Probing Ambiguous Base‐Pairs by Genetic Transformation with XNA Templates

The templating potential of anhydrohexitol oligonucleotides bearing ambiguous bases was studied in vivo, by using a selection screen for mosaic heteroduplex plasmids in Escherichia coli. 1,5‐Anhydro‐2,3‐dideoxy‐2‐(5‐nitroindazol‐1‐yl)‐D ‐arabino‐hexitol showed the greatest ambiguity among the three nucleosides tested. At most two successive ambiguous bases could be tolerated on hexitol templates read in bacterial cells. Hexitol nucleosides bearing simplified heterocycles thus stand as promising monomers for generating random DNA sequences in vivo from defined synthetic oligonucleotides.     

Hydrogen Production by the Thermophilic Bacterium Thermotoga neapolitana

As the only fuel that is not chemically bound to carbon, hydrogen has gained interest as an energy carrier to face the current environmental issues of greenhouse gas emissions and to substitute the depleting non-renewable reserves. In the last years, there has been a significant increase in the number of publications about the bacterium Thermotoga neapolitana that is responsible for production yields of H₂ that are among the highest achievements reported in the literature. Here we present an extensive overview of the most recent studies on this hyperthermophilic bacterium together with a critical discussion of the potential of fermentative production by this bacterium. The review article is organized into sections focused on biochemical, microbiological and technical issues, including the effect of substrate, reactor type, gas sparging, temperature, pH, hydraulic retention time and organic loading parameters on rate and yield of gas production.     

State multiplicity in CSTR-separator-recycle polymerisation systems

This article continues earlier work (Comput. Chem. Eng. 24 (2000) 209) concerning the design and control of isothermal reactor-separator-recycle systems. The multiplicity behaviour of six reaction systems of increasing complexity, from one-reactant, first-order reaction to chain-growth polymerisation, is investigated. Below a critical value of the plant Damkohler number, Da<Da^cr, the only steady state involves infinite flow rates. Feasible steady states become possible if the critical value is exceeded, Da>Da^cr. For one-reaction systems, one stable steady state is born at a transcritical bifurcation. For consecutive-reaction systems, including polymerisation, a fold bifurcation can lead to two feasible steady states. Moreover, the transcritical bifurcation is destroyed when two reactants are involved. If the gel-effect is included, a maximum of four steady states are possible. When multiple steady states exist, the achievable conversion is constrained by the instability of the low-conversion branch. This has practical importance for polymerisation systems when the radicals’ quasi-steady state assumption is not valid or the gel effect is significant.     

截面分析法对界面过渡区厚度的放大作用

在采用截面法分析研究截面过渡区厚度时，由于截平面并不一定正好垂直于集料的表面，导致得到的表观界面过渡区厚度与实际界面过渡区厚度是不同的。以3种规则形状(球形、椭圆形截面以及矩形截面)的集料为例，从几何概率角度研究了截面分析法对界面过渡区厚度的放大问题。研究结果表明，截面分析法得到的表观界面过渡区厚度都大于实际的界面过渡区厚度，平均放大倍数与集料的粒形有关。对正方体性集料而言，平均表观界面过渡区的厚度是实际界面厚度的1．12倍；对球形集料而言，实际界面过渡区厚度被放大了π／2倍。     

Syndiospecific polymerization of propene under different processes with different bridged [(RPh)2C(Cp)(2,7-BuFlu)]ZrCl2 metallocene catalysts

The synthesis of syndiotactic polypropene was achieved by using new C_S-symmetric ansa-metallocene catalysts of the type [Ph′₂C(Cp)(2,7-^tertBu₂Flu)]ZrCl₂ (Ph′₂=Ph₂, (4-MePh)₂, 3,4′-Me₂Ph₂, (4-OCH₃Ph)₂). Applying these catalysts, the influence of the substitution pattern of the bridge on the polymerization performance can be studied and highly syndiotactic polypropene (rrrr>99%) with high molar masses and high melting temperatures (up to 153 °C) was obtained.Propene was polymerized at different temperatures under four sets of conditions: in toluene solution, bulk, toluene slurry, and gas phase with NaCl as stirred bed material. Methylaluminoxane (MAO) and methylaluminoxane supported on silicagel (MAO/SiO₂) were used as cocatalyst, respectively. In order to estimate the influence of the process on the single site properties of the catalysts, comparisons were made between polymer properties, i.e. microstructure, melting temperature, molar mass, and polymer morphology, thus allowing the effect of the support on the catalyst to be observed.     

水泥基复合材料集料与浆体界面研究综述(一):实验技术

关于界面研究,概括起来主要可以从以下5个方面考虑：(1)界面研究的相关技术手段;(2)界面微观结构特征的研究;(3)界面微观结构的形成及劣化机理;(4)影响界面微观结构因素的研究;(5)界面过渡区的性能对材料宏观性能(包括：力学性能和耐久性)影响的研究。对这些问题的研究是为了回答以下2个问题：(1)各种层次的界面过渡区到底在多大程度上影响着整个材料的力学性能和耐久性;(2)通过改善界面来达到改善水泥基复合材料的性能这一措施是否可行。由于界面研究的技术手段与方法随着其它相关技术与设备的引入而不断取得新的进展,促进了水泥基复合材料集料与浆体界面相关研究也不断取得新的成果。关于界面研究的新实验技术和方法,从如下4个方面进行了描述：(1)与界面过渡区微观结构表征相关的实验技术;(2)与界面过渡区力学性能(包括：粘结强度、刚度和断裂力学性能)相关的技术和方法;(3)与界面过渡区传输性能相关的技术和方法;(4)与界面过渡区收缩性能相关的技术和方法。     

