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Showing papers by "Oak Ridge National Laboratory published in 2011"


Journal ArticleDOI
19 Aug 2011-Science
TL;DR: The total forest sink estimate is equivalent in magnitude to the terrestrial sink deduced from fossil fuel emissions and land-use change sources minus ocean and atmospheric sinks, with tropical estimates having the largest uncertainties.
Abstract: The terrestrial carbon sink has been large in recent decades, but its size and location remain uncertain. Using forest inventory data and long-term ecosystem carbon studies, we estimate a total forest sink of 2.4 ± 0.4 petagrams of carbon per year (Pg C year–1) globally for 1990 to 2007. We also estimate a source of 1.3 ± 0.7 Pg C year–1 from tropical land-use change, consisting of a gross tropical deforestation emission of 2.9 ± 0.5 Pg C year–1 partially compensated by a carbon sink in tropical forest regrowth of 1.6 ± 0.5 Pg C year–1. Together, the fluxes comprise a net global forest sink of 1.1 ± 0.8 Pg C year–1, with tropical estimates having the largest uncertainties. Our total forest sink estimate is equivalent in magnitude to the terrestrial sink deduced from fossil fuel emissions and land-use change sources minus ocean and atmospheric sinks.

4,948 citations


Journal ArticleDOI
TL;DR: Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.
Abstract: Platinum-based heterogeneous catalysts are critical to many important commercial chemical processes, but their efficiency is extremely low on a per metal atom basis, because only the surface active-site atoms are used. Catalysts with single-atom dispersions are thus highly desirable to maximize atom efficiency, but making them is challenging. Here we report the synthesis of a single-atom catalyst that consists of only isolated single Pt atoms anchored to the surfaces of iron oxide nanocrystallites. This single-atom catalyst has extremely high atom efficiency and shows excellent stability and high activity for both CO oxidation and preferential oxidation of CO in H-2. Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.

4,446 citations


Journal ArticleDOI
22 Apr 2011-Science
TL;DR: A family of non–precious metal catalysts that approach the performance of platinum-based systems at a cost sustainable for high-power fuel cell applications, possibly including automotive power.
Abstract: The prohibitive cost of platinum for catalyzing the cathodic oxygen reduction reaction (ORR) has hampered the widespread use of polymer electrolyte fuel cells. We describe a family of non-precious metal catalysts that approach the performance of platinum-based systems at a cost sustainable for high-power fuel cell applications, possibly including automotive power. The approach uses polyaniline as a precursor to a carbon-nitrogen template for high-temperature synthesis of catalysts incorporating iron and cobalt. The most active materials in the group catalyze the ORR at potentials within ~60 millivolts of that delivered by state-of-the-art carbon-supported platinum, combining their high activity with remarkable performance stability for non-precious metal catalysts (700 hours at a fuel cell voltage of 0.4 volts) as well as excellent four-electron selectivity (hydrogen peroxide yield <1.0%).

3,464 citations


Journal ArticleDOI
TL;DR: The fourth version of the Community Climate System Model (CCSM4) was recently completed and released to the climate community as mentioned in this paper, which describes developments to all CCSM components, and documents fully coupled preindustrial control runs compared to the previous version.
Abstract: The fourth version of the Community Climate System Model (CCSM4) was recently completed and released to the climate community. This paper describes developments to all CCSM components, and documents fully coupled preindustrial control runs compared to the previous version, CCSM3. Using the standard atmosphere and land resolution of 1° results in the sea surface temperature biases in the major upwelling regions being comparable to the 1.4°-resolution CCSM3. Two changes to the deep convection scheme in the atmosphere component result in CCSM4 producing El Nino–Southern Oscillation variability with a much more realistic frequency distribution than in CCSM3, although the amplitude is too large compared to observations. These changes also improve the Madden–Julian oscillation and the frequency distribution of tropical precipitation. A new overflow parameterization in the ocean component leads to an improved simulation of the Gulf Stream path and the North Atlantic Ocean meridional overturning circulati...

2,835 citations


Journal ArticleDOI
TL;DR: In order to further improve the power and energy densities of the capacitors, carbon-based composites combining electrical double layer capacitors (EDLC)-capacitance and pseudo-Capacitance have been explored and show not only enhanced capacitance, but as well good cyclability.
Abstract: Carbon materials have attracted intense interests as electrode materials for electrochemical capacitors, because of their high surface area, electrical conductivity, chemical stability and low cost. Activated carbons produced by different activation processes from various precursors are the most widely used electrodes. Recently, with the rapid growth of nanotechnology, nanostructured electrode materials, such as carbon nanotubes and template-synthesized porous carbons have been developed. Their unique electrical properties and well controlled pore sizes and structures facilitate fast ion and electron transportation. In order to further improve the power and energy densities of the capacitors, carbon-based composites combining electrical double layer capacitors (EDLC)-capacitance and pseudo-capacitance have been explored. They show not only enhanced capacitance, but as well good cyclability. In this review, recent progresses on carbon-based electrode materials are summarized, including activated carbons, carbon nanotubes, and template-synthesized porous carbons, in particular mesoporous carbons. Their advantages and disadvantages as electrochemical capacitors are discussed. At the end of this review, the future trends of electrochemical capacitors with high energy and power are proposed.

