The layer‐structured MoS2 is a typical hydrogen evolution reaction (HER) electrocatalyst but it possesses poor activity for the oxygen evolution reaction (OER). In this work, a cobalt covalent doping ...approach capable of inducing HER and OER bifunctionality into MoS2 for efficient overall water splitting is reported. The results demonstrate that covalently doping cobalt into MoS2 can lead to dramatically enhanced HER activity while simultaneously inducing remarkable OER activity. The catalyst with optimal cobalt doping density can readily achieve HER and OER onset potentials of −0.02 and 1.45 V (vs reversible hydrogen electrode (RHE)) in 1.0 m KOH. Importantly, it can deliver high current densities of 10, 100, and 200 mA cm−2 at low HER and OER overpotentials of 48, 132, 165 mV and 260, 350, 390 mV, respectively. The reported catalyst activation approach can be adapted for bifunctionalization of other transition metal dichalcogenides.
A cobalt covalent doping catalyst activation approach to induce hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) bifunctionality of MoS2 is proposed and experimentally validated, demonstrating superior bifunctional electrocatalytic activities with great application potential for overall water splitting in alkaline media.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Pancreatic ductal adenocarcinoma (PDAC) is the most common type of pancreatic cancer featured with high intra-tumoral heterogeneity and poor prognosis. To comprehensively delineate the PDAC ...intra-tumoral heterogeneity and the underlying mechanism for PDAC progression, we employed single-cell RNA-seq (scRNA-seq) to acquire the transcriptomic atlas of 57,530 individual pancreatic cells from primary PDAC tumors and control pancreases, and identified diverse malignant and stromal cell types, including two ductal subtypes with abnormal and malignant gene expression profiles respectively, in PDAC. We found that the heterogenous malignant subtype was composed of several subpopulations with differential proliferative and migratory potentials. Cell trajectory analysis revealed that components of multiple tumor-related pathways and transcription factors (TFs) were differentially expressed along PDAC progression. Furthermore, we found a subset of ductal cells with unique proliferative features were associated with an inactivation state in tumor-infiltrating T cells, providing novel markers for the prediction of antitumor immune response. Together, our findings provide a valuable resource for deciphering the intra-tumoral heterogeneity in PDAC and uncover a connection between tumor intrinsic transcriptional state and T cell activation, suggesting potential biomarkers for anticancer treatment such as targeted therapy and immunotherapy.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Spaceborne synthetic aperture radar (SAR) real-time imaging is especially important for disaster emergencies and real-time monitoring applications with highly desired real-time requirements. ...Therefore, the continuous improvement of real-time imaging efficiency is an important development trend. At present, traditional real-time imaging algorithms based on constant pulse repetition frequency (PRF) have low accuracy when processing spaceborne SAR data with nonlinear trajectory. For this problem, the existing methods usually introduce some complex signal processing steps, such as scaling or interpolation processing, to improve the accuracy of the real-time imaging, but this will reduce its efficiency. Therefore, this article proposes a new real-time imaging algorithm based on variable PRF for nonlinear trajectory spaceborne SAR. By introducing the variable PRF, the proposed algorithm is equivalent to complete the complex signal processing steps in the radar signal transmission stage, which can greatly improve the efficiency of real-time imaging. Simulation experiments verify the effectiveness of the algorithm.
The exact role of moist deep convection and associated latent heating in the tropical Hadley circulation has been debated for many years. This study investigates the connection between moist ...convection and the strength of the upper‐level meridional circulation over the tropical Atlantic, focusing mainly on one particular boreal winter season. There is a close relationship between events of strong organised deep convection and enhanced meridional upper‐level wind on many occasions. A process‐based analysis of specific events suggests that moist convection impacts Hadley circulation variability on time‐scales of days to months through equatorial wave dynamics. Equatorial waves play an important role, both directly by contributing to the Hadley circulation via their meridional wind component and also indirectly by triggering moist convection through low‐level convergence. Specific Hadley circulation surge events, short‐term, regionally confined intensifications of the upper‐level meridional circulation, can be attributed to enhanced organised moist convection and equatorial wave activity in many cases, with implications for trade wind cloudiness. The findings thus elucidate how the mean Hadley circulation is shaped by and composed of temporally and spatially varying convection–circulation interactions.
