bluuebunny/crossref_metadata_2025 huggingface dataset:
Las finalidades de las relaciones de sucesos y los elementos que aumentan su efectividad: El caso de un mesonero avaricioso
Authors: Iglesias Castellano Abel
Published: July 2013

Resumen: Las «relaciones de sucesos», unos escritos de carácter fundamentalmente popular, tuvieron durante el siglo XVII una notable difusión. A menudo, la finalidad de estos impresos era moralizante. Es el caso de una jácara publicada hacia 1687, la cual constituye un ataque a la avaricia, personificada en un mesonero de Yebes, pueblo del término de Alcalá de Henares. Los elementos que aportan veracidad al relato, el sensacionalismo y la existencia de una serie de lugares comunes hacían aumentar la efectividad del exemplum. Por otra parte, este tipo de relatos solían acoger en sus páginas una visión de las estructuras económicas que interesaba a los poderes establecidos. Además, sus versos proyectaban las ideas religiosas imperantes.Palabras clave: Relaciones de sucesos, Jácara, Exemplum, Avaricia, EconomíaAbstract: The following «pamphlets» –essentially popular writings– spread throughout 17th century. Quite often, the ending of these leaflets was moralistic. In the case of a tale published about 1687, which instigated an attack of greed, relates to an innkeeper from Yebes, a town in the district of Alcalá de Henares. The elements that contributed to the story were sensationalism and the existence of a series of common places that augmented the effectiveness of the exemplum. On the other hand, this type of legend always embraces a perception of the economic structures that call the attention of the established authorities. Moreover, its verses reflect the religious ideas.Keywords: Pamphlets, Tale, Exemplum, Avarice, Economy
Fluidics
Authors: Austin Suthanthiraraj Pearlson P. , Graves Steven W.
Published: July 2013

The use of fluidics is implicit in a technology named “flow cytometry,” which flows a cell or particle through a sensing volume to obtain serial analysis of particles on a one by one basis. This flow of particles enables flow cytometry to collect information on multiple particle populations, giving it a distinct advantage over bulk analysis approaches. Moreover, flow cytometers can analyze thousands of particles per second in a single flowing stream. Additionally, use of volumetric sample delivery makes it possible for flow cytometers to accurately count cells and particles. Furthermore, the analysis results can be coupled with a fluidic diversion mechanism to sort and collect particles based on desired properties. Finally, when high‐throughput sampling technologies are employed to rapidly change the input of the sample stream, a flow cytometer can become an integral tool for high‐throughput screening. The above properties have made flow cytometry useful in a wide range of biomedical applications. In this unit we will present an overview of fluidic systems that make flow cytometry possible. This will introduce historical approaches, explanations of the commonly implemented current fluidics, and brief discussions of potential future fluidics where appropriate. Curr. Protoc. Cytom. 65:1.2.1‐1.2.14. © 2013 by John Wiley & Sons, Inc.
Association of Tobacco Exposure and Reduction of Radiographic Progression in Early Rheumatoid Arthritis: Results From a French Multicenter Cohort
Authors: Vesperini Veronique , Lukas Cedric , Fautrel Bruno , Le Loet Xavier , Rincheval Nathalie , Combe Bernard
Published: July 2013

Objective

To investigate the initial response to treatment and risk of radiographic disease progression in current smokers (S), ex‐smokers (EX), and nonsmokers (NS) in a prospective early arthritis cohort and to analyze the influence of smoking cessation on arthritis outcome.

Methods

The ESPOIR cohort is a prospective cohort study monitoring clinical, biologic, and radiographic data for patients with inflammatory arthritis lasting 6 weeks to 6 months. We examined the influence of smoking status on disease presentation (baseline characteristics) and therapeutic response at 1 year. Risk of structural progression at 12 months, defined as change in the modified Sharp/van der Heijde score ≥1, was analyzed by multivariate regression adjusted for potential confounders (age, sex, joint erosion at inclusion, educational level, positivity for rheumatoid factor or anti–cyclic citrullinated peptide 2 antibodies, and shared HLA–DRB1 epitope).

Results

A total of 813 patients were included; 641 (79%) fulfilled the 2010 American College of Rheumatology/European League Against Rheumatism (EULAR) criteria for rheumatoid arthritis (RA). At inclusion, 138 (21.5%) were S patients, 168 (26.2%) were EX patients, and 335 (52.3%) were NS patients. Baseline acute‐phase indicator values were significantly lower for S patients than EX and NS patients (mean ± SD erythrocyte sedimentation rate was 24.2 ± 18.2 mm/hour versus 33.4 ± 28.0 and 31.4 ± 25.0 [P = 0.02], respectively, and mean ± SD C‐reactive protein level was 17.7 ± 28.0 mg/dl versus 28.5 ± 42.5 and 21.4 ± 29.0 [P = 0.01], respectively). Smoking status had no influence on Disease Activity Score in 28 joints, Health Assessment Questionnaire score, EULAR response, or use of disease‐modifying antirheumatic drugs and biologic therapy in the first 12 months of followup (P > 0.05). The adjusted risk for structural disease progression was associated with active smokers (odds ratio 0.50 [95% confidence interval 0.27–0.93], P = 0.028). Sixteen patients had stopped smoking at 12 months, with no significant difference in observed outcomes from other patients.