2,497 citations


Journal ArticleDOI
TL;DR: The ENDF/B-VII.1 library as mentioned in this paper is the most widely used data set for nuclear data analysis and has been updated several times over the last five years. But the most recent version of the ENDF-B-VI.0 library is based on the JENDL-4.0 standard.

2,171 citations


Journal ArticleDOI
Jens Kattge1, Sandra Díaz2, Sandra Lavorel3, Iain Colin Prentice4, Paul Leadley5, Gerhard Bönisch1, Eric Garnier3, Mark Westoby4, Peter B. Reich6, Peter B. Reich7, Ian J. Wright4, Johannes H. C. Cornelissen8, Cyrille Violle3, Sandy P. Harrison4, P.M. van Bodegom8, Markus Reichstein1, Brian J. Enquist9, Nadejda A. Soudzilovskaia8, David D. Ackerly10, Madhur Anand11, Owen K. Atkin12, Michael Bahn13, Timothy R. Baker14, Dennis D. Baldocchi10, Renée M. Bekker15, Carolina C. Blanco16, Benjamin Blonder9, William J. Bond17, Ross A. Bradstock18, Daniel E. Bunker19, Fernando Casanoves20, Jeannine Cavender-Bares7, Jeffrey Q. Chambers21, F. S. Chapin22, Jérôme Chave3, David A. Coomes23, William K. Cornwell8, Joseph M. Craine24, B. H. Dobrin9, Leandro da Silva Duarte16, Walter Durka25, James J. Elser26, Gerd Esser27, Marc Estiarte28, William F. Fagan29, Jingyun Fang, Fernando Fernández-Méndez30, Alessandra Fidelis31, Bryan Finegan20, Olivier Flores32, H. Ford33, Dorothea Frank1, Grégoire T. Freschet34, Nikolaos M. Fyllas14, Rachael V. Gallagher4, Walton A. Green35, Alvaro G. Gutiérrez25, Thomas Hickler, Steven I. Higgins36, John G. Hodgson37, Adel Jalili, Steven Jansen38, Carlos Alfredo Joly39, Andrew J. Kerkhoff40, Don Kirkup41, Kaoru Kitajima42, Michael Kleyer43, Stefan Klotz25, Johannes M. H. Knops44, Koen Kramer, Ingolf Kühn16, Hiroko Kurokawa45, Daniel C. Laughlin46, Tali D. Lee47, Michelle R. Leishman4, Frederic Lens48, Tanja Lenz4, Simon L. Lewis14, Jon Lloyd49, Jon Lloyd14, Joan Llusià28, Frédérique Louault50, Siyan Ma10, Miguel D. Mahecha1, Peter Manning51, Tara Joy Massad1, Belinda E. Medlyn4, Julie Messier9, Angela T. Moles52, Sandra Cristina Müller16, Karin Nadrowski53, Shahid Naeem54, Ülo Niinemets55, S. Nöllert1, A. Nüske1, Romà Ogaya28, Jacek Oleksyn56, Vladimir G. Onipchenko57, Yusuke Onoda58, Jenny C. Ordoñez59, Gerhard E. Overbeck16, Wim A. Ozinga59, Sandra Patiño14, Susana Paula60, Juli G. Pausas60, Josep Peñuelas28, Oliver L. Phillips14, Valério D. Pillar16, Hendrik Poorter, Lourens Poorter59, Peter Poschlod61, Andreas Prinzing62, Raphaël Proulx63, Anja Rammig64, Sabine Reinsch65, Björn Reu1, Lawren Sack66, Beatriz Salgado-Negret20, Jordi Sardans28, Satomi Shiodera67, Bill Shipley68, Andrew Siefert69, Enio E. Sosinski70, Jean-François Soussana50, Emily Swaine71, Nathan G. Swenson72, Ken Thompson37, Peter E. Thornton73, Matthew S. Waldram74, Evan Weiher47, Michael T. White75, S. White11, S. J. Wright76, Benjamin Yguel3, Sönke Zaehle1, Amy E. Zanne77, Christian Wirth58 
Max Planck Society1, National University of Cordoba2, Centre national de la recherche scientifique3, Macquarie University4, University of Paris-Sud5, University of Western Sydney6, University of Minnesota7, VU University Amsterdam8, University of Arizona9, University of California, Berkeley10, University of Guelph11, Australian National University12, University of Innsbruck13, University of Leeds14, University of Groningen15, Universidade Federal do Rio Grande do Sul16, University of Cape Town17, University of Wollongong18, New Jersey Institute of Technology19, Centro Agronómico Tropical de Investigación y Enseñanza20, Lawrence Berkeley National Laboratory21, University of Alaska Fairbanks22, University of Cambridge23, Kansas State University24, Helmholtz Centre for Environmental Research - UFZ25, Arizona State University26, University of Giessen27, Autonomous University of Barcelona28, University of Maryland, College Park29, Universidad del Tolima30, University of São Paulo31, University of La Réunion32, University of York33, University of Sydney34, Harvard University35, Goethe University Frankfurt36, University of Sheffield37, University of Ulm38, State University of Campinas39, Kenyon College40, Royal Botanic Gardens41, University of Florida42, University of Oldenburg43, University of Nebraska–Lincoln44, Tohoku University45, Northern Arizona University46, University of Wisconsin–Eau Claire47, Naturalis48, James Cook University49, Institut national de la recherche agronomique50, Newcastle University51, University of New South Wales52, Leipzig University53, Columbia University54, Estonian University of Life Sciences55, Polish Academy of Sciences56, Moscow State University57, Kyushu University58, Wageningen University and Research Centre59, Spanish National Research Council60, University of Regensburg61, University of Rennes62, Université du Québec à Trois-Rivières63, Potsdam Institute for Climate Impact Research64, Technical University of Denmark65, University of California, Los Angeles66, Hokkaido University67, Université de Sherbrooke68, Syracuse University69, Empresa Brasileira de Pesquisa Agropecuária70, University of Aberdeen71, Michigan State University72, Oak Ridge National Laboratory73, University of Leicester74, Utah State University75, Smithsonian Institution76, University of Missouri77
01 Sep 2011
TL;DR: TRY as discussed by the authors is a global database of plant traits, including morphological, anatomical, physiological, biochemical and phenological characteristics of plants and their organs, which can be used for a wide range of research from evolutionary biology, community and functional ecology to biogeography.
Abstract: Plant traits – the morphological, anatomical, physiological, biochemical and phenological characteristics of plants and their organs – determine how primary producers respond to environmental factors, affect other trophic levels, influence ecosystem processes and services and provide a link from species richness to ecosystem functional diversity. Trait data thus represent the raw material for a wide range of research from evolutionary biology, community and functional ecology to biogeography. Here we present the global database initiative named TRY, which has united a wide range of the plant trait research community worldwide and gained an unprecedented buy-in of trait data: so far 93 trait databases have been contributed. The data repository currently contains almost three million trait entries for 69 000 out of the world's 300 000 plant species, with a focus on 52 groups of traits characterizing the vegetative and regeneration stages of the plant life cycle, including growth, dispersal, establishment and persistence. A first data analysis shows that most plant traits are approximately log-normally distributed, with widely differing ranges of variation across traits. Most trait variation is between species (interspecific), but significant intraspecific variation is also documented, up to 40% of the overall variation. Plant functional types (PFTs), as commonly used in vegetation models, capture a substantial fraction of the observed variation – but for several traits most variation occurs within PFTs, up to 75% of the overall variation. In the context of vegetation models these traits would better be represented by state variables rather than fixed parameter values. The improved availability of plant trait data in the unified global database is expected to support a paradigm shift from species to trait-based ecology, offer new opportunities for synthetic plant trait research and enable a more realistic and empirically grounded representation of terrestrial vegetation in Earth system models.

