ABSTRACT
The iron(III) salen complex (R,R)-N,N'-bis(salicylidene)-1,2-cyclohexanediamineiron(III) chloride has been developed as a catalyst for the acceptorless dehydrogenation of alcohols. The complex catalyzes the direct synthesis of imines in good yields from different primary alcohols and amines with the liberation of hydrogen gas. The mechanism has been investigated experimentally with labelled substrates and theoretically with density functional theory calculations. In contrast to the corresponding manganese(III) salen-catalyzed dehydrogenation, it has not been possible to identify a homogeneous catalytic pathway with the iron complex. Instead, poisoning experiments with trimethylphosphine and mercury indicated that the catalytically active species are heterogeneous small iron particles.
ABSTRACT
Plasmonic hot electrons have shown great potential in photocatalysis, but little is known about the hot hole-driven chemical reactions due to the lack of desired plasmonic metal/p-type semiconductor architectures. Herein, we describe a general and robust strategy for the site-selective growth of a p-type semiconductor, Cu2O on Au nanocrystals (NCs), to produce diverse spatially separated Au/Cu2O heterostructures. The preferential growth of Cu2O on the tips/ends/edges of Au NCs is directed by the sparse coverage of the surfactant molecules at the high-curvature sites of Au NCs. The obtained dumbbell-shaped nanostructures serve as the ideal platforms for probing the hot-hole-mediated CO2 reduction reaction. Benefiting from the hot-hole injection, a new reaction pathway is unlocked, and the C2 product activity and selectivity are significantly improved. This study demonstrates the genuine superiority of the dumbbell-shaped nanostructures in photocatalysis, offering a new unique avenue to explore the underlying mechanism of hot-hole-mediated chemical reactions.
ABSTRACT
Personal protective behaviors and their dynamic change are known to play a major role in the community spread of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), the causal pathogen of the coronavirus disease 2019 (COVID-19) pandemic. In this study, a total of 3229 students in Chinese universities completed an online survey about their knowledge on transmission and personal protective behavior before and after COVID-19 vaccination. Of the respondents, 87.6% had been vaccinated. Most students believed that the large droplet (97.0%) and short-range airborne (89.3%) routes were the two most likely SARS-CoV-2 transmission routes, whereas only 24.1% considered long-range airborne transmission to be possible. Students who would be expected to possess better knowledge about virus transmission (e.g., students of medicine) reported better personal protective behaviors. Female students reported relatively better personal hygiene practices than male students, so did the confident students than their diffident peers. Students washed their hands on average of 5.76 times per day during the pandemic. Students at universities in southern regions washed their hands more frequently but paid less attention to indoor ventilation than did their northern counterparts. Interestingly, students who are fear of being infected had the bad personal hygiene. University students wore 22% less masks in public indoor environments after vaccination. Chinese university students weakened their personal protective behavior after vaccination and it may increase the potential risk of infection in the new waves of variant virus (e.g. delta).
ABSTRACT
To determine the effects of Ti and mixing entropy (ΔSmix) on the structure and mechanical proper-ties of Zr-Ta alloys and then find a new potential energetic structural material with good me-chanical properties and more reactive elements, TixZr2.5-xTa (x = 0, 0.5, 1.0, 1.5, 2.0) alloys were investigated. The XRD experimental results showed that the phase transformation of TixZr2.5-xTa nonequal-ratio ternary alloys depended not on the value of ΔSmix, but on the amount of Ti atoms. With the addition of Ti, the content of the HCP phase decreased gradually. SEM analyses revealed that dendrite morphology and component segregation increasingly developed and then weakened gradually. When x increases to 2.0, TixZr2.5-xTa with the best mechanical properties can be ob-tained. The yield strength, compressive strength and fracture strain of Ti2.0Zr0.5Ta reached 883 MPa, 1568 MPa and 34.58%, respectively. The dependence of the phase transformation and me-chanical properties confirms that improving the properties of Zr-Ta alloys by doping Ti is feasible.
