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Temporal compressive coherent diffraction imaging is a lensless imaging technique with the capability to capture fast-moving small objects. However, the accuracy of imaging reconstruction is often hindered by the loss of frequency domain information, a critical factor limiting the quality of the reconstructed images. To improve the quality of these reconstructed images, a method dual-domain mean-reverting diffusion model-enhanced temporal compressive coherent diffraction imaging (DMDTC) has been introduced. DMDTC leverages the mean-reverting diffusion model to acquire prior information in both frequency and spatial domain through sample learning. The frequency domain mean-reverting diffusion model is employed to recover missing information, while hybrid input-output algorithm is carried out to reconstruct the spatial domain image. The spatial domain mean-reverting diffusion model is utilized for denoising and image restoration. DMDTC has demonstrated a significant enhancement in the quality of the reconstructed images. The results indicate that the structural similarity and peak signal-to-noise ratio of images reconstructed by DMDTC surpass those obtained through conventional methods. DMDTC enables high temporal frame rates and high spatial resolution in coherent diffraction imaging.
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Developing pure inorganic catalysts for low-energy transfer hydrogenation of biomass-derived furfural and alcohols below 100 °C is still challenging. This work reports highly dispersed Zr(IV) species catalysts prepared by irreversible adsorption of different solvent-dissolved Zr(IV) cations such as Zr4+ or [Zr4(OH)8(H2O)16]8+ on/in SBA-15 through Zr-O coordination, without adding an alkaline precipitant and calcination treatment. In the transfer hydrogenation of furfural to furfuryl alcohol, the Zr(IV) species catalysts exhibited unexpectedly outstanding transfer hydrogenation activity at low temperatures of 70 and 85 °C, superior to other transition-metal (Zr4+, Hf4+, Fe3+, etc.)- and main-group metal (Al3+, etc.)-based inorganic catalysts, which need high reaction temperatures above 100 °C, and comparable to the best-performing metal-organic hybrid catalysts with precise defect engineering modification or specific macromolecular ligands, and had negligible Zr leaching amounts (<0.01%) in water and in the collected liquid reaction medium from 7 cycles of reactions. In addition, the large strong Lewis acidic site amount rather than the large total acidic amount is a crucial condition for the catalysts to obtain high transfer hydrogenation activity, and basic sites were also involved in catalysis, and their absence would induce the acetalization side reaction. Furthermore, the catalysts were universal for low-temperature transfer hydrogenation of other aldehydes.
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Construction of pyrrolidinyl-spiroindoles with easily available starting materials has attracted considerable attention from the synthesis community and is in great demand. Here, we describe a base-promoted formal (3 + 2) cycloaddition of α-halohydroxamates with alkenyl-iminoindolines. The present methodology features mild reaction conditions and a broad substrate scope with up to 99% yield and excellent diastereoselectivity. The versatility of this approach is demonstrated through valuable synthetic transformations. Preliminary mechanistic studies shed light on the mechanism of this cycloaddition process.
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The limited characterization and detection capacity of unknown compounds hinder our understanding of the molecular composition of toxic compounds in PM2.5. The present study applied Fourier transform ion cyclotron resonance mass spectrometry coupled with negative and positive electrospray ionization sources (ESI-/ESI+ FT-ICR-MS) to probe the molecular characteristics and dynamic formation processes of the effective proinflammatory components in organic aerosols (OAs) of PM2.5 in Guangzhou for one year. We detected abundant proinflammatory molecules in OAs, mainly classified as CHON compounds (compounds composed of C, H, O, and N atoms) in elemental and nitroaromatic compounds (NACs) in structures. From the perspective of the formation process, we discovered that these proinflammatory molecules, especially toxic NACs, were largely driven by secondary nitrate formation and biomass burning (in emission source), as well as SO2 (in atmospheric evolution). In addition, our results indicated that the secondary processes had replaced the primary emission as the main contributing source of the toxic proinflammatory compounds in OAs. This study highlights the importance of community measures to control the production of nitroaromatic compounds derived from secondary nitrate formation and biomass burning in urban areas.
