Showing papers by "Pacific Northwest National Laboratory published in 2019"
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Northern Arizona University1, National Institutes of Health2, University of Minnesota3, University of California, Davis4, Woods Hole Oceanographic Institution5, Massachusetts Institute of Technology6, University of Copenhagen7, University of Trento8, Chinese Academy of Sciences9, University of California, San Francisco10, University of Pennsylvania11, Pacific Northwest National Laboratory12, North Carolina State University13, University of California, San Diego14, Institute for Systems Biology15, Dalhousie University16, University of British Columbia17, Statens Serum Institut18, Anschutz Medical Campus19, University of Washington20, Michigan State University21, Stanford University22, Harvard University23, Broad Institute24, Australian National University25, University of Düsseldorf26, University of New South Wales27, Sookmyung Women's University28, San Diego State University29, Howard Hughes Medical Institute30, Cornell University31, Max Planck Society32, Colorado State University33, Google34, Syracuse University35, Webster University36, United States Department of Agriculture37, University of Arkansas for Medical Sciences38, Colorado School of Mines39, University of Southern Mississippi40, National Oceanic and Atmospheric Administration41, University of California, Merced42, Wageningen University and Research Centre43, University of Arizona44, Environment Agency45, University of Florida46, Merck & Co.47
TL;DR: QIIME 2 development was primarily funded by NSF Awards 1565100 to J.G.C. and R.K.P. and partial support was also provided by the following: grants NIH U54CA143925 and U54MD012388.
Abstract: QIIME 2 development was primarily funded by NSF Awards 1565100 to J.G.C. and 1565057 to R.K. Partial support was also provided by the following: grants NIH U54CA143925 (J.G.C. and T.P.) and U54MD012388 (J.G.C. and T.P.); grants from the Alfred P. Sloan Foundation (J.G.C. and R.K.); ERCSTG project MetaPG (N.S.); the Strategic Priority Research Program of the Chinese Academy of Sciences QYZDB-SSW-SMC021 (Y.B.); the Australian National Health and Medical Research Council APP1085372 (G.A.H., J.G.C., Von Bing Yap and R.K.); the Natural Sciences and Engineering Research Council (NSERC) to D.L.G.; and the State of Arizona Technology and Research Initiative Fund (TRIF), administered by the Arizona Board of Regents, through Northern Arizona University. All NCI coauthors were supported by the Intramural Research Program of the National Cancer Institute. S.M.G. and C. Diener were supported by the Washington Research Foundation Distinguished Investigator Award.
8,821 citations
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TL;DR: Liu et al. as mentioned in this paper discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg −1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials.
Abstract: State-of-the-art lithium (Li)-ion batteries are approaching their specific energy limits yet are challenged by the ever-increasing demand of today’s energy storage and power applications, especially for electric vehicles. Li metal is considered an ultimate anode material for future high-energy rechargeable batteries when combined with existing or emerging high-capacity cathode materials. However, much current research focuses on the battery materials level, and there have been very few accounts of cell design principles. Here we discuss crucial conditions needed to achieve a specific energy higher than 350 Wh kg−1, up to 500 Wh kg−1, for rechargeable Li metal batteries using high-nickel-content lithium nickel manganese cobalt oxides as cathode materials. We also provide an analysis of key factors such as cathode loading, electrolyte amount and Li foil thickness that impact the cell-level cycle life. Furthermore, we identify several important strategies to reduce electrolyte-Li reaction, protect Li surfaces and stabilize anode architectures for long-cycling high-specific-energy cells. Jun Liu and Battery500 Consortium colleagues contemplate the way forward towards high-energy and long-cycling practical batteries.
1,747 citations
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Broad Institute1, Harvard University2, Baylor College of Medicine3, Pacific Northwest National Laboratory4, University of California, Los Angeles5, University of California, San Diego6, Cincinnati Children's Hospital Medical Center7, Cedars-Sinai Medical Center8, Emory University9, Umeå University10, University of Cincinnati Academic Health Center11, Washington University in St. Louis12, Massachusetts Institute of Technology13
TL;DR: It is demonstrated that periods of disease activity were also marked by increases in temporal variability, with characteristic taxonomic, functional, and biochemical shifts, and integrative analysis identified microbial, biochemical, and host factors central to this dysregulation.
