Dual‐atom catalysts (DACs) have emerged as efficient electrocatalysts for CO2 reduction owing to the synergistic effect between the binary metal sites. However, rationally modulating the electronic ...structure of DACs to optimize the catalytic performance remains a great challenge. Herein, we report the electronic structure modulation of three Ni2 DACs (namely, Ni2−N7, Ni2−N5C2 and Ni2−N3C4) by the regulation of the coordination environments around the dual‐atom Ni2 centres. As a result, Ni2−N3C4 exhibits significantly improved electrocatalytic activity for CO2 reduction, not only better than the corresponding single‐atom Ni catalyst (Ni−N2C2), but also higher than Ni2−N7 and Ni2−N5C2 DACs. Density functional theory (DFT) calculations revealed that the high electrocatalytic activity of Ni2−N3C4 for CO2 reduction could be attributed to the electronic structure modulation to the Ni centre and the resulted proper binding energies to COOH* and CO* intermediates.
Three Ni2 dual‐atom catalysts (DACs) with electronic structures tailored by the regulation of the coordination environment of Ni atoms, have been prepared for electrocatalytic CO2 reduction. The optimal Ni2−N3C4 exhibits the highest performance for the reduction of CO2 to CO, highlighting the significance of the electronic structure for electrocatalytic CO2 reduction in DACs.
We report acute antibody responses to SARS-CoV-2 in 285 patients with COVID-19. Within 19 days after symptom onset, 100% of patients tested positive for antiviral immunoglobulin-G (IgG). ...Seroconversion for IgG and IgM occurred simultaneously or sequentially. Both IgG and IgM titers plateaued within 6 days after seroconversion. Serological testing may be helpful for the diagnosis of suspected patients with negative RT-PCR results and for the identification of asymptomatic infections.
To achieve high‐efficiency deep‐blue electroluminescence satisfying Rec.2020 standard blue gamut, two thermally activated delayed fluorescent (TADF) emitters are developed: ...5‐(2,12‐di‐tert‐butyl‐5,9‐dioxa‐13b‐boranaphtho3,2,1‐deanthracen‐7‐yl)‐10,10‐diphenyl‐5,10‐dihydrodibenzob,e1,4azasiline (TDBA‐PAS) and 10‐(2,12‐di‐tert‐butyl‐5,9‐dioxa‐13b‐boranaphtho3,2,1‐deanthracen‐7‐yl)‐9,9‐diphenyl‐9,10‐dihydroacridine (TDBA‐DPAC). Inheriting from their parented organoboron multi‐resonance core, both emitters show very promising deep‐blue emissions with relatively narrow full width at half‐maximum (FWHM, ≈50 nm in solution), high photoluminescence quantum yield (up to 92.3%), and short emission lifetime (≤2.49 µs) with fast reverse intersystem crossing (>106 s−1) in doped films. More importantly, replacing the spiro‐centered sp3 C atom (TDBA‐DPAC) with the larger‐radius sp3 Si atom (TDBA‐PAS), enhanced conformational heterogeneities in bulky‐group‐shielded TADF molecules are observed in solution, doped film, and device. Consequently, OLEDs based on TDBA‐PAS retain high maximum external quantum efficiencies ≈20% with suppressed efficiency roll‐off and color index close to Rec.2020 blue gamut over a wide doping range of 10–50 wt%. This study highlights a new strategy to restrain spectral broadening and redshifting and efficiency roll‐off in the design of deep‐blue TADF emitters.
Conformational heterogeneity in bulky‐group‐shielded deep‐blue thermally activated delayed fluorescent emitters enables suppression of spectral broadening, redshifting, and concentration quenching. Devices based on the emitter present high external quantum efficiency up to 22.35% with suppressed efficiency roll‐off and color indices close to Rec.2020 blue gamut over a wide doping range of 10–50 wt%.
Background and Aims
The mechanism underlying HCC metastasis remains unclear, many oncogenes are known to regulate this process. However, the role of alternative splicing (AS) in pro‐metastatic HCC is ...poorly understood.
Approach and Results
By performing RNA sequencing on nine pairs of primary HCC tissues with extrahepatic metastasis (EHMH) and nine pairs of metastasis‐free HCC (MFH) tissues, we depicted the AS landscape in HCC and found a higher frequency of AS events in EHMH compared with MFH. Moreover, 28 differentially expressed splicing regulators were identified in EHMH compared with MFH. Among these, DEAD‐box RNA helicase 17 (DDX17) was significantly up‐regulated in EHMH and was strongly associated with patient outcome. Functional studies indicated that DDX17 knockout inhibited the degradation of the extracellular matrix, and diminished the invasive ability of HCC cells. A significant reduction in lung metastasis induced by DDX17 deficiency was also demonstrated in a diethylnitrosamine‐induced DDX17HKO mouse model. Mechanistically, high DDX17 induced intron 3 retention of PXN‐AS1 and produced a transcript (termed PXN‐AS1‐IR3). The transcript PXN‐AS1‐IR3 acted as an important promoter of HCC metastasis by inducing MYC transcription activation via recruiting the complex of testis expressed 10 and p300 to the MYC enhancer region, which led to transcriptional activation of several metastasis‐associated downstream genes. Finally, the PXN‐AS1‐IR3 level was significantly higher in serum and HCC tissues with extrahepatic metastasis.
Conclusions
DDX17 and PXN‐AS1‐IR3 act as important metastatic promoters by modulating MYC signaling, suggesting that DDX17 and PXN‐AS1‐IR3 may be potential prognostic markers for metastatic HCC.
