Bisphenol A (BPA), a typical endocrine disrupting chemical, is widespread in aqueous environment and cannot be efficiently treated by traditional water treatment technologies. Bismuth oxybromide ...(BiOBr) is a promising photocatalyst with a special layered structure. However, its band gap (2.8 eV) is not narrow enough for the efficient harvesting of visible light, severely restricting its practical use. Given that the band gap of Bi2S3 is only 1.3 eV, S-doping modification could be used to tailor the band structure of BiOBr. Here, series of S-doped BiOBr nanosheets was prepared through a facile hydrothermal procedure. The as-prepared S0.2-BiOBr nanosheets showed a narrower band gap of 2.33 eV. The intrinsic photocatalytic activity of S0.2-BiOBr sample for the degradation of BPA was 2.78 times higher than that of BiOBr under visible light degradation. Moreover, the mechanism of BPA degradation over the S-doped BiOBr under visible light irradiation was elucidated based on the experimental results and density functional theoretical calculations. Overall, a feasible and effective doping method was proposed to improve the utilization efficiency of visible light.
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•S-doped BiOBr nanosheets were synthesized using a facile hydrothermal procedure.•Bisphenol A was efficiently degraded over S-doped BiOBr under visible light irradiation.•The efficiency of the doped S element was confirmed using DFT calculation.•Superoxide radical produced by the photogenerated e− was the main active species for the degradation of BPA.
Post-translational modifications (PTMs) diversify the molecular structures of proteins and play essential roles in regulating their functions. Abnormal PTM status has been linked to a variety of ...developmental disorders and human diseases, highlighting the importance of studying PTMs in understanding physiological processes and discovering novel nodes and links with therapeutic intervention potential. Classical biochemical methods are suitable for studying PTMs on individual proteins; however, global profiling of PTMs in proteomes remains a challenging task. In this feature article, we start with a brief review of the traditional affinity-based strategies and shift the emphasis to summarizing recent progress in the development and application of chemical and computational proteomic strategies to delineate the global landscapes of functional PTMs. Finally, we discuss current challenges in PTM detection and provide future perspectives on how the field can be further advanced.
We propose all‐dielectric metasurfaces that can be actively re‐configured using the phase‐change material Ge2Sb2Te5 (GST) alloy. With selectively controlled phase transitions on the composing GST ...elements, metasurfaces can be tailored to exhibit varied functionalities. Using phase‐change GST rod as the basic building block, we have modelled metamolecules with tunable optical response when phase change occurs on select constituent GST rods. Tunable gradient metasurfaces can be realized with variable supercell period consisting of different patterns of the GST rods in their amorphous and crystalline states. Simulation results indicate a range of functions can be delivered, including multilevel signal modulating, near‐field coupling of GST rods, and anomalous reflection angle controlling. This work opens up a new space in exploring active meta‐devices with broader applications that cannot be achieved in their passive counterparts with permanent properties once fabricated.
The all‐dielectric reconfigurable metasurfaces based on switchable phase‐change material Ge2Sb2Te5 with functional diversity for light modulation are shown. The tunability of EIT resonance on phase‐change metamolecule and the steering of gradient metasurface are demonstrated by selectively modifying the phase of selected constituent Ge2Sb2Te5 rods.
A high-efficient, low-cost, and eco-friendly catalyst is highly desired to activate peroxides for environmental remediation. Due to the potential synergistic effect between bimetallic oxides’ two ...different metal cations, these oxides exhibit superior performance in the catalytic activation of peroxymonosulfate (PMS). In this work, novel Mn1.8Fe1.2O4 nanospheres were synthesized and used to activate PMS for the degradation of bisphenol A (BPA), a typical refractory pollutant. The catalytic performance of the Mn1.8Fe1.2O4 nanospheres was substantially greater than that of the Mn/Fe monometallic oxides and remained efficient in a wide pH range from 4 to 10. More importantly, a synergistic effect between solid-state Mn and Fe was identified in control experiments with Mn3O4 and Fe3O4. Mn was inferred to be the primary active site in the surface of the Mn1.8Fe1.2O4 nanospheres, while Fe(III) was found to play a key role in the synergism with Mn by acting as the main adsorption site for the reaction substrates. Both sulfate and hydroxyl radicals were generated in the PMS activation process. The intermediates of BPA degradation were identified and the degradation pathways were proposed. This work is expected to help to elucidate the rational design and efficient synthesis of bimetallic materials for PMS activation.
