Showing papers by "Oak Ridge National Laboratory published in 2014"
TL;DR: This work examined a five-element high-entropy alloy, CrMnFeCoNi, which forms a single-phase face-centered cubic solid solution, and found it to have exceptional damage tolerance with tensile strengths above 1 GPa and fracture toughness values exceeding 200 MPa·m1/2.
Abstract: High-entropy alloys are equiatomic, multi-element systems that can crystallize as a single phase, despite containing multiple elements with different crystal structures. A rationale for this is that the configurational entropy contribution to the total free energy in alloys with five or more major elements may stabilize the solid-solution state relative to multiphase microstructures. We examined a five-element high-entropy alloy, CrMnFeCoNi, which forms a single-phase face-centered cubic solid solution, and found it to have exceptional damage tolerance with tensile strengths above 1 GPa and fracture toughness values exceeding 200 MPa·m(1/2). Furthermore, its mechanical properties actually improve at cryogenic temperatures; we attribute this to a transition from planar-slip dislocation activity at room temperature to deformation by mechanical nanotwinning with decreasing temperature, which results in continuous steady strain hardening.
3,704 citations
TL;DR: Recent developments in genetic engineering, enhanced extraction methods, and a deeper understanding of the structure of lignin are yielding promising opportunities for efficient conversion of this renewable resource to carbon fibers, polymers, commodity chemicals, and fuels.
Abstract: Background Lignin, nature’s dominant aromatic polymer, is found in most terrestrial plants in the approximate range of 15 to 40% dry weight and provides structural integrity. Traditionally, most large-scale industrial processes that use plant polysaccharides have burned lignin to generate the power needed to productively transform biomass. The advent of biorefineries that convert cellulosic biomass into liquid transportation fuels will generate substantially more lignin than necessary to power the operation, and therefore efforts are underway to transform it to value-added products. Production of biofuels from cellulosic biomass requires separation of large quantities of the aromatic polymer lignin. In planta genetic engineering, enhanced extraction methods, and a deeper understanding of the structure of lignin are yielding promising opportunities for efficient conversion of this renewable resource to carbon fibers, polymers, commodity chemicals, and fuels. [Credit: Oak Ridge National Laboratory, U.S. Department of Energy] Advances Bioengineering to modify lignin structure and/or incorporate atypical components has shown promise toward facilitating recovery and chemical transformation of lignin under biorefinery conditions. The flexibility in lignin monomer composition has proven useful for enhancing extraction efficiency. Both the mining of genetic variants in native populations of bioenergy crops and direct genetic manipulation of biosynthesis pathways have produced lignin feedstocks with unique properties for coproduct development. Advances in analytical chemistry and computational modeling detail the structure of the modified lignin and direct bioengineering strategies for targeted properties. Refinement of biomass pretreatment technologies has further facilitated lignin recovery and enables catalytic modifications for desired chemical and physical properties. Outlook Potential high-value products from isolated lignin include low-cost carbon fiber, engineering plastics and thermoplastic elastomers, polymeric foams and membranes, and a variety of fuels and chemicals all currently sourced from petroleum. These lignin coproducts must be low cost and perform as well as petroleum-derived counterparts. Each product stream has its own distinct challenges. Development of renewable lignin-based polymers requires improved processing technologies coupled to tailored bioenergy crops incorporating lignin with the desired chemical and physical properties. For fuels and chemicals, multiple strategies have emerged for lignin depolymerization and upgrading, including thermochemical treatments and homogeneous and heterogeneous catalysis. The multifunctional nature of lignin has historically yielded multiple product streams, which require extensive separation and purification procedures, but engineering plant feedstocks for greater structural homogeneity and tailored functionality reduces this challenge.
2,958 citations
TL;DR: A highly active and durable class of electrocatalysts is synthesized by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals by exploitingThe starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility.
Abstract: Control of structure at the atomic level can precisely and effectively tune catalytic properties of materials, enabling enhancement in both activity and durability. We synthesized a highly active and durable class of electrocatalysts by exploiting the structural evolution of platinum-nickel (Pt-Ni) bimetallic nanocrystals. The starting material, crystalline PtNi3 polyhedra, transforms in solution by interior erosion into Pt3Ni nanoframes with surfaces that offer three-dimensional molecular accessibility. The edges of the Pt-rich PtNi3 polyhedra are maintained in the final Pt3Ni nanoframes. Both the interior and exterior catalytic surfaces of this open-framework structure are composed of the nanosegregated Pt-skin structure, which exhibits enhanced oxygen reduction reaction (ORR) activity. The Pt3Ni nanoframe catalysts achieved a factor of 36 enhancement in mass activity and a factor of 22 enhancement in specific activity, respectively, for this reaction (relative to state-of-the-art platinum-carbon catalysts) during prolonged exposure to reaction conditions.
