data for LH 2 could be found in seven experimental studies, five of them from the same source. Based on the 91 data points, it is suggested that the correlation of Katto and Ohno (1984) be used to predict the flow CHF of LH 2 . No useful data could be found for flow boiling CHF of LCH 4 or LO 2 . The available databases for flow boiling of LCH 4 and LO 2 are generally deficient in all boiling regimes. This deficiency is particularly serious with respect to flow boiling.
Multi-Phase Flow↗
Critical Heat Flux of Liquid Hydrogen, Liquid Methane, and Liquid Oxygen: A Review of Available Data and Predictive Tools
Available experimental data dealing with critical heat flux (CHF) of liquid hydrogen (LH2), liquid methane (LCH4), and liquid oxygen (LO2) in pool and flow boiling are compiled. The compiled data are compared with widely used correlations. Experimental pool boiling CHF data for the aforementioned cryogens are scarce. Based on only 25 data points found in five independent sources, the correlation of Sun and Lienhard (1970) is recommended for predicting the pool CHF of LH2. Only two experiments with useful CHF data for the pool boiling of LCH4 could be found. Four different correlations including the correlation of Lurie and Noyes (1964) can predict the pool boiling CHF of LCH4 within a factor of two for more than 70% of the data. Furthermore, based on the 19 data points taken from only two available sources, the correlation of Sun and Lienhard (1970) is recommended for the prediction of pool CHF of LO2. Flow boiling CHF data for LH2 could be found in seven experimental studies, five of them from the same source. Based on the 91 data points, it is suggested that the correlation of Katto and Ohno (1984) be used to predict the flow CHF of LH2. No useful data could be found for flow boiling CHF of LCH4 or LO2. The available databases for flow boiling of LCH4 and LO2 are generally deficient in all boiling regimes. This deficiency is particularly serious with respect to flow boiling.
Multi-Phase Flow↗
Nanodomains and Their Temperature Dependence in a Phosphonium-Based Ionic Liquid: A Single-Molecule Tracking Study
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Opare-Addo, Jemima↗
Solvent effects on extractant conformational energetics in liquid–liquid extraction: a simulation study of molecular solvents and ionic liquids
Extractant design in liquid–liquid extraction (LLE) is a research frontier of metal ion separations that typically focuses on the direct extractant–metal interactions. However, a more detailed understanding of energetic drivers of separations beyond primary metal coordination is often lacking, including the role of solvent in the extractant phase. In this work, we propose a new mechanism for enhancing metal-complexant energetics with nanostructured solvents. Using molecular dynamics simulations with umbrella sampling, we find that the organic solvent can reshape the energetics of the extractant's intramolecular conformational landscape. Here, we calculate free energy profiles of different conformations of a representative bidentate extractant, n-octyl(phenyl)-N,N-diisobutyl carbamoyl methyl phosphinoxide (CMPO), in four different solvents: dodecane, tributyl phosphate (TBP), and dry and wet ionic liquid (IL) 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIM][Tf 2 N]). By promoting reorganization of the extractant molecule into its binding conformation, our findings reveal how particular solvents can ameliorate this unfavorable step of the metal separation process. In particular, the charge alternating nanodomains formed in ILs substantially reduce the free energy penalty associated with extractant reorganization. Importantly, using alchemical free energy calculations, we find that this stabilization persists even when we explicitly include the extracted cation. These findings provide insight into the energetic drivers of metal ion separations and potentially suggest a new approach to designing effective separations using a molecular-level understanding of solvent effects.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Photoresponsive Structured Liquids Enabled by Molecular Recognition at Liquid–Liquid Interfaces
Using host-guest molecular recognition at the oil-water interface, a new type of photoresponsive nanoparticle surfactant (NPS) was designed and prepared to structure liquids. With the help of a polymeric surfactant, the interfacial host-guest interactions can be significantly enhanced, leading to the rapid formation and assembly of a NP monolayer and offering sufficient binding energy to hold the NPs in a jammed state. The assembly of the NPSs can be reversibly manipulated via a photoswitchable jamming-to-unjamming transition, endowing the interface as well as the macroscopic assemblies with responsiveness to the external trigger (photons). Finally, this study for the first time opens a pathway for the construction of multiresponsive, structured all-liquid systems by introducing host-guest chemistry, showing promising potential applications in encapsulation, delivery systems, and unique microfluidic devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Microfluidic liquid-liquid contactor
An assembly comprises a first liquid guide having an inlet, an outlet, and a liquid-conducting layer comprising a first material. The liquid-conducting layer extends between the inlet and the outlet. A second liquid guide has an inlet, an outlet, and a liquid-conducting layer comprising a second material. The liquid-conducting layer extends between the inlet and the outlet. At least a portion of the liquid-conducting layer of the second liquid guide overlaps the liquid-conducting layer of the first liquid guide such that, when a first liquid flows along the liquid-conducting layer of the first liquid guide and a second liquid flows along the liquid-conducting layer of the second liquid guide, the second liquid contacts the first liquid along the portion of the liquid-conducting layer of the second liquid guide that overlaps the liquid-conducting layer of the first liquid guide.