The wound-healing process is a natural response to burn injury. Resveratrol (RES) may have potential as a therapy for wound healing, but how and whether RES regulates skin repair remains poorly ...understood. Human epidermal keratinocyte (HaCaT) cells were treated with lipopolysaccharide (LPS), and a mouse skin wound-healing model was established. Cell viability and apoptosis were analyzed by 3-(4,5-dimethyl-2-thiazolyl)−2,5-diphenyl-2-H-tetrazolium bromide or flow cytometry. Cell proliferation was assessed by cell viability and colony-formation analyses. Cell migration was tested by wound-healing analysis. The microRNA-212 (miR-212) and caspase-8 (CASP8) levels were determined by quantitative reverse transcription polymerase chain reaction and western blotting. The correlation between miR-212 and CASP8 was analyzed by dual-luciferase reporter analysis. Skin wound healing in mice was assessed by measuring the wound area and gap after hematoxylin–eosin (HE) staining. RES reduced the LPS-induced reduction in viability and apoptosis in HaCaT cells. miR-212 expression was reduced by LPS and increased by exposure to RES. RES promoted cell proliferation and migration after LPS treatment by increasing miR-212 levels. CASP8 was a target of miR-212. CASP8 silencing promoted cell proliferation and migration, which was reversed by miR-212 knockdown in LPS-treated HaCaT cells. RES promoted skin wound healing in mice, which was reduced by miR-212 knockdown. Thus, RES facilitates cell proliferation and migration in LPS-treated HaCaT cells and promotes skin wound-healing in a mouse model by regulating the miR-212/CASP8 axis.
The authors aimed to provide new insights into the pathogenesis and treatment of cutaneous burns. They show that the plant polyphenol resveratrol contributes to cell proliferation and migration in lipopolysaccharide-stimulated human epidermal keratinocyte cells. Resveratrol promotes wound healing in a mouse skin wound model via regulation of the miR-212/CASP8 axis.
Itaconate has been recently recognized as an anti-inflammatory metabolite involved in the pathogen-macrophage interface. Due to its weak electrophilicity, itaconate could modify cysteines of the ...protein KEAP1 and glutathione, which contribute to its anti-inflammatory effect. However, the substrates of itaconate modification in macrophages have not been systematically profiled, which largely impedes the understanding of its roles in immune responses. Here, we developed a specific thiol-reactive probe, 1-OH-Az, for quantitative chemoproteomic profiling of cysteine modifications by itaconate, and provided a global portrait of its proteome reactivity. We found that itaconate covalently modifies key glycolytic enzymes and impairs glycolytic flux mainly through inhibition of fructose-bisphosphate aldolase A (ALDOA). Moreover, itaconate attenuates the inflammatory response in stimulated macrophages by impairing the glycolysis. Our study provides a valuable resource of protein targets of itaconate in macrophages and establishes a negative-feedback link between glycolysis and itaconate, elucidating new functional insights for this anti-inflammatory metabolite.
We report here the development of a suite of biocompatible SuFEx transformations from the SOF4‐derived iminosulfur oxydifluoride hub in aqueous buffer conditions. These biocompatible SuFEx reactions ...of iminosulfur oxydifluorides (R‐N=SOF2) with primary amines give sulfamides (8 examples, up to 98 %), while the reaction with secondary amines furnish sulfuramidimidoyl fluoride products (8 examples, up to 97 %). Likewise, under mild buffered conditions, phenols react with the iminosulfur oxydifluorides (Ar‐N=SOF2) to produce sulfurofluoridoimidates (13 examples, up to 99 %), which can themselves be further modified by nucleophiles. These transformations open the potential for asymmetric and trisubstituted linkages projecting from the sulfur(VI) center, including versatile S−N and S−O connectivity (9 examples, up to 94 %). Finally, the SuFEx bioconjugation of iminosulfur oxydifluorides to amine‐tagged single‐stranded DNA and to BSA protein demonstrate the potential of SOF4‐derived SuFEx click chemistry in biological applications.
SuFEx goes biology: New biocompatible SOF4‐based SuFEx reactions operating at low concentration in aqueous solution under mild pH and temperature conditions provide access to asymmetric and trisubstituted products at the sulfur(VI) center with versatile S−N and S−O connectivity. The SuFEx bioconjugation of iminosulfur oxydifluorides to either BSA protein or to single‐stranded DNA is demonstrated.
Chemical isotope labeling (CIL) LC-MS is a powerful tool for metabolome analysis with high metabolomic coverage and quantification accuracy. In CIL LC-MS, the overall metabolite detection efficiency ...using Orbitrap MS can be further improved by employing a segment scan method where the full m/z range is divided into multiple segments for spectral acquisition with a significant increase in the in-spectrum dynamic range. Considering the metabolic complexity in different types of biological samples (e.g., feces, urine, serum/plasma, cell/tissue extracts, saliva, etc.), we report the development and evaluation of the segment scan method for metabolome analysis of different sample types.