2,252 citations
TL;DR: A one-step growth strategy for the creation of high-quality vertically stacked as well as in-plane interconnected heterostructures of WS2/MoS2 via control of the growth temperature is reported.
Abstract: Layer-by-layer stacking or lateral interfacing of atomic monolayers has opened up unprecedented opportunities to engineer two-dimensional heteromaterials. Fabrication of such artificial heterostructures with atomically clean and sharp interfaces, however, is challenging. Here, we report a one-step growth strategy for the creation of high-quality vertically stacked as well as in-plane interconnected heterostructures of WS2/MoS2 via control of the growth temperature. Vertically stacked bilayers with WS2 epitaxially grown on top of the MoS2 monolayer are formed with preferred stacking order at high temperature. A strong interlayer excitonic transition is observed due to the type II band alignment and to the clean interface of these bilayers. Vapour growth at low temperature, on the other hand, leads to lateral epitaxy of WS2 on MoS2 edges, creating seamless and atomically sharp in-plane heterostructures that generate strong localized photoluminescence enhancement and intrinsic p-n junctions. The fabrication of heterostructures from monolayers, using simple and scalable growth, paves the way for the creation of unprecedented two-dimensional materials with exciting properties.
1,919 citations
Duke University1, University of Texas at Austin2, Heidelberg Institute for Theoretical Studies3, American Museum of Natural History4, Xi'an Jiaotong University5, Beijing Genomics Institute6, New Mexico State University7, University of Sydney8, University of California9, Uppsala University10, University of Copenhagen11, Okinawa Institute of Science and Technology12, University of Georgia13, Griffith University14, Catalan Institution for Research and Advanced Studies15, Joint Institute for Nuclear Research16, Oak Ridge National Laboratory17, Aarhus University18, Washington University in St. Louis19, University of California, Santa Cruz20, Cardiff University21, Kunming Institute of Zoology22, China Agricultural University23, Louisiana State University24, Tulane University25, Copenhagen Zoo26, Federal University of Pará27, Oregon Health & Science University28, Technical University of Denmark29, Canterbury Museum30, Curtin University31, Novosibirsk State University32, Smithsonian Institution33, National University of Singapore34, National Museum of Natural History35, Nova Southeastern University36, Occidental College37, University of Edinburgh38, Harvard University39, University of California, San Francisco40, University of Florida41, University of Illinois at Urbana–Champaign42
TL;DR: A genome-scale phylogenetic analysis of 48 species representing all orders of Neoaves recovered a highly resolved tree that confirms previously controversial sister or close relationships and identifies the first divergence in Neoaves, two groups the authors named Passerea and Columbea.
Abstract: To better determine the history of modern birds, we performed a genome-scale phylogenetic analysis of 48 species representing all orders of Neoaves using phylogenomic methods created to handle genome-scale data. We recovered a highly resolved tree that confirms previously controversial sister or close relationships. We identified the first divergence in Neoaves, two groups we named Passerea and Columbea, representing independent lineages of diverse and convergently evolved land and water bird species. Among Passerea, we infer the common ancestor of core landbirds to have been an apex predator and confirm independent gains of vocal learning. Among Columbea, we identify pigeons and flamingoes as belonging to sister clades. Even with whole genomes, some of the earliest branches in Neoaves proved challenging to resolve, which was best explained by massive protein-coding sequence convergence and high levels of incomplete lineage sorting that occurred during a rapid radiation after the Cretaceous-Paleogene mass extinction event about 66 million years ago.
1,624 citations
TL;DR: In this article, the most recent advance in the applications of 0D (nanoparticles), 1D(nanowires and nanotubes), and 2D (thin film) silicon nanomaterials in lithium-ion batteries are summarized.