The role of moist convection in the Hadley circulation has been debated for many years. Tropical moist convection can be vigorous, with updraft velocities in deep convective clouds of several meters per second, and often occurs in organised convective systems. In this study we present strong evidence that tropical moist convection is an important driver of regional Hadley circulation variability over the Atlantic on time‐scales of days to months, and that equatorial waves play a mediating role in the process.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
This study presents an analysis of the equatorial waves in the ERA5 reanalysis and forecasts of the Met Office Global Seasonal Forecast System version 5 (GloSea5), by projecting dynamical fields onto ...theoretical equatorial wave modes. The seasonal and interannual variation of equatorial wave activity in GloSea5 is evaluated against ERA5 waves. We find that in ERA5 the seasonal and spatial variations of eastward‐moving Kelvin wave activity are mainly determined by the ambient zonal flow, with wave activity being stronger in easterlies than westerlies. For the westward‐moving mixed Rossby–gravity waves and equatorial Rossby waves, the seasonal and spatial variations of the upper‐tropospheric wave activity are determined by both the ambient flow and extratropical forcing with stronger wave activity generally in the westerlies, whilst the lower‐tropospheric wave activity is related to the ambient flow and tropical convection. In GloSea5, the Kelvin wave activity is not well simulated in the upper troposphere, and in general the wave activity and wave‐related convective signal are too weak. In contrast, GloSea5 performs better for the westward‐moving equatorial waves, including their Doppler‐shifted eastward‐moving components, despite a significant overestimation in the Atlantic and African region. The phase of ENSO has a substantial impact on equatorial waves in both ERA5 and GloSea5. The mechanism of the impact is through changes in the ENSO‐related ambient flow, upper‐tropospheric extratropical forcing, and tropical convection. GloSea5 can capture the low‐level Kelvin wave–ENSO relationship reasonably well, with stronger wave activity over the eastern Pacific in El Niño, although the ENSO‐driven variation is too weak. The wave–ENSO relationship for westward‐moving waves is well represented in GloSea5, especially in the upper‐level eastern‐Pacific westerly duct region in the extended boreal winter and the low‐level Indo‐Pacific in all seasons. We conclude that in GloSea5 the representation of the wave–ENSO teleconnection is the key driver for the performance of interannual variability in the wave activity.
This study presents an analysis and comparison of equatorial waves in the ERA5 reanalysis and GloSea5 forecasts, by projecting dynamical fields onto theoretical equatorial wave modes. The seasonal and spatial variations of Kelvin wave activity is mainly determined by the ambient zonal flow, with wave activity being stronger in the ambient easterlies than westerlies. In GloSea5 the Kelvin wave activity is generally too weak, consistent with that the Kelvin wave‐related convective signal is nearly missing in GloSea5.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Cancer stem cells (CSCs), also known as tumor-initiating cells (TICs), are suggested to be responsible for drug resistance and cancer relapse due in part to their ability to self-renew themselves and ...differentiate into heterogeneous lineages of cancer cells. Thus, it is important to understand the characteristics and mechanisms by which CSCs display resistance to therapeutic agents. In this review, we highlight the key features and mechanisms that regulate CSC function in drug resistance as well as recent breakthroughs of therapeutic approaches for targeting CSCs. This promises new insights of CSCs in drug resistance and provides better therapeutic rationales to accompany novel anticancer therapeutics.