Abstract: Inflammatory bowel diseases, which include Crohn's disease and ulcerative colitis, affect several million individuals worldwide. Crohn's disease and ulcerative colitis are complex diseases that are heterogeneous at the clinical, immunological, molecular, genetic, and microbial levels. Individual contributing factors have been the focus of extensive research. As part of the Integrative Human Microbiome Project (HMP2 or iHMP), we followed 132 subjects for one year each to generate integrated longitudinal molecular profiles of host and microbial activity during disease (up to 24 time points each; in total 2,965 stool, biopsy, and blood specimens). Here we present the results, which provide a comprehensive view of functional dysbiosis in the gut microbiome during inflammatory bowel disease activity. We demonstrate a characteristic increase in facultative anaerobes at the expense of obligate anaerobes, as well as molecular disruptions in microbial transcription (for example, among clostridia), metabolite pools (acylcarnitines, bile acids, and short-chain fatty acids), and levels of antibodies in host serum. Periods of disease activity were also marked by increases in temporal variability, with characteristic taxonomic, functional, and biochemical shifts. Finally, integrative analysis identified microbial, biochemical, and host factors central to this dysregulation. The study's infrastructure resources, results, and data, which are available through the Inflammatory Bowel Disease Multi'omics Database ( http://ibdmdb.org ), provide the most comprehensive description to date of host and microbial activities in inflammatory bowel diseases.
1,385 citations
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TL;DR: The Basis Set Exchange has been rewritten, utilizing modern software design and best practices, and the website updated to use the current generation of web development libraries.
Abstract: The Basis Set Exchange (BSE) has been a prominent fixture in the quantum chemistry community. First publicly available in 2007, it is recognized by both users and basis set creators as the de facto source for information related to basis sets. This popular resource has been rewritten, utilizing modern software design and best practices. The basis set data has been separated into a stand-alone library with an accessible API, and the Web site has been updated to use the current generation of web development libraries. The general layout and workflow of the Web site is preserved, while helpful features requested by the user community have been added. Overall, this design should increase adaptability and lend itself well into the future as a dependable resource for the computational chemistry community. This article will discuss the decision to rewrite the BSE, the new architecture and design, and the new features that have been added.
1,016 citations
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University of New South Wales1, Oregon State University2, Braunschweig University of Technology3, University of California, San Diego4, Norwegian University of Life Sciences5, University of Liverpool6, Max Planck Society7, University of Tasmania8, University of Vermont9, ETH Zurich10, Stazione Zoologica Anton Dohrn11, Montana State University12, University of Amsterdam13, University of Southern California14, Pacific Northwest National Laboratory15, University of Hawaii at Manoa16, University of California, Berkeley17, Marine Biological Laboratory18, University of California, Irvine19, University of Georgia20, California Institute of Technology21, University of Edinburgh22, Ohio State University23, University of Sydney24, University of Alberta25, Georgia Institute of Technology26, Australian Institute of Marine Science27, University of Melbourne28, University of Texas Medical Branch29, University of Queensland30
TL;DR: This Consensus Statement documents the central role and global importance of microorganisms in climate change biology and puts humanity on notice that the impact of climate change will depend heavily on responses of micro organisms, which are essential for achieving an environmentally sustainable future.
Abstract: In the Anthropocene, in which we now live, climate change is impacting most life on Earth. Microorganisms support the existence of all higher trophic life forms. To understand how humans and other life forms on Earth (including those we are yet to discover) can withstand anthropogenic climate change, it is vital to incorporate knowledge of the microbial 'unseen majority'. We must learn not just how microorganisms affect climate change (including production and consumption of greenhouse gases) but also how they will be affected by climate change and other human activities. This Consensus Statement documents the central role and global importance of microorganisms in climate change biology. It also puts humanity on notice that the impact of climate change will depend heavily on responses of microorganisms, which are essential for achieving an environmentally sustainable future.
963 citations
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National Center for Atmospheric Research1, Lawrence Berkeley National Laboratory2, Oak Ridge National Laboratory3, Utrecht University4, Columbia University5, Chinese Academy of Sciences6, University of Houston7, California Institute of Technology8, University of California, Los Angeles9, Institute of Arctic and Alpine Research10, Los Alamos National Laboratory11, Harvard University12, Cooperative Institute for Research in Environmental Sciences13, University of Arizona14, University of Colorado Boulder15, Purdue University16, Michigan State University17, Argonne National Laboratory18, University of Michigan19, Auburn University20, Pacific Northwest National Laboratory21, Goddard Space Flight Center22, University of California, Irvine23, Virginia Tech24, University of Sheffield25
TL;DR: The Community Land Model (CLM) is the land component of the Community Earth System Model (CESM) and is used in several global and regional modeling systems.