Abstract: There are growing concerns over the environmental, climate, and health impacts caused by using non-renewable fossil fuels. The utilization of green energy, including solar and wind power, is believed to be one of the most promising alternatives to support more sustainable economic growth. In this regard, lithium-ion batteries (LIBs) can play a critically important role. To further increase the energy and power densities of LIBs, silicon anodes have been intensively explored due to their high capacity, low operation potential, environmental friendliness, and high abundance. The main challenges for the practical implementation of silicon anodes, however, are the huge volume variation during lithiation and delithiation processes and the unstable solid-electrolyte interphase (SEI) films. Recently, significant breakthroughs have been achieved utilizing advanced nanotechnologies in terms of increasing cycle life and enhancing charging rate performance due partially to the excellent mechanical properties of nanomaterials, high surface area, and fast lithium and electron transportation. Here, the most recent advance in the applications of 0D (nanoparticles), 1D (nanowires and nanotubes), and 2D (thin film) silicon nanomaterials in LIBs are summarized. The synthetic routes and electrochemical performance of these Si nanomaterials, and the underlying reaction mechanisms are systematically described.
1,365 citations
TL;DR: N nanoscale nickel oxide/nickel heterostructures formed on carbon nanotube sidewalls as highly effective electrocatalysts for hydrogen evolution reaction with activity similar to platinum are reported.
Abstract: There is ongoing research into new electrocatalysts for hydrogen production from water splitting. Here, the authors report the electrocatalytic performance of nickel/nickel oxide heterostructures on carbon nanotubes, and are able to assemble a water electrolyzer operated by a single-cell 1.5 V battery.
1,345 citations
1,265 citations
11 Nov 2014-Nuclear Instruments & Methods in Physics Research Section A-accelerators Spectrometers Detectors and Associated Equipment
TL;DR: The Mantid framework as discussed by the authors is a software solution developed for the analysis and visualization of neutron scattering and muon spin measurements, which is jointly developed by software engineers and scientists at the ISIS Neutron and Muon Facility and the Oak Ridge National Laboratory.
Abstract: The Mantid framework is a software solution developed for the analysis and visualization of neutron scattering and muon spin measurements. The framework is jointly developed by software engineers and scientists at the ISIS Neutron and Muon Facility and the Oak Ridge National Laboratory. The objectives, functionality and novel design aspects of Mantid are described.
1,247 citations
TL;DR: The growth of a highly aligned meta-stable structure of 2,7-dioctyl[1]benzothieno[3,2-b][1] Benzothiophene (C8-BTBT) is described from a blended solution of C8- BTBT and polystyrene by using a novel off-centre spin-coating method, indicating their potential for transparent, high-performance organic electronics.
Abstract: One of the advantages of organic over inorganic semiconductors is they can be grown from solution, but their electrical mobility is often poor. Yuan et al. report a technique for fabricating organic transistors with mobilities far beyond that of amorphous silicon and close to that of polycrystalline silicon.
1,130 citations
TL;DR: L lithiated oxygen terminated MXenes surfaces are able to adsorb additional Li beyond a monolayer, providing a mechanism to substantially increase capacity, as observed mainly in delaminated MXenes and confirmed by DFT calculations and XAS.
Abstract: A combination of density functional theory (DFT) calculations and experiments is used to shed light on the relation between surface structure and Li-ion storage capacities of the following functionalized two-dimensional (2D) transition-metal carbides or MXenes: Sc2C, Ti2C, Ti3C2, V2C, Cr2C, and Nb2C The Li-ion storage capacities are found to strongly depend on the nature of the surface functional groups, with O groups exhibiting the highest theoretical Li-ion storage capacities MXene surfaces can be initially covered with OH groups, removable by high-temperature treatment or by reactions in the first lithiation cycle This was verified by annealing f-Nb2C and f-Ti3C2 at 673 and 773 K in vacuum for 40 h and in situ X-ray adsorption spectroscopy (XAS) and Li capacity measurements for the first lithiation/delithiation cycle of f-Ti3C2 The high-temperature removal of water and OH was confirmed using X-ray diffraction and inelastic neutron scattering The voltage profile and X-ray adsorption near edge struc
TL;DR: In this paper, the authors investigated the short fiber (02 mm to 04 mm) reinforced acrylonitrile-butadiene-styrene composites as a feedstock for 3D-printing in terms of their processibility, microstructure and mechanical performance.
TL;DR: This work presents an alternative approach to plasmonic metasurfaces by replacing the metallic resonators with high-refractive-index silicon cut-wires in combination with a silver ground plane, and demonstrates optical vortex beam generation using a meta-reflectarray with an azimuthally varied phase profile.
