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At least 1,747 records · Page 97

Net-structured Co{sub 3}O{sub 4}/C nanosheet array with enhanced electrochemical performance toward lithium storage

Graphical abstract: - Highlights: • Co{sub 3}O{sub 4}/C nanosheet array on nickel foam was synthesized by hydrothermal method, followed by magnetron sputtering of a carbon layer. • The Co{sub 3}O{sub 4}/C nanosheet array electrode delivers an initial discharge capacity of 1340.4 mAh g{sup −1} at 0.1 C. • After 100 cycles, the capacity retention of the Co{sub 3}O{sub 4}/C is 88.8% of its initial discharge capacity. • The enhanced electrochemical performances are attributed to the porous nanosheet array and the thin carbon layer coated on Co{sub 3}O{sub 4} nanosheets. - Abstract: Freestanding Co{sub 3}O{sub 4}/C nanosheet array growing directly on nickel foam substrate was synthesized using a hydrothermal approach, followed by a direct current magnetron sputtering of a thin carbon layer. The Co{sub 3}O{sub 4} nanosheets with thicknesses of 10–20 nm are interconnected with each other, forming a highly open net-structure. The Co{sub 3}O{sub 4}/C nanosheet array electrode delivers an initial discharge capacity of 1340.4 mAh g{sup −1} at 0.1 C, and maintains a high specific capacity of 912.1 mAh g{sup −1} at room temperature and can still remain 88.8% of its initial discharge capacity at 55 °C at 1 C after 100 cycles. The enhanced electrochemical performances are attributed to the porous nanosheet array and the thin carbon layer coated on Co{sub 3}O{sub 4} nanosheets, which cannot only facilitate Li{sup +} and electron transportation in the electrode, but also improve its structure stability during cycling.

36 MATERIALS SCIENCE↗

Large-scale synthesis of hierarchical-structured weissite (Cu{sub 2−x}Te) flake arrays and their catalytic properties

Graphical abstract: - Highlights: • Large-scale Cu{sub 2−x}Te flake arrays grown on copper foam were synthesized. • They possess superior catalytic efficiency on methylene blue with the assistance of H{sub 2}O{sub 2}. • The effects of preparing conditions on the growth of Cu{sub 2−x}Te flake arrays were investigated. - Abstract: Large-scale weissite (Cu{sub 2−x}Te) flake arrays with three-dimensional (3D) hierarchical structure have been successfully fabricated via a facile one-step solution-phase strategy through the reaction of tellurium powder and copper foam. At the end of the reaction Cu{sub 2−x}Te flakes were distributed evenly on the surface of a porous solid copper substrate. Field-emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM) analysis showed the abundance of flakes grown on the 3D porous copper architecture, while X-ray diffraction (XRD) and energy-dispersive X-ray spectra (EDS) were used to determine the crystal structure and phase composition of these products. A series of experiments discovered that the size and morphology of the products could be affected by some reactive parameters including the reaction time, synthesis temperature and volume ratio of absolute ethanol/deionized water. Catalysis experiments using the in situ synthesized of Cu{sub 2−x}Te flakes to catalyze the degradation of methylene blue (MB) demonstrated the strong catalytic ability of these flakes.

36 MATERIALS SCIENCE↗

Hierarchical NiCo{sub 2}O{sub 4} nanowalls composed of ultrathin nanosheets as electrode materials for supercapacitor and Li ion battery applications

Highlights: • NiCo{sub 2}O{sub 4} nanowalls composed of ultrathin nanosheets are synthesized by solvothermal reaction. • The prepared NiCo{sub 2}O{sub 4} structures possess excellent electrochemical properies. • The hierarchica electrode materials might potential applications for energy storage devices. - Abstract: In this work, NiCo{sub 2}O{sub 4} nanowalls composed of ultrathin nanosheets are fabricated successfully on Ni foam by a facile one-pot solvothermal method followed by thermolysis of the precursors. The as-prepared NiCo{sub 2}O{sub 4} products are evaluated as electrode materials for supercapacitors and lithium ion batteries. The results show high discharge capacitance of 925 mF/cm{sup 2} at a current density of 5 mA/cm{sup 2}, with remarkable cycling stability (about 24.2% loss after 6000 cycles) and excellent rate performance (71.5% capacitance retention with current density range from 1 mA/cm{sup 2} to 20 mA/cm{sup 2}). In addition, Ni foam supported NiCo{sub 2}O{sub 4} nanowalls possess excellent discharge capacity of 1100 mAh/g as lithium ion battery anode at a current density of 100 mA/g. The excellent electrochemical performance of NiCo{sub 2}O{sub 4} nanowalls could be ascribed to the unique spatial structure composed of interconnected ultrathin nanosheets, which facilitates ion penetration and electron transportation, demonstrating their potential applications as electrode materials for high performance supercapacitors and lithium ion batteries.