2,017 citations


Journal ArticleDOI
TL;DR: In this article, the components of RFBs with a focus on understanding the underlying physical processes are examined and various transport and kinetic phenomena are discussed along with the most common redox couples.
Abstract: Redox flow batteries (RFBs) are enjoying a renaissance due to their ability to store large amounts of electrical energy relatively cheaply and efficiently. In this review, we examine the components of RFBs with a focus on understanding the underlying physical processes. The various transport and kinetic phenomena are discussed along with the most common redox couples.

1,661 citations


Journal ArticleDOI
TL;DR: The Community Land Model (CLM) as discussed by the authors is the land component of the Community Climate System Model (CCSM) and has been extended with a carbon-nitrogen (CN) biogeochemical model that is prognostic with respect to vegetation, litter, and soil carbon and nitrogen states.
Abstract: [1] The Community Land Model is the land component of the Community Climate System Model. Here, we describe a broad set of model improvements and additions that have been provided through the CLM development community to create CLM4. The model is extended with a carbon-nitrogen (CN) biogeochemical model that is prognostic with respect to vegetation, litter, and soil carbon and nitrogen states and vegetation phenology. An urban canyon model is added and a transient land cover and land use change (LCLUC) capability, including wood harvest, is introduced, enabling study of historic and future LCLUC on energy, water, momentum, carbon, and nitrogen fluxes. The hydrology scheme is modified with a revised numerical solution of the Richards equation and a revised ground evaporation parameterization that accounts for litter and within-canopy stability. The new snow model incorporates the SNow and Ice Aerosol Radiation model (SNICAR) - which includes aerosol deposition, grain-size dependent snow aging, and vertically-resolved snowpack heating – as well as new snow cover and snow burial fraction parameterizations. The thermal and hydrologic properties of organic soil are accounted for and the ground column is extended to ∼50-m depth. Several other minor modifications to the land surface types dataset, grass and crop optical properties, surface layer thickness, roughness length and displacement height, and the disposition of snow-capped runoff are also incorporated. The new model exhibits higher snow cover, cooler soil temperatures in organic-rich soils, greater global river discharge, and lower albedos over forests and grasslands, all of which are improvements compared to CLM3.5. When CLM4 is run with CN, the mean biogeophysical simulation is degraded because the vegetation structure is prognostic rather than prescribed, though running in this mode also allows more complex terrestrial interactions with climate and climate change.

