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31.
As it is known, there is no rule satisfying additivity in the complete domain of bankruptcy problems. This paper proposes a notion of partial additivity in this context, to be called μ-additivity. We find out that this property, together with two quite compelling axioms, equal treatment of equals and continuity, identify the minimal overlap rule, introduced by O’Neill (Math. Soc. Sci. 2:345–371, 1982). 相似文献
32.
Florian Tieves Sbastien Jean‐Paul Willot Morten Martinus Cornelis Harald vanSchie Marine Charlne Rene Rauch Sabry Hamdy Hamed Younes Wuyuan Zhang JiaJia Dong Patricia GomezdeSantos John Mick Robbins Bettina Bommarius Miguel Alcalde Andreas Sebastian Bommarius Frank Hollmann 《Angewandte Chemie (International ed. in English)》2019,58(23):7873-7877
An increasing number of biocatalytic oxidation reactions rely on H2O2 as a clean oxidant. The poor robustness of most enzymes towards H2O2, however, necessitates more efficient systems for in situ H2O2 generation. In analogy to the well‐known formate dehydrogenase to promote NADH‐dependent reactions, we here propose employing formate oxidase (FOx) to promote H2O2‐dependent enzymatic oxidation reactions. Even under non‐optimised conditions, high turnover numbers for coupled FOx/peroxygenase catalysis were achieved. 相似文献
33.
Patricia Gomez de Santos Fadia V. Cervantes Florian Tieves Francisco J. Plou Frank Hollmann Miguel Alcalde 《Tetrahedron》2019,75(13):1827-1831
By mimicking the role of human liver P450 monooxygenases, fungal unspecific peroxygenases (UPOs) can perform a range of highly selective oxyfunctionalization reactions on pharmacological compounds, including O-dealkylations and hydroxylations, thereby simulating drug metabolism. Here we have benchmarked human drug metabolite (HDM) synthesis by several evolved UPO mutants, focusing on dextromethorphan, naproxen and tolbutamide. The HDM from dextromethorphan was prepared at the semi-preparative scale as a proof of production. The structural analysis of mutations involved in the synthesis of HDMs highlights the heme access channel as the main feature on which to focus when designing evolved UPOs. These variants are becoming emergent tools for the cost-effective synthesis of HDMs from next-generation drugs. 相似文献
34.
Aparicio S Alcalde R Dávila MJ García B Leal JM 《The journal of physical chemistry. B》2007,111(12):3167-3177
This paper reports on an experimental and theoretical study of 1,8-cineole, one of the main components of essential oils in different plants. The pressure-volume-temperature behavior of this fluid was evaluated accurately over wide temperature and pressure ranges and correlated successfully with the empirical TRIDEN equation. From the measured data, the relevant derived coefficients isothermal compressibility, isobaric expansibility, and internal pressure were calculated. The isobaric heat capacities at high pressure were extrapolated from the data measured at atmospheric pressure. The cubic equations of state by Soave, Peng-Robinson, Stryjek-Vera modification of Peng-Robinson, Patel-Teja, Sako-Wu-Prausnitz, and the SAFT and PC-SAFT molecularly based equations of state were used to predict the PVT behavior. The SAFT and PC-SAFT parameters for 1,8-cineole were obtained from correlation of available saturation literature data; the best results were provided by Sako-Wu-Prausnitz and PC-SAFT equations of state, whereas the classical ones were shown to be inadequate. The molecular structure was studied by quantum computations at the B3LYP/6-311++g(d) level and classical molecular dynamics simulations in the NPT ensemble with the OPLS-AA forcefield. On the basis of both macroscopic and microscopic studies, a complex fluid structure was inferred. 相似文献
35.
Zumárraga M Bulter T Shleev S Polaina J Martínez-Arias A Plou FJ Ballesteros A Alcalde M 《Chemistry & biology》2007,14(9):1052-1064
Fungal laccases are remarkable green catalysts that have a broad substrate specificity and many potential applications in bioremediation, lignocellulose processing, organic synthesis, and more. However, most of these transformations must be carried out at high concentrations of organic cosolvents in which laccases undergo unfolding, thereby losing their activity. We have tailored a thermostable laccase that tolerates high concentrations of cosolvents, the genetic product of five rounds of directed evolution expressed in Saccharomyces cerevisiae. This evolved laccase--R2 variant--was capable of resisting a wide array of cosolvents at concentrations as high as 50% (v/v). Intrinsic laccase features such as the redox potential and the geometry of catalytic copper varied slightly during the course of the molecular evolution. Some mutations at the protein surface stabilized the laccase by allowing additional electrostatic and hydrogen bonding to occur. 相似文献
36.