36 MATERIALS SCIENCE↗

Conversion of Nuclear Waste into Nuclear Waste Glass: Experimental Investigation and Mathematical Modeling

The melter feed, slurry, or calcine charged on the top of a pool of molten glass forms a floating layer of reacting material called the cold cap. Between the cold-cap top, which is covered with boiling slurry, and its bottom, where bubbles separate it from molten glass, the temperature changes by up to 1000 K. The processes that occur over this temperature interval within the cold cap include liberation of gases, conduction and consumption of heat, dissolution of quartz particles, formation and dissolution of intermediate crystalline phases, and generation of foam and gas cavities. These processes have been investigated using thermal analyses, optical and electronic microscopies, x-ray diffraction, as well as other techniques. Properties of the reacting feed, such as heat conductivity and density, were measured as functions of temperature. Investigating the structure of quenched cold caps produced in a laboratory-scale melter complemented the crucible studies. The cold cap consists of two main layers. The top layer contains solid particles dissolving in the glass-forming melt and open pores through which gases are escaping. The bottom layer contains bubbly melt or foam where bubbles coalesce into larger cavities that move sideways and release the gas to the atmosphere. The feed-to-glass conversion became sufficiently understood for representing the cold-cap processes via mathematical models. These models, which comprise heat transfer, mass transfer, and reaction kinetics models, have been developed with the final goal to relate feed parameters to the rate of glass melting.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Exploring strain rate effects upon 3D materials using high speed in situ X-ray tomoscopy

Cellular materials are ubiquitous in our modern society. They may be stochastic gas-blown foams (e.g., polyurethane), foamed starches (e.g., cereals), or, in this case, 3D printed microlattices. Failure in these materials is often driven by surface or sub-surface defects, which may be nucleated at a surface roughness, an interior void, or inclusion interfaces that may not be typically observable. Obfuscating our understanding further, bulk materials are known to exhibit strain-rate-dependent mechanical response, making a subsurface understanding of damage even more critical. For the first time, an in situ uniaxial mechanical loading stage that simultaneously rotates specimens up to 18 Hz was fielded at a synchrotron for 3D tomographic imaging. This capability opens a plethora of materials science opportunities to explore strain rate effects in materials and examining deformation, fracture, and delamination’s (in composites) for a complete 3D picture (movie) of material response. We demonstrate the deformation of 3D printed polymer lattice structures, of three different material types, at 0.25, 1.1, and 2.2 s −1 strain rates. We successfully imaged the 3D deformation of these materials and can directly compare the same printed structure to the three material types at three strain rates, all in 3D. Material point method simulations were applied to one of the materials to better understand the role of voids on the 3D printed structure’s performance.

36 MATERIALS SCIENCE↗

Ritonavir binds to and downregulates estrogen receptors: Molecular mechanism of promoting early atherosclerosis

Estrogenic actions are closely related to cardiovascular disease. Ritonavir (RTV), a human immunodeficiency virus (HIV) protease inhibitor, induces atherosclerosis in an estrogen-related manner. However, how RTV induce pathological phenotypes through estrogen pathway remains unclear. In this study, we found that RTV increases thickness of coronary artery walls of Sprague Dawley rats and plasma free fatty acids (FFA) levels. In addition, RTV could induce foam cell formation, downregulate both estrogen receptor α (ERα) and ERβ expression, upregulate G protein-coupled estrogen receptor (GPER) expression, and all of them could be partially blocked by 17β-estradiol (E2), suggesting RTV acts as an antagonist for E2. Computational modeling shows a similar interaction with ERα between RTV and 2-aryl indoles, which are highly subtype-selective ligands for ERα. We also found that RTV directly bound to ERα and selectively inhibited the nuclear localization of ERα, and residue Leu536 in the hydrophobic core of ligand binding domain (LBD) was essential for the interaction with RTV. In addition, RTV did not change the secondary structure of ERα-LBD like E2, which explained how ERα lost the capacity of nuclear translocation under the treatment of RTV. All of the evidences suggest that ritonavir acts as an antagonist for 17β-estradiol in regulating α subtype estrogen receptor function and early events of atherosclerosis. - Graphical abstract: RTV directly binds to ERα and Leu536 in the hydrophobic core of ligand binding domain is essential for the interaction. - Highlights: • RTV increases the thickness of rat coronary artery wall and foam cell formation. • RTV downregulates the expression of ERα and ERβ. • RTV inhibits ERα promoter activity. • RTV directly binds to ERα and the key amino acid is Leu536. • RTV inhibits the nuclear translocation of ERα and GPER.

