Iridium-catalyzed boron-hydrogen bond insertion reactions of trimethylamine-borane and sulfoxonium ylides have been demonstrated, furnishing α-boryl ketones in moderate to excellent yields in most ...cases (51 examples; up to 84%). This practical and scalable insertion reaction showed broad substrate scope, high functional-group compatibility and could be applied in late-stage modification of structurally complex drug compounds. Further synthetic applications were also demonstrated.
Iridium-catalyzed boron-hydrogen bond insertion reactions of trimethylamine-borane and sulfoxonium ylides have been demonstrated, furnishing α-boryl ketones in moderate to excellent yields in most cases (51 examples; up to 84%).
Visible-light photoredox catalysis has been established as a popular and powerful tool for organic transformations owing to its inherent characterization of environmental friendliness and ...sustainability in the past decades. The thiol-ene/yne reactions, the direct hydrothiolation of alkenes/alkynes with thiols, represents one of the most efficient and atom-economic approaches for the carbon-sulfur bonds construction. In traditional methodologies, harsh conditions such as stoichiometric reagents or a specialized UV photo-apparatus were necessary suffering from various disadvantages. In particular, visible-light photoredox catalysis has also been demonstrated to be a greener and milder protocol for the thiol-ene/yne reactions in recent years. Additionally, unprecedented advancements have been achieved in this area during the past decade. In this review, we will summarize the recent advances in visible-light photoredox catalyzed thiol-ene/yne reactions from 2015 to 2021. Synthetic strategies, substrate scope, and proposed reaction pathways are mainly discussed.
In order to develop promising anode materials for sodium-ion batteries (SIBs), a novel pie-like FeS@C (P-FeS@C) nanohybrid, in which all ultrasmall FeS nanocrystals (NCs) are completely embedded into ...the carbon network and sealed by a protective carbon shell, has been prepared. The unique pie-like structure can effectively speed up the kinetics of electrode reactions, while the carbon shell stabilizes the FeS NCs inside. Studies show that the electrochemical reaction processes of P-FeS@C electrodes are dominated by the pseudocapacitive behavior, leading to an ultrafast Na+-insertion/extraction reaction. Hence, the prepared P-FeS@C nanohybrid exhibits superior Na-storage properties especially high rate capability in half cells. For example, it can deliver reversible capacities of 555.1 mA h g-1 at 0.2 A g-1 over 150 cycles and about 60.4 mA h g-1 at 80 A g-1 (an ultrahigh current density even higher than that of the capacitor test). Furthermore, an advanced P-FeS@C//Na3V2(PO4)2O2F full cell has been assembled out, which delivers a stable specific capacity of 441.2 mA h g-1 after 80 cycles at 0.5 A g-1 with a capacity retention of 91.8%.
For the low security and compression performance of the existing joint image encryption and compression technology, an improvement algorithm for joint image compression and encryption is proposed. ...The algorithm employs the discrete cosine transformation dictionary to sparsely represent the color image and then combines it with the encryption algorithm based on the hyper-chaotic system to achieve image compression and encryption simultaneously. Through the experimental analysis, the algorithm proposed in this paper has a good performance in security and compression.
The response of the Indian Ocean dipole (IOD) mode to global warming is investigated based on simulations from phase 5 of the Coupled Model Intercomparison Project (CMIP5). In response to increased ...greenhouse gases, an IOD-like warming pattern appears in the equatorial Indian Ocean, with reduced (enhanced) warming in the east (west), an easterly wind trend, and thermocline shoaling in the east. Despite a shoaling thermocline and strengthened thermocline feedback in the eastern equatorial Indian Ocean, the interannual variance of the IOD mode remains largely unchanged in sea surface temperature (SST) as atmospheric feedback and zonal wind variance weaken under global warming. The negative skewness in eastern Indian Ocean SST is reduced as a result of the shoaling thermocline. The change in interannual IOD variance exhibits some variability among models, and this intermodel variability is correlated with the change in thermocline feedback. The results herein illustrate that mean state changes modulate interannual modes, and suggest that recent changes in the IOD mode are likely due to natural variations.
The Indian Ocean Dipole (IOD) is one of the leading modes of interannual sea surface temperature (SST) variability in the tropical Indian Ocean (TIO). The response of IOD to global warming is quite ...uncertain in climate model projections. In this study, the uncertainty in IOD change under global warming, especially that resulting from internal variability, is investigated based on the community earth system model large ensemble (CESM-LE). For the IOD amplitude change, the inter-member uncertainty in CESM-LE is about 50% of the intermodel uncertainty in the phase 5 of the coupled model intercomparison project (CMIP5) multimodel ensemble, indicating the important role of internal variability in IOD future projection. In CESM-LE, both the ensemble mean and spread in mean SST warming show a zonal positive IOD-like (pIOD-like) pattern in the TIO. This pIOD-like mean warming regulates ocean-atmospheric feedbacks of the interannual IOD mode, and weakens the skewness of the interannual variability. However, as the changes in oceanic and atmospheric feedbacks counteract each other, the inter-member variability in IOD amplitude change is not correlated with that of the mean state change. Instead, the ensemble spread in IOD amplitude change is correlated with that in ENSO amplitude change in CESM-LE, reflecting the close inter-basin relationship between the tropical Pacific and Indian Ocean in this model.