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Nitratos , Compostos Orgânicos , Nitratos/análise , Biomassa , Espectrometria de Massas , Compostos Orgânicos/análise , Material Particulado/análise , Aerossóis/análise , BioensaioRESUMO
By annealing an Fe(III)-coordination compound (Fe-CC), [FeCl3(Hbta)2] (Hbta = benzotriazole) in the presence of a carbon nanotube precursor (PCNT) template, an Fe4N/Fe3N/Fe/CNT heterostructure was successfully synthesized without an extra nitrogen source. The decomposition of the Hbta in Fe-CC under high-temperature annealing can produce carbon sheets and reduced graphene oxide (rGO), and the presence of CNTs can alleviate the stacking of thein situ-generated carbon materials. Meanwhile, iron nitride nanoparticles (NPs) can be anchored on the carbon sheets, and the anchoring effect efficiently prevents the agglomeration of NPs and increases the amount of active catalytic sites for the oxygen evolution reaction (OER). Fe4N/Fe3N/Fe/CNT shows an excellent OER activity with a Tafel slope of 63 mV dec-1as well as overpotentials of 121 (η10) and 275 mV (η100) at 10 and 100 mA cm-2, respectively - far exceeding commercial RuO2and other catalysts. Density functional theory calculations show that the excellent OER performance of Fe4N/Fe3N/Fe/CNT is associated with the Fe4N/Fe3N heterojunction, which can improve the electron conductivity and boost the electron transfer from N to Fe. The Fe4N/Fe3N/Fe/CNT catalyst exhibits long-term OER activity during 100 h of electrolysis at 20 mA cm-2. This is related to the dual coatings of thein situ-generated thin carbon shell and few-layered rGO on the surface of the iron nitride NPs, which can protect the fast leaching of iron nitride during the OER process. Furthermore, the effects of the annealing temperature, the PCNT template and the heating rate on the calcined products were investigated.
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Based on a coordination polymer, FeCl2(4,4'-bpy) (4,4'-bpy = 4,4'-bipyridine) and the carbon nanotube (CNT)/NaCl dual template, Fe3N nanoparticles (NPs) were synthesized via chemical thermolysis in the absence of an extra nitrogen source. The decomposition of 4,4'-bpy under high temperature produces thin carbon coating for Fe3N NPs. Also, the CNT template anchors the Fe3N NPs to avoid aggregation. The sample (denoted as Fe3N-C N) exhibits excellent electrocatalytic oxygen evolution reaction (OER) behavior even with a small molar ratio of Fe3N (Fe: 4.9 at. %), which can deliver a current density of 10 mA cm-2 at an overpotential of 218 mV with a Tafel slope of 84 mV dec-1 and long-term OER activity during 60 h electrolysis at 20 mA cm-2. Furthermore, the sample after 20 h electrolysis, denoted as Post-Fe3N-C N (20 h), displays enhanced OER activity with a smaller Tafel slope of 41 mV dec-1 and overpotentials of 195 and 327 mV at 10 and 100 mA cm-2, respectively, which is mainly due to the partial transformation of Fe3N into FeOOH. The OER mechanism is investigated by density functional theory calculations, and it is found that the surface partial oxidation of Fe3N leads to the effective OER electrolysis, which changes the electron density of the superficial atoms and induces the moderate adsorption for the intermediates.
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Although lead associated with intelligence decline in children has long been reported, studies combining intelligence determination, molecular mechanisms exploration, and biomarker screen are quite rare. In this study, based on 333 children aged 9-11, we determined the role of DNA methylation (DNAm) in the relationship of lead exposure with children's intelligence. DNAm was measured from children's blood DNA specimens, and mediation analysis was performed to identify DNAm biomarkers mediating the lead-intelligence relationship. We identified forty-three differentially methylated regions (DMRs), and two fragments (FAM50B1 and PTCHD3) significantly mediated the lead-intelligence relationship, with contribution rates of 30.36% (p = 0.010) and 60.36% (p < 0.001), respectively. In addition, blood lead levels (BLLs) lower than 100 µg/L still adversely affected children's IQs and DNAm of the two fragments. Our data suggests that DNAm mediates lead-associated cognitive delay in children and blood lead reference value for school-aged children (100 µg/L) should be revised, and the candidate biomarkers can be used in related neurological diseases in future.