Abstract: Plasmonic metasurfaces have recently attracted much attention due to their ability to abruptly change the phase of light, allowing subwavelength optical elements for polarization and wavefront control. However, most previously demonstrated metasurface designs suffer from low coupling efficiency and are based on metallic resonators, leading to ohmic loss. Here, we present an alternative approach to plasmonic metasurfaces by replacing the metallic resonators with high-refractive-index silicon cut-wires in combination with a silver ground plane. We experimentally demonstrate that this meta-reflectarray can be used to realize linear polarization conversion with more than 98% conversion efficiency over a 200 nm bandwidth in the short-wavelength infrared band. We also demonstrate optical vortex beam generation using a meta-reflectarray with an azimuthally varied phase profile. The vortex beam generation is shown to have high efficiency over a wavelength range from 1500 to 1600 nm. The use of dielectric resonato...
TL;DR: It is shown that the dielectric metasurfaces can be engineered to confine the optical field in either the silicon resonator or the environment, allowing one to tailor light-matter interaction at the nanoscale.
Abstract: Metasurface analogues of electromagnetically induced transparency (EIT) have been a focus of the nanophotonics field in recent years, due to their ability to produce high-quality factor (Q-factor) resonances. Such resonances are expected to be useful for applications such as low-loss slow-light devices and highly sensitive optical sensors. However, ohmic losses limit the achievable Q-factors in conventional plasmonic EIT metasurfaces to values <~10, significantly hampering device performance. Here we experimentally demonstrate a classical analogue of EIT using all-dielectric silicon-based metasurfaces. Due to extremely low absorption loss and coherent interaction of neighbouring meta-atoms, a Q-factor of 483 is observed, leading to a refractive index sensor with a figure-of-merit of 103. Furthermore, we show that the dielectric metasurfaces can be engineered to confine the optical field in either the silicon resonator or the environment, allowing one to tailor light-matter interaction at the nanoscale.
TL;DR: In this paper, a class of two-dimensional transition-metal carbides, called MXene nanosheets, are predicted to serve as highperforming anodes for non-lithium-ion batteries by combined first-principles simulations and experimental measurements.
Abstract: Rechargeable non-lithium-ion (Na+, K+, Mg2+, Ca2+, and Al3+) batteries have attracted great attention as emerging low-cost and high energy-density technologies for large-scale renewable energy storage applications. However, the development of these batteries is hindered by the limited choice of high-performance electrode materials. In this work, MXene nanosheets, a class of two-dimensional transition-metal carbides, are predicted to serve as high-performing anodes for non-lithium-ion batteries by combined first-principles simulations and experimental measurements. Both O-terminated and bare MXenes are shown to be promising anode materials with high capacities and good rate capabilities, while bare MXenes show better performance. Our experiments clearly demonstrate the feasibility of Na- and K-ion intercalation into terminated MXenes. Moreover, stable multilayer adsorption is predicted for Mg and Al, which significantly increases their theoretical capacities. We also show that O-terminated MXenes can decom...
Columbia University1, University of California, San Diego2, Michigan State University3, Stanford University4, Georgia Institute of Technology5, Southern Methodist University6, Florida State University7, Nvidia8, University of Colorado Boulder9, University of Edinburgh10, Oak Ridge National Laboratory11, University of California, Santa Cruz12, University of California, Berkeley13, University of Arizona14, Hokkaido University15, ETH Zurich16, American Museum of Natural History17, Princeton University18
TL;DR: Enzo as discussed by the authors uses block-structured adaptive mesh refinement to provide high spatial and temporal resolution for modeling astrophysical fluid flows, which can be run in one, two, and three dimensions, and supports a wide variety of physics, including hydrodynamics, ideal and non-ideal magnetohydrodynamic, N-body dynamics, primordial gas chemistry, optically thin radiative cooling of primordial and metal-enriched plasmas, and models for star formation and feedback in a cosmological context.
Abstract: This paper describes the open-source code Enzo, which uses block-structured adaptive mesh refinement to provide high spatial and temporal resolution for modeling astrophysical fluid flows. The code is Cartesian, can be run in one, two, and three dimensions, and supports a wide variety of physics including hydrodynamics, ideal and non-ideal magnetohydrodynamics, N-body dynamics (and, more broadly, self-gravity of fluids and particles), primordial gas chemistry, optically thin radiative cooling of primordial and metal-enriched plasmas (as well as some optically-thick cooling models), radiation transport, cosmological expansion, and models for star formation and feedback in a cosmological context. In addition to explaining the algorithms implemented, we present solutions for a wide range of test problems, demonstrate the code's parallel performance, and discuss the Enzo collaboration's code development methodology.