Abstract: The Community Land Model (CLM) is the land component of the Community Earth System Model (CESM) and is used in several global and regional modeling systems. In this paper, we introduce model developments included in CLM version 5 (CLM5), which is the default land component for CESM2. We assess an ensemble of simulations, including prescribed and prognostic vegetation state, multiple forcing data sets, and CLM4, CLM4.5, and CLM5, against a range of metrics including from the International Land Model Benchmarking (ILAMBv2) package. CLM5 includes new and updated processes and parameterizations: (1) dynamic land units, (2) updated parameterizations and structure for hydrology and snow (spatially explicit soil depth, dry surface layer, revised groundwater scheme, revised canopy interception and canopy snow processes, updated fresh snow density, simple firn model, and Model for Scale Adaptive River Transport), (3) plant hydraulics and hydraulic redistribution, (4) revised nitrogen cycling (flexible leaf stoichiometry, leaf N optimization for photosynthesis, and carbon costs for plant nitrogen uptake), (5) global crop model with six crop types and time‐evolving irrigated areas and fertilization rates, (6) updated urban building energy, (7) carbon isotopes, and (8) updated stomatal physiology. New optional features include demographically structured dynamic vegetation model (Functionally Assembled Terrestrial Ecosystem Simulator), ozone damage to plants, and fire trace gas emissions coupling to the atmosphere. Conclusive establishment of improvement or degradation of individual variables or metrics is challenged by forcing uncertainty, parametric uncertainty, and model structural complexity, but the multivariate metrics presented here suggest a general broad improvement from CLM4 to CLM5.
661 citations
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TL;DR: A comprehensive review of this field is presented by emphasizing the emerging issues including the predictive design and controllable construction of porous structures and doping configurations, mechanistic understanding from the model catalysts, integrated experimental and theoretical studies, and performance evaluation in full cells.
Abstract: Replacing precious platinum with earth-abundant materials for the oxygen reduction reaction (ORR) in fuel cells has been the objective worldwide for several decades. In the last 10 years, the fastest-growing branch in this area has been carbon-based metal-free ORR electrocatalysts. Great progress has been made in promoting the performance and understanding the underlying fundamentals. Here, a comprehensive review of this field is presented by emphasizing the emerging issues including the predictive design and controllable construction of porous structures and doping configurations, mechanistic understanding from the model catalysts, integrated experimental and theoretical studies, and performance evaluation in full cells. Centering on these topics, the most up-to-date results are presented, along with remarks and perspectives for the future development of carbon-based metal-free ORR electrocatalysts.
642 citations
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TL;DR: It is proposed that the gut microbiota regulates behaviors in mice via production of neuroactive metabolites, suggesting that gut-brain connections contribute to the pathophysiology of ASD.
598 citations
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Chinese Academy of Sciences1, University of California, Los Angeles2, University of Gothenburg3, Ohio State University4, University of Maryland, College Park5, Fudan University6, University of California, Santa Barbara7, Peking University8, Japan Agency for Marine-Earth Science and Technology9, University of Tsukuba10, Nanjing University11, San Diego State University12, University of Twente13, National Center for Atmospheric Research14, Texas A&M University15, Pacific Northwest National Laboratory16, Chengdu University of Information Technology17
TL;DR: The Third Pole (TP) is experiencing rapid warming and is currently in its warmest period in the past 2,000 years as mentioned in this paper, and the latest development in multidisciplinary TP research is reviewed in this paper.
Abstract: The Third Pole (TP) is experiencing rapid warming and is currently in its warmest period in the past 2,000 years. This paper reviews the latest development in multidisciplinary TP research ...
530 citations
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TL;DR: In this article, a fluorinated orthoformate-based electrolyte was used to prevent dendritic Li formation and minimise Li loss and volumetric expansion in Li-metal batteries.
Abstract: Lithium (Li) pulverization and associated large volume expansion during cycling is one of the most critical barriers for the safe operation of Li-metal batteries. Here, we report an approach to minimize the Li pulverization using an electrolyte based on a fluorinated orthoformate solvent. The solid–electrolyte interphase (SEI) formed in this electrolyte clearly exhibits a monolithic feature, which is in sharp contrast with the widely reported mosaic- or multilayer-type SEIs that are not homogeneous and could lead to uneven Li stripping/plating and fast Li and electrolyte depletion over cycling. The highly homogeneous and amorphous SEI not only prevents dendritic Li formation, but also minimizes Li loss and volumetric expansion. Furthermore, this new electrolyte strongly suppresses the phase transformation of the LiNi0.8Co0.1Mn0.1O2 cathode (from layered structure to rock salt) and stabilizes its structure. Tests of high-voltage Li||NMC811 cells show long-term cycling stability and high rate capability, as well as reduced safety concerns. Parasitic reactions between Li metal and electrolytes need to be mitigated in Li-metal batteries. Here, the authors report the use of a fluorinated orthoformate-based electrolyte, leading to a monolithic solid–electrolyte interphase and subsequently a high-performance Li-metal battery.
512 citations
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TL;DR: This review summarizes the latest cutting-edge innovations of lignin chemical valorization with the focus on the aforementioned three key aspects.
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TL;DR: Li et al. as mentioned in this paper proposed an ether-based localized high-concentration electrolyte that can greatly enhance the stability of a Ni-rich LiNi0.8Mn0.1Co 0.1O2 (NMC811) cathode.