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Metilação de DNA , Chumbo , Criança , China , Exposição Ambiental , Humanos , Inteligência , Instituições AcadêmicasRESUMO
Six month old Cinnamomum cassia seedlings were used to simulate drought stress with polyethylene glycol(PEG 6000). The physiological indicators(osmotic substances, antioxidant enzymes, etc.) and chemical components of seedlings under different drought levels and the correlation between the two were studied. The results showed that the chlorophyll content and relative water content decreased gradually with the increase of PGE 6000(0, 5%, 10%, 15%) concentration and time(3, 5, 7 d), while the soluble protein content, soluble sugar content and catalase(CAT) activity increased, but the rising rate slowed down with the time. The activities of peroxidase(POD), superoxide dismutase(SOD), malondialdehyde(MDA) and proline content increased at first and then decreased. The content of coumarin, cinnamaldehyde, cinnamic acid and dimethoxycinnamaldehyde decreased, while the content of cinnamyl alcohol continued to increase.Under drought stress, the fluorescence signals of reactive oxygen species and no contents in roots of C. cassia seedlings were significantly stronger than those of the control.Further correlation analysis showed that coumarin content, di-methoxycinnamaldehyde content and osmoregulation substance content were significantly negatively correlated(P<0.05), cinnamic acid content was significantly negatively correlated with POD and SOD activities(P<0.01).It was found that C. cassia seedlings showed a certain degree of drought tolerance under short-term or mild drought stress, but if the drought exceeded a certain degree, the physiological metabolism of the seedlings would be unbalanced.
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Cinnamomum aromaticum , Plântula , Catalase , Secas , Malondialdeído , Estresse Fisiológico , Superóxido DismutaseRESUMO
MicroRNA 182 is important for the clonal expansion of CD4+ T cells (Th) following IL-2 stimulation and is a potential therapeutic target for autoimmune diseases. In the present study, we investigated the role of microRNA 182 in the differentiation of pro-inflammatory CD4+ T helper cell by overexpressing or silencing microRNA 182 expression both in in vivo and in vitro settings. We report that in the studied Chinese cohort, microRNA 182 is upregulated in patients with relapse and remitting multiple sclerosis (RRMS) and this upregulation is associated with increased IFN-γ producing CD4+ Th1 cells in the circulation. In the murine experimental autoimmune encephalomyelitis (EAE) model, global microRNA 182 overexpression exacerbates clinical symptoms and results in augmented CD4+ IFN-γ+ Th1 and CD4+ IL-17+ Th17 differentiation in vivo. Addition of microRNA 182 mimics in vitro represses both the protein expression and transcriptional activity of hypoxia induced factor 1α (HIF-1α) but increases the level of IFN-γ transcripts in sorted murine CD4+ T cells. Together, our results provide evidence that microRNA 182 may be one of the transitional hubs contribution to regulate Th cells expansion in response to self-antigens and differentiation of antigen specific Th cells during the progression of autoimmune inflammations.
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Diferenciação Celular/imunologia , Encefalomielite Autoimune Experimental/imunologia , Subunidade alfa do Fator 1 Induzível por Hipóxia/imunologia , MicroRNAs/imunologia , Esclerose Múltipla/imunologia , Células Th1/imunologia , Animais , Encefalomielite Autoimune Experimental/patologia , Feminino , Interferon gama/imunologia , Interleucina-17/imunologia , Camundongos , Esclerose Múltipla/patologia , Células Th1/patologia , Células Th17/imunologia , Células Th17/patologiaRESUMO
Pluripotency of embryonic stem cells (ESCs) can be functionally assessed according to the developmental potency. Tetraploid complementation, through which an entire organism is produced from the pluripotent donor cells, is taken as the most stringent test for pluripotency. It remains unclear whether ESCs of other species besides mice can pass this test. Here we show that the rat ESCs derived under 2i (two small molecule inhibitors) conditions at very early passages are able to produce fertile offspring by tetraploid complementation. However, they lose this capacity rapidly during culture due to a nearly complete loss of genomic imprinting. Our findings support that the naïve ground state pluripotency can be captured in rat ESCs but also point to the species-specific differences in its regulation and maintenance, which have implications for the derivation and application of naïve pluripotent stem cells in other species including human.