McCulloch, Quinn↗
In situ liquid SIMS analysis of uranium oxide
Trace analysis of nuclear materials in solid particles collected in the environment or particles in liquid slurry generated in nuclear material manufacturing processes can pinpoint elemental, organic, and isotopic signatures of nuclear fuel cycle activities and processes. Such information can support nuclear safeguards programs by increasing our ability to detect undeclared nuclear materials, routine activities for safeguarding at declared facilities, and illicit activities. However, trace radioactive material analysis in liquids and slurries is challenging using bulk approaches. For example, one drawback of sensitive analysis such as inductively coupled plasma mass spectrometry (ICP-MS) is that sample is consumed or destroyed as a result of the technical approach. We developed a vacuum compatible microfluidic interface to enable surface analysis of liquids and liquid-solid interactions using time-of-flight secondary ion mass spectrometry (ToF-SIMS). In this work, we illustrate initial results of liquid standards containing uranium using in situ liquid SIMS. Specifically a series of diluted uranium standards used for ICPMS analysis were studied and the limit of detection was estimated. Since the liquid SIMS analysis is almost nondestructive, the same sample can be analyzed by other more destructive approaches afterwards or saved for future references. Consequently, multimodal analysis is possible. Our results demonstrate that in situ liquid SIMS can be used as a new approach to analyze radioactive materials in liquid and slurry forms of relevance to the IAEA safeguards missions.
In situ liquid ToF-SIMS, uranium, limit of detecti↗
Colloidal Three-Dimensional Covalent Organic Frameworks and Their Application as Porous Liquids
Developing solid porous materials into free-flowing liquids with permanent porosity is a promising strategy for overcoming certain limitations of conventional sorbent materials employed in gas storage and separation applications. The ability to control the pore size and chemical functionalities of organic frameworks gives these particular nanoporous materials distinct advantages over other small cage-like molecules or hollow particles that have been developed into porous liquids. Here, we describe the synthesis of a 3D imine-linked colloidal covalent organic framework (COF)-based porous liquid, designed for efficient size-exclusion of solvent, as well as for long-term stability. By tethering ionic liquids to the colloid surface, the colloids can be dried, purified, and resuspended in a variety of solvents without irreversible aggregation typically observed of COF colloids. Colloid size could be controlled between 50 and 400 nm, with surface areas as high as 800 m2/g. The 3D intertwining morphology of the colloids had pore sizes ranging from 5 to 14 Å, allowing them to efficiently sizeexclude bulky ionic liquids. The COF colloids were stable towards flocculation in an ionic liquid for > 1 year. Permanent porosity was confirmed with a combination of 19F NMR measurements and gas sorption techniques. CO2 and CH4 uptake in these porous liquids increased more than 10 and 20-fold, respectively, over non-porous, neat ionic liquid control samples. The work not only advances the state of COF-based colloid science but also represents a practical advance towards developing more robust, tunable framework-based porous liquid materials for a host of gas storage and separation applications.