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TL;DR: This survey paper aims to offer a detailed overview of existing distributed optimization algorithms and their applications in power systems, and focuses on the application of distributed optimization in the optimal coordination of distributed energy resources.
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TL;DR: Comparative proteomic and phosphoproteomic analysis of paired tumor and normal adjacent tissues produced a catalog of colon cancer-associated proteins and phosphosites, including known and putative new biomarkers, drug targets, and cancer/testis antigens, which suggested glycolysis as a potential target to overcome the resistance of MSI-H tumors to immune checkpoint blockade.
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Lawrence Livermore National Laboratory1, Los Alamos National Laboratory2, University of Houston3, Oak Ridge National Laboratory4, Lawrence Berkeley National Laboratory5, University of Arizona6, Pacific Northwest National Laboratory7, University of British Columbia8, Sandia National Laboratories9, Argonne National Laboratory10, University of Michigan11, University of Wisconsin–Milwaukee12, National Center for Atmospheric Research13, Brookhaven National Laboratory14, University of California, San Diego15, House of Representatives16, Gwangju Institute of Science and Technology17, University of California, Irvine18
TL;DR: Energy Exascale Earth System Model (E3SM) project as mentioned in this paper is a project of the U.S. Department of Energy that aims to develop and validate the E3SM model.
Abstract: Energy Exascale Earth System Model (E3SM) project - U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research; Climate Model Development and Validation activity - Office of Biological and Environmental Research in the US Department of Energy Office of Science; Regional and Global Modeling and Analysis Program of the U.S. Department of Energy, Office of Science, Office of Biological and Environmental Research; National Research Foundation [NRF_2017R1A2b4007480]; Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]; DOE Office of Science User Facility [DE-AC05-00OR22725]; U.S. Department of Energy by Lawrence Livermore National Laboratory [DE-AC52-07NA27344]; DOE [DE-AC05-76RLO1830]; National Center for Atmospheric Research - National Science Foundation [1852977];[DE-SC0012778]
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Pacific Northwest National Laboratory1, Virginia Tech2, Montana State University3, Colorado School of Mines4, Virginia–Maryland Regional College of Veterinary Medicine5, University of Delaware6, Kyushu University7, University of Akron8, University of Georgia9, Arizona State University10, East China Normal University11
TL;DR: The sources and impacts of natural nanomaterials, which are not created directly through human actions; incidental nanom material, which form unintentionally during human activities; and engineered nanomMaterials,Which are created for specific applications are reviewed.
Abstract: BACKGROUND Natural nanomaterials have always been abundant during Earth’s formation and throughout its evolution over the past 4.54 billion years. Incidental nanomaterials, which arise as a by-product from human activity, have become unintentionally abundant since the beginning of the Industrial Revolution. Nanomaterials can also be engineered to have unusual, tunable properties that can be used to improve products in applications from human health to electronics, and in energy, water, and food production. Engineered nanomaterials are very much a recent phenomenon, not yet a century old, and are just a small mass fraction of the natural and incidental varieties. As with natural and incidental nanomaterials, engineered nanomaterials can have both positive and negative consequences in our environment. Despite the ubiquity of nanomaterials on Earth, only in the past 20 years or so have their impacts on the Earth system been studied intensively. This is mostly due to a much better understanding of the distinct behavior of materials at the nanoscale and to multiple advances in analytic techniques. This progress continues to expand rapidly as it becomes clear that nanomaterials are relevant from molecular to planetary dimensions and that they operate from the shortest to the longest time scales over the entire Earth system. ADVANCES Nanomaterials can be defined as any organic, inorganic, or organometallic material that present chemical, physical, and/or electrical properties that change as a function of the size and shape of the material. This behavior is most often observed in the size range between 1 nm up to a few to several tens of nanometers in at least one dimension. These materials have very high proportions of surface atoms relative to interior ones. Also, they are often subject to property variation as a function of size owing to quantum confinement effects. Nanomaterial growth, dissolution or evaporation, surface reactivity, and aggregation states play key roles in their lifetime, behaviors, and local interactions in both natural and engineered environments, often with global consequences. It is now possible to recognize and identify critical roles played by nanomaterials in vital Earth system components, including direct human impact. For example, nanomaterial surfaces may have been responsible for promoting the self-assembly of protocells in the origin of life and in the early evolution of bacterial cell walls. Also, weathering reactions on the continents produce various bioavailable iron (oxy)hydroxide natural and incidental nanomaterials, which are transported to the oceans via riverine and atmospheric pathways and which influence ocean surface primary productivity and thus the global carbon cycle. A third example involves nanomaterials in the atmosphere that travel locally, regionally, and globally. When inhaled, the smallest nanoparticles can pass through the alveolar membranes of the lungs and directly enter the bloodstream. From there, they enter vital organs, including the brain, with possible deleterious consequences. OUTLOOK Earth system nanoscience requires a convergent approach that combines physical, biological, and social sciences, as well as engineering and economic disciplines. This convergence will drive developments for all types of intelligent and anticipatory conceptual models assisted by new analytical techniques and computational simulations. Ultimately, scientists must learn how to recognize key roles of natural, incidental, and engineered nanomaterials in the complex Earth system, so that this understanding can be included in models of Earth processes and Earth history, as well as in ethical considerations regarding their positive and negative effects on present and predicted future environmental and human health issues.
