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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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A Stepwise "Micellization-Crystallization" Route to Oblate Ellipsoidal, Cylindrical, and Bilayer Micelles with Polyethylene Cores in Water
Micellar polymorphism from block copolymers has been well documented, but most attention has focused on noncrystalline hydrophobic systems. We have investigated the micellization in water of model diblock copolymers with semicrystalline polyethylene (PE) as the core-forming component. Poly(N,N-dimethylacrylamide)–polyethylene (AE) diblock copolymers were synthesized by a combination of anionic and RAFT polymerizations. The bulk nanostructures were probed by small-angle X-ray scattering (SAXS) and AE diblock copolymers were found to be moderately segregated at 140 °C. Dispersions of AE amphiphiles in water were prepared by direct dissolution at 120 °C (i.e., above the melting transition of PE) followed by cooling to 25 °C. By manipulating the composition of AE diblock copolymers, discrete structures with oblate ellipsoidal, cylindrical, and bilayer morphologies were produced, as evidenced in cryogenic transmission electron microscopy (cryo-TEM). The self-assembled aggregates were also studied by small-angle neutron scattering (SANS) and dilute solution rheology. The semicrystalline nature of the nanostructures was further revealed by differential scanning calorimetry (DSC) and wide-angle X-ray scattering (WAXS). A stepwise “micellization–crystallization” process was proposed as the micelle formation mechanism, as supported by the existence of similar nanostructures at 120 °C using SANS. This strategy holds promise for a general protocol toward the production of giant wormlike micelles and vesicles with semicrystalline polymeric cores.
Synthesis of Patched or Stacked Graphene and hBN Flakes: A Route to Hybrid Structure Discovery
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Unconventional Route to Encapsulated Ultrasmall Gold Nanoparticles for High-Temperature Catalysis
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A fast quantum route to random numbers
Here, using a quantum computer to speed up one step in a textbook approach to generating random numbers proves to be a savvy strategy, and one that could make good use of quantum computers that will be available in the near future.
High pressure route to generate magnetic monopole dimers in spin ice
The gas of magnetic monopoles in spin ice is governed by one key parameter: the monopole chemical potential. A significant variation of this parameter could access hitherto undiscovered magnetic phenomena arising from monopole correlations, as observed in the analogous electrical Coulomb gas, like monopole dimerization, critical phase separation, or charge ordering. However, all known spin ices have values of chemical potential imposed by their structure and chemistry that place them deeply within the weakly correlated regime, where none of these interesting phenomena occur. Here we use high-pressure synthesis to create a new monopole host, Dy 2 Ge 2 O 7 , with a radically altered chemical potential that stabilizes a large fraction of monopole dimers. The system is found to be ideally described by the classic Debye–Huckel–Bjerrum theory of charge correlations. We thus show how to tune the monopole chemical potential in spin ice and how to access the diverse collective properties of magnetic monopoles.
Anisotropic phase segregation and migration of Pt in nanocrystals en route to nanoframe catalysts
Compositional heterogeneity in shaped, bimetallic nanocrystals offers additional variables to manoeuvre the functionality of the nanocrystal. However, understanding how to manipulate anisotropic elemental distributions in a nanocrystal is a great challenge in reaching higher tiers of nanocatalyst design. In this study, we present the evolutionary trajectory of phase segregation in Pt-Ni rhombic dodecahedra. The anisotropic growth of a Pt-rich phase along the $\langle$111$\rangle$ and $\langle$200$\rangle$ directions at the initial growth stage results in Pt segregation to the 14 axes of a rhombic dodecahedron, forming a highly branched, Pt-rich tetradecapod structure embedded in a Ni-rich shell. With longer growth time, the Pt-rich phase selectively migrates outwards through the 14 axes to the 24 edges such that the rhombic dodecahedron becomes a Pt-rich frame enclosing a Ni-rich interior phase. The revealed anisotropic phase segregation and migration mechanism offers a radically different approach to fabrication of nanocatalysts with desired compositional distributions and performance.
Harnessing strong metal–support interactions via a reverse route
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Drivers and implications of alternative routes to fuels decarbonization in net-zero energy systems
Energy transition scenarios are characterized by increasing electrification and improving efficiency of energy end uses, rapid decarbonization of the electric power sector, and deployment of carbon dioxide removal (CDR) technologies to offset remaining emissions. Although hydrocarbon fuels typically decline in such scenarios, significant volumes remain in many scenarios even at the time of net-zero emissions. While scenarios rely on different approaches for decarbonizing remaining fuels, the underlying drivers for these differences are unclear. Here we develop several illustrative net-zero systems in a simple structural energy model and show that, for a given set of final energy demands, assumptions about the use of biomass and CO2 sequestration drive key differences in how emissions from remaining fuels are mitigated. Limiting one resource may increase reliance on another, implying that decisions about using or restricting resources in pursuit of net-zero objectives could have significant tradeoffs that will need to be evaluated and managed.
A general flame aerosol route to kinetically stabilized metal-organic frameworks
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In-situ thermo-mechano-chemical transformation and consolidation of Sm-Co powders via a single-step route for bulk magnet fabrication
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Nonlocal Coulomb interaction and spin-freezing crossover as a route to valence-skipping charge order
Abstract Multiorbital systems away from global half-filling host intriguing physical properties promoted by Hund’s coupling. Despite increasing awareness of this regime dubbed Hund’s metal, effect of nonlocal interaction is still elusive. Here we study a three-orbital model with 1/3 filling (two electrons per site) including the intersite Coulomb interaction ( V ). Using the G W plus extended dynamical mean-field theory, the valence-skipping charge order transition is shown to be driven by V . Most interestingly, the instability to this transition is significantly enhanced in the spin-freezing crossover regime, thereby lowering the critical V to the formation of charge order. This behavior is found to be closely related to the population profile of the atomic multiplet states in the spin-freezing regime. In this regime, maximum spin states are dominant in each total charge subspace with substantial amount of one- and three-electron occupations, which leads to almost equal population of one- and the maximum spin three-electron state. Our finding unveils another feature of the Hund’s metal and has potential implications for the broad range of multiorbital systems as well as the recently discovered charge order in iron pnictides.