TL;DR: The ability to tune the selectivity of graphene through controlled generation of subnanometer pores addresses a significant challenge in the development of advanced nanoporous graphene membranes for nanofiltration, desalination, gas separation, and other applications.
Abstract: We report selective ionic transport through controlled, high-density, subnanometer diameter pores in macroscopic single-layer graphene membranes. Isolated, reactive defects were first introduced into the graphene lattice through ion bombardment and subsequently enlarged by oxidative etching into permeable pores with diameters of 0.40 ± 0.24 nm and densities exceeding 1012 cm–2, while retaining structural integrity of the graphene. Transport measurements across ion-irradiated graphene membranes subjected to in situ etching revealed that the created pores were cation-selective at short oxidation times, consistent with electrostatic repulsion from negatively charged functional groups terminating the pore edges. At longer oxidation times, the pores allowed transport of salt but prevented the transport of a larger organic molecule, indicative of steric size exclusion. The ability to tune the selectivity of graphene through controlled generation of subnanometer pores addresses a significant challenge in the dev...
TL;DR: In this article, three general strategies for accident tolerant fuels are explored: modification of current state-of-the-art zirconium alloy cladding to further improve oxidation resistance (including use of coatings), replacement of Zr Alloy cladding with an alternative oxidation resistant high-performance cladding, and replacement of the monolithic ceramic oxide fuel with alternative fuel forms.
Betty Abelev1, Luke David Hanratty2, M. Esposito3, Edmundo Javier Garcia-Solis4 +940 more•Institutions (90)
TL;DR: The ALICE experiment at the CERN Large Hadron Collider as mentioned in this paper continuously took data during the first physics campaign of the machine from fall 2009 until early 2013, using proton and lead-ion beams.
Abstract: ALICE is the heavy-ion experiment at the CERN Large Hadron Collider. The experiment continuously took data during the first physics campaign of the machine from fall 2009 until early 2013, using proton and lead-ion beams. In this paper we describe the running environment and the data handling procedures, and discuss the performance of the ALICE detectors and analysis methods for various physics observables.
University of Pretoria1, Universidade Católica de Brasília2, Empresa Brasileira de Pesquisa Agropecuária3, United States Department of Energy4, Oak Ridge National Laboratory5, Joint Genome Institute6, Ghent University7, Institut national de la recherche agronomique8, University of Toulouse9, University of British Columbia10, University of Münster11, University of Düsseldorf12, Oregon State University13, Federal University of Rio de Janeiro14, University of São Paulo15, Australian National University16, Indian Institute of Chemical Technology17, University of Arizona18, Universidade Federal de Viçosa19, Universidade Federal do Rio Grande do Sul20, Department of Environment and Primary Industries21, University of Melbourne22, University of Tasmania23, University of the Sunshine Coast24, University of Brasília25
TL;DR: Of 36,376 predicted protein-coding genes, 34% occur in tandem duplications, the largest proportion thus far in plant genomes, which shows the highest diversity of genes for specialized metabolites such as terpenes that act as chemical defence and provide unique pharmaceutical oils.
Abstract: Eucalypts are the world's most widely planted hardwood trees. Their outstanding diversity, adaptability and growth have made them a global renewable resource of fibre and energy. We sequenced and assembled >94% of the 640-megabase genome of Eucalyptus grandis. Of 36,376 predicted protein-coding genes, 34% occur in tandem duplications, the largest proportion thus far in plant genomes. Eucalyptus also shows the highest diversity of genes for specialized metabolites such as terpenes that act as chemical defence and provide unique pharmaceutical oils. Genome sequencing of the E. grandis sister species E. globulus and a set of inbred E. grandis tree genomes reveals dynamic genome evolution and hotspots of inbreeding depression. The E. grandis genome is the first reference for the eudicot order Myrtales and is placed here sister to the eurosids. This resource expands our understanding of the unique biology of large woody perennials and provides a powerful tool to accelerate comparative biology, breeding and biotechnology.
