Although considerable progress has been made in carbon dioxide (CO) hydrogenation to various C chemicals, it is still a great challenge to synthesize value-added products with two or more carbons, such as gasoline, directly from CO because of the extreme inertness of CO and a high C-C coupling barrier. Here we present a bifunctional catalyst composed of reducible indium oxides (InO) and zeolites that yields a high selectivity to gasoline-range hydrocarbons (78.6%) with a very low methane selectivity (1%). The oxygen vacancies on the InO surfaces activate CO and hydrogen to form methanol, and C-C coupling subsequently occurs inside zeolite pores to produce gasoline-range hydrocarbons with a high octane number. The proximity of these two components plays a crucial role in suppressing the undesired reverse water gas shift reaction and giving a high selectivity for gasoline-range hydrocarbons. Moreover, the pellet catalyst exhibits a much better performance during an industry-relevant test, which suggests promising prospects for industrial applications.
Carbapenem-resistant (CRE) infection is highly endemic in China, but estimates of the infection burden are lacking. We established the incidence of CRE infection from a multicenter study that covered 25 tertiary hospitals in 14 provinces. CRE cases defined as carbapenem-nonsusceptible, ,, or infections during January to December 2015 were collected and reviewed from medical records. Antimicrobial susceptibility testing and carbapenemase gene identification were performed. Among 664 CRE cases, most were caused by (73.9%), followed by (16.6%) and (7.1%). The overall CRE infection incidence per 10,000 discharges was 4.0 and differed significantly by region, with the highest in Jiangsu (14.97) and the lowest in Qinghai (0.34). Underlying comorbidities were found in 83.8% of patients; the median patient age was 62 years (range, 45 to 74 years), and 450 (67.8%) patients were male. Lower respiratory tract infections (65.4%) were the most common, followed by urinary tract infection (16.6%), intra-abdominal infection (7.7%), and bacteremia (7.7%). The overall hospital mortality rate was 33.5%. All isolates showed nonsusceptibility to carbapenems and cephalosporins. The susceptibility rate of polymyxin B was >90%. Tigecycline demonstrated a higher susceptibility rate against than against (90.9% versus 40.2%). Of 155 clinical isolates analyzed, 89% produced carbapenemases, with a majority of isolates producing KPC (50%) or NDM (33.5%)-type beta-lactamases among and The incidence of CRE infection in China was 4.0 per 10,000 discharges. The patient-based disease burden in tertiary hospitals in China is severe, suggesting an urgent need to enhance infection control.
Nitrogen fixation in a simulated natural environment (i.e., near ambient pressure, room temperature, pure water, and incident light) would provide a desirable approach to future nitrogen conversion. As the NN triple bond has a thermodynamically high cleavage energy, nitrogen reduction under such mild conditions typically undergoes associative alternating or distal pathways rather than following a dissociative mechanism. Here, we report that surface plasmon can supply sufficient energy to activate N 2 through a dissociative mechanism in the presence of water and incident light, as evidenced by in situ synchrotron radiationbased infrared spectroscopy and near ambient pressure X-ray photoelectron spectroscopy. Theoretical simulation indicates that the electric field enhanced by surface plasmon, together with plasmonic hot electrons and interfacial hybridization, may play a critical role in NN dissociation. Specifically, AuRu coreantenna nanostructures with broadened light adsorption cross section and active sites achieve an ammonia production rate of 101.4 μmol g −1 h −1 without any sacrificial agent at room temperature and 2 atm pressure. This work highlights the significance of surface plasmon to activation of inert molecules, serving as a promising platform for developing novel catalytic systems.
Renewable energy-driven methanol synthesis from CO2 and green hydrogen is a viable and key process in both the “methanol economy” and “liquid sunshine” visions. Recently, In2O3-based catalysts have shown great promise in overcoming the disadvantages of traditional Cu-based catalysts. Here, we report a successful case of theory-guided rational design of a much higher performance In2O3 nanocatalyst. Density functional theory calculations of CO2 hydrogenation pathways over stable facets of cubic and hexagonal In2O3 predict the hexagonal In2O3(104) surface to have far superior catalytic performance. This promotes the synthesis and evaluation of In2O3 in pure phases with different morphologies. Confirming our theoretical prediction, a novel hexagonal In2O3 nanomaterial with high proportion of the exposed {104} surface exhibits the highest activity and methanol selectivity with high catalytic stability. The synergy between theory and experiment proves highly effective in the rational design and experimental realization of oxide catalysts for industry-relevant reactions.
Adsorption is one of the widely used processes in the chemical industry environmental application. As compared to mathematical models proposed to describe batch adsorption in terms of isotherm and kinetic behavior, insufficient models are available to describe and predict fixed-bed or column adsorption, though the latter one is the main option in practical application. The present review first provides a brief summary on basic concepts and mathematic models to describe the mass transfer and isotherm behavior of batch adsorption, which dominate the column adsorption behavior in nature. Afterwards, the widely used models developed to predict the breakthrough curve, i.e., the general rate models, linear driving force (LDF) model, wave propagation theory model, constant pattern model, Clark model, Thomas model, Bohart-Adams model, Yoon-Nelson model, Wang model, Wolborska model, and modified dose-response model, are briefly introduced from the mechanism and mathematical viewpoint. Their basic characteristics, including the advantages and inherit shortcomings, are also discussed. This review could help those interested in column adsorption to reasonably choose or develop an accurate and convenient model for their study and practical application.
Cellulose based ZnO nanocomposite (RCZ) films were prepared from cellulose carbamate-NaOH/ZnO solutions through one-step coagulation in Na2SO4 aqueous solutions. The structure and properties of RCZ films were characterized using XRD, FTIR, XPS, SEM, TEM, TG, tensile testing, and antibacterial activity tests. The content of ZnO in RCZ films was obtained in the range of 2.7-15.1 wt %. ZnO nanoparticles with a hexagonal wurtzite structure agglomerated into large particles, which firmly embedded in the cellulose matrix. RCZ films displayed good mechanical properties and high thermal stability. Moreover, the films exhibited excellent UV-blocking properties and antibacterial activities against Staphylococcus aureus and Escherichia coli. A dramatic reduction in viable bacteria was observed within 3 h of exposure, while all of the bacteria were killed within 6 h. This work provided a novel and simple pathway for the preparation of regenerated cellulose films with ZnO nanoparticles for application as functional biomaterials.
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