1,295 citations


Journal ArticleDOI
TL;DR: The results firmly show that high power factors can be realized by adjusting the total filling fraction of fillers with different charge states to reach the optimum carrier density, and lattice thermal conductivity can also be significantly reduced, to values near the glass limit of these materials.
Abstract: Skutterudites CoSb3 with multiple cofillers Ba, La, and Yb were synthesized and very high thermoelectric figure of merit ZT = 1.7 at 850 K was realized. X-ray diffraction of the densified multiple-filled bulk samples reveals all samples are phase pure. High-resolution scanning transmission electron microscopy (STEM) and energy dispersive X-ray spectroscopy (EDS) analysis confirm that multiple guest fillers occupy the nanoscale-cages in the skutterudites. The fillers are further shown to be uniformly distributed and the Co−Sb skutterudite framework is virtually unperturbed from atomic scale to a few micrometers. Our results firmly show that high power factors can be realized by adjusting the total filling fraction of fillers with different charge states to reach the optimum carrier density, at the same time, lattice thermal conductivity can also be significantly reduced, to values near the glass limit of these materials, through combining filler species of different rattling frequencies to achieve broad-fr...

1,222 citations


Journal ArticleDOI
TL;DR: An "in-plane" fabrication approach for ultrathin supercapacitors based on electrodes comprised of pristine graphene and multilayer reduced graphene oxide to provide a prototype for a broad range of thin-film based energy storage devices.
Abstract: With the advent of atomically thin and flat layers of conducting materials such as graphene, new designs for thin film energy storage devices with good performance have become possible. Here, we report an “in-plane” fabrication approach for ultrathin supercapacitors based on electrodes comprised of pristine graphene and multilayer reduced graphene oxide. The in-plane design is straightforward to implement and exploits efficiently the surface of each graphene layer for energy storage. The open architecture and the effect of graphene edges enable even the thinnest of devices, made from as grown 1−2 graphene layers, to reach specific capacities up to 80 μFcm−2, while much higher (394 μFcm−2) specific capacities are observed multilayer reduced graphene oxide electrodes. The performances of devices with pristine as well as thicker graphene-based structures are examined using a combination of experiments and model calculations. The demonstrated all solid-state supercapacitors provide a prototype for a broad ran...

Journal ArticleDOI
TL;DR: In this paper, a harmonized set of land-use scenarios is presented that smoothly connects historical reconstructions of land use with future projections, in the format required by ESMs, in preparation for the fifth Assessment Report (AR5) of the Intergovernmental Panel on Climate Change (IPCC).
Abstract: In preparation for the fifth Assessment Report (AR5) of the Intergovernmental Panel on Climate Change (IPCC), the international community is developing new advanced Earth System Models (ESMs) to assess the combined effects of human activities (e.g. land use and fossil fuel emissions) on the carbon-climate system. In addition, four Representative Concentration Pathway (RCP) scenarios of the future (2005–2100) are being provided by four Integrated Assessment Model (IAM) teams to be used as input to the ESMs for future carbon-climate projections (Moss et al. 2010). The diversity of approaches and requirements among IAMs and ESMs for tracking land-use change, along with the dependence of model projections on land-use history, presents a challenge for effectively passing data between these communities and for smoothly transitioning from the historical estimates to future projections. Here, a harmonized set of land-use scenarios are presented that smoothly connects historical reconstructions of land use with future projections, in the format required by ESMs. The land-use harmonization strategy estimates fractional land-use patterns and underlying land-use transitions annually for the time period 1500–2100 at 0.5° × 0.5° resolution. Inputs include new gridded historical maps of crop and pasture data from HYDE 3.1 for 1500–2005, updated estimates of historical national wood harvest and of shifting cultivation, and future information on crop, pasture, and wood harvest from the IAM implementations of the RCPs for the period 2005–2100. The computational method integrates these multiple data sources, while minimizing differences at the transition between the historical reconstruction ending conditions and IAM initial conditions, and working to preserve the future changes depicted by the IAMs at the grid cell level. This study for the first time harmonizes land-use history data together with future scenario information from multiple IAMs into a single consistent, spatially gridded, set of land-use change scenarios for studies of human impacts on the past, present, and future Earth system.

