Recent developments in polyester synthesis have established several systems based on zinc, chromium, cobalt, and aluminum catalysts for the ring-opening alternating copolymerization of epoxides with ...cyclic anhydrides. However, to date, regioselective processes for this copolymerization have remained relatively unexplored. Herein we report the development of a highly active, regioselective system for the copolymerization of a variety of terminal epoxides and cyclic anhydrides. Unexpectedly, electron withdrawing substituents on the salen framework resulted in a more redox stable Co(III) species and longer catalyst lifetime. Using enantiopure propylene oxide, we synthesized semicrystalline polyesters via the copolymerization of a range of epoxide/anhydride monomer pairs.
Two-dimensional covalent organic frameworks (2D COFs) are ideally suited for organizing redox-active subunits into periodic, permanently porous polymer networks of interest for pseudocapacitive ...energy storage. Here we describe a method for synthesizing crystalline, oriented thin films of a redox-active 2D COF on Au working electrodes. The thickness of the COF film was controlled by varying the initial monomer concentration. A large percentage (80–99%) of the anthraquinone groups are electrochemically accessible in films thinner than 200 nm, an order of magnitude improvement over the same COF prepared as a randomly oriented microcrystalline powder. As a result, electrodes functionalized with oriented COF films exhibit a 400% increase in capacitance scaled to electrode area as compared to those functionalized with the randomly oriented COF powder. These results demonstrate the promise of redox-active COFs for electrical energy storage and highlight the importance of controlling morphology for optimal performance.
Intensity and frequency of extreme novel epidemics Marani, Marco; Katul, Gabriel G; Pan, William K ...
Proceedings of the National Academy of Sciences - PNAS,
08/2021, Letnik:
118, Številka:
35
Journal Article
Recenzirano
Odprti dostop
Observational knowledge of the epidemic intensity, defined as the number of deaths divided by global population and epidemic duration, and of the rate of emergence of infectious disease outbreaks is ...necessary to test theory and models and to inform public health risk assessment by quantifying the probability of extreme pandemics such as COVID-19. Despite its significance, assembling and analyzing a comprehensive global historical record spanning a variety of diseases remains an unexplored task. A global dataset of historical epidemics from 1600 to present is here compiled and examined using novel statistical methods to estimate the yearly probability of occurrence of extreme epidemics. Historical observations covering four orders of magnitude of epidemic intensity follow a common probability distribution with a slowly decaying power-law tail (generalized Pareto distribution, asymptotic exponent = -0.71). The yearly number of epidemics varies ninefold and shows systematic trends. Yearly occurrence probabilities of extreme epidemics, P
, vary widely: P
of an event with the intensity of the "Spanish influenza" (1918 to 1920) varies between 0.27 and 1.9% from 1600 to present, while its mean recurrence time today is 400 y (95% CI: 332 to 489 y). The slow decay of probability with epidemic intensity implies that extreme epidemics are relatively likely, a property previously undetected due to short observational records and stationary analysis methods. Using recent estimates of the rate of increase in disease emergence from zoonotic reservoirs associated with environmental change, we estimate that the yearly probability of occurrence of extreme epidemics can increase up to threefold in the coming decades.
Urban heat islands (UHIs) exacerbate the risk of heat-related mortality associated with global climate change. The intensity of UHIs varies with population size and mean annual precipitation, but a ...unifying explanation for this variation is lacking, and there are no geographically targeted guidelines for heat mitigation. Here we analyse summertime differences between urban and rural surface temperatures (ΔT
) worldwide and find a nonlinear increase in ΔT
with precipitation that is controlled by water or energy limitations on evapotranspiration and that modulates the scaling of ΔT
with city size. We introduce a coarse-grained model that links population, background climate, and UHI intensity, and show that urban-rural differences in evapotranspiration and convection efficiency are the main determinants of warming. The direct implication of these nonlinearities is that mitigation strategies aimed at increasing green cover and albedo are more efficient in dry regions, whereas the challenge of cooling tropical cities will require innovative solutions.
The ability to fight bacterial infections with antibiotics has been a longstanding cornerstone of modern medicine. However, wide-spread overuse and misuse of antibiotics has led to unintended ...consequences, which in turn require large-scale changes of policy for mitigation. In this review, we address two broad classes of corollaries of antibiotics overuse and misuse. Firstly, we discuss the spread of antibiotic resistance from hotspots of resistance evolution to the environment, with special concerns given to potential vectors of resistance transmission. Secondly, we outline the effects of antibiotic pollution independent of resistance evolution on natural microbial populations, as well as invertebrates and vertebrates. We close with an overview of current regional policies tasked with curbing the effects of antibiotics pollution and outline areas in which such policies are still under development.
Leptin is a hormone produced by the adipose tissue that acts in the brain, stimulating white fat breakdown. We find that the lipolytic effect of leptin is mediated through the action of sympathetic ...nerve fibers that innervate the adipose tissue. Using intravital two-photon microscopy, we observe that sympathetic nerve fibers establish neuro-adipose junctions, directly “enveloping” adipocytes. Local optogenetic stimulation of sympathetic inputs induces a local lipolytic response and depletion of white adipose mass. Conversely, genetic ablation of sympathetic inputs onto fat pads blocks leptin-stimulated phosphorylation of hormone-sensitive lipase and consequent lipolysis, as do knockouts of dopamine β-hydroxylase, an enzyme required for catecholamine synthesis. Thus, neuro-adipose junctions are necessary and sufficient for the induction of lipolysis in white adipose tissue and are an efferent effector of leptin action. Direct activation of sympathetic inputs to adipose tissues may represent an alternative approach to induce fat loss, circumventing central leptin resistance.