Mow, Rachel E.↗
Can a Nuclear-Assisted Biofuels System Enable Liquid Biofuels as the Economic Low-carbon Replacement for All Liquid Fossil Fuels and Hydrocarbon Feedstocks and Enable Negative Carbon Emissions?
This report integrates the results of a series of studies and workshops to address the question: Can a nuclear-assisted biofuels system enable liquid biofuels as the economic low-carbon replacement for all liquid fossil fuels and hydrocarbon feedstocks and simultaneously enable negative carbon emissions? “Economic” is defined as economically competitive relative to other low-carbon replacement options for crude oil. “All” refers to the capability to replace the 18 million barrels of oil per day used by the United States. “Nuclear-assisted” refers to the provision of massive quantities of low-carbon heat and hydrogen at the refinery to fully utilize the carbon content of the cellulosic biomass feedstocks for liquid hydrocarbon production. A system is proposed that decarbonizes about half of the U.S. economy while improving long-term soil productivity and sequestering carbon from the atmosphere. In the U.S. almost half the energy consumed by the final customer is in the form of liquid hydrocarbons produced from crude oil. Liquid hydrocarbons are used as (1) an energy source, (2) a method for daily-to-seasonal energy storage, (3) a chemical feedstock, (4) a chemical reducing agent, (5) a method to enhance high-temperature heat transfer in many furnaces and industrial processes and (6) other purposes. As a consequence, the U.S. consumes ~18 million barrels of crude oil per day to produce liquid hydrocarbons. While there are substitutes for liquid hydrocarbons for some applications, our assessment is that the costs and difficulty will dramatically increase if liquid hydrocarbon use goes much below the equivalent of 10 million barrels per day of crude oil. New uses of liquid hydrocarbons to partly replace coal and natural gas could increase demand beyond the equivalent of 10 million barrels of oil per day. One can produce and burn liquid hydrocarbons from biomass without any net addition of carbon dioxide to the atmosphere. Plants grow by removing carbon dioxide from the atmosphere; thus, burning biomass does not result in any net addition of carbon dioxide to the atmosphere. Biomass is typically 40% oxygen. To remove this oxygen to create hydrocarbon liquids, there are two options. The first option is to use biomass as (1) a feedstock, (2) an energy source to operate the process and (3) a supply of carbon to remove the biomass oxygen as carbon dioxide. The second option is to use external heat and hydrogen to remove the oxygen as water and produce liquid hydrocarbons. The use of massive quantities of external heat and hydrogen for hydrocarbon liquid fuels production reduces the biomass feedstock per unit of liquid hydrocarbon product by more than a factor of two reducing land use by more than a factor of two. Many cellulosic feedstocks unsuitable for liquid hydrocarbon production are viable feedstocks with external heat and hydrogen inputs. As a result, there is sufficient cellulosic feedstocks to meet U.S. and global liquid fuels hydrocarbon demand without significant impacts on food and fiber prices. The heat and hydrogen (heat plus electricity) are produced using base-load nuclear power plants—the most economic form of nuclear energy. If low-price natural gas, there is also the option of producing hydrogen from natural gas with sequestration of the carbon dioxide. The biomass is locally processed in depots to produce commodity feedstocks that can be shipped long distances to large biorefineries (250,000 barrels per day, oil equivalent) similar to existing refineries except modifications of front-end processes. The depot system enables local recycle of nutrients back to the soil. The biorefinery can produce variable quantities of liquid hydrocarbon fuels and carbon dioxide for sequestration enabling removal of carbon dioxide from the atmosphere. Preliminary estimates are that the liquid hydrocarbon costs are equivalent to crude oil at between $60 and $70 per barrel. The largest cost is for hydrogen with biomass feedstocks and refinery costs a smaller fraction of the total cost.
