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RESEARCH HIGHLIGHTS: Urate tophi were found in the kidneys, liver, spleen and lungs.IFA confirmed the co-expression of GoAstV-I and II antigens in the same kidney.
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Infecciones por Astroviridae , Astroviridae , Avastrovirus , Coinfección , Gota , Enfermedades de las Aves de Corral , Animales , Gansos , Infecciones por Astroviridae/veterinaria , Coinfección/veterinaria , Astroviridae/genética , Gota/veterinaria , Avastrovirus/genética , ChinaRESUMEN
Boron-based nonmetallic materials (such as B2O3 and BN) emerge as promising catalysts for selective oxidation of light alkanes by O2 to form value-added products, resulting from their unique advantage in suppressing CO2 formation. However, the site requirements and reaction mechanism of these boron-based catalysts are still in vigorous debate, especially for methane (the most stable and abundant alkane). Here, we show that hexagonal BN (h-BN) exhibits high selectivities to formaldehyde and CO in catalyzing aerobic oxidation of methane, similar to Al2O3-supported B2O3 catalysts, while h-BN requires an extra induction period to reach a steady state. According to various structural characterizations, we find that active boron oxide species are gradually formed in situ on the surface of h-BN, which accounts for the observed induction period. Unexpectedly, kinetic studies on the effects of void space, catalyst loading, and methane conversion all indicate that h-BN merely acts as a radical generator to induce gas-phase radical reactions of methane oxidation, in contrast to the predominant surface reactions on B2O3/Al2O3 catalysts. Consequently, a revised kinetic model is developed to accurately describe the gas-phase radical feature of methane oxidation over h-BN. With the aid of in situ synchrotron vacuum ultraviolet photoionization mass spectroscopy, the methyl radical (CH3â¢) is further verified as the primary reactive species that triggers the gas-phase methane oxidation network. Theoretical calculations elucidate that the moderate H-abstraction ability of predominant CH3⢠and CH3OO⢠radicals renders an easier control of the methane oxidation selectivity compared to other oxygen-containing radicals generally proposed for such processes, bringing deeper understanding of the excellent anti-overoxidation ability of boron-based catalysts.
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Whole-genome duplication (WGD) occurs broadly and repeatedly across the history of eukaryotes and is recognized as a prominent evolutionary force, especially in plants. Immediately following WGD, most genes are present in two copies as paralogs. Due to this redundancy, one copy of a paralog pair commonly undergoes pseudogenization and is eventually lost. When speciation occurs shortly after WGD; however, differential loss of paralogs may lead to spurious phylogenetic inference resulting from the inclusion of pseudoorthologs-paralogous genes mistakenly identified as orthologs because they are present in single copies within each sampled species. The influence and impact of including pseudoorthologs versus true orthologs as a result of gene extinction (or incomplete laboratory sampling) are only recently gaining empirical attention in the phylogenomics community. Moreover, few studies have yet to investigate this phenomenon in an explicit coalescent framework. Here, using mathematical models, numerous simulated data sets, and two newly assembled empirical data sets, we assess the effect of pseudoorthologs on species tree estimation under varying degrees of incomplete lineage sorting (ILS) and differential gene loss scenarios following WGD. When gene loss occurs along the terminal branches of the species tree, alignment-based (BPP) and gene-tree-based (ASTRAL, MP-EST, and STAR) coalescent methods are adversely affected as the degree of ILS increases. This can be greatly improved by sampling a sufficiently large number of genes. Under the same circumstances, however, concatenation methods consistently estimate incorrect species trees as the number of genes increases. Additionally, pseudoorthologs can greatly mislead species tree inference when gene loss occurs along the internal branches of the species tree. Here, both coalescent and concatenation methods yield inconsistent results. These results underscore the importance of understanding the influence of pseudoorthologs in the phylogenomics era. [Coalescent method; concatenation method; incomplete lineage sorting; pseudoorthologs; single-copy gene; whole-genome duplication.].