Synthesis and Anti‐herpetic Activity of Phosphoramidate ProTides

Among the many prodrug approaches aimed at delivering nucleoside monophosphates into cells, the phosphoramidate ProTide approach is one that has shown success, which has made it possible for some of the phosphoramidates to enter into clinical trials. Herein, we report the synthesis and antiviral activity of a series of phosphoramidate ProTides designed to bypass the thymidine kinase (TK) dependence of the parent nucleoside analogues. Phosphoramidate derivatives of (E)‐5‐(2‐bromovinyl)‐2′‐deoxyuridine (BVDU) that contain L ‐alanine or pivaloyloxymethyl iminodiacetate (IDA‐POM) exhibit anti‐HSV‐1 and anti‐VZV activity in cell cultures, but they largely lost antiviral potency against TK‐deficient virus strains. Among deazapurine nucleosides and their phosphoramidate derivatives, the 7‐deazaadenine containing nucleosides and their phosphoramidate triester derivatives showed weak antiviral activity against VZV. Apparently, intracellular nucleotide delivery with these phosphoramidates is partly successful. However, none of the compound prodrugs showed superior activity to their parent drugs.     

Discovery of an Acyclic Nucleoside Phosphonate that Inhibits Mycobacterium tuberculosis ThyX Based on the Binding Mode of a 5‐Alkynyl Substrate Analogue

The urgent need for new antibiotics poses a challenge to target un(der)exploited vital cellular processes. Thymidylate biosynthesis is one such process due to its crucial role in DNA replication and repair. Thymidylate synthases (TS) catalyze a crucial step in the biosynthesis of thymidine 5‐triphosphate (TTP), an elementary building block required for DNA synthesis and repair. To date, TS inhibitors have only been successfully applied in anticancer therapy due to their lack of specificity for antimicrobial versus human enzymes. However, the discovery of a new family of TS enzymes (ThyX) in a range of pathogenic bacteria that is structurally and biochemically different from the “classic” TS (ThyA) has opened the possibility to develop selective ThyX inhibitors as potent antimicrobial drugs. Here, the interaction of the known inhibitor 5‐(3‐octanamidoprop‐1yn‐1yl)‐2′‐deoxyuridine‐5′‐monophosphate ( 1 ) with Mycobacterium tuberculosis ThyX enzyme is explored using molecular modeling starting from published crystal structures, with further confirmation through NMR experiments. While the deoxyuridylate (dUMP) moiety of compound 1 occupies the cavity of the natural substrate in ThyX, the rest of the ligand (the “5‐alkynyl tail”) extends to the outside of the enzyme between two of its four subunits. The hydrophobic pocket that accommodates the alkyl part of the tail is formed by displacement of Tyr 44.C, Tyr 108.A and Lys 165.A. Changes to the resonance of the Lys 165 NH₃ group upon ligand binding were monitored in a titration experiment by 2D HISQC NMR. Guided by the results of the modeling and NMR studies, and inspired by the success of acyclic antiviral nucleosides, compounds where a 5‐alkynyl uracyl moiety is coupled to an acyclic nucleoside phosphonate (ANP) were synthesized and evaluated. Of the compounds evaluated, sodium (6‐(5‐(3‐octanamidoprop‐1‐yn‐1‐yl)‐2,4‐dioxo‐3,4‐dihydropyrimidin‐1(2H)‐yl)hexyl)phosphonate ( 3 e ) exhibited 43 % of inhibitory effect on ThyX at 50 μM . While only modest activity was achieved, this is the first example of an ANP inhibiting ThyX, and these results can be used to further guide structural modifications to this class to develop more potent compounds with potential application as antibacterial agents acting through a novel mechanism of action.     

Pilot Plant Results with Three Different Types of UV Lamps for Advanced Oxidation

Three different types of ultraviolet lamps were tested for the advanced oxidation process application on pre-treated surface water in a pilot plant. The pilot setup consisted of three parallel reactors with either medium pressure, low pressure or dielectric barrier discharge UV lamps. Four model compounds (atrazine, bromacil, ibuprofen and N-nitroso-dimethylamine (NDMA)) and 0, 5 or 10 ppm hydrogen peroxide were dosed. Low pressure lamps were shown to have the lowest energy demand, calculated as electrical energy per order, followed by dielectric barrier discharge lamps and then medium pressure lamps. Medium pressure lamps gave the highest formation of genotoxic activity and nitrite formation, whereas no formation of genotoxic activity was observed for either of the other lamp types.     

Local porosity analysis of pore structure in cement paste

Three-dimensional (3-D) local porosity theory (LPT) was originally proposed by Hilfer and recently used for the analysis of pore space geometry in model sandstone. LPT pursues to define the probability density functions of porosity and porosity connectivity. In doing so, heterogeneity differences in various sandstone samples were assessed. However, fundamental issues as to the stochastic concept of geometric heterogeneity are ignored in Hilfer's LPT theory. This paper focuses on proper sampling procedures that should be based on stochastic approaches to multistage sampling and geometric heterogeneity. Standard LPT analysis provides a 3-D microscopic modeling approach to materials. Traditional experimental techniques yield two-dimensional (2-D) section images, however. Therefore, this paper replaces the method for assessing material data in standard LPT theory to a more practical one, based on stereological, 3-D interpretation of quantitative image analysis data. The developed methodology is used to characterize the pore structure in hardened cement paste with various water/cement ratios (w/c) at different hydration stages.