60 APPLIED LIFE SCIENCES↗

Dissolving Nonionic Surfactants in CO 2 to Improve Oil Recovery in Unconventional Reservoirs via Wettability Alteration

CO 2 injection is a promising method for enhanced oil recovery (EOR) in unconventional shale reservoirs. Here, in this work, we postulate that CO 2 EOR may be improved by the dissolution of surfactants into CO 2 . Although CO 2 is a relatively good solvent for oil, we show that CO 2 and Eagle Ford oil are immiscible at compositions above 70 wt % CO 2 , even at pressures as high as 62 MPa. The presence of a CO 2 –oil interface at reservoir conditions indicates that the addition of a surfactant has the potential to improve oil recovery–via wettability alteration from oil-wet to CO 2 -wet, CO 2 –oil interfacial tension (IFT) reduction, or both. Three nonionic surfactants (branched tridecyl ethoxylate Indorama SURFONIC TDA-9, branched nonylphenol ethoxylate Indorama SURFONIC N-100, and linear dodecyl ethoxylate Indorama SURFONIC L12-6) were evaluated for CO 2 -solubility, shale wettability alteration, effect on CO 2 –oil IFT, ability to generate CO 2 –oil foams, and ability to increase oil extraction from Eagle Ford, Mancos, and Bakken shale cores. Each surfactant dissolved in CO 2 up to 1 wt % at pressures and temperatures commensurate with CO 2 EOR. CO 2 -dissolved surfactants did not significantly affect CO 2 –oil IFT or generate CO2–oil foams, but they did induce a dramatic change in the contact angle of an oil droplet on an oil-aged shale chip in CO 2 from strongly oil-wet (11°) toward intermediate CO 2 –oil wettability (82°) (at 80 °C, 27.6 MPa). The branched tridecyl ethoxylated surfactant, SURFONIC TDA-9, afforded the highest oil recovery in core soaking experiments–75%, compared to 71% by pure CO 2 . Analysis of oil extracts by gas chromatography revealed that heavier oil components were produced when the surfactant was added to CO 2 . These results indicate that CO 2 -dissolved surfactants may increase oil recovery from shale by wettability alteration from oil-wet toward CO 2 -wet.

04 OIL SHALES AND TAR SANDS↗

Materials Engineering and Scale Up of Fluid Phase Chemical Hydrogen Storage for Automotive Applications

Among candidates for chemical hydrogen storage in PEM fuel cell automotive applications, ammonia borane (AB, NH3BH3) is considered to be one of the most promising materials due to its high hydrogen content of 14-16 wt% below 200°C and high volumetric density. In our previous paper, we selected AB in silicone oil as a role model for a slurry hydrogen storage system. Materials engineering properties were optimized by increasing solid loading by using an ultra-sonic process. In this paper, we proceeded to scale up to liter size batches with solid loadings up to 50 wt% (8 wt% H2) with dynamic viscosities less than 1000cP at 25°C. The use of a non-ionic surfactant, Triton X-15, shows significant promise in controlling the level of foaming produced during the thermal dehydrogenation of the AB. Through the development of new and efficient processing techniques and the ability to adequately control the foaming, stable homogenous slurries of high solid loading have been demonstrated as a viable hydrogen delivery source.

ammonia borane↗

Assessment of Plant and Microalgal Oil-Derived Nonisocyanate Polyurethane Products for Potential Commercialization

Green pathways for nonisocyanate polyurethane (NIPU) production have attracted increasing levels of interest. The reaction between 5-membered cyclic carbonate and polyamines is one of the most promising pathways to produce NIPU polymers. Though promising, major technical hurdles such as slow polymerization rate and poor performance hinder the commercialization of NIPU. In this paper, we screened several commercially available triglyceride oil feedstocks for NIPU products, focusing on polymerization kinetics and product performance for industrial application. The impact of carbonated group density on polymerization rate and mechanical strength was determined. We have demonstrated a remarkably higher reactivity of carbonated oil derived from feedstocks with polyunsaturated fatty acid (PUFA). The NIPU derived from such feedstocks also showed improved performance for industrial application. Unlike traditional polyurethane foam production that uses isocyanate and water to generate CO2 as a blowing reagent, there is no gas formation in NIPU polymerization. We have demonstrated a practical and cost-effective approach to produce NIPU foam material using bicarbonate as a blowing reagent. Furthermore, we conducted the first-ever technoeconomic analysis (TEA), revealing that profitable commercial NIPU production can be achieved when operating at sufficient production capacities.