It was found that sample complexity significantly influenced the performance of the segment scan method. In metabolically complex samples such as feces and urine, the method yielded a substantial increase (up to 94 %) in detected peak pairs or metabolites, compared to conventional full scan. Conversely, less complex samples like saliva exhibited more modest gains (approximately 25 %). Based on the observations, a 120-m/z segment scan method was determined as a routine approach for CIL LC-Orbitrap-MS-based metabolomics with good compatibility with different types of biological samples. For this method, a further investigation on relative quantification accuracy was done. The peak area ratios of 12C-/13-labeled metabolites were slightly reduced with 72%–84 % of peak pairs falling within the ±25 % range of the anticipated peak ratio of 1.0 among different samples, as opposed to 81%–90 % in the full scan, which was attributed to the inclusion of more low-abundance peak pairs within the narrow MS segments. However, the overall peak ratio measurement precision was not significantly affected by the segment scan.
The segment scan method was found to be useful for CIL LC-Orbitrap-MS-based metabolome analysis of different types of samples with significant improvement in metabolite detectability (25–94 % increase), compared to the conventional full scan method.
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•Segment-scan-assisted LC-Orbitrap-MS was developed and evaluated for analyzing different types of samples.•The complexity of biological samples significantly influenced the performance of the segment scan method.•The more complex a sample the more gain of detectability the segment scan method offers.•A 120-m/z segment scan method was determined as a suitable routine approach for metabolomics.
Chemical isotope labeling (CIL) LC-MS is a powerful tool for metabolome analysis with markedly improved metabolomic coverage and quantification accuracy over the conventional LC-MS technique. In ...addition, with differential isotope labeling, each labeled metabolite is detected as a peak pair in the mass spectra, offering the possibility of differentiating true metabolite peaks from the singlet noise or background peaks. In this study, we examined the effects of instrument type on the detectability of true metabolites with a focus on the comparison of quadrupole time-of-flight (QTOF) and Orbitrap mass spectrometers. Using the same ultra-high-performance liquid chromatography setup and optimized running conditions for QTOF and Orbitrap, we compared the total number of peak pairs detected and identified from the two instruments using human urine and serum as the test samples. Many common peak pairs were detected from the two instruments; however, there were a significant number of unique peak pairs detected in each type of instrument. By combining the datasets obtained using QTOF and Orbitrap, the total number of peak pairs detected could be significantly increased. We also examined the effect of mass resolving power on peak pair detection in Orbitrap (60,000 vs. 120,000 resolution). The observed differences in peak pair detectability were much less than those of QTOF vs. Orbitrap. However, the type of peak pairs detected using different resolutions could be somewhat different, offering the possibility of increasing the overall number of peak pairs by combining the two datasets obtained at two different resolutions. The results from this study clearly indicate that instrument type can have a profound effect on metabolite detection in CIL LC-MS. Therefore, comparison of metabolome data generated using different instruments needs to be carefully done. Moreover, future research (e.g., hardware modifications) is warranted to minimize the differences in order to generate more reproducible metabolome data from different types of instruments.
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•QTOF and Orbitrap had different metabolite detectability from dansylated urine and serum.•Orbitrap operated at 60 k and 120 k resolutions also showed different metabolite detectability.•Combined datasets from different MS instruments increased the metabolome coverage.•Same type of instrument should be used for detecting common metabolites in comparative samples.
To unravel the potential of Licochalcone B as an anti-tumour phytochemical agent and evaluate its underlying mechanisms, we analyzed the mRNAs and miRNAs expression profiles of HepG2 cells in ...response to Licochalcone B (120 μM). mRNA and miRNA expression libraries were conducted and functional analysis for differential expression mRNAs was carried out utilizing Clue GO. We found 763 Licochalcone B -responsive differently expressed genes, among them, 572 mRNAs were up-regulated and 191 mRNAs were down-regulated, many of which were related to the MAPK signaling pathway. A protein-protein interaction network was constructed to discover the hub genes, and IL6, FOS, JUN, NOTCH1, UBC, UBB, CXCL8, CDKN1A, IL1B, ATF3, and GATA3 genes were screened out. Additionally, miRNAs engaged in Licochalcone B -mediated regulation on HepG2 cells were also studied. 85 differential expression miRNAs were identified, including 39 up-regulated miRNAs and 46 down-regulated miRNAs. Co-expression of miRNA-mRNA network was created and two key miRNAs (hsa-miR-29b-3p and hsa-miR-96-5p) were identified. These recognized key genes, miRNA, and the miRNA-mRNA regulatory network may provide clues to understand the molecular mechanism of Licochalcone B as an apoptotic inducer which may offer hint for its application as a functional food component.
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•The mRNAs and miRNAs expression profiles of HepG2 cells in response to Licochalcone B (120 μM) was investigated.•Licochalcone B up-regulated 572 mRNAs and down-regulated 191 mRNAs on HepG2 cells.•IL6, FOS, JUN, NOTCH1, UBC, UBB, CXCL8, CDKN1A, IL1B, ATF3, and GATA3 were filtered as hub genes.•Licochalcone B up-regulated 39 miRNAs and down-regulated 46 miRNAs on HepG2 cells.•Co-expression of miRNA-mRNA network was created and hsa-miR-96-5p were key miRNAs.
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