14 research outputs found
Gas transport behavior of mixed-matrix membranes composed of silica nanoparticles in a polymer of intrinsic microporosity (PIM-1)
Recently, high-free volume, glassy ladder-type polymers, referred to as polymers of intrinsic microporosity (PIM), have been developed and their reported gas transport performance exceeded the Robeson upper bound trade-off for O2/N2 and CO2/CH4. The present work reports the gas transport behavior of PIM-1/silica nanocomposite membranes. The changes in free volume, as well as the presence and volume of the void cavities, were investigated by analyzing the density, thermal stability, and nano-structural morphology. The enhancement in gas permeability (e.g., He, H2, O2, N2, and CO2) with increasing filler content shows that the trend is related to the true silica volume and void volume fraction.Peer reviewed: YesNRC publication: Ye
Forecasting type-specific seasonal influenza after 26 weeks in the United States using influenza activities in other countries.
To identify countries that have seasonal patterns similar to the time series of influenza surveillance data in the United States and other countries, and to forecast the 2018-2019 seasonal influenza outbreak in the U.S., we collected the surveillance data of 164 countries using the FluNet database, search queries from Google Trends, and temperature from 2010 to 2018. Data for influenza-like illness (ILI) in the U.S. were collected from the Fluview database. We identified the time lag between two time-series which were weekly surveillances for ILI, total influenza (Total INF), influenza A (INF A), and influenza B (INF B) viruses between two countries using cross-correlation analysis. In order to forecast ILI, Total INF, INF A, and INF B of next season (after 26 weeks) in the U.S., we developed prediction models using linear regression, auto regressive integrated moving average, and an artificial neural network (ANN). As a result of cross-correlation analysis between the countries located in northern and southern hemisphere, the seasonal influenza patterns in Australia and Chile showed a high correlation with those of the U.S. 22 weeks and 28 weeks earlier, respectively. The R2 score of ANN models for ILI for validation set in 2015-2019 was 0.758 despite how hard it is to forecast 26 weeks ahead. Our prediction models forecast that the ILI for the U.S. in 2018-2019 may be later and less severe than those in 2017-2018, judging from the influenza activity for Australia and Chile in 2018. It allows to estimate peak timing, peak intensity, and type-specific influenza activities for next season at 40th week. The correlation between seasonal influenza patterns in the U.S., Australia, and Chile could be used to forecast the next seasonal influenza pattern, which can help to determine influenza vaccine strategy approximately six months ahead in the U.S
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Fluorination‐Enhanced Surface Stability of Disordered Rocksalt Cathodes
Cation-disordered rocksalt (DRX) oxides are a promising new class of high-energy-density cathode materials for next-generation Li-ion batteries. However, their capacity fade presents a major challenge. Partial fluorine (F) substitution into the oxygen (O) lattice appears to be an effective strategy for improving the cycling stability, but the underlying atomistic mechanism remains elusive. Here, using a combination of advanced transmission electron microscopy based imaging and spectroscopy techniques, the structural and chemical evolution upon cycling of Mn-based DRX cathodes with an increasing F content (Li-Mn-Nb-O-Fx , x = 0, 0.05, 0.2) are probed. The atomic origin behind the beneficial effect of high-level fluorination for enhancing the surface stability of the DRX is revealed. It is discovered that, due to the reduced O redox activity while with increasing F concentration, F in the DRX lattice mitigates the formation of an O-deficient surface layer upon cycling. For low F-substituted DRX, the O loss near the surface results in the formation of an amorphous cathode-electrolyte interphase layer and nanoscale voids after extended cycling. Increased F concentration in the DRX lattice minimizes both O loss and the interfacial reactions between DRX and the liquid electrolyte, enhancing the surface stability of DRX. These results provide guidance on the development of next-generation cathode materials through anion substitution
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Ultrahigh‐Capacity Rocksalt Cathodes Enabled by Cycling‐Activated Structural Changes