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Duplicación de Gen , Especiación Genética , Evolución Biológica , Simulación por Computador , Modelos Genéticos , FilogeniaRESUMEN
Constructed wetlands (CWs) added with biochar were built to study pollutant removal efficiencies, nitrous oxide (N2O) emission characteristics, and biological mechanisms in nitrogen transformation. The results showed that biochar addition enhanced the average removal rates of ammonium (NH4+-N), total nitrogen, and chemical oxygen demand by 4.03-18.5%, 2.90-4.99%, and 2.87-5.20% respectively while reducing N2O emissions by 25.85-83.41%. Based on 15N stable isotope tracing, it was found that nitrification, denitrification, and simultaneous nitrification and denitrification were the main processes contributing to N2O emission. The addition of biochar resulted in maximum reduction rates of 71.50%, 80.66%, and 73.09% for these three processes, respectively. The relative abundance of nitrogen-transforming microbes, such as Nitrospira, Dechloromonas, and Denitratisoma, increased after the addition of biochar, promoting nitrogen removal and reducing N2O emissions. Adding biochar could increase the functional gene copy number and enzyme activity responsible for nitrogen conversion, which helped achieve efficient NH4+-N oxidation and eliminate nitrite accumulation, thereby reducing N2O emissions.
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Desnitrificación , Humedales , Carbón Orgánico/metabolismo , Nitrógeno , Óxido Nitroso/metabolismoRESUMEN
Ceria (CeO2 ) supports are unique in their ability to trap ionic platinum (Pt), providing exceptional stability for isolated single atoms of Pt. The reactivity and stability of single-atom Pt species was explored for the industrially important light alkane dehydrogenation reaction. The single-atom Pt/CeO2 catalysts are stable during propane dehydrogenation, but are not selective for propylene. DFT calculations show strong adsorption of the olefin produced, leading to further unwanted reactions. In contrast, when tin (Sn) is added to CeO2 , the single-atom Pt catalyst undergoes an activation phase where it transforms into Pt-Sn clusters under reaction conditions. Formation of small Pt-Sn clusters allows the catalyst to achieve high selectivity towards propylene because of facile desorption of the product. The CeO2 -supported Pt-Sn clusters are very stable, even during extended reaction at 680 °C. Coke formation is almost completely suppressed by adding water vapor to the feed. Furthermore, upon oxidation the Pt-Sn clusters readily revert to the atomically dispersed species on CeO2 , making Pt-Sn/CeO2 a fully regenerable catalyst.
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Conversion of biomass-derived molecules involves catalytic reactions under harsh conditions in the liquid phase (e.g., temperatures of 250 °C and possibly under either acidic or basic conditions). Conventional oxide-supported catalysts undergo pore structure collapse and surface area reduction leading to deactivation under these conditions. Here we demonstrate an approach to deposit graphitic carbon to protect the oxide surface. The heterogeneous catalysts supported on the graphitic carbon/oxide composite exhibit excellent stability (even under acidic conditions) for biomass conversion reactions.
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Biomasa , Grafito/química , Óxidos/química , Carbono/química , Catálisis , Hidrogenación , Modelos Moleculares , Porosidad , Propiedades de Superficie , TemperaturaRESUMEN
Conversion of CO2 into high-value chemicals using solar energy is one of promising approaches to achieve carbon neutrality. However, the oxidation of water in the photocatalytic CO2 reduction is kinetically unfavorable due to multi-electron and proton transfer processes, along with the difficulty in generating O-O bonds. To tackle these challenges, this study investigated the coupling reaction of photocatalytic CO2 reduction and selective propane oxidation using the Pd/P25 (1â wt%) catalyst. Our findings reveal a significant improvement in CO2 reduction, nearly fivefold higher, achieved by substituting water oxidation with selective propane oxidation. This substitution not only accelerates the process of CO2 reduction but also yields valuable propylene. The relative ease of propane oxidation, compared to water, appears to increase the density of photogenerated electrons, ultimately enhancing the efficiency of CO2 reduction. We further found that hydroxyl radicals and reduced intermediate (carboxylate species) played important roles in the photocatalytic reaction. These findings not only propose a potential approach for the efficient utilization of CO2 through the coupling of selective propane oxidation into propylene, but also provide insights into the mechanistic understanding of the coupling reaction.
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Transition metal oxides are promising catalysts for catalytic oxidation reactions but are hampered by low room-temperature activities. Such low activities are normally caused by sparse reactive sites and insufficient capacity for molecular oxygen (O2) activation. Here, we present a dual-stimulation strategy to tackle these two issues. Specifically, we import highly dispersed nickel (Ni) atoms onto MnO2 to enrich its oxygen vacancies (reactive sites). Then, we use molecular ozone (O3) with a lower activation energy as an oxidant instead of molecular O2. With such dual stimulations, the constructed O3-Ni/MnO2 catalytic system shows boosted room-temperature activity for toluene oxidation with a toluene conversion of up to 98%, compared with the O3-MnO2 (Ni-free) system with only 50% conversion and the inactive O2-Ni/MnO2 (O3-free) system. This leap realizes efficient room-temperature catalytic oxidation of transition metal oxides, which is constantly pursued but has always been difficult to truly achieve.
