| 1. |
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| 2. |
- Nguyen, Thanh N, et al.
(författare)
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Global Impact of the COVID-19 Pandemic on Stroke Volumes and Cerebrovascular Events: A 1-Year Follow-up.
- 2023
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Ingår i: Neurology. - 1526-632X. ; 100:4
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Tidskriftsartikel (refereegranskat)abstract
- Declines in stroke admission, IV thrombolysis (IVT), and mechanical thrombectomy volumes were reported during the first wave of the COVID-19 pandemic. There is a paucity of data on the longer-term effect of the pandemic on stroke volumes over the course of a year and through the second wave of the pandemic. We sought to measure the effect of the COVID-19 pandemic on the volumes of stroke admissions, intracranial hemorrhage (ICH), IVT, and mechanical thrombectomy over a 1-year period at the onset of the pandemic (March 1, 2020, to February 28, 2021) compared with the immediately preceding year (March 1, 2019, to February 29, 2020).We conducted a longitudinal retrospective study across 6 continents, 56 countries, and 275 stroke centers. We collected volume data for COVID-19 admissions and 4 stroke metrics: ischemic stroke admissions, ICH admissions, IVT treatments, and mechanical thrombectomy procedures. Diagnoses were identified by their ICD-10 codes or classifications in stroke databases.There were 148,895 stroke admissions in the 1 year immediately before compared with 138,453 admissions during the 1-year pandemic, representing a 7% decline (95% CI [95% CI 7.1-6.9]; p < 0.0001). ICH volumes declined from 29,585 to 28,156 (4.8% [5.1-4.6]; p < 0.0001) and IVT volume from 24,584 to 23,077 (6.1% [6.4-5.8]; p < 0.0001). Larger declines were observed at high-volume compared with low-volume centers (all p < 0.0001). There was no significant change in mechanical thrombectomy volumes (0.7% [0.6-0.9]; p = 0.49). Stroke was diagnosed in 1.3% [1.31-1.38] of 406,792 COVID-19 hospitalizations. SARS-CoV-2 infection was present in 2.9% ([2.82-2.97], 5,656/195,539) of all stroke hospitalizations.There was a global decline and shift to lower-volume centers of stroke admission volumes, ICH volumes, and IVT volumes during the 1st year of the COVID-19 pandemic compared with the prior year. Mechanical thrombectomy volumes were preserved. These results suggest preservation in the stroke care of higher severity of disease through the first pandemic year.This study is registered under NCT04934020.
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| 3. |
- Chien, Yu-Chuan, 1990-, et al.
(författare)
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Rapid determination of solid-state diffusion coefficients in Li-based batteries via intermittent current interruption method
- 2023
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 14:1
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Tidskriftsartikel (refereegranskat)abstract
- The galvanostatic intermittent titration technique (GITT) is considered the go-to method for determining the Li+ diffusion coefficients in insertion electrode materials. However, GITT-based methods are either time-consuming, prone to analysis pitfalls or require sophisticated interpretation models. Here, we propose the intermittent current interruption (ICI) method as a reliable, accurate and faster alternative to GITT-based methods. Using Fick’s laws, we prove that the ICI method renders the same information as the GITT within a certain duration of time since the current interruption. Via experimental measurements, we also demonstrate that the results from ICI and GITT methods match where the assumption of semi-infinite diffusion applies. Moreover, the benefit of the non-disruptive ICI method to operando materials characterization is exhibited by correlating the continuously monitored diffusion coefficient of Li+ in a LiNi0.8Mn0.1Co0.1O2-based electrode to its structural changes captured by operando X-ray diffraction measurements.
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| 4. |
- Chien, Yu-Chuan, 1990-, et al.
(författare)
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Simultaneous Monitoring of Crystalline Active Materials and Resistance Evolution in Lithium-Sulfur Batteries
- 2020
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Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 142:3, s. 1449-1456
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Tidskriftsartikel (refereegranskat)abstract
- Operando X-ray diffraction (XRD) is a valuable tool for studying secondary battery materials as it allows for the direct correlation of electrochemical behavior with structural changes of crystalline active materials. This is especially true for the lithium-sulfur chemistry, in which energy storage capability depends on the complex growth and dissolution kinetics of lithium sulfide (Li2S) and sulfur (S-8) during discharge and charge, respectively. In this work, we present a novel development of this method through combining operando XRD with simultaneous and continuous resistance measurement using an intermittent current interruption (ICI) method. We show that a coefficient of diffusion resistance, which reflects the transport properties in the sulfur/carbon composite electrode, can be determined from analysis of each current interruption. Its relationship to the established Warburg impedance model is validated theoretically and experimentally. We also demonstrate for an optimized electrode formulation and cell construction that the diffusion resistance increases sharply at the discharge end point, which is consistent with the blocking of pores in the carbon host matrix. The combination of XRD with ICI allows for a direct correlation of structural changes with not only electrochemical properties but also energy loss processes at a nonequilibrium state and, therefore, is a valuable technique for the study of a wide range of energy storage chemistries.