Journal ArticleDOI
TL;DR: Improved constraints are placed on a cosmological origin for the DAMA/LIBRA effect and an irreducible excess of bulklike events below 3 keV in ionization energy are discussed.
Abstract: We report on several features in the energy spectrum from an ultralow-noise germanium detector operated deep underground. By implementing a new technique able to reject surface events, a number of cosmogenic peaks can be observed for the first time. We discuss an irreducible excess of bulklike events below 3 keV in ionization energy. These could be caused by unknown backgrounds, but also dark matter interactions consistent with DAMA/LIBRA. It is not yet possible to determine their origin. Improved constraints are placed on a cosmological origin for the DAMA/LIBRA effect.

Journal ArticleDOI
TL;DR: The structural parameters of fluid phase bilayers composed of phosphatidylcholines with fully saturated, mixed, and branched fatty acid chains, at several temperatures, have been determined by simultaneously analyzing small-angle neutron and X-ray scattering data to assess the effect of temperature and hydrocarbon chain composition on bilayer structure.

Journal ArticleDOI
TL;DR: This work focuses on overcoming recalcitrance with biochemical conversion, which uses low-severity thermochemical pretreatment followed by enzymatic hydrolysis to produce soluble sugars.
Abstract: Plants represent a vast, renewable resource and are well suited to provide sustainably for humankind’s transportation fuel needs. To produce infrastructure-compatible fuels from biomass, two challenges remain: overcoming plant cell wall recalcitrance to extract sugar and phenolic intermediates, and reduction of oxygenated intermediates to fuel molecules. To compete with fossil-based fuels, two primary routes to deconstruct cell walls are under development, namely biochemical and thermochemical conversion. Here, we focus on overcoming recalcitrance with biochemical conversion, which uses low-severity thermochemical pretreatment followed by enzymatic hydrolysis to produce soluble sugars. Many challenges remain, including understanding how pretreatments affect the physicochemical nature of heterogeneous cell walls; determination of how enzymes deconstruct the cell wall effectively with the aim of designing superior catalysts; and resolution of issues associated with the co-optimization of pretreatment, enzymatic hydrolysis, and fermentation. Here, we highlight some of the scientific challenges and open questions with a particular focus on problems across multiple length scales.

Journal ArticleDOI
01 Jul 2011-ACS Nano
TL;DR: Graphene chemical vapor deposition growth on copper foil using methane as a carbon source is strongly affected by hydrogen, which appears to serve a dual role: an activator of the surface bound carbon that is necessary for monolayer growth and an etching reagent that controls the size and morphology of the graphene domains.
Abstract: We show that graphene chemical vapor deposition growth on copper foil using methane as a carbon source is strongly affected by hydrogen, which appears to serve a dual role: an activator of the surface bound carbon that is necessary for monolayer growth and an etching reagent that controls the size and morphology of the graphene domains. The resulting growth rate for a fixed methane partial pressure has a maximum at hydrogen partial pressures 200–400 times that of methane. The morphology and size of the graphene domains, as well as the number of layers, change with hydrogen pressure from irregularly shaped incomplete bilayers to well-defined perfect single layer hexagons. Raman spectra suggest the zigzag termination in the hexagons as more stable than the armchair edges.

Journal ArticleDOI
TL;DR: In this paper, the authors outline the climate forcings and setup of the Met Office Hadley Centre ESM, HadGEM2-ES for the CMIP5 set of centennial experiments.
Abstract: . The scientific understanding of the Earth's climate system, including the central question of how the climate system is likely to respond to human-induced perturbations, is comprehensively captured in GCMs and Earth System Models (ESM). Diagnosing the simulated climate response, and comparing responses across different models, is crucially dependent on transparent assumptions of how the GCM/ESM has been driven – especially because the implementation can involve subjective decisions and may differ between modelling groups performing the same experiment. This paper outlines the climate forcings and setup of the Met Office Hadley Centre ESM, HadGEM2-ES for the CMIP5 set of centennial experiments. We document the prescribed greenhouse gas concentrations, aerosol precursors, stratospheric and tropospheric ozone assumptions, as well as implementation of land-use change and natural forcings for the HadGEM2-ES historical and future experiments following the Representative Concentration Pathways. In addition, we provide details of how HadGEM2-ES ensemble members were initialised from the control run and how the palaeoclimate and AMIP experiments, as well as the "emission-driven" RCP experiments were performed.

Journal ArticleDOI
TL;DR: In this paper, a new annual estimate of anthropogenic global and regional sulfur dioxide emissions has been constructed spanning the period 1850-2005 using a bottom-up mass balance method, calibrated to country-level inventory data.
Abstract: . Sulfur aerosols impact human health, ecosystems, agriculture, and global and regional climate. A new annual estimate of anthropogenic global and regional sulfur dioxide emissions has been constructed spanning the period 1850–2005 using a bottom-up mass balance method, calibrated to country-level inventory data. Global emissions peaked in the early 1970s and decreased until 2000, with an increase in recent years due to increased emissions in China, international shipping, and developing countries in general. An uncertainty analysis was conducted including both random and systemic uncertainties. The overall global uncertainty in sulfur dioxide emissions is relatively small, but regional uncertainties ranged up to 30%. The largest contributors to uncertainty at present are emissions from China and international shipping. Emissions were distributed on a 0.5° grid by sector for use in coordinated climate model experiments.