09 BIOMASS FUELS↗

Low-surface-area hard carbon anode for Na-ion batteries via graphene oxide as a dehydration agent

Na-ion batteries are emerging as one of the most promising energy storage technologies, particularly for grid-level applications. Among anode candidate materials, hard carbon is very attractive due to its high capacity and low cost. However, hard carbon anodes often suffer a low first-cycle Coulombic efficiency and fast capacity fading. In this study, we discover that doping graphene oxide into sucrose, the precursor for hard carbon, can effectively reduce the specific surface area of hard carbon to as low as 5.4 m²/g. We further reveal that such doping can effectively prevent foaming during caramelization of sucrose and extend the pyrolysis burn-off of sucrose caramel over a wider temperature range. Thus, the obtained low-surface-area hard carbon greatly improves the first-cycle Coulombic efficiency from 74% to 83% and delivers a very stable cyclic life with 95% of capacity retention after 200 cycles.

25 ENERGY STORAGE↗

Investigation of Fluoroethylene Carbonate Effects on Tin-based Lithium-Ion Battery Electrodes

Electroless plating of tin on copper foil (2-D) and foams (3-D) was used to create carbon- and binder-free thin films for solid electrolyte interphase (SEI) property investigation. When electrochemically cycled vs lithium metal in coin cells, the foam electrodes exhibited better cycling performance than the planar electrodes due to electrode curvature. The effect of the additive/cosolvent fluoroethylene carbonate (FEC) was found to drastically improve the capacity retention and Coulombic efficiency of the cells. The additive amount of 2% FEC is enough to derive the benefits in the cells at a slow (C/9) cycling rate. The interfacial properties of Sn thin film electrodes in electrolyte with/without FEC additive were investigated using in situ electrochemical quartz crystal microbalance with dissipation (EQCM-D). The processes of the decomposition of the electrolyte on the electrode surface and Li alloying/dealloying with Sn were characterized quantitatively by surface mass change at the molecular level. FEC-containing electrolytes deposited less than electrolyte without FEC on the initial reduction sweep, yet increased the overall thickness/mass of SEI after several cyclic voltammetry cycles. EQCM-D studies demonstrate that the mass accumulated per mole of electrons (mpe) was varied in different voltage ranges, which reveals that the reduction products of the electrolyte with/without FEC are different.

25 ENERGY STORAGE↗

Intramyocardial hemorrhage drives fatty degeneration of infarcted myocardium

Sudden blockage of arteries supplying the heart muscle contributes to millions of heart attacks (myocardial infarction, MI) around the world. Although re-opening these arteries (reperfusion) saves MI patients from immediate death, approximately 50% of these patients go on to develop chronic heart failure (CHF) and die within a 5-year period; however, why some patients accelerate towards CHF while others do not remains unclear. Here we show, using large animal models of reperfused MI, that intramyocardial hemorrhage - the most damaging form of reperfusion injury (evident in nearly 40% of reperfused ST-elevation MI patients) - drives delayed infarct healing and is centrally responsible for continuous fatty degeneration of the infarcted myocardium contributing to adverse remodeling of the heart. Specifically, we show that the fatty degeneration of the hemorrhagic MI zone stems from iron-induced macrophage activation, lipid peroxidation, foam cell formation, ceroid production, foam cell apoptosis and iron recycling. We also demonstrate that timely reduction of iron within the hemorrhagic MI zone reduces fatty infiltration and directs the heart towards favorable remodeling. Collectively, our findings elucidate why some, but not all, MIs are destined to CHF and help define a potential therapeutic strategy to mitigate post-MI CHF independent of MI size.

60 APPLIED LIFE SCIENCES↗

Enhanced solar evaporation of water from porous media, through capillary mediated forces and surface treatment

The relative influence of the capillary, Marangoni, and hydrophobic forces in mediating the evaporation of water from carbon foam based porous media, in response to incident solar radiation, are investigated. It is indicated that inducing hydrophilic interactions on the surface, through nitric acid treatment of the foams, has a similar effect to reduced pore diameter and the ensuing capillary forces. The efficiency of water evaporation may be parameterized through the Capillary number (Ca), with a lower Ca being preferred. The proposed study is of much relevance to efficient solar energy utilization.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Controlling shockwave dynamics using architecture in periodic porous materials

