The megacity of Beijing has experienced frequent severe fine particle pollution during the last decade. Although the sources and formation mechanisms of aerosol particles have been extensively ...investigated on the basis of ground measurements, real-time characterization of aerosol particle composition and sources above the urban canopy in Beijing is rare. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) composition at 260 m at the Beijing 325 m meteorological tower (BMT) from 10 October to 12 November 2014, by using an aerosol chemical speciation monitor (ACSM) along with synchronous measurements of size-resolved NR-PM1 composition near ground level using a high-resolution time-of-flight aerosol mass spectrometer (HR–ToF–AMS). The NR-PM1 composition above the urban canopy was dominated by organics (46 %), followed by nitrate (27 %) and sulfate (13 %). The high contribution of nitrate and high NO3− / SO42− mass ratios illustrates an important role of nitrate in particulate matter (PM) pollution during the study period. The organic aerosol (OA) was mainly composed of secondary OA (SOA), accounting for 61 % on an average. Different from that measured at the ground site, primary OA (POA) correlated moderately with SOA, likely suggesting a high contribution from regional transport above the urban canopy. The Asia–Pacific Economic Cooperation (APEC) summit with strict emission controls provides a unique opportunity to study the impacts of emission controls on aerosol chemistry. All aerosol species were shown to have significant decreases of 40–80 % during APEC from those measured before APEC, suggesting that emission controls over regional scales substantially reduced PM levels. However, the bulk aerosol composition was relatively similar before and during APEC as a result of synergetic controls of aerosol precursors. In addition to emission controls, the routine circulations of mountain–valley breezes were also found to play an important role in alleviating PM levels and achieving the "APEC blue" effect. The evolution of vertical differences between 260 m and the ground level was also investigated. Our results show complex vertical differences during the formation and evolution of severe haze episodes that are closely related to aerosol sources and boundary-layer dynamics.
The Tibetan Plateau is the highest and one of the most demanding environments ever inhabited by humans. We investigated the timing and mechanisms of its initial colonization at the Nwya Devu site, ...located nearly 4600 meters above sea level. This site, dating from 40,000 to 30,000 years ago, is the highest Paleolithic archaeological site yet identified globally. Nwya Devu has yielded an abundant blade tool assemblage, indicating hitherto-unknown capacities for the survival of modern humans who camped in this environment. This site deepens the history of the peopling of the "roof of the world" and the antiquity of human high-altitude occupations more generally.
This paper studies the fault detection process (FDP) and fault correction process (FCP) with the incorporation of testing effort function and imperfect debugging. In order to ensure high reliability, ...it is essential for software to undergo a testing phase, during which faults can be detected and corrected by debuggers. The testing resource allocation during this phase, which is usually depicted by the testing effort function, considerably influences not only the fault detection rate but also the time to correct a detected fault. In addition, testing is usually far from perfect such that new faults may be introduced. In this paper, we first show how to incorporate testing effort function and fault introduction into FDP and then develop FCP as delayed FDP with a correction effort. Various specific paired FDP and FCP models are obtained based on different assumptions of fault introduction and correction effort. An illustrative example is presented. The optimal release policy under different criteria is also discussed.
In this paper, we report the formation of a series Zr–(Cu,Ag)–Al bulk metallic glasses (BMGs) with diameters at least 20
mm and demonstrate the formation of about 25
g amorphous metallic ingots in a ...wide Zr–(Cu,Ag)–Al composition range using a conventional arc-melting machine. The origin of high glass-forming ability (GFA) of the Zr–(Cu,Ag)–Al alloy system has been investigated from the structural, thermodynamic and kinetic points of view. The high GFA of the Zr–(Cu,Ag)–Al system is attributed to denser local atomic packing and the smaller difference in Gibbs free energy between amorphous and crystalline phases. The thermal, mechanical and corrosion properties, as well as elastic constants for the newly developed Zr–(Cu,Ag)–Al BMGs, are also presented. These newly developed Ni-free Zr–(Cu,Ag)–Al BMGs exhibit excellent combined properties: strong GFA, high strength, high compressive plasticity, cheap and non-toxic raw materials and biocompatible property, as compared with other BMGs, leading to their potential industrial applications.