Journal ArticleDOI
TL;DR: In this article, a detailed lithium de-intercalation mechanism was proposed for high voltage high energy density cathode materials, which showed clear evidence of a new spinel-like solid phase formed on the surface of the electrode materials after high-voltage cycling.
Abstract: High voltage cathode materials Li-excess layered oxide compounds Li[NixLi1/3−2x/3Mn2/3−x/3]O2 (0 < x < 1/2) are investigated in a joint study combining both computational and experimental methods. The bulk and surface structures of pristine and cycled samples of Li[Ni1/5Li1/5Mn3/5]O2 are characterized by synchrotron X-Ray diffraction together with aberration corrected Scanning Transmission Electron Microscopy (a-S/TEM). Electron Energy Loss Spectroscopy (EELS) is carried out to investigate the surface changes of the samples before/after electrochemical cycling. Combining first principles computational investigation with our experimental observations, a detailed lithium de-intercalation mechanism is proposed for this family of Li-excess layered oxides. The most striking characteristics in these high voltage high energy density cathode materials are 1) formation of tetrahedral lithium ions at voltage less than 4.45 V and 2) the transition metal (TM) ions migration leading to phase transformation on the surface of the materials. We show clear evidence of a new spinel-like solid phase formed on the surface of the electrode materials after high-voltage cycling. It is proposed that such surface phase transformation is one of the factors contributing to the first cycle irreversible capacity and the main reason for the intrinsic poor rate capability of these materials.

Journal ArticleDOI
TL;DR: A facile and versatile synthesis using dopamine as a carbon source gives hollow carbon spheres and yolk-shell Au{at}Carbon nanocomposites that endow the products with high structural integrity.
Abstract: A facile and versatile synthesis using dopamine as a carbon source gives hollow carbon spheres and yolk-shell Au{at}Carbon nanocomposites. The uniform nature of dopamine coatings and their high carbon yield endow the products with high structural integrity. The Au{at}C nanocomposites are catalytically active.

Journal ArticleDOI
TL;DR: In this article, a case study of three municipalities in Sydney, Australia in 2008 shows that climate adaptation was widely accepted as an important issue for planning conducted by local governments, but it was yet to be embedded in planning practice which retained a strong mitigation bias in relation to climate change.
Abstract: Municipal planning represents a key avenue for local adaptation, but is subject to recognised constraints. To date, these constraints have focused on simplistic factors such as limited resources and lack of information. In this paper we argue that this focus has obscured a wider set of constraints which need to be acknowledged and addressed if adaptation is likely to advance through municipal planning. Although these recognised constraints are relevant, we argue that what underpins these issues are more fundamental challenges affecting local, placed-based planning by drawing on the related field of community-based environmental planning (CBEP). In considering a wider set of constraints to practical attempts towards adaptation, the paper considers planning based on a case study of three municipalities in Sydney, Australia in 2008. The results demonstrate that climate adaptation was widely accepted as an important issue for planning conducted by local governments. However, it was yet to be embedded in planning practice which retained a strong mitigation bias in relation to climate change. In considering the case study, we draw attention to factors thus far under-acknowledged in the climate adaptation literature. These include leadership, institutional context and competing planning agendas. These factors can serve as constraints or enabling mechanisms for achieving climate adaptation depending upon how they are exploited in any given situation. The paper concludes that, through addressing these issues, local, place-based planning can play a greater role in achieving climate adaptation.

Journal ArticleDOI
TL;DR: The dramatic up-regulation of transcripts coding for small secreted proteins, secreted hydrolytic enzymes, and transporters in planta suggests that they play a role in host infection and nutrient acquisition.
Abstract: Rust fungi are some of the most devastating pathogens of crop plants. They are obligate biotrophs, which extract nutrients only from living plant tissues and cannot grow apart from their hosts. Their lifestyle has slowed the dissection of molecular mechanisms underlying host invasion and avoidance or suppression of plant innate immunity. We sequenced the 101-Mb genome of Melampsora larici-populina, the causal agent of poplar leaf rust, and the 89-Mb genome of Puccinia graminis f. sp. tritici, the causal agent of wheat and barley stem rust. We then compared the 16,399 predicted proteins of M. larici-populina with the 17,773 predicted proteins of P. graminis f. sp tritici. Genomic features related to their obligate biotrophic lifestyle include expanded lineage-specific gene families, a large repertoire of effector-like small secreted proteins, impaired nitrogen and sulfur assimilation pathways, and expanded families of amino acid and oligopeptide membrane transporters. The dramatic up-regulation of transcripts coding for small secreted proteins, secreted hydrolytic enzymes, and transporters in planta suggests that they play a role in host infection and nutrient acquisition. Some of these genomic hallmarks are mirrored in the genomes of other microbial eukaryotes that have independently evolved to infect plants, indicating convergent adaptation to a biotrophic existence inside plant cells.