Conclusion

In this large prospective cohort of patients with early arthritis, smoking status had no significant effect on disease activity and disability but did reduce 1‐year radiographic disease progression. The antiinflammatory role of nicotine may explain the lower systemic inflammation and structural disease progression in current smokers with early RA.
Exploratory Study of Radiographic Change in Patients With Tophaceous Gout Treated With Intensive Urate‐Lowering Therapy
Authors: Dalbeth Nicola , Doyle Anthony J. , McQueen Fiona M. , Sundy John , Baraf Herbert S. B.
Published: July 2013

Objective

Tophi are strongly associated with structural damage in gout, and urate‐lowering therapy reduces tophus size. Pegloticase leads to dramatic reductions in serum urate and subcutaneous tophi in treatment responders. The aim of this analysis was to examine whether profound urate lowering can alter radiographic findings in gout.

Methods

Serial plain radiographs of the hands and feet were obtained from 8 patients with tophaceous gout treated with pegloticase. Radiographs were scored for erosion and joint space narrowing (JSN) according to the gout‐modified Sharp/van der Heijde method. Scorers were blinded to each other's scores and to the clinical characteristics of the patients (including the clinical response to pegloticase). A detailed qualitative site‐by‐site analysis was undertaken to define additional changes observed from baseline.

Results

All patients experienced a profound urate‐lowering response (serum urate level <1 mg/dl) during pegloticase treatment. For the entire group, the median total radiographic scores reduced from 69.25 (range 1.5–138) at baseline to 57.25 (range 1.5–110) at 12 months (P = 0.02). Median erosion scores reduced over 1 year (P = 0.008), but JSN scores did not change (P = 0.50). Further reductions were observed in total scores and erosion scores in 5 patients with 24‐month followup films (one‐way analysis of variance P = 0.009 for total score, 0.02 for erosion, and 0.95 for JSN). Qualitative site‐by‐site analysis identified regression of soft tissue masses, increased sclerosis, and filling in of erosions in the followup films.

Conclusion

This exploratory study suggests that profound urate lowering can lead to improvement in structural damage, particularly bone erosion, in patients with tophaceous gout.
Prophylaxis for Latent Tuberculosis Infection Prior to Anti–Tumor Necrosis Factor Therapy in Low‐Risk Elderly Patients With Rheumatoid Arthritis: A Decision Analysis
Authors: Hazlewood Glen S. , Naimark David , Gardam Michael , Bykerk Vivian , Bombardier Claire
Published: July 2013

Objective

To determine if low‐risk elderly patients with rheumatoid arthritis (RA) who screen positive for latent tuberculosis (TB) infection prior to anti–tumor necrosis factor (anti‐TNF) therapy should be given isoniazid (INH).

Methods

A Markov model was developed. The base case was a patient age 65 years with RA starting anti‐TNF therapy with a positive tuberculin skin test (TST) finding of 5–9 mm, who was born in a country with low TB prevalence and had no other TB risk factors. The decision was 9 months of INH or not. The primary outcome was quality‐adjusted life expectancy. Multiple sensitivity analyses were performed.

Results

No prophylaxis was favored, with a gain of 1.1 quality‐adjusted life days, but the decision was sensitive to several variables. Prophylaxis was favored for patients ages <61 years, if the relative risk (RR) of TB reactivation with RA alone was >2.5, if the RR with anti‐TNF therapy was >5.8, or if the utility associated with INH therapy was >0.98. Prophylaxis was also preferred for patients with a TST result >10 mm and for patients from higher risk countries. If 6 months of INH or 4 months of rifampin were used, prophylaxis was preferred, providing that therapy reduced the risk of TB reactivation by >47% and >27%, respectively.

Conclusion

Withholding prophylaxis prior to anti‐TNF therapy may be reasonable for low‐risk elderly RA patients with a TST finding of 5–9 mm, although the decision is sensitive to patient preferences. For patients age <61 years from a higher risk country, or with a TST finding >10 mm, prophylaxis is preferred.
Covalently Tethered Polyoxometalate–Pyrene Hybrids for Noncovalent Sidewall Functionalization of Single‐Walled Carbon Nanotubes as High‐Performance Anode Material
Authors: Ma Dui , Liang Liying , Chen Wei , Liu Haimei , Song Yu‐Fei
Published: July 2013

A covalently tethered polyoxometalate (POM)–pyrene hybrid (Py–SiW11) is utilized for the noncovalent functionalization of single‐walled carbon nanotubes (SWNTs). The resulting SWNTs/Py–SiW11 nanocomposite shows that both SiW11 and pyrene moieties could interact with SWNTs without causing any chemical decomposition. When used as anode material in lithium‐ion batteries, the SWNTs/Py–SiW11 nanocomposite exhibits higher discharge capacities, and better rate capacity and cycling stability than the individual components. When the current density is 0.5 mA cm−2, the nanocomposite exhibits the initial discharge capacity of 1569.8 mAh g−1, and a high discharge capacity of 580 mAh g−1 for up to 100 cycles.
Synthesis and Characterization of Polyaniline/Zinc Sulfite Composite Films and Investigation of Properties
Authors: Tuncer Ebru , Turac Ersen
Published: July 2013