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Identification of active sites in catalytic materials is important and helps establish approaches to the precise design of catalysts for achieving high reactivity. Generally, active sites of conventional heterogeneous catalysts can be single atom, nanoparticle or a metal/oxide interface. Herein, we report that metal/oxide reverse interfaces can also be active sites which are created from the coordinated migration of metal and oxide atoms. As an example, a Pd1/CeO2 single-atom catalyst prepared via atom trapping, which is otherwise inactive at 30 °C, is able to completely oxidize formaldehyde after steam treatment. The enhanced reactivity is due to the formation of a Ce2O3-Pd nanoparticle domain interface, which is generated by the migration of both Ce and Pd atoms on the atom-trapped Pd1/CeO2 catalyst during steam treatment. We show that the generation of metal oxide-metal interfaces can be achieved in other heterogeneous catalysts due to the coordinated mobility of metal and oxide atoms, demonstrating the formation of a new active interface when using metal single-atom material as catalyst precursor.
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Pulmonary collectins have been reported to bind carbohydrates on pathogens and inhibit infection by agglutination, neutralization, and opsonization. In this study, surfactant protein A (SP-A) was identified from goose lung and characterized at expression- and agglutination-functional levels. The deduced amino acid sequence of goose surfactant protein A (gSP-A) has two characteristic structures: a shorter, collagen-like region and a carbohydrate recognition domain. The latter contains two conserved motifs in its Ca2+-binding site: EPN (Glu-Pro-Asn) and WND (Trp-Asn-Asp). Expression analysis using qRT-PCR and fluorescence IHC revealed that gSP-A was highly expressed in the air sac and present in several other tissues, including the lung and trachea. We went on to produce recombinant gSP-A (RgSP-A) using a baculovirus/insect cell system and purified using a Ni2+ affinity column. A biological activity assay showed that all bacterial strains tested in this study were aggregated by RgSP-A, but only Escherichia coli AE17 (E. coli AE17, O2) and E. coli AE158 (O78) were susceptible to RgSP-A-mediated growth inhibition at 2-6 h. Moreover, the swarming motility of the two bacterial strains were weakened with increasing RgSP-A concentration, and their membrane permeability was compromised at 3 h, as determined by flow cytometry and laser confocal microscopy. Therefore, RgSP-A is capable of reducing bacterial viability of E. coli O2 and O78 via an aggregation-dependent mechanism which involves decreasing motility and increasing the bacterial membrane permeability. These data will facilitate detailed studies into the role of gSP-A in innate immune defense as well as for development of antibacterial agents.
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Infecciones por Escherichia coli , Escherichia coli , Gansos , Inmunidad Innata , Proteína A Asociada a Surfactante Pulmonar , Animales , Escherichia coli/crecimiento & desarrollo , Escherichia coli/inmunología , Gansos/inmunología , Gansos/microbiología , Proteína A Asociada a Surfactante Pulmonar/genética , Proteína A Asociada a Surfactante Pulmonar/metabolismo , Pulmón/metabolismo , Proteínas Recombinantes/genética , Proteínas Recombinantes/metabolismo , Infecciones por Escherichia coli/inmunología , Infecciones por Escherichia coli/microbiología , Infecciones por Escherichia coli/veterinariaRESUMEN
Methane (CH4 ) is an attractive energy source and important greenhouse gas. Therefore, from the economic and environmental point of view, scientists are working hard to activate and convert CH4 into various products or less harmful gas at low-temperature. Although the inert nature of CH bonds requires high dissociation energy at high temperatures, the efforts of researchers have demonstrated the feasibility of catalysts to activate CH4 at low temperatures. In this review, the efficient catalysts designed to reduce the CH4 oxidation temperature and improve conversion efficiencies are described. First, noble metals and transition metal-based catalysts are summarized for activating CH4 in temperatures ranging from 50 to 500 °C. After that, the partial oxidation of CH4 at relatively low temperatures, including thermocatalysis in the liquid phase, photocatalysis, electrocatalysis, and nonthermal plasma technologies, is briefly discussed. Finally, the challenges and perspectives are presented to provide a systematic guideline for designing and synthesizing the highly efficient catalysts in the complete/partial oxidation of CH4 at low temperatures.