TL;DR: In this article, the authors investigated various binary, ternary and quaternary alloys made from the equiatomic high-entropy alloy FeNiCoCrMn.
TL;DR: In the case of an earlier spring and a later autumn, carbon uptake (photosynthesis) increases considerably more than carbon release (respiration) in temperate forests in the eastern US as mentioned in this paper.
Abstract: The timing of life-history events has a strong impact on ecosystems. Now, analysis of the phenology of temperate forests in the eastern US indicates that in the case of an earlier spring and a later autumn, carbon uptake (photosynthesis) increases considerably more than carbon release (respiration).
TL;DR: An overview of the international efforts on these reactor types carried out in the framework of Generation-IV can be found in this article, where the authors give an overview of international R&D efforts.
Western Kentucky University1, Cooperative Institute for Research in Environmental Sciences2, University of Nebraska–Lincoln3, Purdue University4, University of Queensland5, Pennsylvania State University6, Cooperative Institute for Research in the Atmosphere7, Agriculture and Agri-Food Canada8, John Deere9, Oak Ridge National Laboratory10, University of Alabama in Huntsville11, University of Delaware12, University of Georgia13, Chinese Academy of Sciences14, University of Colorado Boulder15, Texas A&M University16, Tuskegee University17
TL;DR: In this article, the authors provide an overview and synthesis of some of the most notable types of land cover changes and their impacts on climate, including agriculture, deforestation and afforestation, desertification, and urbanization.
Abstract: Land cover changes (LCCs) play an important role in the climate system. Research over recent decades highlights the impacts of these changes on atmospheric temperature, humidity, cloud cover, circulation, and precipitation. These impacts range from the local- and regional-scale to sub-continental and global-scale. It has been found that the impacts of regional-scale LCC in one area may also be manifested in other parts of the world as a climatic teleconnection. In light of these findings, this article provides an overview and synthesis of some of the most notable types of LCC and their impacts on climate. These LCC types include agriculture, deforestation and afforestation, desertification, and urbanization. In addition, this article provides a discussion on challenges to, and future research directions in, assessing the climatic impacts of LCC.
TL;DR: It is shown that 40-nanometre-wide graphene nanoribbons epitaxially grown on silicon carbide are single-channel room-temperature ballistic conductors on a length scale greater than ten micrometres, which is similar to the performance of metallic carbon nanotubes.
Abstract: Graphene nanoribbons will be essential components in future graphene nanoelectronics. However, in typical nanoribbons produced from lithographically patterned exfoliated graphene, the charge carriers travel only about ten nanometres between scattering events, resulting in minimum sheet resistances of about one kilohm per square. Here we show that 40-nanometre-wide graphene nanoribbons epitaxially grown on silicon carbide are single-channel room-temperature ballistic conductors on a length scale greater than ten micrometres, which is similar to the performance of metallic carbon nanotubes. This is equivalent to sheet resistances below 1 ohm per square, surpassing theoretical predictions for perfect graphene by at least an order of magnitude. In neutral graphene ribbons, we show that transport is dominated by two modes. One is ballistic and temperature independent; the other is thermally activated. Transport is protected from back-scattering, possibly reflecting ground-state properties of neutral graphene. At room temperature, the resistance of both modes is found to increase abruptly at a particular length--the ballistic mode at 16 micrometres and the other at 160 nanometres. Our epitaxial graphene nanoribbons will be important not only in fundamental science, but also--because they can be readily produced in thousands--in advanced nanoelectronics, which can make use of their room-temperature ballistic transport properties.
TL;DR: This work investigates the mechanism of oxygen-vacancy-mediated redox pseudocapacitance for a nanostructured lanthanum-based perovskite, LaMnO3, which is the first example of anion-based intercalation pseudocAPacitance as well as the first time oxygen interCalation has been exploited for fast energy storage.
Abstract: Perovskite oxides have attracted significant attention as energy conversion materials for metal-air battery and solid-oxide fuel-cell electrodes owing to their unique physical and electronic properties. Amongst these unique properties is the structural stability of the cation array in perovskites that can accommodate mobile oxygen ions under electrical polarization. Despite oxygen ion mobility and vacancies having been shown to play an important role in catalysis, their role in charge storage has yet to be explored. Herein we investigate the mechanism of oxygen-vacancy-mediated redox pseudocapacitance for a nanostructured lanthanum-based perovskite, LaMnO3. This is the first example of anion-based intercalation pseudocapacitance as well as the first time oxygen intercalation has been exploited for fast energy storage. Whereas previous pseudocapacitor and rechargeable battery charge storage studies have focused on cation intercalation, the anion-based mechanism presented here offers a new paradigm for electrochemical energy storage.