Varea T Alcalde A López de Dicastillo C Ramírez de Arellano C Cossío FP Asensio G 《The Journal of organic chemistry》2012,77(14):6327-6331
Double addition (1,2-1,4) of vinyl magnesium bromide to squaric acid derivatives allows the preparation of polyoxygenated cyclopentenones (8) in a "one-pot" procedure. The reaction occurs through the intermediate formation of octatetraenes (6). Protonation of this latter intermediate at -78 °C with TFE occurs selectively at the vinyl CH(2) closer to the metallic centers. DFT studies of the cyclization step justify the observed diastereoselectivity. 相似文献
37.
A broad and simple method permitted halide ions in quaternary heteroaromatic and ammonium salts to be exchanged for a variety of anions using an anion exchange resin (A(-) form) in non-aqueous media. The anion loading of the AER (OH(-) form) was examined using two different anion sources, acids or ammonium salts, and changing the polarity of the solvents. The AER (A(-) form) method in organic solvents was then applied to several quaternary heteroaromatic salts and ILs, and the anion exchange proceeded in excellent to quantitative yields, concomitantly removing halide impurities. Relying on the hydrophobicity of the targeted ion pair for the counteranion swap, organic solvents with variable polarity were used, such as CH(3)OH, CH(3)CN and the dipolar nonhydroxylic solvent mixture CH(3)CN:CH(2)Cl(2) (3:7) and the anion exchange was equally successful with both lipophilic cations and anions. 相似文献
38.
Barrero AF Herrador MM Arteaga P Gil J González JA Alcalde E Cerdá-Olmedo E 《Organic & biomolecular chemistry》2011,9(20):7190-7195
Mixed cultures of strains of opposite sex ("mated" cultures) of Blakeslea trispora contain trisporic acids and other apocarotenoids, some of which mediate the sexual responses of this fungus and other Mucorales. In mated cultures of the wild-type strains F986 and F921 we identified eleven apocarotenoids: two C(18) trisporoids, three C(15) compounds with a monocyclofarnesane skeleton, a C(13) compound, and five C(7) compounds with a 2-methylhexane skeleton. Six of them are new natural products and two others are new for Blakeslea. Their structures were established by NMR and mass spectra and those of the C(7) and C(13) compounds were confirmed by chemical synthesis. The finding of these compounds and the presence of approximately equimolecular amounts of the C(18), C(15), and C(7) families led to the conclusion that β-carotene is initially split in three fragments by cleavage of its 13,14 and 11',12' double bonds. 相似文献
39.
de Abreu MA Alvaro-Benito M Plou FJ Fernández-Lobato M Alcalde M 《Combinatorial chemistry & high throughput screening》2011,14(8):730-738
β-Fructofuranosidases can divert their hydrolytic activity towards transglycosylation for the synthesis of high value-added products, including prebiotic fructooligosaccharides (FOS). A directed evolution strategy has been employed to enhance the transferase rate of the β-fructofuranosidase (SoINV) from the Schwanniomyces occidentalis yeast for the production of β-(2→6)-linked FOS. To screen for transferase activity of the SoINV functionally expressed in Saccharomyces cerevisiae, a high-throughput screening protocol based on two colorimetric assays was validated (with coefficient of variance below 11%). Mutagenic libraries were constructed by error-prone PCR and clones showing higher glucose:fructose ratio with respect to the parental type were identified. Further analysis by anion-exchange chromatography coupled with pulsed amperometric detection helped to identify mutants with improved yields for the synthesis of β-(2→6) fructooligosaccharides. Selected mutants displayed transferase initial rates enhanced ~2-fold over parent type, reaching production levels up to 47 g/L after 48 h of reaction for the formation of 6-kestose. 相似文献
40.
S. J. Prado C. Trallero-Giner V. Lpez-Richard A. M. Alcalde G. E. Marques 《Physica E: Low-dimensional Systems and Nanostructures》2004,20(3-4):286
We present a systematic theoretical study, based on the Kane–Weiler 8×8 k·p model, of the linear Zeeman splitting introduced by the interaction between the angular momentum and the magnetic field which can give a measure of the non-linear Zeeman effect associated with interband coupling and diamagnetic contributions. The conduction and valence bands g-factors are calculated for InSb spherical and semi-spherical quantum dots. The calculations of the g-factors showed an almost linear dependence, for the ground state, on the magnetic field. We have also found that the strong magnetic field dependence as well as the dependence on the dot size of the effective spin splitting can be unambiguously attributed to the strength of the inter-level mixing. 相似文献