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FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, UL, UM, UPUK
Although 5-methylcytosine (m
C) is a widespread modification in RNAs, its regulation and biological role in pathological conditions (such as cancer) remain unknown. Here, we provide the ...single-nucleotide resolution landscape of messenger RNA m
C modifications in human urothelial carcinoma of the bladder (UCB). We identify numerous oncogene RNAs with hypermethylated m
C sites causally linked to their upregulation in UCBs and further demonstrate YBX1 as an m
C 'reader' recognizing m
C-modified mRNAs through the indole ring of W65 in its cold-shock domain. YBX1 maintains the stability of its target mRNA by recruiting ELAVL1. Moreover, NSUN2 and YBX1 are demonstrated to drive UCB pathogenesis by targeting the m
C methylation site in the HDGF 3' untranslated region. Clinically, a high coexpression of NUSN2, YBX1 and HDGF predicts the poorest survival. Our findings reveal an unprecedented mechanism of RNA m
C-regulated oncogene activation, providing a potential therapeutic strategy for UCB.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
2D covalent organic frameworks (2D COFs) have been recognized as a novel class of photoactive materials owing to their extended π‐electron conjugation and high chemical stabilities. Herein, a new ...covalent organic framework (Tph‐BDP) is facilely synthesized by using a porphyrin derivative and an organic dye BODIPY derivative (5,5‐difluoro‐2,8‐diformyl‐1,3,7,9‐tetramethyl‐10‐phenyl‐5H‐dipyrrolo1,2‐c:2′,1′‐f1,3,2diazabori‐nin‐4‐ium‐5‐uide) as monomers for the first time, and their unique photosensitive properties endow them excellent simulated oxidase activity under 635 nm laser irradiation that can catalyze the oxidation of 3,3′,5,5′‐tetramethylbenzidine (TMB). Further findings demonstrate that the presence of uranium (UO22+) can coordinate with imines of the oxidation products of TMB, thus modulating the charge transfer process of the colored products accompanied with intensive aggregation and remarkable color fading. This research provides a preparation strategy for COFs with excellent photocatalytic properties and nanozyme activity, and broadens the applications of the simple colorimetric methods for sensitive and selective radionuclide detection.
A new covalent organic framework is facilely synthesized and its unique photosensitive property endows excellent simulated oxidase activity that can catalyze the oxidation of 3,3′,5,5′‐tetramethylbenzidine (TMB). The presence of uranium can coordinate with imines of the oxidation products of TMB, thus modulating the charge transfer process of the colored products accompanied with intensive aggregation and remarkable color fading.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
A combined strategy of building blocks recognition and molecular network construction, termed the building blocks‐based molecular network (BBMN), was first presented to facilitate the efficient ...discovery of novel natural products. By mapping the BBMN of the total alkaloid fraction of Flueggea suffruticosa, three Securinega alkaloids (SEAs) with unusual chemical architectures, suffranidines A–C (1–3), were discovered and isolated. Compound 1 characterizes an unprecedented 8/5/6/5/6/6/6/6‐fused octacyclic scaffold with a unique cage‐shaped 3‐azatricyclo6.4.0.03,11dodecane core. Compounds 2 and 3 are highly modified SEA dimers that incorporate additional C6 motifs. A hypothetical biosynthetic pathway for 1–3 was proposed. In addition, 1 significantly induced neuronal differentiation and neurite extension by upregulating eukaryotic elongation factor 2 (eEF2)‐mediated protein synthesis.
A building blocks‐based molecular network (BBMN) strategy was first presented and resulted in the discovery of three novel Securinega alkaloids. Compound 1 features an unprecedented 8/5/6/5/6/6/6/6‐fused octacyclic scaffold with a unique cage‐shaped 3‐azatricyclo6.4.0.03,11dodecane core, which also exhibited remarkable effects on neuronal differentiation and neurite extension.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Surface engineering has been shown critical for the success of perovskite solar cells by passivating the surface enriched defects and mobile species. The discovery of surface modulators with superior ...interaction strength to perovskite is of paramount importance since they can retain reliable passivation under various environments. Here, we report a chelation strategy for surface engineering of CsPbI
Br perovskite, in which dithiocarbamate molecules can be coordinate to surface Pb sites via strong bidentate chelating bonding. Such chelated CsPbI
Br perovskite can realize excellent passivation of surface under-coordinated defects, reaching a champion power conversion efficiency of 17.03% and an open-circuit voltage of 1.37 V of CsPbI
Br solar cells. More importantly, our chelation strategy enabled excellent device stability by maintaining 98% of their initial efficiency for over 1400 h in ambient condition. Our findings provide scientific insights on the surface engineering of perovskite that can facilitate the further development and application of perovskite optoelectronics.
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