Coordinatively unsaturated ferrous (CUF) sites confined in nanosized matrices are active centers in a wide range of enzyme and homogeneous catalytic reactions. Preparation of the analogous active sites at supported catalysts is of great importance in heterogeneous catalysis but remains a challenge. On the basis of surface science measurements and density functional calculations, we show that the interface confinement effect can be used to stabilize the CUF sites by taking advantage of strong adhesion between ferrous oxides and metal substrates. The interface-confined CUF sites together with the metal supports are active for dioxygen activation, producing reactive dissociated oxygen atoms. We show that the structural ensemble was highly efficient for carbon monoxide oxidation at low temperature under typical operating conditions of a proton-exchange membrane fuel cell.
Liver enzyme abnormalities in patients with COVID-19 are associated with disease severity. Patients with liver enzyme abnormalities have higher A-aDO2 and GGT, lower albumin and decreased circulating CD4+ T cells and B lymphocytes. SARS-CoV-2 is able to infect the liver and cause conspicuous hepatic cytopathy. Massive apoptosis and binuclear hepatocytes were the predominant histological features of SARS-CoV-2-infected liver.
The catalytic activity of noble-metal nanocrystals is mainly determined by their sizes and the facets exposed on the surface. For single crystals, it has been demonstrated that the Pd(100) surface is catalytically more active than both Pd(110) and Pd(111) surfaces for the CO oxidation reaction. Here we report the synthesis of Pd nanocrystals enclosed by {100} facets with controllable sizes in the range of 6-18 nm by manipulating the rate of reduction of the precursor. UV-vis spectroscopy studies indicate that the rate of reduction of Na 2 PdCl 4 can be controlled by adjusting the concentrations of Br -and Cl -ions added to the reaction mixture. Pd nanocrystals with different sizes were immobilized on ZnO nanowires and evaluated as catalysts for CO oxidation. We found that the activity of this catalytic system for CO oxidation showed a strong dependence on the nanocrystal size. When the size of the Pd nanocrystals was reduced from 18 nm to 6 nm, the maximum conversion rate was significantly enhanced by a factor of ~10 and the corresponding maximum conversion temperature was lowered by ~80 °C . KEYWORDS
As a derivative of LiNiO 2 , NCA (LiNi 1-x-y Co x Al y O 2 ) is widely used in the electric vehicle industry because of its high energy density. It is thought that Co and Al both play important roles in enhancing NCA material properties. However, there is no solid evidence in the literature that clearly shows that Co is required in NCA with high nickel (e.g. when 1-x-y > 0.9) content. Therefore, a systematic study on the roles of different cation substituents in a series of LiNi 1-n M n O 2 (M = Al, Mn, Mg, or Co) materials was made. In-situ X-ray diffraction (XRD) and differential capacity versus voltage (dQ/dV vs. V) studies showed that the multiple phase transitions in Li x NiO 2 during charge and discharge, thought to cause poor charge-discharge capacity retention, were suppressed in Li x Ni 0.95 M 0.05 O 2 (M = Al, Mn, or Mg), while 5% Co failed to suppress the phase transitions. First principles calculations were made to understand the function of each substituent. Accelerating rate calorimetry shows that unlike Al, Mn, or Mg, Co has no contribution to safety improvement. Therefore, we believe that Co brings little or no value at all to NCA-type materials with high Ni content (> 90% Ni in the transition metal layer) and we hope this paper will spur more interest in Co-free materials.
Ni-rich transition metal layered oxide materials are of great interest as positive electrode materials for lithium ion batteries. As the popular electrode materials NMC (LiNi 1-x-y Mn x Co y O 2 ) and NCA (LiNi 1-x-y Co x Al y O 2 ) become more and more Ni-rich, they approach LiNiO 2 . Therefore it is important to benchmark the structure and electrochemistry of state of the art Li x NiO 2 for the convenience of researchers in the field. In this work, LiNiO 2 synthesized from a commercial Ni(OH) 2 precursor and modern synthesis methods shows a specific capacity close to the theoretical specific capacity of 274 mAh/g. In-situ X-ray diffraction (XRD) measurements were conducted to obtain accurate structural information versus lithium content, x. The known multiple phase transitions of Li x NiO 2 during charge and discharge were clearly observed, and the variation in unit cell lattice constants and volume was measured. Differential capacity versus voltage (dQ/dV vs. V) studies were used to investigate the electrochemical properties including regions of composition that show very slow kinetics. It is hoped that this work will be a useful reference for those working on Ni-rich positive electrode materials for Li-ion cells.