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TL;DR: A unified framework is proposed to clarify the important concepts related to DSE, forecasting-aided state estimation, trackingstate estimation, and static state estimation and provide future research needs and directions for the power engineering community.
Abstract: This paper summarizes the technical activities of the Task Force on Power System Dynamic State and Parameter Estimation. This Task Force was established by the IEEE Working Group on State Estimation Algorithms to investigate the added benefits of dynamic state and parameter estimation for the enhancement of the reliability, security, and resilience of electric power systems. The motivations and engineering values of dynamic state estimation (DSE) are discussed in detail. Then, a set of potential applications that will rely on DSE is presented and discussed. Furthermore, a unified framework is proposed to clarify the important concepts related to DSE, forecasting-aided state estimation, tracking state estimation, and static state estimation. An overview of the current progress in DSE and dynamic parameter estimation is provided. The paper also provides future research needs and directions for the power engineering community.
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TL;DR: Liu et al. as discussed by the authors developed a prototype Li metal pouch cell by integrating a Li metal anode, a LiNi0.6Mn0.2Co 0.2O2 cathode and a compatible electrolyte.
Abstract: Lithium metal anodes have attracted much attention as candidates for high-energy batteries, but there have been few reports of long cycling behaviour, and the degradation mechanism of realistic high-energy Li metal cells remains unclear. Here, we develop a prototypical 300 Wh kg−1 (1.0 Ah) pouch cell by integrating a Li metal anode, a LiNi0.6Mn0.2Co0.2O2 cathode and a compatible electrolyte. Under small uniform external pressure, the cell undergoes 200 cycles with 86% capacity retention and 83% energy retention. In the initial 50 cycles, flat Li foil converts into large Li particles that are entangled in the solid-electrolyte interphase, which leads to rapid volume expansion of the anode (cell thickening of 48%). As cycling continues, the external pressure helps the Li anode maintain good contact between the Li particles, which ensures a conducting percolation pathway for both ions and electrons, and thus the electrochemical reactions continue to occur. Accordingly, the solid Li particles evolve into a porous structure, which manifests in substantially reduced cell swelling by 19% in the subsequent 150 cycles. Much has been said about the high-energy, long-lasting potential of Li metal batteries, and yet little has been demonstrated at the cell scale. Here, Jun Liu and colleagues demonstrate a Li metal pouch cell with a 300 Wh kg−1 energy density and a 200-cycle lifetime.
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TL;DR: A self-smoothing lithium–carbon anode structure based on mesoporous carbon nanofibres, coupled with a lithium nickel–manganese–cobalt oxide cathode with a high nickel content, can lead to a cell-level energy density of 350–380 Wh kg−1 and a stable cycling life up to 200 cycles.
Abstract: Despite considerable efforts to stabilize lithium metal anode structures and prevent dendrite formation, achieving long cycling life in high-energy batteries under realistic conditions remains extremely difficult due to a combination of complex failure modes that involve accelerated anode degradation and the depletion of electrolyte and lithium metal. Here we report a self-smoothing lithium–carbon anode structure based on mesoporous carbon nanofibres, which, coupled with a lithium nickel–manganese–cobalt oxide cathode with a high nickel content, can lead to a cell-level energy density of 350–380 Wh kg−1 (counting all the active and inactive components) and a stable cycling life up to 200 cycles. These performances are achieved under the realistic conditions required for practical high-energy rechargeable lithium metal batteries: cathode loading ≥4.0 mAh cm−2, negative to positive electrode capacity ratio ≤2 and electrolyte weight to cathode capacity ratio ≤3 g Ah−1. The high stability of our anode is due to the amine functionalization and the mesoporous carbon structures that favour smooth lithium deposition. Metallic lithium wets a functionalized mesoporous carbon film to create a self-smoothing anode that, in conjunction with a standard lithium nickel–manganese–cobalt cathode, delivers long cycling life, 350 Wh kg−1 high-energy cells under realistic conditions.
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TL;DR: Of several possible degradation mechanisms, demetalation and carbon oxidation are found to be the most likely reasons for M-N-C catalysts/cathodes degradation.