ABSTRACT
Acquiring spatial control of nanoscopic metal clusters is central to their function as efficient multi-electron catalysts. However, dispersing metal clusters on surfaces or in porous hosts is accompanied by an intrinsic heterogeneity that hampers detailed understanding of the chemical structure and its relation to reactivities. Tethering pre-assembled molecular metal clusters into polymeric, crystalline 2D or 3D networks constitutes an unproven approach to realizing ordered arrays of chemically well-defined metal clusters. Herein, we report the facile synthesis of a {Pd3} cluster-based organometallic framework from a molecular triangulo-Pd3(CNXyl)6 (Xyl = xylyl; Pd3) cluster under chemically mild conditions. The formally zero-valent Pd3 cluster readily engages in a complete ligand exchange when exposed to a similar, ditopic isocyanide ligand, resulting in polymerization into a 2D coordination network (Pd3-MOF). The structure of Pd3-MOF could be unambiguously determined by continuous rotation 3D electron diffraction (3D-ED) experiments to a resolution of ~1.0 Å (>99% completeness), showcasing the applicability of 3D-ED to nanocrystalline, organometallic polymers. Pd3-MOF displays Pd03 cluster nodes, which possess significant thermal and aerobic stability, and activity towards hydrogenation catalysis. Importantly, the realization of Pd3-MOF paves the way for the exploitation of metal clusters as building blocks for rigidly interlocked metal nanoparticles at the molecular limit.
ABSTRACT
The corticospinal tract (CST) is the principal neural pathway responsible for conducting voluntary movement in the vertebrate nervous system. Netrin-1 is a well-known guidance molecule for midline crossing of commissural axons during embryonic development. Families with inherited Netrin-1 mutations display congenital mirror movements (CMM), which are associated with malformations of pyramidal decussation in most cases. Here, we investigated the role of Netrin-1 in CST formation by generating conditional knockout (CKO) mice using a Gfap-driven Cre line. A large proportion of CST axons spread laterally in the ventral medulla oblongata, failed to decussate and descended in the ipsilateral spinal white matter of Ntn1Gfap CKO mice. Netrin-1 mRNA was expressed in the ventral ventricular zone (VZ) and midline, while Netrin-1 protein was transported by radial glial cells to the ventral medulla, through which CST axons pass. The level of transported Netrin-1 protein was significantly reduced in Ntn1Gfap CKO mice. In addition, Ntn1Gfap CKO mice displayed increased symmetric movements. Our findings indicate that VZ-derived Netrin-1 deletion leads to an abnormal trajectory of the CST in the spinal cord due to the failure of CST midline crossing and provides novel evidence supporting the idea that the Netrin-1 signalling pathway is involved in the pathogenesis of CMM.
Subject(s)
Netrin-1 , Pyramidal Tracts , Animals , Mice , Axons/metabolism , Axons/pathology , Mice, Knockout , Netrin-1/metabolism , Netrin-1/genetics , Pyramidal Tracts/metabolism , Pyramidal Tracts/pathology , Movement/physiologyABSTRACT
Probiotic supplementation has become a prominent method of decreasing ammonia emissions in poultry production. The present study was conducted to investigate the influence of Lactobacillus plantarum on ammonia emission, immune responses, antioxidant capacity, cecal microflora and short chain fatty acids, and serum metabolites in broilers challenged with ammonia. A total of 360 1-day-old yellow-feathered broilers were randomly divided into three treatment groups: birds fed with a basal diet (CON), a basal diet supplemented with ammonia (AN), and a basal diet supplemented with 2.5 × 108 CFU L. plantarum kg-1 and challenged with ammonia (LP). Data showed that L. plantarum supplementation decreased ammonia more than 30% from day 48, and significantly reduced the levels of serum urea nitrogen and ammonia, fecal urease, and ammonium nitrogen compared with those on CON. Compared with AN and CON treatments, LP administration increased (p < 0.05) the concentration of serum immunoglobulin Y (IgY), IgM, and IL-10, as well as the serum total-antioxidant capacity (T-AOC) and GSH-Px, and decreased (p < 0.05) IL-1ß, IL-6, and TNF-α. Furthermore, birds supplemented with LP had higher (p < 0.05) cecal contents of short chain fatty acids (SCFAs) than AN birds and had more butyrate than CON birds. Data from 16s high throughput sequencing showed that LP supplementation significantly increased (p < 0.05) the Shannon and Simpson indices of bird cecal microflora, and Alloprevotella dominated the LP birds. The function prediction of cecal microflora indicated that LP treatment significantly increased alanine aspartate and glutamate metabolism, starch and sucrose metabolism, exosome, mismatch repair, homologous recombination, DNA repair and recombination proteins, and amino acid-related enzymes. The serum metabolome showed that LP supplementation significantly changed the aminoacyl-tRNA, pantothenate and acetyl-coenzyme A, arginine, phenylalanine, tyrosine and tryptophan, valine, leucine, and isoleucine biosynthesis; purine, beta-alanine, galactose, histidine, alanine, aspartate and glutamate, glyoxylate and dicarboxylate, pyruvate and thiamine metabolism, melanogenesis, and citrate cycle.