09 BIOMASS FUELS↗
Understanding liquid–liquid equilibria in binary mixtures of hydrocarbons with a thermally robust perarylphosphonium-based ionic liquid
Binary mixtures of hydrocarbons and a thermally robust ionic liquid (IL) incorporating a perarylphosphonium-based cation are investigated experimentally and computationally.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The interaction of an atmospheric pressure plasma jet with liquid water: dimple dynamics and its impact on crystal violet decomposition
Not Available
Kondeti, V. S. Santosh K. (ORCID:000000018825845X)↗
New Insights into Secondary Organic Aerosol Formation at the Air–Liquid Interface
Air-liquid interfacial processing of volatile organic compound oxidation has been suggested as an important source of secondary organic aerosols. However, owing to the lack of techniques for in situ air-liquid interface analysis, the detailed interfacial mechanism remains speculative. To obviate this, the analysis of air-liquid interfacial reactions and the dynamics of glyoxal oxidation as a model volatile organic compound using in situ liquid synchrotron-based vacuum ultraviolet single photon ionization mass spectrometry enabled by the system for analysis at the liquid vacuum interface microreactor is reported. This approach allows for determination of reaction intermediates and oxidation products including polymers and oligomers at the air-liquid interface by mass spectral analysis and appearance energy measurements. Furthermore, an expanded reaction mechanism of photooxidation free radical induced reactions as a source of aqueous secondary organic aerosol formation is proposed based on these new results, suggesting that single photon ionization could be applied to provide unique insights into interfacial chemistry changing the earth atmospheric composition.
aqueous secondary organic aerosol, glyoxal, photoo↗
Role of Bifunctional Ru/Acid Catalysts in the Selective Hydrocracking of Polyethylene and Polypropylene Waste to Liquid Hydrocarbons
Hydrogenolysis of C–C bonds over Ru-based catalysts has emerged as a deconstruction strategy to convert single-use polyolefin waste to liquid alkanes at relatively mild conditions, but this approach exhibits limitations, including methane formation resulting from terminal C–C bond scission. In this study, a variety of catalysts were investigated for the reductive deconstruction of polyethylene (PE) and polypropylene (PP) to identify supports that promote nonterminal C–C bond scission. We found that Ru nanoparticles supported on Brønsted-acidic zeolites with the faujasite (FAU) and Beta (BEA) topologies were highly active for the cleavage of C–C bonds in PE and PP, exhibiting improved liquid yields and suppressed methane formation. For the deconstruction of PE, supporting ruthenium nanoparticles (5 wt %) on FAU increased the yields of liquid alkanes to 67% compared to 33% over an inert silica support (5 wt % Ru/SiO 2 ) at 200 °C, 16 h, under 30 bar of H2. A dramatic selectivity enhancement toward liquid hydrocarbons was also observed for PP over Ru/FAU and Ru/BEA compared to Ru/SiO 2 . To understand the origin of this selectivity improvement, a combination of ex situ and operando characterization techniques were used to reveal that both catalyst structure and acidity play key roles in PE and PP conversion. Operando X-ray absorption spectroscopy studies with model polyolefins over Ru-supported catalysts with varying acidity levels revealed that the local chemical environment of Ru [0] during the reaction is consistent across multiple acidic supports, although the onset of reduction during synthesis of the nanoparticles varies across different supports. These results, combined with reactivity data, demonstrate the importance of the acid-noble metal cooperativity in promoting selective C–C bond scission toward liquid alkanes that shifts the mechanism from hydrogenolysis to ideal hydrocracking.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Chemical and bonding analysis of liquids using liquid cell electron microscopy
Liquid cell transmission electron microscopy (TEM) has become an essential tool for studying the structure and properties of both hard and soft condensed-matter samples, as well as liquids themselves. Liquid cell sample holders, often consisting of two thin window layers separating the liquid sample from the high vacuum of the microscope column, have been designed to control in situ conditions, including temperature, voltage/current, or flow through the window region. While high-resolution and time-resolved TEM imaging probes the structure, shape, and dynamics of liquid cell samples, information about the chemical composition and spatially resolved bonding is often difficult to obtain due to the liquid thickness, the window layers, the holder configuration, or beam-induced radiolysis. Here, we review different approaches to quantitative liquid cell electron microscopy, including recent developments to perform energy-dispersive x-ray and electron energy-loss spectroscopy experiments on samples in a liquid environment or the liquid itself. We also cover graphene liquid cells and other ultrathin window layer holders.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