In the present work, we explore the opportunity to deposit zinc sulfide (ZnS)/polyaniline (PANI) composite films through an electrochemical route. The structural and the optical characterization showed the interaction between ZnS nanoparticular and PANI. The structure of the PANI–ZnS composite films was characterized by scanning electron microscopy, atomic force microscopy, and UV–vis spectroscopy. Cyclic voltammetry was used to investigate the electrochemical behavior of the resulting material. The existence of Zn and S on PANI–ZnS composite films was proved by the EDX‐mapping method. The conductivity measurements of PANI–ZnS composite films and PANI were accomplished by the four‐probe technique. © 2013 Wiley Periodicals, Inc. Adv Polym Technol 2013, 32, 21373; View this article online at wileyonlinelibrary.com. DOI 10.1002/adv.21373
CKM unitarity normalization tests, present and future
Authors: Hardy John C. , Towner Ian S.
Published: July 2013

The Cabibbo‐Kobayashi‐Maskawa (CKM) quark‐mixing matrix is a central pillar of the Electroweak Standard Model. The elements of the matrix must be determined from experiment, but the Model requires the matrix itself to be unitary. Any deviation from unitarity would signal the presence of “new physics” beyond the Standard Model, so tests of CKM unitarity have attracted considerable attention. Currently the most precise test is of the normalization of the top row, which has now reached a precision of 0.06% based on measurements of superallowed 0+ nuclear β decay and of kaon semileptonic and leptonic decays. This work overviews the status of the normalization tests and speculates on likely future improvements.
Structure and dielectric breakdown strength of nano calcium carbonate/polypropylene composites
Authors: Virtanen Suvi , Ranta Hannes , Ahonen Susanna , Karttunen Mikko , Pelto Jani , Kannus Kari , Pettersson Mika
Published: July 2013

Nanodielectrics, a 21st‐century phenomena, is envisioned to be the answer for material challenges in progressive high‐voltage technology. It is well known that the proper dispersion of nanoparticles plays a key role in improving the dielectric properties of a material, but to understand where changes in the properties of a material originate, it is also essential to reveal the multiscale structure of the material. In this study, the dielectric permittivity, breakdown strength, and structure of nano calcium carbonate (nano‐CaCO3)/polypropylene composites with 1.8–8.1 wt % doping were characterized systematically. The combined results from transmission electron microscopy, Raman microscopy, and optical microscopy show that the quality of nanodispersion was similar in all of the filler concentrations studied. However, all of the samples also contained smoothly distributed microparticles. The density of the microparticles increased exponentially when the concentration of nano‐CaCO3 was increased in the manufacturing process. The dielectric direct‐current breakdown of the composites had a maximum at 1.8 wt % concentration and then decreased as the filler concentration was increased. The differences could be explained by the existence of large microparticles rather than the quality of the nanoparticle dispersion; this indicated the importance of multiscale characterization. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 39504.
Graphene nanoplatelet‐polyetherimide composites: Revealed morphology and relation to properties
Authors: Wu Huang , Drzal Lawrence T.
Published: July 2013

In this research, a novel sample preparation technique was applied to reveal the morphology exfoliated graphene nanoplatelets [GNP, ∼10 nm thick and ∼5 µm in diameter)] and Polyetherimide (PEId) nanocomposite and study the relationship between processing and properties. The morphology of nanoscale fillers used to be hard to capture through conventional sample preparation. The polish‐plasma etching approach presented in this article successfully created contrast between filler and matrix. As a result, distribution and orientation of the fillers were obtained to study the effect of injection molding, compression molding and annealing. It was found that the orientation was significantly different depending on processing routes. The information obtained from morphology study also led to the modification of Tandon–Weng model, resulting in improved prediction of elastic modulus of the composite. The SEM images also clearly revealed change of filler orientation after annealing. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 4081–4089, 2013
Micropatterning of polymethacrylates by single‐ or two‐photon irradiation using π‐conjugated o‐nitrobenzyl ester phototrigger as side chains
Authors: Jin Ming , Xu Haoran , Hong Hong , Bao Chunyan , Pu Hongting , Wan Decheng , Zhu Linyong
Published: July 2013