Abstract: In recent years, significant progress has been achieved in the development of platinum group metal-free (PGM-free) oxygen reduction reaction (ORR) catalysts for proton exchange membrane (PEM) fuel cells. At the same time the limited durability of these catalysts remains a great challenge that needs to be addressed. This mini-review summarizes the recent progress in understanding the main causes of instability of PGM-free ORR catalysts in acidic environments, focusing on transition metal/nitrogen codoped systems (M-N-C catalysts, M: Fe, Co, Mn), particularly MNx moiety active sites. Of several possible degradation mechanisms, demetalation and carbon oxidation are found to be the most likely reasons for M-N-C catalysts/cathodes degradation.
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TL;DR: The vibrational normal modes in a single molecule are imaged using tip-enhanced Raman spectromicroscopy performed in the atomistic near-field, and ångström-scale resolution is attained at subatomic separation between the tip atom and a molecule in the quantum tunnelling regime of plasmons.
Abstract: The internal vibrations of molecules drive the structural transformations that underpin chemistry and cellular function. While vibrational frequencies are measured by spectroscopy, the normal modes of motion are inferred through theory because their visualization would require microscopy with angstrom-scale spatial resolution—nearly three orders of magnitude smaller than the diffraction limit in optics1. Using a metallic tip to focus light and taking advantage of the surface-enhanced Raman effect2 to amplify the signal from individual molecules, tip-enhanced Raman spectromicroscopy (TER-SM)3,4 reaches the requisite sub-molecular spatial resolution5, confirming that light can be confined in picocavities6–10 and anticipating the direct visualization of molecular vibrations11–13. Here, by using TER-SM at the precisely controllable junction of a cryogenic ultrahigh-vacuum scanning tunnelling microscope14–16, we show that angstrom-scale resolution is attained at subatomic separation between the tip atom and a molecule in the quantum tunnelling regime of plasmons6,8,9,17. We record vibrational spectra within a single molecule, obtain images of normal modes and atomically parse the intramolecular charges and currents driven by vibrations. Our analysis provides a paradigm for optics in the atomistic near-field. The vibrational normal modes in a single molecule are imaged using tip-enhanced Raman spectromicroscopy performed in the atomistic near-field.
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TL;DR: This Perspective discussed the best practices for reporting lab-scale performance metrics in battery papers, and explained metrics such as anode energy density, voltage hysteresis, mass of non-active cell components and anode/cathode mass ratio.
Abstract: Batteries have shaped much of our modern world. This success is the result of intense collaboration between academia and industry over the past several decades, culminating with the advent of and improvements in rechargeable lithium-ion batteries. As applications become more demanding, there is the risk that stunted growth in the performance of commercial batteries will slow the adoption of important technologies such as electric vehicles. Yet the scientific literature includes many reports describing material designs with allegedly superior performance. A considerable gap needs to be filled if we wish these laboratory-based achievements to reach commercialization. In this Perspective, we discuss some of the most relevant testing parameters that are often overlooked in academic literature but are critical for practical applicability outside the laboratory. We explain metrics such as anode energy density, voltage hysteresis, mass of non-active cell components and anode/cathode mass ratio, and we make recommendations for future reporting. We hope that this Perspective, together with other similar guiding principles that have recently started to emerge, will aid the transition from lab-scale research to next-generation practical batteries. This Perspective discussed the best practices for reporting lab-scale performance metrics in battery papers.
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University of California, Riverside1, Purdue University2, Pacific Northwest National Laboratory3, Rensselaer Polytechnic Institute4, SUNY Downstate Medical Center5, University of Michigan6, Brown University7, University of Pennsylvania8, University of California, Santa Barbara9, Stanford University10
TL;DR: It is demonstrated that machine learning and multiscale modeling can naturally complement each other to create robust predictive models that integrate the underlying physics to manage ill-posed problems and explore massive design spaces.
Abstract: Fueled by breakthrough technology developments, the biological, biomedical, and behavioral sciences are now collecting more data than ever before. There is a critical need for time- and cost-efficient strategies to analyze and interpret these data to advance human health. The recent rise of machine learning as a powerful technique to integrate multimodality, multifidelity data, and reveal correlations between intertwined phenomena presents a special opportunity in this regard. However, machine learning alone ignores the fundamental laws of physics and can result in ill-posed problems or non-physical solutions. Multiscale modeling is a successful strategy to integrate multiscale, multiphysics data and uncover mechanisms that explain the emergence of function. However, multiscale modeling alone often fails to efficiently combine large datasets from different sources and different levels of resolution. Here we demonstrate that machine learning and multiscale modeling can naturally complement each other to create robust predictive models that integrate the underlying physics to manage ill-posed problems and explore massive design spaces. We review the current literature, highlight applications and opportunities, address open questions, and discuss potential challenges and limitations in four overarching topical areas: ordinary differential equations, partial differential equations, data-driven approaches, and theory-driven approaches. Towards these goals, we leverage expertise in applied mathematics, computer science, computational biology, biophysics, biomechanics, engineering mechanics, experimentation, and medicine. Our multidisciplinary perspective suggests that integrating machine learning and multiscale modeling can provide new insights into disease mechanisms, help identify new targets and treatment strategies, and inform decision making for the benefit of human health.