ABSTRACT
Classrooms are high-risk indoor environments, so analysis of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) transmission in classrooms is important for determining optimal interventions. Due to the absence of human behavior data, it is challenging to accurately determine virus exposure in classrooms. A wearable device for close contact behavior detection was developed, and we recorded >250,000 data points of close contact behaviors of students from grades 1 to 12. Combined with a survey on students' behaviors, we analyzed virus transmission in classrooms. Close contact rates for students were 37 ± 11% during classes and 48 ± 13% during breaks. Students in lower grades had higher close contact rates and virus transmission potential. The long-range airborne transmission route is dominant, accounting for 90 ± 3.6% and 75 ± 7.7% with and without mask wearing, respectively. During breaks, the short-range airborne route became more important, contributing 48 ± 3.1% in grades 1 to 9 (without wearing masks). Ventilation alone cannot always meet the demands of COVID-19 control; 30 m3/h/person is suggested as the threshold outdoor air ventilation rate in a classroom. This study provides scientific support for COVID-19 prevention and control in classrooms, and our proposed human behavior detection and analysis methods offer a powerful tool to understand virus transmission characteristics and can be employed in various indoor environments.
ABSTRACT
Medium-high temperature Daqu is a characteristic starter for Chinese strong-flavor Baijiu fermentation, and its final quality determines the character and type of Baijiu. Nonetheless, its formation is affected by the interaction of physical and chemical, environmental and microbial interaction, and the differences in seasonal fermentation performance emerge. Here, the differences in the two seasons' Daqu fermentation properties were revealed by the detection of the enzyme activity. The respective dominant enzyme in summer Daqu (SUD) was protease and amylase, while cellulase and glucoamylase in spring Daqu (SPD). The underlying causes of this phenomenon were then investigated through an evaluation of nonbiological variables and microbial community structure. A greater absolute number of microorganisms, particularly Thermoactinomyces, were created in the SPD as a result of the superior growth environment (higher water activity). Additionally, the correlation network and discriminant analysis hypothesized that the volatile organic compound (VOC) guaiacol, which had a different content between SUD and SPD, may be a contributing element to the microbial composition. In contrast to SUD, the enzyme system activity related to guaiacol production in SPD was significantly higher. To support this notion that the volatile flavor chemicals mediate microbial interactions in Daqu, the growth effect of guaiacol on several bacteria isolated from the Daqu was examined in both a contact and non-contact manner. This study emphasized that VOCs not only have the basic characteristics of flavor compounds but also have ecological significance. Because the strains' varied structures and enzyme activities affected how the microorganisms interacted, the VOCs produced in this way ultimately had a synergistic effect on the various effects of Daqu fermentation.
Subject(s)
Alcoholic Beverages , Bacteria , Fermentation , Alcoholic Beverages/analysis , Seasons , AmylasesABSTRACT
Close contact routes, including short-range airborne and large-droplet routes, play an important role in the transmission of SARS-CoV-2 in indoor environments. However, the exposure risk of such routes is difficult to quantify due to the lack of data on the close contact behavior of individuals. In this study, a digital wearable device, based on semi-supervised learning, was developed to automatically record human close contact behavior. We collected 337,056 s of indoor close contact of school and university students from 194.5 h of depth video recordings in 10 types of indoor environments. The correlation between aerosol exposure and close contact behaviors was then evaluated. Individuals in restaurants had the highest close contact ratio (64%), as well as the highest probability of face-to-face pattern (78%) during close contact. Accordingly, university students showed greater exposure potential in dormitories than school students in homes, however, a lower exposure was observed in classrooms and postgraduate student offices in comparison with school students in classrooms. In addition, restaurants had the highest aerosol exposure volume for both short-range inhalation and direct deposition on the facial mucosa. Thus, the classroom was established as the primary indoor environment where school students are exposed to aerosols.