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| 5. |
- Chien, Yu-Chuan, 1990-, et al.
(författare)
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Understanding the Impact of Precipitation Kinetics on the Electrochemical Performance of Lithium–Sulfur Batteries by Operando X-ray Diffraction
- 2022
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 126:6, s. 2971-2979
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Tidskriftsartikel (refereegranskat)abstract
- The complex reaction mechanism of the lithium–sulfur battery system consists of re-petitive dissolution and precipitation of the sulfur-containing species in the positiveelectrode. In particular, the precipitation of lithium sulfide (Li2S) during discharge hasbeen considered a crucial factor for achieving a high degree of active material utiliza-tion. Here, the influence of electrolyte amount, electrode thickness, applied current andelectrolyte salt on the formation of Li2S is systematically investigated in a series ofoperando X-ray diffraction experiments. Through a combination of simultaneous dif-fraction and resistance measurements, the evolution of the intensity from Li2S is di-rectly correlated to the variation in internal resistance and transport properties insidethe positive electrode. The correlation indicates that at different stages, the Li2S precip-itation both facilitates and impedes the discharge process. The kinetic information ofLi2S formation offers mechanistic explanations for the strong impact of different elec-trochemical cell parameters on the performance and thus, directions for holistic optimi-zations to achieve high sulfur utilization.
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| 6. |
- Fritze, Stefan, et al.
(författare)
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Magnetron sputtering of carbon supersaturated tungsten films-A chemical approach to increase strength
- 2021
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Ingår i: Materials & design. - : Elsevier. - 0264-1275 .- 1873-4197. ; 208
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Tidskriftsartikel (refereegranskat)abstract
- Tungsten (W)-based materials attract significant attention due to their superior mechanical properties. Here, we present a chemical approach based on the addition of carbon (C) for increased strength via the combination of three strengthening mechanisms in W thin films. W:C thin films with C concentrations up to-4 at.% were deposited by magnetron sputtering. All films exhibit a body-centred-cubic structure with strong texture and columnar growth behaviour. X-ray and electron diffraction measurements suggest the formation of supersaturated W:C solid solution phases. The addition of C reduced the average column width from-133 nm for W to-20 nm for the film containing-4 at.% C. The column refinement is explained by a mechanism where C acts as re-nucleation sites. The W film is-13 GPa hard, while the W:C films achieve a peak hardness of-24 GPa. The W:C films are-11 GPa harder than the W film, which is explained by a combination of grain refinement strengthening, solid solution strengthening and increased dislocation density. Additional micropillar compression tests showed that the flow stress increased upon C addition, from-3.8 to-8.3 GPa and no brittle fracture was observed.
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| 7. |
- Menon, Ashok S., et al.
(författare)
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Influence of Synthesis Routes on the Crystallography, Morphology, and Electrochemistry of Li2MnO3
- 2020
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 12:5, s. 5939-5950
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Tidskriftsartikel (refereegranskat)abstract
- With the potential of delivering reversible capacities of up to 300 mAh/g, Li-rich transition-metal oxides hold great promise as cathode materials for future Li-ion batteries. However, a cohesive synthesis-structure-electrochemistry relationship is still lacking for these materials, which impedes progress in the field. This work investigates how and why different synthesis routes, specifically solid-state and modified Pechini sol-gel methods, affect the properties of Li2MnO3, a compositionally simple member of this material system. Through a comprehensive investigation of the synthesis mechanism along with crystallographic, morphological, and electrochemical characterization, the effects of different synthesis routes were found to predominantly influence the degree of stacking faults and particle morphology. That is, the modified Pechini method produced isotropic spherical particles with approximately 57% faulting and the solid-state samples possessed heterogeneous morphology with approximately 43% faulting probability. Inevitably, these differences lead to variations in electrochemical performance. This study accentuates the importance of understanding how synthesis affects the electrochemistry of these materials, which is critical considering the crystallographic and electrochemical complexities of the class of materials more generally. The methodology employed here is extendable to studying synthesis-property relationships of other compositionally complex Li-rich layered oxide systems.
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| 8. |
- Menon, Ashok S., et al.