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TL;DR: A body-centered cubic W-based refractory high entropy alloy with outstanding radiation resistance has been developed, grown as thin films showing a bimodal grain size distribution in the nanocrystalline and ultrafine regimes and a unique 4-nm lamella-like structure revealed by atom probe tomography.
Abstract: A body-centered cubic W-based refractory high entropy alloy with outstanding radiation resistance has been developed. The alloy was grown as thin films showing a bimodal grain size distribution in the nanocrystalline and ultrafine regimes and a unique 4-nm lamella-like structure revealed by atom probe tomography (APT). Transmission electron microscopy (TEM) and x-ray diffraction show certain black spots appearing after thermal annealing at elevated temperatures. TEM and APT analysis correlated the black spots with second-phase particles rich in Cr and V. No sign of irradiation-created dislocation loops, even after 8 dpa, was observed. Furthermore, nanomechanical testing shows a large hardness of 14 GPa in the as-deposited samples, with near negligible irradiation hardening. Theoretical modeling combining ab initio and Monte Carlo techniques predicts the formation of Cr- and V-rich second-phase particles and points at equal mobilities of point defects as the origin of the exceptional radiation tolerance.
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Northern Arizona University1, National Institutes of Health2, University of Minnesota3, University of California, Davis4, Woods Hole Oceanographic Institution5, Massachusetts Institute of Technology6, University of Copenhagen7, University of Trento8, Chinese Academy of Sciences9, University of California, San Francisco10, University of Pennsylvania11, Pacific Northwest National Laboratory12, North Carolina State University13, University of Montana14, Institute for Systems Biology15, Dalhousie University16, University of British Columbia17, Statens Serum Institut18, Anschutz Medical Campus19, University of Washington20, University of California, San Diego21, Michigan State University22, Stanford University23, Broad Institute24, Harvard University25, Australian National University26, University of Düsseldorf27, University of New South Wales28, Sookmyung Women's University29, San Diego State University30, Howard Hughes Medical Institute31, Max Planck Society32, Cornell University33, Colorado State University34, Google35, Syracuse University36, Webster University37, United States Department of Agriculture38, University of Arkansas for Medical Sciences39, Colorado School of Mines40, National Oceanic and Atmospheric Administration41, University of Southern Mississippi42, University of California, Merced43, Wageningen University and Research Centre44, University of Arizona45, Environment Agency46, University of Florida47, Merck & Co.48
TL;DR: An amendment to this paper has been published and can be accessed via a link at the top of the paper.
Abstract: In the version of this article initially published, some reference citations were incorrect. The three references to Jupyter Notebooks should have cited Kluyver et al. instead of Gonzalez et al. The reference to Qiita should have cited Gonzalez et al. instead of Schloss et al. The reference to mothur should have cited Schloss et al. instead of McMurdie & Holmes. The reference to phyloseq should have cited McMurdie & Holmes instead of Huber et al. The reference to Bioconductor should have cited Huber et al. instead of Franzosa et al. And the reference to the biobakery suite should have cited Franzosa et al. instead of Kluyver et al. The errors have been corrected in the HTML and PDF versions of the article.
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TL;DR: In this article, the critical experimental parameters that determine the cycle number of coin cells were investigated to understand the performance variations reported in the literature, and a representative Li-metal pouch cell with specific energy of 300 Wh/kg was exemplified to provide an effective validation of electrode materials and accurate cell performance evaluations.
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TL;DR: A better fundamental understanding of the interfacial reactions during charging and discharging that dictate cell performance has developed and inspired a reevaluation of the use of Li metal anodes in rechargeable batteries.
Abstract: Studies of interfacial reactions and mass transport may allow safe use of lithium metal anodes Conventional rechargeable lithium (Li)–ion batteries generally use graphite as the anode, where Li ions are stored in the layered graphite. However, the use of Li metal as the anode is now being reconsidered. These next-generation battery technologies could potentially double the cell energy of conventional Li-ion batteries (1). Rechargeable Li metal batteries were commercialized more than four decades ago but were in use only briefly because of safety concerns (2). With the advancements of electrolyte (3, 4), electrode architecture (5), and characterization techniques (6) in recent years, a better fundamental understanding of the interfacial reactions during charging and discharging that dictate cell performance has developed and inspired a reevaluation of the use of Li metal anodes in rechargeable batteries.