Mn-redox-based oxides and oxyfluorides are considered the most promising earth-abundant high-energy cathode materials for next-generation lithium-ion batteries. While high capacities are obtained in high-Mn content cathodes such as Li- and Mn-rich layered and spinel-type materials, local structure changes and structural distortions (often lead to voltage fade, capacity decay, and impedance rise, resulting in unacceptable electrochemical performance upon cycling. In the present study, structural transformations that exploit the high capacity of Mn-rich oxyfluorides while enabling stable cycling, in stark contrast to commonly observed structural changes that result in rapid performance degradation, are reported. It is shown that upon cycling of a cation-disordered rocksalt (DRX) cathode (Li1.1Mn0.8Ti0.1O1.9F0.1, an ultrahigh capacity of ≈320 mAh g−1 (energy density of ≈900 Wh kg−1) can be obtained through dynamic structural rearrangements upon cycling, along with a unique voltage profile evolution and capacity rise. At high voltage, the presence of Mn4+ and Li+ vacancies promotes local cation ordering, leading to the formation of domains of a “δ phase” within the disordered framework. On deep discharge, Mn4+ reduction, along with Li+ insertion transform the structure to a partially ordered DRX phase with a β′-LiFeO2-type arrangement. At the nanoscale, domains of the in situ formed phases are randomly oriented, allowing highly reversible structural changes and stable electrochemical cycling. These new insights not only help explain the superior electrochemical performance of high-Mn DRXbut also provide guidance for the future development of Mn-based, high-energy density oxide, and oxyfluoride cathode materials
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Exceptional Cycling Performance Enabled by Local Structural Rearrangements in Disordered Rocksalt Cathodes
The capacity of lithium transition-metal (TM) oxide cathodes is directly linked to the magnitude and accessibility of the redox reservoir associated with TM cations and/or oxygen anions, which traditionally decreases with cycling as a result of chemical, structural, or mechanical fatigue. Here, it is shown that a capacity increase over 125% can be achieved upon cycling of high-energy Mn- and F-rich cation-disordered rocksalt oxyfluoride cathodes. This study reveals that in Li1.2Mn0.7Nb0.1O1.8F0.2, repeated Li extraction/reinsertion utilizing Mn3+/Mn4+ redox along with some degree of O-redox participation leads to local structural rearrangements and formation of domains with off-stoichiometry spinel-like features. The effective integration of these local “structure-domains” within the cubic disordered rocksalt framework promotes better Li diffusion and improves material utilization, consequently increased capacity upon cycling. This study provides important new insights into materials design strategies to further exploit the rich compositional and structural space of Mn chemistry for developing sustainable, high-energy cathode materials
Nanoscale Zirconium-Abundant Surface Layers on Lithium- and Manganese-Rich Layered Oxides for High-Rate Lithium-Ion Batteries
Battery
performance, such as the rate capability and cycle stability
of lithium transition metal oxides, is strongly correlated with the
surface properties of active particles. For lithium-rich layered oxides,
transition metal segregation in the initial state and migration upon
cycling leads to a significant structural rearrangement, which eventually
degrades the electrode performance. Here, we show that a fine-tuning
of surface chemistry on the particular crystal facet can facilitate
ionic diffusion and thus improve the rate capability dramatically,
delivering a specific capacity of ∼110 mAh g<sup>–1</sup> at 30C. This high rate performance is realized by creating a nanoscale
zirconium-abundant rock-salt-like surface phase epitaxially grown
on the layered bulk. This surface layer is spontaneously formed on
the Li<sup>+</sup>-diffusive crystallographic facets during the synthesis
and is also durable upon electrochemical cycling. As a result, Li-ions
can move rapidly through this nanoscale surface layer over hundreds
of cycles. This study provides a promising new strategy for designing
and preparing a high-performance lithium-rich layered oxide cathode
material
Experimental study of siphon breaking phenomenon in the real-scaled research reactor pool
Pipe rupture is one of the main causes of loss-of-coolant accident (LOCA). A siphon-breaking system would provide a passive mean of preventing LOCA, increasing the safety of research reactors. But despite the need for such a system, previous research on siphon breaking has not been conducted in a systematic manner. In this study, specific lines and holes were selected to act as siphon breakers, and the effect of size and other variables were investigated using an experimental facility similar on the scale of a real reactor. The performance of various siphon breakers was evaluated experimentally for different siphon-breaker sizes, pipe-rupture points, and pipe-rupture sizes. The effect of an orifice was also considered. Visualization of siphon breaking and examination of transient pressure data were used to analyze siphon-breaking phenomena. Filling a horizontal main pipe at the highest point by entrained air had a large effect on triggering siphon breaking; however, the stacked air entrained during the siphon-breaking event alone was insufficient to cause the phenomenon. All of the experimental parameters were investigated by comparing the undershooting height and transient pressure data trends. Experimental investigation and observation could give the possible postulate that all experimental parameters could be described as physical parameters, such as air flow rate, water flow rate and air quantity. (C) 2012 Elsevier B.V. All rights reserved.X1179sciescopu