A new single‐/two‐photon sensitive monomer, (E)‐5‐(4‐ethoxystyryl)−2‐nitrobenzyl methacrylate (ENbMA), was synthesized and copolymerized with methyl methacrylate (MMA) to form a series of photosensitive copolymers P(ENbMA–MMA)s that were well characterized by 1H NMR and GPC. The photochemical and photophysical properties of both photosensitive monomer and copolymers upon visible light irradiation were studied by UV–Vis, FTIR, and HPLC spectra, which confirmed that 5‐(4‐ethoxystyryl)‐2‐nitrobenzyl ester can be photolyzed effectively with generation of the corresponding 5‐(4‐ethoxystyryl)‐2‐nitrosobenzaldehyde and carboxylic acid groups. The successful photocleavage endowed the optimized copolymers with excellent micropatterning property due to the effective generation of alkaline‐soluble carboxylic acid groups. Moreover, the high two‐photon absorption cross‐sections (over 20 GM at 800 nm) and the comparable photolysis upon two‐photon NIR light irradiation of the chromophores provided the copolymers with significant application in two‐photon microfabrication. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 4099–4106, 2013
Synthesis and properties of fluorine‐ and siloxane‐containing polybenzimidazoles for high temperature proton exchange membrane fuel cells
Authors: Hsu Steve Lien‐Chung , Lin Yung‐Chung , Tasi Tsung‐Yu , Jheng Li‐Cheng , Shen Cheng‐Hsun
Published: July 2013

In this study, new fluorine–siloxane‐containing polybenzimidazole (PBI) copolymers were synthesized by copolymerization of 3,3′‐diaminobenzidine, 2,2‐bis(4‐carboxyphenyl)‐hexafluoropropane (HFA), and 1,3 bis(carboxypropyl)tetramethyldisiloxane (BTMDS) with different molar ratios. PBI copolymer membranes were prepared by solution‐casting and then doped with phosphoric acid. The structures of PBI copolymers were characterized by FTIR and X‐ray diffraction. The solubility of the PBI copolymers was significantly increased by the introduction of the bulky HFA group and the flexible BTMDS group into the polymer backbone. The PBI copolymers still maintained good thermal stability and mechanical properties. Because of the introduction of the flexible and hydrophobic siloxane group in the polymer backbone, the methanol permeability was reduced and the proton conductivity under anhydrous condition at high temperatures was increased compared to the PBI without the siloxane group. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 4107–4112, 2013
The response of otters to environmental changes imposed by the construction of large dams
Authors: Pedroso Nuno M. , Marques Tiago A. , Santos‐Reis Margarida
Published: July 2013

The number of dams is progressively increasing, but nonetheless there are few examples of long‐term studies involving otters and these structures.

This study assessed how Eurasian otter Lutra lutra responded over time to environmental changes imposed by the construction of a large reservoir, the Alqueva Dam (250 km2, SE Portugal).

Otter distribution was monitored over four phases (pre‐deforestation/flooding, deforestation, flooding, and post‐flooding) from 2000 to 2006 in both the flooded and surrounding areas. During each phase, presence was assessed at two resolutions: 25 km2 (76 survey sites in wet and dry seasons) and 1 km2 (39 survey sites, every three months). In addition, otter spraints were collected at eight survey sites in 2000 (pre‐dam) and 2006 (post‐dam) to assess and compare otter diet with prey availability.

Otters were widespread before dam construction (>82.4% positive cells), decreased during deforestation (68.5%), and particularly during the flooding phase (33.3%), recovered during the post‐flooding phase, although not at the level recorded before dam construction (61.5–83.3%). Otter diet was dominated by fish and American crayfish Procambarus clarkii during the pre‐deforestation/flooding phase (56.7% fish, 35.3% crayfish) and at the end of the post‐flooding phase (60.7% fish, 33.2% crayfish). Species richness of fish prey decreased with flooding (16 to 8), as did the ratio of native/non‐native fish species (1.7 to 0.3).

Changes in the availability of the main ecological requirements of otter were similar to the changes in the observed otter distribution in the flooded area throughout the impact phases, and decreased during deforestation and flooding with some recovery in the post‐flooding phase.

The results emphasize the importance of long‐term monitoring studies that include several post‐impact phases, to evaluate species response to impacts. This will allow better planning of mitigation and compensation measures.

Copyright © 2013 John Wiley & Sons, Ltd.
Tibetan ice core evidence for an intensification of the East Asian jet stream since the 1870s
Authors: Moore G. W. K.
Published: July 2013

The subtropical jet stream plays a significant role in the climate system and there exists evidence that it has intensified since the 1950s. However, the lack of upper‐air observations before this time makes it difficult to place this trend in a longer term context. Here, we show that a Tibetan ice core's snow accumulation and dust concentration records are respectively correlated and anti‐correlated with wind speeds in the jet stream over Asia as represented in both the NCEP and the 20th Century Reanalyses. This behavior is consistent with an intensification of this jet stream that began in the 1870s.
Reputation Management: Evidence for Ability But Reduced Propensity in Autism
Authors: Cage Eilidh , Pellicano Elizabeth , Shah Punit , Bird Geoffrey
Published: July 2013