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University of Bordeaux1, Wichita State University2, University of Manchester3, Mansfield University of Pennsylvania4, Florida State University5, Pacific Northwest National Laboratory6, University of Washington7, Amgen8, University of Natural Resources and Life Sciences, Vienna9, Washington State University10, Loughborough University11, University of Liège12, Florida International University13, Agilent Technologies14, Waters Corporation15, University of Bern16, University of Minnesota17, Vanderbilt University18, French Institute of Health and Medical Research19, Birkbeck, University of London20, West Virginia University21
TL;DR: A guide to ion mobility mass spectrometry experiments, which covers both linear and nonlinear methods: what is measured, how the measurements are done, and how to report the results, including the uncertainties of mobility and collision cross section values.
Abstract: Here we present a guide to ion mobility mass spectrometry experiments, which covers both linear and nonlinear methods: what is measured, how the measurements are done, and how to report the results, including the uncertainties of mobility and collision cross section values. The guide aims to clarify some possibly confusing concepts, and the reporting recommendations should help researchers, authors and reviewers to contribute comprehensive reports, so that the ion mobility data can be reused more confidently. Starting from the concept of the definition of the measurand, we emphasize that (i) mobility values (K0) depend intrinsically on ion structure, the nature of the bath gas, temperature, and E/N; (ii) ion mobility does not measure molecular surfaces directly, but collision cross section (CCS) values are derived from mobility values using a physical model; (iii) methods relying on calibration are empirical (and thus may provide method‐dependent results) only if the gas nature, temperature or E/N cannot match those of the primary method. Our analysis highlights the urgency of a community effort toward establishing primary standards and reference materials for ion mobility, and provides recommendations to do so.
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TL;DR: A coupled redox dynamic that needs to be taken into account when designing high-capacity layered cathode materials for high-voltage lithium-ion batteries is unveiled.
Abstract: Surfaces, interfaces and grain boundaries are classically known to be sinks of defects generated within the bulk lattice. Here, we report an inverse case by which the defects generated at the particle surface are continuously pumped into the bulk lattice. We show that, during operation of a rechargeable battery, oxygen vacancies produced at the surfaces of lithium-rich layered cathode particles migrate towards the inside lattice. This process is associated with a high cutoff voltage at which an anionic redox process is activated. First-principle calculations reveal that triggering of this redox process leads to a sharp decrease of both the formation energy of oxygen vacancies and the migration barrier of oxidized oxide ions, therefore enabling the migration of oxygen vacancies into the bulk lattice of the cathode. This work unveils a coupled redox dynamic that needs to be taken into account when designing high-capacity layered cathode materials for high-voltage lithium-ion batteries.
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Rutgers University1, National Center for Atmospheric Research2, University of Virginia3, Pennsylvania State University4, University of Utah5, University of California, Berkeley6, Boise State University7, Oregon State University8, ETH Zurich9, University at Buffalo10, University of Saskatchewan11, United States Geological Survey12, University of Kansas13, University of California, Santa Barbara14, University of California, Riverside15, Duke University16, University of Arizona17, University of Freiburg18, Ghent University19, University of Bristol20, Northeastern University21, Purdue University22, Pacific Northwest National Laboratory23, University of Colorado Boulder24, Texas A&M University25, University of Washington26, United States Department of Agriculture27, University of California, Merced28, University of Nevada, Reno29, University of Tokyo30
TL;DR: In this paper, the authors bring together hydrologists, critical zone scientists, and ESM developers to explore how hillslope structures may modulate ESM grid-level water, energy, and biogeochemical fluxes.
Abstract: Earth System Models (ESMs) are essential tools for understanding and predicting global change, but they cannot explicitly resolve hillslope‐scale terrain structures that fundamentally organize water, energy, and biogeochemical stores and fluxes at subgrid scales. Here we bring together hydrologists, Critical Zone scientists, and ESM developers, to explore how hillslope structures may modulate ESM grid‐level water, energy, and biogeochemical fluxes. In contrast to the one‐dimensional (1‐D), 2‐ to 3‐m deep, and free‐draining soil hydrology in most ESM land models, we hypothesize that 3‐D, lateral ridge‐to‐valley flow through shallow and deep paths and insolation contrasts between sunny and shady slopes are the top two globally quantifiable organizers of water and energy (and vegetation) within an ESM grid cell. We hypothesize that these two processes are likely to impact ESM predictions where (and when) water and/or energy are limiting. We further hypothesize that, if implemented in ESM land models, these processes will increase simulated continental water storage and residence time, buffering terrestrial ecosystems against seasonal and interannual droughts. We explore efficient ways to capture these mechanisms in ESMs and identify critical knowledge gaps preventing us from scaling up hillslope to global processes. One such gap is our extremely limited knowledge of the subsurface, where water is stored (supporting vegetation) and released to stream baseflow (supporting aquatic ecosystems). We conclude with a set of organizing hypotheses and a call for global syntheses activities and model experiments to assess the impact of hillslope hydrology on global change predictions.