Abstract
Background
Severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), a novel β-coronavirus, causes severe pneumonia and has spread throughout the globe rapidly. The disease associated ...with SARS-CoV-2 infection is named coronavirus disease 2019 (COVID-19). To date, real-time reverse-transcription polymerase chain reaction (RT-PCR) is the only test able to confirm this infection. However, the accuracy of RT-PCR depends on several factors; variations in these factors might significantly lower the sensitivity of detection.
Methods
In this study, we developed a peptide-based luminescent immunoassay that detected immunoglobulin (Ig)G and IgM. The assay cutoff value was determined by evaluating the sera from healthy and infected patients for pathogens other than SARS-CoV-2.
Results
To evaluate assay performance, we detected IgG and IgM in the sera from confirmed patients. The positive rate of IgG and IgM was 71.4% and 57.2%, respectively.
Conclusions
Therefore, combining our immunoassay with real-time RT-PCR might enhance the diagnostic accuracy of COVID-19.
A peptide-based magnetic chemiluminescence enzyme immunoassay for the detection of SARS-CoV-2 antibodies was developed; 71.4% (197 of 276) and 57.2% (158 of 276) of the COVID-19 inpatients were positive for IgG and IgM against SARS-CoV-2.
Atypical porcine pestivirus (APPV) was recently reported to be associated with neurologic disorders in newborn piglets. Investigations of 1,460 serum samples of apparently healthy pigs from different ...parts of Europe and Asia demonstrate a geographically wide distribution of genetically highly variable APPV and high APPV genome and antibody detection rates.
Cellular metabolism plays a central role in the regulation of both innate and adaptive immunity. Immune cells utilize metabolic pathways to modulate the cellular differentiation or death. The ...intricate interplay between metabolism and immune response is critical for maintaining homeostasis and effective antiviral activities. In recent years, immunometabolism induced by viral infections has been extensively investigated, and accumulating evidence has indicated that cellular metabolism can be hijacked to facilitate viral replication. Generally, virus-induced changes in cellular metabolism lead to the reprogramming of metabolites and metabolic enzymes in different pathways (glucose, lipid, and amino acid metabolism). Metabolic reprogramming affects the function of immune cells, regulates the expression of immune molecules and determines cell fate. Therefore, it is important to explore the effector molecules with immunomodulatory properties, including metabolites, metabolic enzymes, and other immunometabolism-related molecules as the antivirals. This review summarizes the relevant advances in the field of metabolic reprogramming induced by viral infections, providing novel insights for the development of antivirals.
Revealing the contribution of π-π stacking interactions in supramolecular assembly is important for understanding the intrinsic nature of molecular assembly fundamentally. However, because they are ...much weaker than covalent bonds, π-π stacking interactions are usually ignored in the construction of porous materials. Obtaining stable porous materials that are only dependent on π-π stacking interactions, despite being very challenging, could address this concern. Here, we present a porous supramolecular framework (
) stabilized only by intermolecular π-π stacking interactions.
shows good thermal and chemical stability not only in various organic solvents but also in aqueous solution in a broad pH range. Furthermore, featuring one-dimensional channels with dangling thiolate groups,
exhibits excellent Hg
removal performance, with adsorption capacity as high as 786.67 mg g
and an adsorption ratio as high as 99.998%. In addition,
also shows high adsorption selectivity to Hg
in the presence of a series of interfering ions.
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•Carbon-dot (CD) hydrogels were prepared for PFOS removal.•CD hydrogels adsorbed PFOS with a maximum capacity of 2.82 g/g.•CD hydrogels could be regenerated and reused.•CD hydrogels ...could remove PFOS in firefighting and environmental wastewaters.
Efficiently removing perfluorooctane sulfonate (PFOS) from wastewaters is a hot topic in environmental field. Herein, crosslinking the nano-sized and zero-dimensional carbon dots (CDs) with polyethylene glycol diglycidyl ether (PEG) and polypropylene glycol diglycidyl ether (PPG) resulted in CD hydrogels that were verified by TEM, SEM, FTIR and XPS. The obtained CD hydrogels could efficiently adsorb PFOS from water through their CD moieties. The kinetic curves were fitted well by the pseudo-second order model, indicating the involvement of chemisorption in the rate-limiting step. The adsorption isotherm measurements showed that the hydrogel with the highest CD content had a PFOS maximum uptake capacity of ca. 2.82 g/g (5.64 mmol/g) in the neutral water, which was much higher than the ever-reported carbonaceous materials, and also ranked the top three among the superior positively-charged adsorbents. The superior PFOS adsorption of CD hydrogels could be attributed to good dispersion of the nanoscale CDs in the PEG/PPG hydrogel matrix, leading to the substantial exposure of the binding sites of CDs towards PFOS molecules. Moreover, CD hydrogels did not show pronounced loss of adsorption capacity after experiencing five adsorption-desorption cycles. As for the real wastewaters, CD hydrogels could efficiently treat not only the high concentration of PFOS in the neutral firefighting wastewaters, but also the extremely low concentration of PFOS in the neutral environmental wastewater, where the residual PFOS concentration could be reduced less than 5 ng/L, satisfying the standard of the U.S. Environmental Protection Agency.
Using an experimental approach, the role of metal catalysis has been investigated in the in situ cycloaddition reaction of nitrile with azide to form tetrazoles. It has been shown that metal ...catalysis serves to activate the cyano group in the nitrile reagent by a coordinative interaction.
A key role: Using an experimental approach, the role of metal catalysis has been investigated in the in situ cycloaddition reaction of nitrile with azide to form tetrazoles. X‐ray crystallography and IR spectroscopy are used to show that the metal species acts as a catalyst, activating the cyano group in the nitrile‐containing reagent by a coordinative interaction.
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