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•The neuro-adipose junction in white adipose tissue is visualized in vivo•Adipocyte-projecting neurons can completely envelop an adipocyte•Leptin stimulates lipolysis via sympathetic neurons in fat•Optogenetic activation of sympathetic fibers in fat drives lipolysis and fat mass reduction
The lipolytic effect of leptin is mediated by sympathetic neurons that innervate adipocytes, forming neuro-adipose junctions that directly mediate fat breakdown. Anti-obesity strategies targeting the sympathetic neurons in fat have the potential to circumvent central leptin resistance.
The SIR ('susceptible-infectious-recovered') formulation is used to uncover the generic spread mechanisms observed by COVID-19 dynamics globally, especially in the early phases of infectious spread. ...During this early period, potential controls were not effectively put in place or enforced in many countries. Hence, the early phases of COVID-19 spread in countries where controls were weak offer a unique perspective on the ensemble-behavior of COVID-19 basic reproduction number Ro inferred from SIR formulation. The work here shows that there is global convergence (i.e., across many nations) to an uncontrolled Ro = 4.5 that describes the early time spread of COVID-19. This value is in agreement with independent estimates from other sources reviewed here and adds to the growing consensus that the early estimate of Ro = 2.2 adopted by the World Health Organization is low. A reconciliation between power-law and exponential growth predictions is also featured within the confines of the SIR formulation. The effects of testing ramp-up and the role of 'super-spreaders' on the inference of Ro are analyzed using idealized scenarios. Implications for evaluating potential control strategies from this uncontrolled Ro are briefly discussed in the context of the maximum possible infected fraction of the population (needed to assess health care capacity) and mortality (especially in the USA given diverging projections). Model results indicate that if intervention measures still result in Ro > 2.7 within 44 days after first infection, intervention is unlikely to be effective in general for COVID-19.
Structural and transcriptional changes during early brain maturation follow fixed developmental programs defined by genetics. However, whether this is true for functional network activity remains ...unknown, primarily due to experimental inaccessibility of the initial stages of the living human brain. Here, we developed human cortical organoids that dynamically change cellular populations during maturation and exhibited consistent increases in electrical activity over the span of several months. The spontaneous network formation displayed periodic and regular oscillatory events that were dependent on glutamatergic and GABAergic signaling. The oscillatory activity transitioned to more spatiotemporally irregular patterns, and synchronous network events resembled features similar to those observed in preterm human electroencephalography. These results show that the development of structured network activity in a human neocortex model may follow stable genetic programming. Our approach provides opportunities for investigating and manipulating the role of network activity in the developing human cortex.
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•Long-term, single-cell transcriptomics reveals cortical organoid developmental dynamics•Cortical organoids exhibit phase-amplitude coupling during network-synchronous events•Differential role of glutamate and GABA in initiating and maintaining oscillations•Network-level events are similar to the human preterm neonatal EEG features
Oscillatory activity is a candidate mechanism for how neural populations are temporally organized. Cortical organoids exhibit periodic and highly regular nested oscillatory network events that are dependent on glutamatergic and GABAergic signaling. The emerging development of network activity transitions to more spatiotemporally complex activity, capturing features of preterm infant electroencephalography.
Functional magnetic resonance imaging (fMRI) and particularly resting state fMRI (rs-fMRI) is widely used to investigate resting state brain networks (RSNs) on the systems level. Echo planar imaging ...(EPI) is the state-of-the-art imaging technique for most fMRI studies. Therefore, improvements of EPI might lead to increased sensitivity for a large amount of studies performed every day. A number of developments to shorten acquisition time have been recently proposed and the multiband technique, allowing the simultaneous acquisition of multiple slices yielding an equivalent reduction of measurement time, is the most promising among them. While the prospect to significantly reduce acquisition time by means of high multiband acceleration factors (M) appears tempting, signal quality parameters and the sensitivity to detect common RSNs with increasing M-factor have only been partially investigated up to now. In this study, we therefore acquired rs-fMRI data from 20 healthy volunteers to systematically investigate signal characteristics and sensitivity for brain network activity in datasets with increasing M-factor, M = 2 - 4. Combined with an inplane, sensitivity encoding (SENSE), acceleration factor, S = 2, we applied a maximal acceleration factor of 8 (S2×M4). Our results suggest that an M-factor of 2 (total acceleration of 4) only causes negligible SNR decrease but reveals common RSN with increased sensitivity and stability. Further M-factor increase produced random artifacts as revealed by signal quality measures that may affect interpretation of RSNs under common scanning conditions. Given appropriate hardware, a mb-EPI sequence with a total acceleration of 4 significantly reduces overall scanning time and clearly increases sensitivity to detect common RSNs. Together, our results suggest mb-EPI at moderate acceleration factors as a novel standard for fMRI that might increase our understanding of network dynamics in healthy and diseased brains.
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