Previous research has reported that autistic adults do not manage their reputation, purportedly due to problems with theory of mind [Izuma, Matsumoto, Camerer, & Adolphs]. The current study aimed to test alternative explanations for this apparent lack of reputation management. Twenty typical and 19 autistic adults donated to charity and to a person, both when alone and when observed. In an additional manipulation, for half of the participants, the observer was also the recipient of their donations, and participants were told that this observer would subsequently have the opportunity to donate to them (motivation condition). This manipulation was designed to encourage an expectation of a reciprocal “tit‐for‐tat” strategy in the participant, which may motivate participants to change their behavior to receive more donations. The remaining participants were told that the person watching was just observing the procedure (no motivation condition). Our results replicated Izuma et al.'s finding that autistic adults did not donate more to charity when observed. Yet, in the motivation condition, both typical and autistic adults donated significantly more to the observer when watched, although this effect was significantly attenuated in autistic individuals. Results indicate that, while individuals with autism may have the ability to think about reputation, a reduced expectation of reciprocal behavior from others may reduce the degree to which they engage in reputation management. Autism Res 2013, ●●: ●●–●●. © 2013 International Society for Autism Research, Wiley Periodicals, Inc.
Rare missense variants in DVL1, one of the human counterparts of the Drosophila dishevelled gene, do not confer increased risk for neural tube defects
Authors: Merello Elisa , Kibar Zoha , Allache Redouane , Piatelli Gianluca , Cama Armando , Capra Valeria , De Marco Patrizia
Published: July 2013

BACKGROUND

Neural tube defects (NTDs) are severe malformations that arise when the neural tube fails to close during embryogenesis. The planar cell polarity pathway is involved in neural tube closure and has been implicated in the pathogenesis of NTDs both in animal models and human cohorts. Dishevelled (Dvl/Dsh) is a multi‐module protein and a key regulator of both the canonical Wnt and the PCP pathway. In mouse, all Dvl1−/−; Dvl2−/− double mutants display craniorachischisis, a severe form of open NTDs. Recently, we have reported a possible role for rare variants of DVL2 as risk factors for NTDs.

METHODS

In view of these data, we hypothesized that DVL1 mutations might increase the risk for NTDs in some cases. Resequencing of the DVL1 gene in a cohort of 473 NTDs patients and 150 ethnically matched controls was performed. Prediction of the downstream effects of the nonsynonymous variants was done using computational methods.

RESULTS

We identified six missense variants that were absent in our ethnically matched controls group, and four of them (p.Arg153Cys; p.Glu544Arg; p.Arg568Trp; p.Val644Phe) were predicted to have a functional effect on protein structure by one or more bioinformatic programs. However, there was no difference in the overall rate of deleterious variants between the patients and controls (four in patients and three in controls; p = 0.36).

CONCLUSION

Our findings did not provide evidence for the implication of DVL1 in the pathogenesis of human NTDs. Birth Defects Research (Part A) 97:452–455, 2013. © 2013 Wiley Periodicals, Inc.
Sensitive determination of 2‐methoxyestradiol in pharmaceutical preparations and serum samples using flow injection chemiluminescence
Authors: Yao Hanchun , Zhang Min , Zeng Wenyuan , Zeng Xiaoying , Zhang Zhenzhong
Published: July 2013

A rapid and sensitive flow injection chemiluminescence (FI–CL) method is described for the determination of 2‐methoxyestradiol (2ME) based on enhancement of the CL intensity from a potassium ferricyanide–calcein system in sodium hydroxide medium. The optimum conditions for the CL emission were investigated. Under optimized conditions, a linear calibration graph was obtained over the range 1.0 × 10‐8 to 1.0 × 10‐6 mol/L (r = 0.998) 2ME with a detection limit (3σ) of 5.4 × 10‐9 mol/L. The relative standard deviation (RSD) for 5.0 × 10‐7 mol/L 2ME was 1.7%. As a preliminary application, the proposed method was successfully applied to the determination of 2ME in injection solutions and serum samples. The possible CL mechanism was also proposed. Copyright © 2013 John Wiley & Sons, Ltd.
Influence of the cycle length on the production of PHA and polyglucose from glycerol by bacterial enrichments in sequencing batch reactors
Authors: Moralejo‐Gárate Helena , Palmeiro‐Sánchez Tania , Kleerebezem Robbert , Mosquera‐Corral Anuska , Campos José Luis , van Loosdrecht Mark C.M.
Published: July 2013

PHA, a naturally occurring biopolymer produced by a wide range of microorganisms, is known for its applications as bioplastic. In recent years the use of agro‐industrial wastewater as substrate for PHA production by bacterial enrichments has attracted considerable research attention. Crude glycerol as generated during biodiesel production is a waste stream that due to its high organic matter content and low price could be an interesting substrate for PHA production. Previously we have demonstrated that when glycerol is used as substrate in a feast‐famine regime, PHA and polyglucose are simultaneously produced as storage polymers. The work described in this paper aimed at understanding the effect of the cycle length on the bacterial enrichment process with emphasis on the distribution of glycerol towards PHA and polyglucose. Two sequencing batch reactors where operated with the same hydraulic and biomass retention time. A short cycle length (6 h) favored polyglucose production over PHA, whereas at long cycle length (24 h) PHA was more favored. In both communities the same microorganism appeared dominating, suggesting a metabolic rather than a microbial competition response. Moreover, the presence of ammonium during polymer accumulation did not influence the maximum amount of PHA that was attained. Biotechnol. Bioeng. 2013;110: 3148–3155. © 2013 Wiley Periodicals, Inc.
Metabolic engineering of Saccharomyces cerevisiae for the production of 2‐phenylethanol via Ehrlich pathway
Authors: Kim Bosu , Cho Bo‐Ram , Hahn Ji‐Sook
Published: July 2013

