RESUMO
Molybdenum disulfide (MoS2) has been recognized as a promising cost-effective catalyst for water-splitting hydrogen production. However, the desired performance of MoS2 is often limited by insufficient edge-terminated active sites, poor electrical conductivity, and inefficient contact to the supporting substrate. To address these limitations, we developed a unique nanoarchitecture (namely, winged Au@MoS2 heterostructures enabled by our discovery of the "seeding effect" of Au nanoparticles for the chemical vapor deposition synthesis of vertically aligned few-layer MoS2 wings). The winged Au@MoS2 heterostructures provide an abundance of edge-terminated active sites and are found to exhibit dramatically improved electrocatalytic activity for the hydrogen evolution reaction. Theoretical simulations conducted for this unique heterostructure reveal that the hydrogen evolution is dominated by the proton adsorption step, which can be significantly promoted by introducing sufficient edge active sites. Our study introduces a new morphological engineering strategy to make the pristine MoS2 layered structures highly competitive earth-abundant catalysts for efficient hydrogen production.
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Two sequencing batch reactors (SBRs) were operated for 100days under aerobic conditions, with one being fed with unsterilized municipal wastewater (USBR), and the other fed with sterilized municipal wastewater (SSBR). Respirometric assays and fluorescence in situ hybridization (FISH) results show that active nitrifiers were present in the unsterilized influent municipal wastewater. The maximum ammonia utilization rate (AUR) and nitrite utilization rate (NUR) of the unsterilized influent were 0.32±0.12mg NH4+-N/(L·hr) and 0.71±0.18mg NO2--N/(L·hr). Based on the maximum utilization rates, the estimated seeding intensity for the ammonia oxidizing bacteria (AOB) and nitrite oxidizing bacteria (NOB) of the USBR was 0.08g AOB/(g AOB·day) and 0.20g NOB/(g NOB·day) respectively. The fraction of nitrifiers/total bacteria in the influent was 5.35%±2.1%, the dominant AOB was Nitrosomonas spp., Nitrosococcus mobilis hybridizated with Nsm156, and the dominant NOB was Nitrospira hybridizated with Ntspa662. The influent nitrifiers potentially seeded the activated sludge of the bioreactor and hence demonstrated a mitigation of the acclimatization times and instability during start-up and early operation. The AUR and NUR in the USBR was 15% and 13% higher than the SSBR respectively during the stable stage, FISH results showed that nitrifiers population especially the Nitrospira in the USBR was higher than that in the SSBR. These results indicate that the natural continuous immigration of nitrifiers from municipal influent streams may have some repercussions on the modeling and design of bioreactors.
Assuntos
Reatores Biológicos/microbiologia , Nitrificação , Esgotos/microbiologiaRESUMO
Amyloid ß-protein (Aß) aggregation is considered to be a critical step in the neurodegeneration of Alzheimer's disease (AD). In addition to Aß, many proteins aggregate into the amyloid state, in which they form elongated fibers with spines comprising stranded ß-sheets. However, the cross-seeding effects of other protein aggregates on Aß aggregation pathways are not completely clear. To investigate the cross-seeding effects of exogenous and human non-CNS amyloidogenic proteins on Aß aggregation pathways, we examined whether and how sonicated fibrils of casein, fibroin, sericin, actin, and islet amyloid polypeptide affected Aß40 and Aß42 aggregation pathways using the thioflavin T assay and electron microscopy. Interestingly, the fibrillar seeds of all amyloidogenic proteins functioned as seeds. The cross-seeding effect of actin was stronger but that of fibroin was weaker than that of other proteins. Furthermore, our nuclear magnetic resonance spectroscopic studies identified the binding sites of Aß with the amyloidogenic proteins. Our results indicate that the amyloidogenic proteins, including those contained in foods and cosmetics, contribute to Aß aggregation by binding to Aß, suggesting their possible roles in the propagation of Aß amyloidosis.
Assuntos
Peptídeos beta-Amiloides/química , Proteínas Amiloidogênicas/farmacologia , Amiloidose/etiologia , Benzotiazóis , Humanos , Espectroscopia de Ressonância Magnética , Microscopia Eletrônica , Tiazóis/metabolismoRESUMO
The slow hardening process of carbonate-activated slag limits its application as a construction material. This paper aims to provide an acceleration method for the early age hydration of carbonate-activated slag by applying calcium silicate hydrate (C-S-H) seeds and unveil the underlying mechanism. The results show that the incorporation of C-S-H seeds significantly accelerates the early age reaction of carbonate-activated slag and shortens the setting time. With 4% of calcium silicate hydrate (C-S-H) seeds, the 1d-compressive strength of carbonate activates slag can achieve 25.4 MPa. The C-S-H seeds acts as the preferred nucleation sites for the strength-giving phase C-A-S-H gel and the carbonate-containing phases (e.g., calcite, gaylussite, hydrotalcite, etc.), and accelerates hydration. The dormant period of samples with C-S-H seeds becomes negligible, confirming that the seeding effect that controls the saturation limits of the pore solution is the major reason for the accelerated hydration.
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Amyloidogenesis, self-propagation of protein or peptide monomers to amyloid fibrils, has been linked to incurable pathogenesis of neurodegenerative diseases such as Alzheimer's disease and prion diseases. Investigations of amyloid structures and how monomers are transformed through seeding are therefore crucial for developing therapeutics toward these diseases. Here we describe a cross-seeding method to explore the amyloid core in prion fibrils that uses preformed amyloid fibrils as a seed to induce the transformation of other protein or peptide monomers to amyloid fibrils.