Composition and size distribution of atmospheric aerosols from Xi'an city (~400 m, altitude) in inland China during the spring of 2009 including a massive dust event on 24 April were measured and ...compared with a parallel measurement at the summit (2060 m, altitude) of Mt. Hua, an alpine site nearby Xi'an. EC (elemental carbon), OC (organic carbon) and major ions in the city were 2-22 times higher than those on the mountaintop during the whole sampling period. Compared to that in the non-dust period a sharp increase in OC was observed at both sites during the dust period, which was mainly caused by an input of biogenic organics from the Gobi desert. However, adsorption/heterogeneous reaction of gaseous organics with dust was another important source of OC in the urban, contributing 22% of OC in the dust event. In contrast to the mountain atmosphere where fine particles were less acidic when dust was present, the urban fine particles became more acidic in the dust event than in the non-dust event, mainly due to enhanced heterogeneous formation of nitrate and diluted NH sub(3). Cl super(-) and NO sub(3) super(-) in the urban air during the dust event significantly shifted toward coarse particles. Such redistributions were further pronounced on the mountaintop when dust was present, resulting in both ions almost entirely staying in coarse particles. On the contrary, no significant spatial difference in size distribution of SO sub(4) super(2-) was found between the urban ground surface and the mountain atmosphere, which dominated in the fine mode (<2.1 mu m) during the nonevent and comparably distributed in the fine (<2.1 mu m) and coarse (>2.1 mu m) modes during the dust event.
The secondary β-relaxation is an intrinsic feature in glassy materials. However, its structural origin is still not well understood. Here we report that the β-relaxations in La50Al15Ni35 and ...La50Al15Cu35 metallic glasses (MGs) mainly depend on the vibration of small Ni and Cu atoms in local cages. By using advanced synchrotron X-ray techniques and theoretical calculations, we elucidate that the tricapped-trigonal-prism-like polyhedra with more large La atoms in shells favor the local vibration of center Ni atoms, leading to the pronounced β-relaxation event. In contrast, the in-cage vibration of Cu atoms is somehow suppressed by the appearance of more shell Cu atoms. Nevertheless, they could easily diffuse out of the cages compared with Ni, thus triggering the onset of α-relaxation. This work provides a pathway to understand the different structural relaxation behaviors in MGs and other disordered materials from their local atomic packing and dynamics points of view.
Based on the central role of the ubiquitin-proteasome system (UPS) in the degradation of cellular proteins, proteasome inhibition has been considered an attractive approach for anticancer therapy. ...Deubiquitinases (DUBs) remove ubiquitin conjugates from diverse substrates; therefore, they are essential regulators of the UPS. DUB inhibitors, especially the inhibitors of proteasomal DUBs are becoming a research hotspot in targeted cancer therapy. Previous studies have shown that metal complexes, such as copper and zinc complexes, can induce cancer cell apoptosis through inhibiting UPS function. Moreover, we have found that copper pyrithione inhibits both 19S proteasome-associated DUBs and 20S proteasome activity with a mechanism distinct from that of the classical 20S proteasome inhibitor bortezomib. In the present study, we reveal that (i) nickel pyrithione complex (NiPT) potently inhibits the UPS via targeting the 19S proteasome-associated DUBs (UCHL5 and USP14), without effecting on the 20S proteasome; (ii) NiPT selectively induces proteasome inhibition and apoptosis in cultured tumor cells and cancer cells from acute myeloid leukemia human patients; and (iii) NiPT inhibits proteasome function and tumor growth in nude mice. This study, for the first time, uncovers a nickel complex as an effective inhibitor of the 19S proteasomal DUBs and suggests a potentially new strategy for cancer treatment.