2‐Phenylethanol (2‐PE), a fragrance compound with a rose‐like odor, is widely used in perfumery and cosmetics. Here, we report the first metabolic engineering approach for 2‐PE production in Saccharomyces cerevisiae. 2‐PE can be produced from the catabolism of L‐phenylalanine via Ehrlich pathway, consisting of transamination to phenylpyruvate by Aro9, decarboxylation to phenylacetaldehyde by Aro10, and reduction to 2‐PE by alcohol dehydrogenases. We demonstrated that Ald3 is mainly responsible for phenylacetaldehyde oxidation, competing with 2‐PE production. ALD3 deletion strain overexpressing ARO9 and ARO10 both by episomal overexpression and by induction of the endogenous genes through overexpression of Aro80 transcription factor, produced 4.8 g/L 2‐PE in a medium containing 10 g/L L‐phenylalanine as a sole nitrogen source. Considering the cytotoxicity of 2‐PE, this production titer is almost the upper limit that can be reached in batch cultures, suggesting the great potential of this yeast strain for 2‐PE production. 2‐PE production was further increased by applying two‐phase fermentation method with polypropylene glycol 1200 as an extractant, reaching 6.1 g/L 2‐PE in organic phase with the molar yield of 82.5%, which is about ninefold increase compared with wild type. Biotechnol. Bioeng. 2014;111: 115–124. © 2013 Wiley Periodicals, Inc.
Regulated expression of polysaccharide utilization and capsular biosynthesis loci in biofilm and planktonic Bacteroides thetaiotaomicron during growth in chemostats
Authors: TerAvest Michaela A. , He Zhen , Rosenbaum Miriam A. , Martens Eric C. , Cotta Michael A. , Gordon Jeffrey I. , Angenent Largus T.
Published: July 2013

Bacteroides thetaiotaomicron is a prominent member of the human distal gut microbiota that specializes in breaking down diet and host‐derived polysaccharides. While polysaccharide utilization has been well studied in B. thetaiotaomicron, other aspects of its behavior are less well characterized, including the factors that allow it to maintain itself in the gut. Biofilm formation may be a mechanism for bacterial retention in the gut. Therefore, we used custom GeneChips to compare the transcriptomes of biofilm and planktonic B. thetaiotaomicron during growth in mono‐colonized chemostats. We identified 1,154 genes with a fold‐change greater than 2, with confidence greater than or equal to 95%. Among the prominent changes observed in biofilm populations were: (i) greater expression of genes in polysaccharide utilization loci that are involved in foraging of O‐glycans normally found in the gut mucosa; and (ii) regulated expression of capsular polysaccharide biosynthesis loci. Hierarchical clustering of the data with different datasets, which were obtained during growth under a range of conditions in minimal media and in intestinal tracts of gnotobiotic mice, revealed that within this group of differentially expressed genes, biofilm communities were more similar to the in vivo samples than to planktonic cells and exhibited features of substrate limitation. The current study also validates the use of chemostats as an in vitro “gnotobiotic” model to study gene expression of attached populations of this bacterium. This is important to gut microbiota research, because bacterial attachment and the consequences of disruptions in attachment are difficult to study in vivo. Biotechnol. Bioeng. 2014;111: 165–173. © 2013 Wiley Periodicals, Inc.
Direct resolution and quantitative analysis of flurbiprofen enantiomers using microcrystalline cellulose triacetate plates: applications to the enantiomeric purity control and optical isomer determination in widely consumed drugs
Authors: Del Bubba M. , Checchini L. , Ciofi L. , Furlanetto S. , Lepri L.
Published: July 2013

Flurbiprofen enantiomers have very different pharmacological properties, since the (S)‐(+) form has a much higher anti‐inflammatory activity than the (R)‐(−) isomer, the latter being responsible for very undesirable side effects, such as gastrointestinal irritation. Based on the different biological properties of flurbiprofen enantiomers, the development of chiral chromatographic methods for the control of the enantiomeric purity is a very important topic. In this study the separation of flurbiprofen enantiomers was achieved using for the first time noncommercial MCTA layers with polyvinyl alcohol as binder, which gives to these plates a mechanical stability equivalent to that of marketed ones. Baseline resolution (α = 1.31; RS = 2.0) was obtained with ethanol–acetic acid solution (pH 3.0 ± 0.1; 60:40, v/v) as eluent and a migration distance of about 14.5 cm. Under these experimental conditions, the thin‐layer chromatography determination of the enantiomeric purity of the pharmacologically active (S)‐(+)‐flurbiprofen in the presence of 1% of the undesired (R)‐(−) form was demonstrated. Moreover, the quantitative analysis of flurbiprofen enantiomers was achieved, obtaining quantification limits and detection limits of 50 and 25 ng of each enantiomer applied to the plate, respectively. The method was succesfully applied to the enantiomer determination in widely consumed drugs, obtaining results consistent with the flurbiprofen content declared in the drug facts. Copyright © 2013 John Wiley & Sons, Ltd.
Kinetic Study on Polyethylenimine‐Assisted Reactive Crystallization of Monodisperse Strontium Sulfate Microcrystals
Authors: Mikami T. , Hirasawa I.
Published: July 2013