Journal ArticleDOI
Pelin Yilmaz1, Pelin Yilmaz2, Renzo Kottmann1, Dawn Field, Rob Knight3, Rob Knight4, James R. Cole5, Linda A. Amaral-Zettler6, Jack A. Gilbert7, Jack A. Gilbert8, Jack A. Gilbert9, Ilene Karsch-Mizrachi10, Anjanette Johnston10, Guy Cochrane, Robert Vaughan, Christopher I. Hunter, Joonhong Park11, Norman Morrison12, Philippe Rocca-Serra13, Peter Sterk, Manimozhiyan Arumugam, Mark J. Bailey, Laura K. Baumgartner3, Bruce W. Birren14, Martin J. Blaser15, Vivien Bonazzi10, Timothy F. Booth, Peer Bork, Frederic D. Bushman16, Pier Luigi Buttigieg1, Pier Luigi Buttigieg2, Patrick S. G. Chain17, Patrick S. G. Chain18, Patrick S. G. Chain5, Emily S. Charlson16, Elizabeth K. Costello3, Heather Huot-Creasy19, Peter Dawyndt20, Todd Z. DeSantis21, Noah Fierer3, Jed A. Fuhrman22, Rachel E. Gallery23, Dirk Gevers14, Richard A. Gibbs24, Inigo San Gil25, Antonio Gonzalez3, Jeffrey I. Gordon26, Robert P. Guralnick3, Wolfgang Hankeln2, Wolfgang Hankeln1, Sarah K. Highlander24, Philip Hugenholtz27, Janet K. Jansson17, Janet K. Jansson21, Andrew L. Kau26, Scott T. Kelley28, Jerry Kennedy3, Dan Knights3, Omry Koren29, Justin Kuczynski3, Nikos C. Kyrpides17, Robert Larsen3, Christian L. Lauber3, Teresa M. Legg3, Ruth E. Ley29, Catherine A. Lozupone3, Wolfgang Ludwig30, Donna Lyons3, Eamonn Maguire13, Barbara A. Methé31, Folker Meyer8, Brian D. Muegge26, Sara Nakielny3, Karen E. Nelson31, Diana R. Nemergut3, Josh D. Neufeld32, Lindsay K. Newbold, Anna Oliver, Norman R. Pace3, Giriprakash Palanisamy33, Jörg Peplies, Joseph F. Petrosino24, Lita M. Proctor10, Elmar Pruesse2, Elmar Pruesse1, Christian Quast1, Jeroen Raes34, Sujeevan Ratnasingham35, Jacques Ravel19, David A. Relman36, David A. Relman37, Susanna Assunta-Sansone13, Patrick D. Schloss, Lynn M. Schriml19, Rohini Sinha16, Michelle I. Smith26, Erica Sodergren26, Aymé Spor29, Jesse Stombaugh3, James M. Tiedje5, Doyle V. Ward14, George M. Weinstock26, Doug Wendel3, Owen White19, Andrew S. Whiteley, Andreas Wilke8, Jennifer R. Wortman19, Tanya Yatsunenko26, Frank Oliver Glöckner1, Frank Oliver Glöckner2 
TL;DR: To establish a unified standard for describing sequence data and to provide a single point of entry for the scientific community to access and learn about GSC checklists, the minimum information about any (x) sequence is presented (MIxS).
Abstract: Here we present a standard developed by the Genomic Standards Consortium (GSC) for reporting marker gene sequences—the minimum information about a marker gene sequence (MIMARKS). We also introduce a system for describing the environment from which a biological sample originates. The ‘environmental packages’ apply to any genome sequence of known origin and can be used in combination with MIMARKS and other GSC checklists. Finally, to establish a unified standard for describing sequence data and to provide a single point of entry for the scientific community to access and learn about GSC checklists, we present the minimum information about any (x) sequence (MIxS). Adoption of MIxS will enhance our ability to analyze natural genetic diversity documented by massive DNA sequencing efforts from myriad ecosystems in our ever-changing biosphere.

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TL;DR: Presently available data support the presence of a modulated component of unknown origin, with parameters prima facie compatible with a galactic halo composed of light-mass WIMPs.
Abstract: Fifteen months of cumulative CoGeNT data are examined for indications of an annual modulation, a predicted signature of weakly interacting massive particle (WIMP) interactions. Presently available data support the presence of a modulated component of unknown origin, with parameters prima facie compatible with a galactic halo composed of light-mass WIMPs. Unoptimized estimators yield a statistical significance for a modulation of $\ensuremath{\sim}2.8\ensuremath{\sigma}$, limited by the short exposure.

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TL;DR: Basic ionic liquids based on a phosphonium hydroxide derivative can be tuned for CO{sub 2} capture by varying the weak proton donors, which have different pK{sub a} values.
Abstract: Basic ionic liquids (ILs) based on a phosphonium hydroxide derivative can be tuned for CO{sub 2} capture by varying the weak proton donors, which have different pK{sub a} values. The stability, absorption capacity, and absorption enthalpy of the ILs could be easily tuned: the best IL for CO{sub 2} capture has good stability (>300 C), energy saving (ca. 56 kJ mol{sup -1}), and equimolar absorption capability.