Drought re-routes soil microbial carbon metabolism towards emission of volatile metabolites in an artificial tropical rainforest
Drought impacts on microbial activity can alter soil carbon fate and lead to the loss of stored carbon to the atmosphere as CO 2 and volatile organic compounds (VOCs). Here we examined drought impacts on carbon allocation by soil microbes in the Biosphere 2 artificial tropical rainforest by tracking 13 C from position-specific 13 C-pyruvate into CO 2 and VOCs in parallel with multi-omics. During drought, efflux of 13 C-enriched acetate, acetone and C 4 H 6 O 2 (diacetyl) increased. These changes represent increased production and buildup of intermediate metabolites driven by decreased carbon cycling efficiency. Simultaneously, 13 C-CO 2 efflux decreased, driven by a decrease in microbial activity. However, the microbial carbon allocation to energy gain relative to biosynthesis was unchanged, signifying maintained energy demand for biosynthesis of VOCs and other drought-stress-induced pathways. Overall, while carbon loss to the atmosphere via CO 2 decreased during drought, carbon loss via efflux of VOCs increased, indicating microbially induced shifts in soil carbon fate.
Facile route to bulk ultrafine-grain steels for high strength and ductility
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Prediction of an alternative high-pressure route to polymeric carbon dioxide as a metastable energetic material
The use of pressure to obtain new materials that can be recovered under ambient conditions is a central problem in high-pressure physics. Despite decades of research, this goal has only been achieved in the laboratory for a few notable examples, such as diamond and cubic boron nitride. An area of significant interest is the transformation under compression of light-element molecular compounds to extended covalent-bonded (polymeric) solids. Among them, CO 2 has been extensively studied because of its status as a prototypical simple molecular system with a rich phase diagram and due to its fundamental role in Earth’s physics and chemistry. One of its polymeric crystalline phases, accessible at extreme pressures and temperatures, has been recently quenched to ambient pressure, but below room temperature. Here we report ab initio calculations predicting that isothermal compression of a carbon monoxide and oxygen mixture (CO+O 2 ), rather than the compound CO 2 , lowers the onset of C-polymerization at room temperature from ~ 118 GPa to ~ 7 GPa (complete by ~ 23 GPa). Moreover, it leads to the formation of an intrinsically different polymer with enhanced metastability. We predict that this dense phase is an energetic material which can potentially be recovered to ambient pressure and temperature.
A bottom-up route to enhance thermoelectric figures of merit in graphene nanoribbons
We propose a hybrid nano-structuring scheme for tailoring thermal and thermoelectric transport properties of graphene nanoribbons. Geometrical structuring and isotope cluster engineering are the elements that constitute the proposed scheme. Using first-principles based force constants and Hamiltonians, we show that the thermal conductance of graphene nanoribbons can be reduced by 98.8% at room temperature and the thermoelectric figure of merit, ZT, can be as high as 3.25 at T 5 800 K. The proposed scheme relies on a recently developed bottom-up fabrication method, which is proven to be feasible for synthesizing graphene nanoribbons with an atomic precision.
New route toward building active ruthenium nanoparticles on ordered mesoporous carbons with extremely high stability
Creating highly active and stable metal catalysts is a persistent goal in the field of heterogeneous catalysis. However, a real catalyst can rarely achieve both of these qualities simultaneously due to limitations in the design of the active site and support. One method to circumvent this problem is to fabricate firmly attached metal species onto the voids of a mesoporous support formed simultaneously. In this study, we developed a new type of ruthenium catalyst that was firmly confined by ordered mesoporous carbons through the fabrication of a cubic Ia3d chitosan-ruthenium-silica mesophase before pyrolysis and silica removal. This facile method generates fine ruthenium nanoparticles (ca. 1.7 nm) that are homogeneously dispersed on a mesoporous carbonaceous framework. This ruthenium catalyst can be recycled 22 times without any loss of reactivity, showing the highest stability of any metal catalysts; this catalyst displays a high activity (23.3 molLAh21 gmetal21 ) during the catalytic hydrogenation of levulinic acid (LA) when the metal loading is 6.1 wt%. Even at an ultralow loading (0.3 wt%), this catalyst still outperforms the most active known Ru/C catalyst. This work reveals new possibilities for designing and fabricating highly stable and active metal catalysts by creating metal sites and mesoporous supports simultaneously.
Route to optimal generation of soft X-ray high harmonics with synthesized two-color laser pulses
High harmonics extending to X-rays have been generated from gases by intense lasers. To establish these coherent broadband radiations as an all-purpose tabletop light source for general applications in science and technology, new methods are needed to overcome the present low conversion efficiencies. Here we show that the conversion efficiency may be drastically increased with an optimized two-color pulse. By employing an optimally synthesized 2-mm mid-infrared laser and a small amount of its third harmonic, we show that harmonic yields from sub- to few-keV energy can be increased typically by ten-fold over the optimized single-color one. By combining with favorable phase-matching and together with the emerging high-repetition MHz mid-infrared lasers, we anticipate efficiency of harmonic yields can be increased by four to five orders in the near future, thus paving the way for employing high harmonics as useful broadband tabletop light sources from the extreme ultraviolet to the X-rays, as well as providing new tools for interrogating ultrafast dynamics of matter at attosecond timescales.