Millimeter-size single-crystal monolayer graphene is synthesized on polycrystalline Cu foil by a method that involves suppressing loss by evaporation of the Cu at high temperature under low pressure. This significantly diminishes the number of graphene domains, and large single crystal domains up to ∼2 mm in size are grown.
BACKGROUND. Coronavirus disease 2019 (COVID-19), caused by severe acute respiratory coronavirus 2 (SARS-CoV-2), has become a pandemic. This study addresses the clinical and immunopathological characteristics of severe COVID-19. METHODS. Sixty-nine patients with COVID-19 were classified into severe and nonsevere groups to analyze their clinical and laboratory characteristics. A panel of blood cytokines was quantified over time. Biopsy specimens from 2 deceased cases were obtained for immunopathological, ultrastructural, and in situ hybridization examinations. RESULTS. Circulating cytokines, including IL-8, IL-6, TNF-α, IP10, MCP1, and RANTES, were significantly elevated in patients with severe COVID-19. Dynamic IL-6 and IL-8 were associated with disease progression. SARS-CoV-2 was demonstrated to infect type II and type I pneumocytes and endothelial cells, leading to severe lung damage through cell pyroptosis and apoptosis. In severe cases, lymphopenia, neutrophilia, depletion of CD4 + and CD8 + T lymphocytes, and massive macrophage and neutrophil infiltrates were observed in both blood and lung tissues. CONCLUSIONS. A panel of circulating cytokines could be used to predict disease deterioration and inform clinical interventions. Severe pulmonary damage was predominantly attributed to both cytopathy caused by SARS-CoV-2 and immunopathologic damage. Strategies that prohibit pulmonary recruitment and overactivation of inflammatory cells by suppressing cytokine storm might improve the outcomes of patients with severe COVID-19.
Single-crystal LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC532) with a grain size of 2-3 μm was compared to conventional polycrystalline uncoated NMC532 and polycrystalline Al 2 O 3 -coated materials in this work. Studies were made to determine how single crystal NMC532 material with large grain size could be synthesized. Ultra high precision coulometry (UHPC), in-situ gas measurements and isothermal microcalorimetry were used to make comparative studies of the three materials in Li-ion pouch cells. All the diagnostic measurements suggested that the single crystal material should yield Li-ion cells with longer lifetime. Long-term cycling tests verified these predictions and showed that cells with single crystal NMC532 exhibited much better capacity retention than cells with the polycrystalline materials at both 40 • C and 55 • C when tested to an upper cutoff potential of 4.4 V. The reasons for the superior performance of the single crystal cells were explored using thermogravimetric analysis/mass spectrometry experiments on the charged electrode materials. The single crystal materials were extremely resistant to oxygen loss below 100 • C compared to the polycrystalline materials. The major drawback of the single crystal material is its slightly lower specific capacity compared to the polycrystalline materials. However, this may not be an issue for Li-ion cells designed for long lifetime applications. Lithium ion batteries with high energy density, long lifetime and low cost need to be developed for applications in electric vehicles and stationary energy storage. The family of Li(Ni x Mn y Co z )O 2 (x + y + z = 1) (NMC) materials with high nickel and low cobalt are used as positive electrode materials in lithium ion cells.1,2 One simple way to increase the energy density of NMC lithium ion cells is to increase their upper cutoff voltage which gives access to higher specific capacity from the positive electrode.3,4 However, increasing the upper cutoff voltage usually decreases the lifetime of cells due to an acceleration of 'unwanted' parasitic reactions between the electrolyte and the delithiated positive electrode surface at high voltages. Such reactions include oxidation of species found in the electrolyte, transition metal dissolution, etc. [5][6][7] In addition, structural reconstruction of the positive electrode surface can occur which can contribute to impedance growth and capacity loss. 3,4 The by-products of oxidation at the positive electrode can migrate to the negative electrode surface and be reduced there. 8,9 Such reactions can lead to the consumption of lithium ions from the electrolyte, (to maintain charge neutrality in the electrolyte), a reduction in lithium inventory, as well as a thickening of the negative electrode solid electrolyte interface (SEI) which together ultimately cause cell-failure.10,11 These processes are accelerated by higher charging potentials and higher temperatures.Methods such as modification of the positive electrode surface with coatings or dopants 12,13 and/or modification of electr...
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