Double‐jet reactive crystallization of SrSO4 was carried out in the presence of polyethylenimine (PEI). A simple kinetic model of primary nucleation as well as crystal growth was investigated under the condition of producing monodisperse microcrystals. Furthermore, surface free energy in the solution of PEI was estimated. PEI addition causes growth inhibition leading to smaller sizes and modifies the Gibbs free energy gap required for occurring nucleation.
A Covalent Reporter of β‐Lactamase Activity for Fluorescent Imaging and Rapid Screening of Antibiotic‐Resistant Bacteria
Authors: Shao Qing , Zheng Yan , Dong Xueming , Tang Kai , Yan Xiaomei , Xing Bengang
Published: July 2013

Bacterial resistance to antibiotics poses a great clinical challenge in fighting serious infectious diseases due to complicated resistant mechanisms and time‐consuming testing methods. Chemical reaction‐directed covalent labeling of resistance‐associated bacterial proteins in the context of a complicated environment offers great opportunity for the in‐depth understanding of the biological basis conferring drug resistance, and for the development of effective diagnostic approaches. In the present study, three fluorogenic reagents LRBL1–3 for resistant bacteria labeling have been designed and prepared on the basis of fluorescence resonance energy transfer (FRET). The hydrolyzed probes could act as reactive electrophiles to attach the enzyme, β‐lactamase, and thus facilitated the covalent labeling of drug resistant bacterial strains. SDS electrophoresis and MALDI‐TOF mass spectrometry characterization confirmed that these probes were sensitive and specific to β‐lactamase and could therefore serve for covalent and localized fluorescence labeling of the enzyme structure. Moreover, this β‐lactamase‐induced covalent labeling provides quantitative analysis of the resistant bacterial population (down to 5 %) by high resolution flow cytometry, and allows single‐cell detection and direct observation of bacterial enzyme activity in resistant pathogenic species. This approach offers great promise for clinical investigations and microbiological research.
Synthesis, Chiroptical Properties and Density Functional Theory Calculations of 3,3’‐Biphenyl‐2,2’‐BiTropone
Authors: Cavazza Marino , Cifelli Mario , Domenici Valentina , Funaioli Tiziana , Mennucci Benedetta , Alberto Veracini Carlo , Zandomeneghi Maurizio
Published: July 2013

The synthesis of new bitropone derivatives, namely, 3,3'‐biphenyl‐2,2'‐bitropone and 7,7’‐biphenyl‐2,2'‐bitropone, are reported. Isolation of enantiomers arising from restricted rotation around the C‐C bond connecting the tropone moieties was attempted by means of chiral high performance liquid chromatography (HPLC). No separation was obtained for 7,7’‐biphenyl‐2,2'‐bitropone. For 3,3'‐biphenyl‐2,2'‐bitropone, difficulties were encountered because of the low separation factor of the peaks and the presence of a rapid racemization process. However, quantitative chiroptical data on the antipodes were obtained by linking a circular dichroism (CD) spectrometer and a UV–vis spectrophotometric detector in series to the HPLC instrument. The analysis of the CD and UV–vis spectra in terms of absolute conformations was done with the help of theoretical calculations performed at the Density Functional Theory (DFT) level. The most stable conformations of the 3,3'‐biphenyl‐2,2'‐bitropone in its ground state were obtained. Starting from these minimum energy conformations, it was possible to compute theoretical CD and UV absorption spectra that fit well with the experimental ones. From this comparison the absolute configuration to the antipodes was assigned. Finally, the effect of the presence of the two lateral phenyl substituents on the structure of the bitropone and hence on the CD spectrum is discussed. Chirality 25:648–655, 2013. © 2013 Wiley Periodicals, Inc.
Two‐Dimensional Nanostructures by the Assembly of n‐Type Tetraazaanthracene‐Based Conjugated Molecules
Authors: He Chunyang , Wu Dongqing , Zhang Fan , Xue Minzhao , Zhuang Xiaodong , Qiu Feng , Feng Xinliang
Published: July 2013

On the basis of our previous communication concerning a new family of thiophene‐armed tetraazaanthracene molecules, we present a further intensive investigation on this class of compounds substituted with different alkyl chains and their self‐assembled two‐dimensional (2D) nanostructures. These tetraazaanthracene molecules with different alkyl chains were prepared in good yields using the synthetic strategy we developed. In addition to the expected typical n‐type character, one compound exhibited aggregation behavior upon electrochemical reduction. Moreover, all molecules in the neutral state showed a strong tendency to aggregate in a binary solvent, as confirmed by optical spectral measurements. To investigate such self‐assembly behavior, a phase‐transfer method with a dichloromethane/methanol (2:3) binary solvent system was used to prepare the nanostructures. By means of atomic force microscopy, transmission electron microscopy, and X‐ray diffraction, we found that the morphology of assembled 2D sheet‐like structures could be adjusted by varying the alkyl chain. The weak interactions arising from the heteroatoms (N and S) in the conjugated backbones play a key role in the formation and stabilization of layered structures.
Homotropic Allosterism: In‐Depth Structural Analysis of the Gas‐Phase Noncovalent Complexes Associating a Double‐Cavity Cucurbit[n]uril‐Type Host and Size‐Selected Protonated Amino Compounds
Authors: Lemaur Vincent , Carroy Glenn , Poussigue Frédéric , Chirot Fabien , De Winter Julien , Isaacs Lyle , Dugourd Philippe , Cornil Jérôme , Gerbaux Pascal
Published: July 2013