Additive manufacturing (AM) is an attractive approach for the design and fabrication of structures capable of achieving controlled mechanical response of the underlying deformation mechanisms. While there are numerous examples illustrating how the quasi-static mechanical responses of polymer foams have been tailored by additive manufacturing, there is limited understanding of the response of these materials under shockwave compression. Dynamic compression experiments coupled with time-resolved X-ray imaging were performed to obtain insights into the in situ evolution of shockwave coupling to porous, periodic polymer foams. We further demonstrate shock wave modulation or “spatially graded-flow” in shock-driven experiments via the spatial control of layer symmetries afforded by additive manufacturing techniques at the micron scale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Design considerations for indirectly driven double shell capsules

Here, double shell capsules are predicted to ignite and burn at relatively low temperature (~3 keV) via volume ignition and are a potential low-convergence path to substantial α-heating and possibly ignition at the National Ignition Facility. Double shells consist of a dense, high-Z pusher, which first shock heats and then performs work due to changes in pressure and volume (PdV work) on deuterium-tritium gas, bringing the entire fuel volume to high pressure thermonuclear conditions near implosion stagnation. The high-Z pusher is accelerated via a shock and subsequent compression of an intervening foam cushion by an ablatively driven low-Z outer shell. A broad capsule design parameter space exists due to the inherent flexibility of potential materials for the outer and inner shells and foam cushion. This is narrowed down by design physics choices and the ability to fabricate and assemble the separate pieces forming a double shell capsule. We describe the key physics for good double shell performance, the trade-offs in various design choices, and the challenges for capsule fabrication. Finally, both 1D and 2D calculations from radiation-hydrodynamic simulations are presented.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The rate of development of atomic mixing and temperature equilibration in inertial confinement fusion implosions

The MARBLE project is a novel inertial confinement fusion platform for studying the development of atomic mixing and temperature equilibration in inertial confinement fusion implosions and their impact on thermonuclear burn. Experiments involve the laser-driven implosion of capsules filled with deuterated engineered foams whose pores are filled with a gaseous mixture of hydrogen and tritium. By varying the size of the foam pores, we can study the timescale of the development of atomic mix relative to the development of thermal equilibrium between species. In contrast, previous separated reactant experiments have only provided information on the total amount of mix mass. Additionally, we report on the series of MARBLE experiments [first reported in Haines et al., Nat. Commun. 11, 544 (2020)] performed on the University of Rochester's OMEGA laser facility and detailed and highly resolved three-dimensional radiation-hydrodynamic simulations of the implosions. In both the experimental and simulation results, we observe that the reactants do not achieve thermal equilibrium during the course of the implosion except in atomically mixed regions—i.e., that atomic mixing develops faster than thermal equilibration between species. The results suggest that ion temperature variations in the mixture are at least as important as reactant concentration variations for determining the fusion reaction rates.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Development of the Marble experimental platform at the National Ignition Facility

The Marble experimental platform at the National Ignition Facility (NIF) was developed to quantify the influence of heterogeneous mix on fusion burn. The platform utilizes a plastic capsule filled with a deuterated plastic foam of controlled coarseness, with tritium gas filling the voids in the foam. The capsule implosion is driven with x rays generated in an NIF Hohlraum in which the time-dependent symmetry of the implosion can be controlled via dynamic beam phasing. Importantly, the Hohlraum drive conditions can be understood via integrated 2D radiation-hydrodynamic simulations, and capsule implosions can be reliably calculated. After several years of development and experimentation, the NIF Marble platform has become successful and has produced important experimental results. Here, the experimental results, which will be presented in a future publication by the LANL Marble team, provide the first definitive examination of the influence of heterogeneous mix on thermonuclear burn.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Deceleration-stage Rayleigh–Taylor growth in a background magnetic field studied in cylindrical and Cartesian geometries

Experiments have identified the Rayleigh–Taylor (RT) instability as one of the greatest obstacles to achieving inertial confinement fusion. Consequently, mitigation strategies to reduce RT growth and fuel–ablator mixing in the hotspot during the deceleration phase of the implosion are of great interest. In this work, the effect of seed magnetic fields on deceleration-phase RT growth are studied in planar and cylindrical geometries under conditions relevant to the National Ignition Facility (NIF) and Omega experiments. The magnetohydrodynamic (MHD) and resistive-MHD capabilities of the FLASH code are used to model imploding cylinders and planar blast-wave-driven targets. Realistic target and laser parameters are presented that suggest the occurrence of morphological differences in late-time RT evolution in the cylindrical NIF case and a measurable difference in spike height of single-mode growth in the planar NIF case. The results of this study indicate the need for target designs to utilize an RT-unstable foam–foam interface in order to achieve sufficient magnetic field amplification to alter RT evolution. Benchmarked FLASH simulations are used to study these magnetic field effects in both resistive and ideal MHD.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