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The direct oxidation of methane to methanol (MTM) remains a significant challenge in heterogeneous catalysis due to the high dissociation energy of the C-H bond in methane and the high desorption energy of methanol. In this work, we demonstrate a breakthrough in selective MTM by achieving a high methanol space-time yield of 2678 mmol molCu-1 h-1 with 93% selectivity in a continuous methane-steam reaction at 400 °C. The superior performance is attributed to the confinement effect of 6-membered ring (6MR) voids in SSZ-13 zeolite, which host isolated Cu-OH single sites. Our results provide a deeper understanding of the role of Cu-zeolites in continuous methane-steam to methanol conversion and pave the way for further improvement.
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Single-atom catalysis is a research Frontier and has attracted extensive interests in catalysis. Significant progresses have been carried out in the synthesis and characterization of metal single-atom catalysts (SACs). However, the stability and catalytic reactivity of metal SAC at elevated temperatures are not well documented because single atoms sinter at elevated temperatures. Therefore, the development of stable and reactive SAC at high temperatures remains a formidable challenge. In this perspective, we summarize recent efforts on the preparation of the thermally-stable SACs synthesized at elevated temperature via the reverse-Ostwald ripening mechanism, including the approaches of atom trapping and vapor-phase self-assembly. The reducibility of lattice oxygen, the loading upper limit and the location of the metal single atom are discussed, combining experiments with simulations. In addition, we demonstrate that the coordination structure of the metal single atom can be tailored to address the relationship of structure and performances of the metal SAC in reactions. We expect that this perspective can provide some insights to guide the study for the rational design of thermally-stable and active single atom catalysts, which are especially suitable for high-temperature reactions.
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Antibiotic-metal complexes (AMCs) formed by antibiotics and metal ions have attracted considerable attentions in recent years. Although different removal methods for AMCs have been reported in the literature, very few investigations have focused on the mechanisms and toxic effects of antibiotic-metal coordination. This review briefly describes the structural characteristics of various commonly used antibiotics and the coordination mechanisms with metal ions. Considering the complexity of the real environment, various environmental factors affecting AMC formation are highlighted. The effects of AMCs on microbial community structure and the role of metal ions in influencing resistant genes from the molecular perspective are of interest within this work. The toxicities and mechanisms of AMCs on different species of biota are also discussed. These findings underline the need for more targeted detection and analysis methods and more suitable toxicity markers to verify the combination of antibiotics with metal ions and reveal environmental toxicities in future. This review presents an innovative idea that antibiotics combined with metal ions will change the toxicity and environmental behavior of antibiotics.
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Antibacterianos , Complejos de Coordinación , Antibacterianos/farmacología , Complejos de Coordinación/química , Iones , Metales/análisisRESUMEN
Volatile organic compounds (VOCs) are detrimental to the environment and human health and must be eliminated before discharging. Oxidation by heterogeneous catalysts is one of the most promising approaches for the VOCs abatement. Precious metal catalysts are highly active for the catalytic oxidation of VOCs, but they are rare and their high price limits large-scale application. Supported metal single-atom catalysts (SACs) have a high atom efficiency and provide the possibility to circumvent such limitations. This Review summarizes recent advances in the use of metal SACs for the complete oxidation of VOCs, such as benzene, toluene, formaldehyde, and methanol, as well as aliphatic and Cl- and S-containing hydrocarbons. The structures of the metal SACs used and the reaction mechanisms of the VOC oxidation are discussed. The most widely used SACs are noble metals supported on oxides, especially on reducible oxides, such as Mn2 O3 and TiO2 . The reactivity of most SACs is related to the activity of surface lattice oxygen of the oxides. Furthermore, several metal SACs show better reactivity and improved S and Cl resistance than the corresponding nanocatalysts, indicating that SACs have potential for application in the oxidation of VOCs. The deactivation and regeneration mechanisms of the metal SACs are also summarized. It is concluded that the application of metal SACs in catalytic oxidation of VOCs is still in its infancy. This Review aims to elucidate structure-performance relationships and to guide the design of highly efficient metal SACs for the catalytic oxidation of VOCs.
