Sulfonylamidine-substituted derivatives of avibactam: Synthesis and antibacterial activity

Avibactam is a clinically approved non-β-lactam based β-lactamase inhibitor. Derivatization of this scaffold with improved inhibition profile is the demand of the day to cope with the future challenges. We successfully synthesized new derivatives of avibactam containing sulfonylamidine moieties at C2 position of the diazabicyclooctane ring. We tested in vitro antibacterial activities of newly synthesized compounds against 10 bacterial strains expressing variable β-lactamases. All compounds did not exhibit antimicrobial profile when assayed individually; however, all compounds minimized the MIC value of the imipenem in combination. Compound 5l proved most potent against all 10 bacterial strains, and showed improved inhibition against six bacterial strains as compared with the control inhibitor, relebactam. The compound 5l may be a lead hit for future development.     

Non-gray chemical composition based radiative property model of fly ash particles

Particle radiation has a spectral dependence and is closely related to the chemical composition of the material. Iron oxide, one of the main components of fly ash, observably affects the complex index of refraction of the particles. In this study, following the theory of the spectrum k-distribution based weighted sum of gray particles model (Guo et al. [4,13]), a non-gray fly ash radiative property model involving the chemical composition was developed. First, four typical fly ash particles with different iron oxide contents were selected, and the corresponding particle radiative parameters were obtained using the Mie theory. Then, the absorption efficiency and weighting factors of the non-gray model were directly obtained from the Gaussian integral points of the k-distribution. The scattering efficiency of the particles was obtained from the Planck mean. The accuracy of the newly developed model was evaluated in a one-dimensional plane-parallel slab system through comparison with the line-by-line (LBL) model and two commonly used gray radiative property models. The results show that the new non-gray model agrees well with the LBL solution and becomes more accurate as the iron oxide content increases. When the iron oxide content of the fly ash increased from 5.47% to 30.50%, the maximum relative error of the radiative heat flux and the radiative source term decreased from 12.50% to 5.68% and from 20.97% to 12.62%, respectively. The new model can improve the prediction accuracy of radiative heat transfer in pulverized coal-fired furnaces.     

Computational Modeling of Boundary Layer Flashback in a Swirling Stratified Flame Using a LES-Based Non-Adiabatic Tabulated Chemistry Approach

When operating under lean fuel–air conditions, flame flashback is an operational safety issue in stationary gas turbines. In particular, with the increased use of hydrogen, the propagation of the flame through the boundary layers into the mixing section becomes feasible. Typically, these mixing regions are not designed to hold a high-temperature flame and can lead to catastrophic failure of the gas turbine. Flame flashback along the boundary layers is a competition between chemical reactions in a turbulent flow, where fuel and air are incompletely mixed, and heat loss to the wall that promotes flame quenching. The focus of this work is to develop a comprehensive simulation approach to model boundary layer flashback, accounting for fuel–air stratification and wall heat loss. A large eddy simulation (LES) based framework is used, along with a tabulation-based combustion model. Different approaches to tabulation and the effect of wall heat loss are studied. An experimental flashback configuration is used to understand the predictive accuracy of the models. It is shown that diffusion-flame-based tabulation methods are better suited due to the flashback occurring in relatively low-strain and lean fuel–air mixtures. Further, the flashback is promoted by the formation of features such as flame tongues, which induce negative velocity separated boundary layer flow that promotes upstream flame motion. The wall heat loss alters the strength of these separated flows, which in turn affects the flashback propensity. Comparisons with experimental data for both non-reacting cases that quantify fuel–air mixing and reacting flashback cases are used to demonstrate predictive accuracy.     

Beam steering characteristics in high-power quantum-cascade lasers emitting at∼4.6µm

A beam steering effect of high-power quantum cascade(QC) lasers emitting at 4.6 μm was investigated. The continuous wave(CW) output power of an uncoated, 6-mm-long, 7.5-μm-wide buried-heterostructure QC laser at 25℃ was as high as 854.2 m W. The maximum beam steering angle was offset by ±14.2° from the facet normal(0°) in pulsed mode. The phenomenon was judged explicitly by combining the diffraction limit theory and Fourier transform of the spectra. It was also verified by finite element method software simulation and the calculation of two-dimensional(2 D)effective-index model. The observed steering is consistent with a theory for coherence between the two lowest order lateral modes. Therefore, we have established an intrinsic linkage between the spectral instabilities and the beam steering by using the Fourier transform of the spectra, and further presented an extremely valid method to judge the beam steering. The content of this method includes both three equidistant peak positions in the Fourier transform of the spectra and the beam quality located between once the diffraction limit(DL) and twice the DL.     