Aims: To examine the mechanism of ozone‐induced damage to cytoplasmic membrane and cell ultrastructure of Pseudomonas aeruginosa ATCC27853. Methods and Results: Cell suspensions of Ps. aeruginosa ...ATCC27853 were treated with ozonated water. The leakages of cellular potassium (K+), magnesium (Mg2+) and adenosine triphosphate (ATP), determined by inductively coupled plasma/mass spectrometry (ICP/MS) and a commercial bioluminescence assay kit, were to assess ozone‐induced damage to the cytoplasmic membrane. Maximum leakages of K+ and Mg2+ were attained, respectively, at 0·53 mg l−1 ozone after 0·5 and 2 min with >99% inactivation of culturable bacteria, while that of ATP was achieved at 0·67 mg l−1 ozone after 1 min. Transmission electron microscopy (TEM) and scanning electron microscopy (SEM) revealed that treated cells retained intact shapes and cytoplasm agglutinations and vacuoles occurred. Conclusions: Ozone inactivates Ps. aeruginosa ATCC27853 by the combined results of increased cytoplasmic membrane permeability and cytoplasm coagulation, rather than by severe membrane disruption and cell lysis. Significance and Impact of the Study: Pseudomonas aeruginosa is a common water‐related pathogen. These insights into the leakage of cytoplasmic components and ultrastructural changes provide evidence for the mechanisms of ozone‐mediated inactivation.
Due to that the high charge density and small radius render In3+ cation a stronger Lewis acidity, multifunctional nanoporous In-MOFs have become one of the most promising catalysts for their high ...activity. Herein, the solvothermal self-assembly by employing 2,4,6-tri (2,4-dicarboxyphenyl)pyridine (H6TDP) as organic linker leads to a robust honeycomb skeleton of {(CH3)2NH2InIIIPbII(TDP) (H2O)⋅3DMF⋅3H2O}n (NUC-52) with the merits of nanoscopic channels, high porosity (61.3%), large specific surface area, and thermal stability. To the best of our knowledge, this is the first 4p-5p heterometallic {InIIIPbII} cluster-based nano-porous host framework, whose activated state possesses the coexistence of Lewis acid-base sites including 7-coordinated Pb2+ ions, 4-coordinated In3+ ions, uncoordinated carboxyl oxygen atoms, and Npyridine atoms. Performed catalytic experiments exhibited that activated NUC-52 owned the high catalytic activity on the cycloaddition reactions of styrene oxide with CO2 under mild conditions with excellent turnover number (2475) and turnover frequency (619 h−1). Moreover, activated NUC-52 could greatly accelerate the deacetalization-Knoevenagel condensation reactions of benzaldehyde dimethyl acetal and malononitrile. Hence, this work lays down the groundwork for constructing heterometallic cluster-based nanoporous MOFs with excellent Lewis acidic catalysis and chemical stability, which should be ascribed to the reasonable coordination arrangement between organic ligands and distinct metal ions according to the hard–soft acid–base (HSAB) theory.
A highly robust {InPb}-organic framework with Lewis acid-base bifunctional features exhibits high catalytic activity on the cycloaddition reactions of epoxides with CO2 and deacetalization-Knoevenagel condensation reactions. Display omitted
•InPb-cluster-based honeycomb framework of NUC-52 can highly catalyze the cycloaddition of CO2 and deacetalization-Knoevenagel condensation.•Performed catalytic experiments exhibited that activated NUC-52 owned the high catalytic activity on the cycloaddition reactions of styrene oxide with CO2 under mild conditions with excellent turnover number (2475) and turnover frequency (619 h-1). Moreover, activated NUC-52 could greatly accelerate the deacetalization-Knoevenagel condensation reactions of benzaldehyde dimethyl acetal and malononitrile.
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