Subject(s)
COVID-19 , SARS-CoV-2 , Humans , Universities , Respiratory Aerosols and Droplets , StudentsABSTRACT
During COVID-19 pandemic, analysis on virus exposure and intervention efficiency in public transports based on real passenger's close contact behaviors is critical to curb infectious disease transmission. A monitoring device was developed to gather a total of 145,821 close contact data in subways based on semi-supervision learning. A virus transmission model considering both short- and long-range inhalation and deposition was established to calculate the virus exposure. During rush-hour, short-range inhalation exposure is 3.2 times higher than deposition exposure and 7.5 times higher than long-range inhalation exposure of all passengers in the subway. The close contact rate was 56.1 % and the average interpersonal distance was 0.8 m. Face-to-back was the main pattern during close contact. Comparing with random distribution, if all passengers stand facing in the same direction, personal virus exposure through inhalation (deposition) can be reduced by 74.1 % (98.5 %). If the talk rate was decreased from 20 % to 5 %, the inhalation (deposition) exposure can be reduced by 69.3 % (73.8 %). In addition, we found that virus exposure could be reduced by 82.0 % if all passengers wear surgical masks. This study provides scientific support for COVID-19 prevention and control in subways based on real human close contact behaviors.
Subject(s)
COVID-19 , Railroads , COVID-19/epidemiology , COVID-19/prevention & control , Humans , Masks , Pandemics/prevention & controlABSTRACT
Personal protective behaviors of healthcare workers (HCWs) and dynamic changes in them are known to play a major role in the hospital transmission of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). In this study, 1,499 HCWs in Chinese hospitals completed an online survey about their knowledge on SARS-CoV-2 transmission and their personal protective behaviors before and after coronavirus disease 2019 (COVID-19) vaccination. Of all the respondents, 89% were vaccinated at the time of the survey and 96% believed that the vaccine was effective or highly effective. Further, 88% of the vaccinated HCWs expressed that they would get revaccinated if the vaccination failed. Compared with HCWs with a lower education level, those with a higher education level had less fear of being infected with SARS-CoV-2 and reported a lower negative impact of the pandemic on how they treated patients. Physicians and nurses were willing to believe that short-range airborne and long-range fomite are possible transmission routes. HCWs with a higher education level had a better knowledge of COVID-19 but worse personal protective behaviors. The fact that HCWs with a longer work experience had worse personal protective behaviors showed that HCWs gradually relax their personal protective behaviors over time. Moreover, vaccination reduced the negative effects of the COVID-19 pandemic on how the HCWs treated patients. Importantly, the survey revealed that after vaccination, HCWs in China did not relax their personal protective behaviors, and it may bring a low potential risk for following waves of variant virus (e.g., delta).
Subject(s)
COVID-19 , COVID-19 Vaccines , Health Personnel , Humans , Pandemics , SARS-CoV-2 , VaccinationABSTRACT
The crude mortality rate in critical pneumonia cases with coronavirus disease 2019 (COVID-19) reaches 49%. This study aimed to test whether levels of blood urea nitrogen (BUN) in combination with D-dimer were predictors of in-hospital mortality in COVID-19 patients. The clinical characteristics of 305 COVID-19 patients were analysed and were compared between the survivor and non-survivor groups. Of the 305 patients, 85 (27.9%) died and 220 (72.1%) were discharged from hospital. Compared with discharged cases, non-survivor cases were older and their BUN and D-dimer levels were significantly higher (P < 0.0001). Least absolute shrinkage and selection operator (LASSO) and multivariable Cox regression analyses identified BUN and D-dimer levels as independent risk factors for poor prognosis. Kaplan-Meier analysis showed that elevated levels of BUN and D-dimer were associated with increased mortality (log-rank, P < 0.0001). The area under the curve for BUN combined with D-dimer was 0.94 (95% CI 0.90-0.97), with a sensitivity of 85% and specificity of 91%. Based on BUN and D-dimer levels on admission, a nomogram model was developed that showed good discrimination, with a concordance index of 0.94. Together, initial BUN and D-dimer levels were associated with mortality in COVID-19 patients. The combination of BUN ≥ 4.6 mmol/L and D-dimer ≥ 0.845 µg/mL appears to identify patients at high risk of in-hospital mortality, therefore it may prove to be a powerful risk assessment tool for severe COVID-19 patients.