Cu2O/SiC高效催化卤代芳烃与酚类的Ullmann偶联反应

卤代苯与酚类化合物反应制取二芳基醚是现代有机合成中的一个重要反应.传统的二苯醚合成方法是铜催化卤代苯与酚类化合物的Ullmann型C-O偶联反应,但是这种方法需要苛刻的反应条件.后来,人们发现了Pd(0)和Cu(Ⅰ)基催化剂,但是前者成本较高,且需要使用昂贵的配体,因此其应用受到了限制,而铜作为一种成本较低的催化剂受到了越来越多的关注.铜催化剂可以分为均相和非均相两大类.均相铜催化剂使用的是铜盐,并且需要加入配体,成本较高,且不易分离和循环利用.非均相铜催化剂研究较多的是CuO,Cu2O及Cu纳米颗粒,其中Cu2O纳米颗粒催化剂对Ullmann型C-O偶联反应具有很高的催化活性,但是它在潮湿的空气中容易被氧化,因此需要寻找一种合适的载体防止Cu2O纳米颗粒被氧化.SiC具有优良的化学稳定性及导电导热性能,并且作为载体己经成功应用到很多热催化及光催化反应中.本文以高比表面积的SiC为载体,以二乙二醇作为溶剂和还原剂,采用传统的两步液相还原法制备了Cu2O/SiC催化剂,并通过X射线衍射、X射线光电子能谱、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和H2程序升温还原等方法对Cu2O/SiC催化剂进行了表征.SEM和TEM结果表明,Cu2O纳米颗粒均匀分散在SiC表面,同时上述表征结果都表明Cu在SiC上主要以Cu2O的形式存在.将制备的Cu2O/SiC催化剂用于催化卤代芳烃与酚类的Ullmann C-O偶联反应中.以碘苯和苯酚的Ullmann C-O偶联反应为模型实验,考察了反应温度、反应时间、溶剂、碱的种类及用量和催化剂用量等条件的影响,得到了碘苯与苯酚UllmannC-O偶联反应的最优反应条件为:卤代芳烃14 mmol,酚类14 mmol,1.0当量的Cs2CO3,Cu2O/SiC(5 wt％) 10 mg,四氢呋喃10mL,在Ar气氛下150℃反应3h.在该条件下,二苯醚收率达到97％,转化频率(TOF)高达1136 h-1.Cu2O/SiC催化剂对Ullmann C-O偶联反应具有很好的普适性,并且对Ullmann C-S偶联反应也表现出很高的活性,TOF高达1186h-1.以碘苯和苯酚的Ullmann C-O偶联反应为基准实验,对催化剂的循环稳定性进行了考察.Cu2O/SiC催化剂五次循环后二苯醚的收率从97％降低至64％,这主要是由于活性组分Cu2O的流失所致.     

An Iterative Module in the Azalomycin F Polyketide Synthase Contains a Switchable Enoylreductase Domain

Detailed analysis of the modular Type I polyketide synthase (PKS) involved in the biosynthesis of the marginolactone azalomycin F in mangrove Streptomyces sp. 211726 has shown that only nineteen extension modules are required to accomplish twenty cycles of polyketide chain elongation. Analysis of the products of a PKS mutant specifically inactivated in the dehydratase domain of extension-module 1 showed that this module catalyzes two successive elongations with different outcomes. Strikingly, the enoylreductase domain of this module can apparently be “toggled” off and on : it functions in only the second of these two cycles. This novel mechanism expands our understanding of PKS assembly-line catalysis and may explain examples of apparent non-colinearity in other modular PKS systems.     

Porous Si/C composite as anode materials for high-performance rechargeable lithium-ion battery

A novel porous silicon was synthesized through a magnesiothermic reduction method of molecular sieve for the first time, the porous silicon was used as anode material, which shows a high initial specific capacity of 2018.5 mAh/g with current density of 0.1 A/g.     

A moderate deviation principle for 2-D stochastic Navier–Stokes equations driven by multiplicative Lévy noises

In this paper, we establish a moderate deviation principle for two-dimensional stochastic Navier–Stokes equations driven by multiplicative Lévy noises. The weak convergence method introduced by Budhiraja, Dupuis and Ganguly in [3] plays a key role.     

Some upper and lower bounds on PSD-rank

Positive semidefinite rank (PSD-rank) is a relatively new complexity measure on matrices, with applications to combinatorial optimization and communication complexity. We first study several basic properties of PSD-rank, and then develop new techniques for showing lower bounds on the PSD-rank. All of these bounds are based on viewing a positive semidefinite factorization of a matrix M as a quantum communication protocol. These lower bounds depend on the entries of the matrix and not only on its support (the zero/nonzero pattern), overcoming a limitation of some previous techniques. We compare these new lower bounds with known bounds, and give examples where the new ones are better. As an application we determine the PSD-rank of (approximations of) some common matrices.     

Fixed points of mixed monotone operators for existence and uniqueness of nonlinear fractional differential equations

In this paper we study the existence and uniqueness of positive solutions for nonlinear fractional differential equation boundary value problems by using new fixed point results of mixed monotone operators on cones.