(författare)
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Synthesis-structure relationships in Li- and Mn-rich layered oxides : phase evolution, superstructure ordering and stacking faults
- 2022
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Ingår i: Dalton Transactions. - : Royal Society of Chemistry. - 1477-9226 .- 1477-9234. ; 51:11, s. 4435-4446
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Tidskriftsartikel (refereegranskat)abstract
- Li- and Mn-rich layered oxides are promising positive electrode materials for future Li-ion batteries. The presence of crystallographic features such as cation-mixing and stacking faults in these compounds make them highly susceptible to synthesis-induced structural changes. Consequently, significant variations exist in the reported structure of these compounds that complicate the understanding of how the crystallographic structure influences its properties. This work investigates the synthesis-structure relations for three widely investigated Li- and Mn-rich layered oxides: Li2MnO3, Li1.2Mn0.6Ni0.2O2 and Li1.2Mn0.54Ni0.13Co0.13O2. For each compound, the average structure is compared between two synthetic routes of differing degrees of precursor mixing and four annealing protocols. Furthermore, thermodynamic and synthesis-specific kinetic factors governing the equilibrium crystallography of each composition are considered. It was found that the structures of these compounds are thermodynamically metastable under the synthesis conditions employed. In addition to a driving force to reduce stacking faults in the structure, these compositions also exhibited a tendency to undergo structural transformations to more stable phases under more intense annealing conditions. Increasing the compositional complexity introduced a kinetic barrier to structural ordering, making Li1.2Mn0.6Ni0.2O2 and Li1.2Mn0.54Ni0.13Co0.13O2 generally more faulted relative to Li2MnO3. Additionally, domains with different degrees of faulting were found to co-exist in the compounds. This study offers insight into the highly synthesis-dependent subtle structural complexities present in these compounds and complements the substantial efforts that have been undertaken to understand and optimise its electrochemical properties.
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| 9. |
- Menon, Ashok S.
(författare)
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Synthesis–Structure–Property Relationships in Li- and Mn-rich Layered Oxides
- 2021
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- The commercialisation of Li-ion batteries over the last decade has provided additional impetus for the improvement of existing energy storage technologies. Towards this, a major portion of the global efforts includes exploratory research aimed at the development of new material chemistries. Aligning with this theme, this Thesis explores the synthesis–structure–property relationships in Li- and Mn-rich layered oxides, a cost-effective high-capacity material system that shows promise as a positive electrode material for future Li-ion batteries. The compositional and crystallographic diversity of Li- and Mn-rich layered oxides make them particularly susceptible to synthesis-dependent variations and exacerbates structural characterisation. Therefore, understanding how synthetic variations influence their structural and electrochemical properties is a crucial step in realising their potential as positive electrode materials.Even for simple compositions like Li2MnO3, dissimilar crystallographic ordering and particle morphologies are produced depending on whether a solid-state or sol-gel synthesis approach was implemented. Subsequently, due to the higher degree of structural disorder and larger surface area, the sol-gel sample exhibited higher initial electrochemical capacities. The structural features present in these compounds such as cation site-mixing and stacking faults, manifest over varying crystallographic regimes. Hence, complementary characterisation techniques that probe different structural length scales are necessary for an accurate structural characterisation of these compounds. This factor, together with their complex crystallography, have led to contradictory single- and multi-phase structure models being reported for complex Li- and Mn-rich layered oxides. By using a combination of diffraction, spectroscopic techniques and magnetic measurements it was discovered that Li1.2Mn0.54Ni0.13Co0.13O2 can exist in both single- and multi-phase structural forms if synthesised through sol-gel and solid-state methods, respectively. Further studies following the same theme revealed that when synthesised under common laboratory conditions these compounds are metastable. Here, the composition and synthesis play a critical role in the thermodynamic and kinetic factors affecting the resultant phase, domain structure and degree of cationic order. Finally, to encompass all the structural features contained in Li- and Mn-rich layered oxides, a supercell-based structure model for Li- and Mn-rich layered oxides, using Li1.2Mn0.6Ni0.2O2 as an example, is presented. Summing all the work together from the thesis, a critical evaluation of commonly used characterisation techniques is also provided as a guideline for future research in this field.
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| 10. |
- Menon, Ashok S., et al.
(författare)
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Synthetic Pathway Determines the Nonequilibrium Crystallography of Li- and Mn-Rich Layered Oxide Cathode Materials
- 2021
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 4:2, s. 1924-1935
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Tidskriftsartikel (refereegranskat)abstract
- Li- and Mn-rich layered oxides show significant promise as electrode materials for future Li-ion batteries. However, an accurate description of its crystallography remains elusive, with both single-phase solid solution and multiphase structures being proposed for high performing materials such as Li1.2Mn0.54Ni0.13Co0.13O2. Herein, we report the synthesis of single- and multiphase variants of this material through sol-gel and solid-state methods, respectively, and demonstrate that its crystallography is a direct consequence of the synthetic route and not necessarily an inherent property of the composition, as previously argued. This was accomplished via complementary techniques that probe the bulk and local structure followed by in situ methods to map the synthetic progression. As the electrochemical performance and anionic redox behavior are often rationalized on the basis of the presumed crystal structure, clarifying the structural ambiguities is an important step toward harnessing its potential as an electrode material.
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