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Compuestos Orgánicos Volátiles , Catálisis , Humanos , Metales , Oxidación-Reducción , Óxidos/química , Compuestos Orgánicos Volátiles/químicaRESUMEN
The host innate defense-pathogen interaction in the lung has always been a topic of concern. The respiratory tract is a common entry route for Avian pathogenic Escherichia coli (APEC). Chicken surfactant protein A (cSP-A) and chicken lung lectin (cLL) can bind to the carbohydrate moieties of various microorganisms. Despite their detection in chickens, their role in the innate immune response is largely unknown. This study aimed to examine whether the expression levels of cSP-A and cLL in the chicken respiratory system were affected by APEC infection. A lung colonization model was established in vivo using 5-day-old specific-pathogen-free chickens infected intratracheally with APEC. The chickens were euthanized 12 h post-infection (hpi) and 1-3 days post-infection (dpi) to detect various indicators. The results of quantitative reverse transcription-polymerase chain reaction and fluorescence multiplex immunohistochemical staining showed that the mRNA and protein expression levels of cSP-A and cLL in the lung and trachea were significantly co-upregulated at 2dpi.Transcriptome RNA-sequencing analysis indicated that the inoculation with APEC AE17 at 2 dpi resulted in differential gene expression of approximately 810 genes compared with control birds, but only a few genes were expressed with astatistically significant â§2-fold difference. cLL and cSP-A were among the significantly upregulated genes involved in innate immunity. These findings indicated that cSP-A and cLL might play an important role in lung innate host defense against APEC infection at the early stage.
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Infecciones por Escherichia coli , Enfermedades de las Aves de Corral , Animales , Pollos , Escherichia coli/genética , Proteína A Asociada a Surfactante Pulmonar , Enfermedades de las Aves de Corral/patología , Lectinas , Infecciones por Escherichia coli/veterinaria , Infecciones por Escherichia coli/patología , Pulmón/patologíaRESUMEN
The thermocatalytic conversion of hexose into valuable chemicals such as methyl lactate under mild conditions is very appealing. Here, we report that Mo, Mg co-modified Sn-ß catalyst can effectively catalyze the transformation of glucose and fructose into alkyl lactate at moderate temperatures. A maximum yield of around 35% of methyl lactate was achieved from the conversion of glucose in methanol at 100°C over Sn-ß catalyst modified with 3 wt% Mo and 0.5 wt% Mg. However, up to 82.8% yield of ethyl lactate was obtained in the case of fructose in ethanol upon the same catalytic condition, suggesting a significant solvent effect. The Mo species plays a key role to enable the retro-aldol condensation of fructose, in which the competing side reactions are significantly suppressed with the assistance of neighboring Mg species probably through a synergetic effect of Lewis acid-base.
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Invited for this month's cover is the group of Haifeng Xiong at Xiamen University. The image shows that single-atom catalysts can work in the catalytic oxidation of volatile organic compounds. The Review itself is available at 10.1002/cssc.202102494.
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Selective conversion of specific functional groups to desired products is highly important but still challenging in industrial catalytic processes. The adsorption state of surface species is the key factor in modulating the conversion of functional groups, which is correspondingly determined by the uniformity of active sites. However, the non-identical number of metal atoms, geometric shape, and morphology of conventional nanometer-sized metal particles/clusters normally lead to the non-uniform active sites with diverse geometric configurations and local coordination environments, which causes the distinct adsorption states of surface species. Hence, it is highly desired to modulate the homogeneity of the active sites so that the catalytic transformations can be better confined to the desired direction. In this review, the construction strategies and characterization techniques of the uniform active sites that are atomically dispersed on various supports are examined. In particular, their unique behavior in boosting the catalytic performance in various chemical transformations is discussed, including selective hydrogenation, selective oxidation, Suzuki coupling, and other catalytic reactions. In addition, the dynamic evolution of the active sites under reaction conditions and the industrial utilization of the single-atom catalysts are highlighted. Finally, the current challenges and frontiers are identified, and the perspectives on this flourishing field is provided.
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The development of highly efficient catalysts for room-temperature formaldehyde (HCHO) oxidation is of great interest for indoor air purification. In this work, it was found that the single-atom Pt1/CeO2 catalyst exhibits a remarkable activity with complete removal of HCHO even at 288 K. Combining density functional theory calculations and in situ DRIFTS experiments, it was revealed that the active OlatticeH site generated on CeO2 in the vicinity of Pt2+ via steam treatment plays a key role in the oxidation of HCHO to formate and its further oxidation to CO2. Such involvement of hydroxyls is fundamentally different from that of cofeeding water which dissociates on metal oxide and catalyzes the acid-base-related chemistry. This study provides an important implication for the design and synthesis of supported Pt catalysts with atom efficiency for a very important practical application-room-temperature HCHO oxidation.