TL;DR: This study shows that the succession of groundwater microbial communities in response to nutrient amendment is primarily stochastic, but that the drivers controlling biodiversity and succession are dynamic rather than static, and identifies the mechanisms controlling microbial community assembly and succession.
Abstract: Unraveling the drivers of community structure and succession in response to environmental change is a central goal in ecology. Although the mechanisms shaping community structure have been intensively examined, those controlling ecological succession remain elusive. To understand the relative importance of stochastic and deterministic processes in mediating microbial community succession, a unique framework composed of four different cases was developed for fluidic and nonfluidic ecosystems. The framework was then tested for one fluidic ecosystem: a groundwater system perturbed by adding emulsified vegetable oil (EVO) for uranium immobilization. Our results revealed that groundwater microbial community diverged substantially away from the initial community after EVO amendment and eventually converged to a new community state, which was closely clustered with its initial state. However, their composition and structure were significantly different from each other. Null model analysis indicated that both deterministic and stochastic processes played important roles in controlling the assembly and succession of the groundwater microbial community, but their relative importance was time dependent. Additionally, consistent with the proposed conceptual framework but contradictory to conventional wisdom, the community succession responding to EVO amendment was primarily controlled by stochastic rather than deterministic processes. During the middle phase of the succession, the roles of stochastic processes in controlling community composition increased substantially, ranging from 81.3% to 92.0%. Finally, there are limited successional studies available to support different cases in the conceptual framework, but further well-replicated explicit time-series experiments are needed to understand the relative importance of deterministic and stochastic processes in controlling community succession.
TL;DR: The addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH)x-(Na or K) ensembles and paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.
Abstract: We report that the addition of alkali ions (sodium or potassium) to gold on KLTL-zeolite and mesoporous MCM-41 silica stabilizes mononuclear gold in Au-O(OH)x-(Na or K) ensembles. This single-site gold species is active for the low-temperature (<200°C) water-gas shift (WGS) reaction. Unexpectedly, gold is thus similar to platinum in creating -O linkages with more than eight alkali ions and establishing an active site on various supports. The intrinsic activity of the single-site gold species is the same on irreducible supports as on reducible ceria, iron oxide, and titania supports, apparently all sharing a common, similarly structured gold active site. This finding paves the way for using earth-abundant supports to disperse and stabilize precious metal atoms with alkali additives for the WGS and potentially other fuel-processing reactions.
TL;DR: In this article, three fundamental options for designing radiation resistance are outlined: Utilize matrix phases with inherent radiation tolerance, select materials in which vacancies are immobile at the design operating temperatures, or engineer materials with high sink densities for point defect recombination.
Abstract: Proposed fusion and advanced (Generation IV) fission energy systems require high-performance materials capable of satisfactory operation up to neutron damage levels approaching 200 atomic displacements per atom with large amounts of transmutant hydrogen and helium isotopes. After a brief overview of fusion reactor concepts and radiation effects phenomena in structural and functional (nonstructural) materials, three fundamental options for designing radiation resistance are outlined: Utilize matrix phases with inherent radiation tolerance, select materials in which vacancies are immobile at the design operating temperatures, or engineer materials with high sink densities for point defect recombination. Environmental and safety considerations impose several additional restrictions on potential materials systems, but reduced-activation ferritic/martensitic steels (including thermomechanically treated and oxide dispersion–strengthened options) and silicon carbide ceramic composites emerge as robust structural...
TL;DR: By adapting the concept of epitaxy to two-dimensional space, this work shows the growth of a single-atomic-layer, in-plane heterostructure of a prototypical material system—graphene and hexagonal boron nitride (h-BN).
Abstract: By adapting the concept of epitaxy to two-dimensional space, we show the growth of a single-atomic-layer, in-plane heterostructure of a prototypical material system--graphene and hexagonal boron nitride (h-BN). Monolayer crystalline h-BN grew from fresh edges of monolayer graphene with atomic lattice coherence, forming an abrupt one-dimensional interface, or boundary. More important, the h-BN lattice orientation is solely determined by the graphene, forgoing configurations favored by the supporting copper substrate.