Assuntos
Amiloidose , Doenças Priônicas , Príons , Humanos , Amiloide/química , Príons/química , Proteínas AmiloidogênicasRESUMO
To assess the problem of sewage treatment under the condition of low carbon sources, we carried out a study of activated sludge and a biofilm symbiosis system (IFAS). The occurrence characteristics and interaction law of microorganisms in two phases of sludge membrane under low carbon source conditions were discussed, and their niche and influence on treatment efficiency were clarified. Through a pilot-scale experiment in actual water plants, the biofilm characteristics, sludge membrane activity, and succession law of flora were analyzed, and the microbial structure and interaction in sludge membrane in two phases under the control of different activated sludge ages were compared. The results showed that the sludge concentration in the reactor increased with the increase in SRT under variable SRT. Because the microbial concentration in SRT-H was much higher than that in SRT-L, the competition between mud films in SRT-H was more intense than that in SRT-L, and the pollutant removal efficiency in SRT-H was lower than that in SRT-L. Under the condition of low-carbon feed water, the sludge activity in the IFAS process decreased with the increase in SRT. Under the condition of low SRT(5 d), the nitrification, denitrification, phosphorus accumulation, and phosphorus absorption rate of activated sludge increased by 122%, 88%, 34%, and 44%, respectively, compared with that of high SRT (25 d). However, SRT had little effect on biofilm activity, and there was little difference in nitrification activity and denitrification activity between the two SRTs. Microbial sequencing analysis showed that the functional bacteria of the IFAS process were enriched and transferred with the change in SRT between the two phases of mud membrane. In SRT-L, the functional bacteria that were enriched and transferred between the two phases of mud film owing to the "seeding" effect were mainly unclassified_g__Enterobacteriaceae, whereas in SRT-H, Acinetobacter was mainly used. At the same time, by analyzing the distribution of dominant functional bacteria, it was found that there was some competition between denitrifying bacteria and phosphorus-accumulating bacteria in activated sludge. Under the condition of a lack of organic substrate in the influent, the relative abundance of denitrifying bacteria was obviously higher than that of phosphorus-accumulating bacteria, which indicated that denitrifying bacteria could better adapt to low-carbon source conditions. Thus, they could occupy a dominant competition position, which was mainly reflected in the increase in the relative abundance of aerobic denitrifying bacteria. In addition, the SRT change in the mud phase reacted in the membrane phase, making the residence time of biofilm change correspondingly, thus changing the flora structure, screening out different dominant bacteria genera, and further increasing the difference.
Assuntos
Reatores Biológicos , Esgotos , Bactérias , Reatores Biológicos/microbiologia , Carbono , Interações Microbianas , Fósforo , Esgotos/microbiologia , ÁguaRESUMO
We investigated the interactions of air and snow over one entire winter accumulation period as well as the importance of chemical markers in a pristine free-tropospheric environment to explain variation in a microbiological dataset. To overcome the limitations of short term bioaerosol sampling, we sampled the atmosphere continuously onto quartzfiber air filters using a DIGITEL high volume PM10 sampler. The bacterial and fungal communities, sequenced using Illumina MiSeq, as well as the chemical components of the atmosphere were compared to those of a late season snow profile. Results reveal strong dynamics in the composition of bacterial and fungal communities in air and snow. In fall the two compartments were similar, suggesting a strong interaction between them. The overlap diminished as the season progressed due to an evolution within the snowpack throughout winter and spring. Certain bacterial and fungal genera were only detected in air samples, which implies that a distinct air microbiome might exist. These organisms are likely not incorporated in clouds and thus not precipitated or scavenged in snow. Although snow appears to be seeded by the atmosphere, both air and snow showed differing bacterial and fungal communities and chemical composition. Season and alpha diversity were major drivers for microbial variability in snow and air, and only a few chemical markers were identified as important in explaining microbial diversity. Air microbial community variation was more related to chemical markers than snow microbial composition. For air microbial communities Cl-, TC/OC, SO4 2-, Mg2+, and Fe/Al, all compounds related to dust or anthropogenic activities, were identified as related to bacterial variability while dust related Ca2+ was significant in snow. The only common driver for snow and air was SO4 2-, a tracer for anthropogenic sources. The occurrence of chemical compounds was coupled with boundary layer injections in the free troposphere (FT). Boundary layer injections also caused the observed variations in community composition and chemistry between the two compartments. Long-term monitoring is required for a more valid insight in post-depositional selection in snow.
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Monolayers of transition metal dichalcogenides (TMDs) are attractive for various modern semiconductor devices. However, the limited control over the location, yield, and size distribution of the products using current synthesis methods has severely limited their large-scale applicability. Herein, we identify the ability to use metal ( e. g., Au) nanoparticles to seed the growth of MoS2 monolayers and thereby provide a means to achieve programmable and controllable synthesis. In this study, prepatterned Au seeds are used as heterogeneous nucleation sites to induce the formation of desired geometries of MoS2 monolayers via chemical vapor deposition. Our experimental and theoretical results shed light on the growth mechanism driving the formation of MoS2 monolayers at these sites, revealing that the seeding effect originates from the favorable formation energy of MoS2 on the Au surface. A field-effect transistor with a predesigned channel geometry exhibits electronic performance that compares nicely with previously reported MoS2 monolayer devices. We believe this study contributes fundamental insights into controlled synthesis of TMD monolayers, making integration of these materials into emerging electronic devices more attainable.