Treponema pallidum (Tp) has a well-known ability to evade the immune system and can cause neurosyphilis by invading the central nervous system (CNS). Microglia are resident macrophages of the CNS ...that are essential for host defense against pathogens, this study aims to investigate the interaction between Tp and microglia and the potential mechanism. Here, we found that Tp can exert significant toxic effects on microglia in vivo in Tg (mpeg1: EGFP) transgenic zebrafish embryos. Single-cell RNA sequencing results showed that Tp downregulated autophagy-related genes in human HMC3 microglial cells, which is negatively associated with apoptotic gene expression. Biochemical and cell biology assays further established that Tp inhibits microglial autophagy by interfering with the autophagosome-lysosome fusion process. Transcription factor EB (TFEB) is a master regulator of lysosome biogenesis, Tp activates the mechanistic target of rapamycin complex 1 (mTORC1) signaling to inhibit the nuclear translocation of TFEB, leading to decreased lysosomal biogenesis and accumulated autophagosome. Importantly, the inhibition of autophagosome formation reversed Tp-induced apoptosis and promoted microglial clearance of Tp. Taken together, these findings show that Tp blocks autophagic flux by inhibiting TFEB-mediated lysosomal biosynthesis in human microglia. Autophagosome accumulation was demonstrated to be a key mechanism underlying the effects of Tp in promoting apoptosis and preventing itself from clearing by human microglia. This study offers novel perspectives on the potential mechanism of immune evasion employed by Tp within CNS. The results not only establish the pivotal role of autophagy dysregulation in the detrimental effects of Tp on microglial cells but also bear considerable implications for the development of therapeutic strategies against Tp, specifically involving mTORC1 inhibitors and autophagosome formation inhibitors, in the context of neurosyphilis patients.
Person re-identification is to match pedestrian images from disjoint camera views detected by pedestrian detectors. Challenges are presented in the form of complex variations of lightings, poses, ...viewpoints, blurring effects, image resolutions, camera settings, occlusions and background clutter across camera views. In addition, misalignment introduced by the pedestrian detector will affect most existing person re-identification methods that use manually cropped pedestrian images and assume perfect detection. In this paper, we propose a novel filter pairing neural network (FPNN) to jointly handle misalignment, photometric and geometric transforms, occlusions and background clutter. All the key components are jointly optimized to maximize the strength of each component when cooperating with others. In contrast to existing works that use handcrafted features, our method automatically learns features optimal for the re-identification task from data. The learned filter pairs encode photometric transforms. Its deep architecture makes it possible to model a mixture of complex photometric and geometric transforms. We build the largest benchmark re-id dataset with 13, 164 images of 1, 360 pedestrians. Unlike existing datasets, which only provide manually cropped pedestrian images, our dataset provides automatically detected bounding boxes for evaluation close to practical applications. Our neural network significantly outperforms state-of-the-art methods on this dataset.
Developing high-efficiency, low-cost and environmental friendly electrode materials for both supercapacitors and overall water splitting are significant for renewable energy storage and conversion. ...Herein, we report a facile consubstantial growth strategy to fabricate subuliform NiCo2S4 nanorod arrays electrode through an in situ growing process, utilizing self-sacrificial Ni foam as substrate and Ni resource. Benefitting from the unique structures, the subuliform NiCo2S4 nanorods can be directly serve as binder-free, trifunctional electrode for overall water splitting with excellent electrocatalytic activity (oxygen evolution reaction with low overpotential of 220 mV at 30 mA cm−2 and hydrogen evolution reaction with low overpotential of 222 mV at 30 mA cm−2) and also as a promising pseudocapacitance electrode with superior electrochemical performance and good stability (high areal capacitance of 8.85 F cm−2 at a current density of 10 mA cm−2 and 94.96% capacitive retention after 10000 cycles). The present work highlights the remarkable advantages of the self-sacrificial strategy for the design of high-performance multifunctional electrode materials.
•The NiCo2S4 nanorod arrays are fabricated by an in situ hydrothermal process.•The integrated configuration of NiCo2S4 can greatly facilitate electron transfer.•The obtained NiCo2S4 electrode exhibit excellent electrochemical performance.
Ischemic stroke is a leading cause of morbidity and mortality worldwide. Resident microglia are the principal immune cells of the brain, and the first to respond to the pathophysiological changes ...induced by ischemic stroke. Traditionally, it has been thought that microglial activation is deleterious in ischemic stroke, and therapies to suppress it have been intensively explored. However, increasing evidence suggests that microglial activation is also critical for neurogenesis, angiogenesis, and synaptic remodeling, thereby promoting functional recovery after cerebral ischemia. Here, we comprehensively review the dual role of microglia during the different phases of ischemic stroke, and the possible mechanisms controlling the post-ischemic activity of microglia. In addition, we discuss the dynamic interactions between microglia and other cells, such as neurons, astrocytes, oligodendrocytes, and endothelial cells within the brain parenchyma and the neurovascular unit.