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TL;DR: Free-air CO2 enrichment (FACE) experiments have provided novel insights into the ecological mechanisms controlling the cycling and storage of carbon in terrestrial ecosystems and contribute to our ability to project how ecosystems respond to increasing CO2 in the Earth's atmosphere as discussed by the authors.
Abstract: Free-air CO2 enrichment (FACE) experiments have provided novel insights into the ecological mechanisms controlling the cycling and storage of carbon in terrestrial ecosystems and contribute to our ability to project how ecosystems respond to increasing CO2 in the Earth’s atmosphere. Important lessons emerge by evaluating a set of hypotheses that initially guided the design and longevity of forested FACE experiments. Net primary productivity is increased by elevated CO2, but the response can diminish over time. Carbon accumulation is driven by the distribution of carbon among plant and soil components with differing turnover rates and by interactions between the carbon and nitrogen cycles. Plant community structure may change, but elevated CO2 has only minor effects on microbial community structure. FACE results provide a strong foundation for next-generation experiments in unexplored ecosystems and inform coupled climate-biogeochemical models of the ecological mechanisms controlling ecosystem response to the rising atmospheric CO2 concentration.

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TL;DR: In this paper, the centrality dependence of the chargedparticle multiplicity density at midrapidity in Pb-Pb collisions at root s(NN) = 2: 76 TeV is presented.
Abstract: The centrality dependence of the charged-particle multiplicity density at midrapidity in Pb-Pb collisions at root s(NN) = 2: 76 TeV is presented. The charged-particle density normalized per participating nucleon pair increases by about a factor of 2 from peripheral (70%-80%) to central (0%-5%) collisions. The centrality dependence is found to be similar to that observed at lower collision energies. The data are compared with models based on different mechanisms for particle production in nuclear collisions.

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TL;DR: The design and synthesis of a Pt-bimetallic catalyst with multilayered Pt-skin surface, which shows superior electrocatalytic performance for the oxygen reduction reaction (ORR) and indicates great potential for improving the material properties by fine-tuning of the nanoscale architecture.
Abstract: Advancement in heterogeneous catalysis relies on the capability of altering material structures at the nanoscale, and that is particularly important for the development of highly active electrocatalysts with uncompromised durability. Here, we report the design and synthesis of a Pt-bimetallic catalyst with multilayered Pt-skin surface, which shows superior electrocatalytic performance for the oxygen reduction reaction (ORR). This novel structure was first established on thin film extended surfaces with tailored composition profiles and then implemented in nanocatalysts by organic solution synthesis. Electrochemical studies for the ORR demonstrated that after prolonged exposure to reaction conditions, the Pt-bimetallic catalyst with multilayered Pt-skin surface exhibited an improvement factor of more than 1 order of magnitude in activity versus conventional Pt catalysts. The substantially enhanced catalytic activity and durability indicate great potential for improving the material properties by fine-tunin...

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TL;DR: A novel distance measure, called a weighted DTW (WDTW), which is a penalty-based DTW that penalizes points with higher phase difference between a reference point and a testing point in order to prevent minimum distance distortion caused by outliers is proposed.

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TL;DR: It is found that stream denitrification produces N2O at rates that increase with stream water nitrate (NO3−) concentrations, but that <1% of denitrified N is converted to N1O, and it is suggested that increased stream NO3− loading stimulatesDenitrification and concomitant N2o production, but does not increase the N2 O yield.
Abstract: Nitrous oxide (N2O) is a potent greenhouse gas that contributes to climate change and stratospheric ozone destruction. Anthropogenic nitrogen (N) loading to river networks is a potentially important source of N2O via microbial denitrification that converts N to N2O and dinitrogen (N2). The fraction of denitrified N that escapes as N2O rather than N2 (i.e., the N2O yield) is an important determinant of how much N2O is produced by river networks, but little is known about the N2O yield in flowing waters. Here, we present the results of whole-stream 15N-tracer additions conducted in 72 headwater streams draining multiple land-use types across the United States. We found that stream denitrification produces N2O at rates that increase with stream water nitrate (NO3−) concentrations, but that <1% of denitrified N is converted to N2O. Unlike some previous studies, we found no relationship between the N2O yield and stream water NO3−. We suggest that increased stream NO3− loading stimulates denitrification and concomitant N2O production, but does not increase the N2O yield. In our study, most streams were sources of N2O to the atmosphere and the highest emission rates were observed in streams draining urban basins. Using a global river network model, we estimate that microbial N transformations (e.g., denitrification and nitrification) convert at least 0.68 Tg·y−1 of anthropogenic N inputs to N2O in river networks, equivalent to 10% of the global anthropogenic N2O emission rate. This estimate of stream and river N2O emissions is three times greater than estimated by the Intergovernmental Panel on Climate Change.