Noncovalent interactions between several protonated amines and an original ditopic receptor, nor‐seco‐cucurbit[10]uril, are investigated by combining mass spectrometry‐based methods and computational chemistry. Electrospray ionization is used to transfer the intact supramolecular assemblies from their acidic solution to the gas phase, provided fine‐tuning of the source parameters is achieved. Ternary complexes, associating two guest molecules and one host cavity, are observed systematically in the mass spectrometry analyses and the quasi‐exclusive occurrence of these 2:1 associations reveals the allosteric nature of the complexation reaction. It is demonstrated that the binary 1:1 complex ions that are detected arise from collision‐induced dissociation processes undergone by the ternary complex ions inside the ion source. Based on ion mobility experiments supported by theoretical calculations, the inclusion nature of the gas‐phase ternary complexes is clearly evidenced independent of the size of the probed guest molecule and the charge state of the complex ions. The allosteric nature of the complexation reactions is dictated by size criteria. This is demonstrated on the basis of mass spectrometry experiments by analyzing solutions containing ligands of different sizes in competition for inclusion within the guest cavity. Computational chemistry is also used to characterize the three‐dimensional structures of the complexes.
ZnO Nanorod Arrays and Hollow Spheres through a Facile Room‐Temperature Solution Route and Their Enhanced Ethanol Gas‐Sensing Properties
Authors: Bao Di , Gao Peng , Wang Longqiang , Wang Ying , Chen Yujin , Chen Guorui , Li Guobao , Chang Cheng , Qin Wei
Published: July 2013

A new two‐phase solution strategy has been developed for the synthesis of multifarious zinc oxide one‐dimensional (1D) nanostructures, in which nanorod arrays (NAs), nanorod hollow spheres (NHSs), nanoribbons, nanowires, nanotubes, and nanonetworks were easily obtained at room temperature without using any catalysts, templates, or precursors. More importantly, an interesting formation mechanism of the 1D nanostructures in the benzene/water system and its distinctive size‐ and morphology‐controlling ability were also discovered. Through a series of directed comparison experiments, it was found that the zinc source, reactant concentration, substrate, and reaction time played significant roles in this dipolar binary liquid technique. In addition, and considering their importance to semiconductor ZnO gas‐sensing properties, the energy state and surface status of the as‐obtained NA and NHS products were investigated through photoluminescence and surface wetting measurements. It was found that a large concentration of oxygen vacancies and high surface energy were present on the surface of the NAs and NHSs, which resulted in their enhanced ethanol gas‐sensing properties at a relatively low temperature.
Formation, Molecular Structure, and Morphology of Humins in Biomass Conversion: Influence of Feedstock and Processing Conditions
Authors: van Zandvoort Ilona , Wang Yuehu , Rasrendra Carolus B. , van Eck Ernst R. H. , Bruijnincx Pieter C. A. , Heeres Hero J. , Weckhuysen Bert M.
Published: July 2013

Neither the routes through which humin byproducts are formed, nor their molecular structure have yet been unequivocally established. A better understanding of the formation and physicochemical properties of humins, however, would aid in making biomass conversion processes more efficient. Here, an extensive multiple‐technique‐based study of the formation, molecular structure, and morphology of humins is presented as a function of sugar feed, the presence of additives (e.g., 1,2,4‐trihydroxybenzene), and the applied processing conditions. Elemental analyses indicate that humins are formed through a dehydration pathway, with humin formation and levulinic acid yields strongly depending on the processing parameters. The addition of implied intermediates to the feedstocks showed that furan and phenol compounds formed during the acid‐catalyzed dehydration of sugars are indeed included in the humin structure. IR spectra, sheared sum projections of solid‐state 2DPASS 13C NMR spectra, and pyrolysis GC–MS data indicate that humins consist of a furan‐rich polymer network containing different oxygen functional groups. The structure is furthermore found to strongly depend on the type of feedstock. A model for the molecular structure of humins is proposed based on the data presented.
Small‐block interleaving for low‐delay cross‐packet forward error correction over burst‐loss channels
Authors: Shih Chi‐Huang , Kuo Chun‐I , Shieh Ce‐Kuen , Chou Yeh‐Kai
Published: July 2013

By adding the redundant packets into source packet block, cross‐packet forward error correction (FEC) scheme performs error correction across packets and can recover both congestion packet loss and wireless bit errors accordingly. Because cross‐packet FEC typically trades the additional latency to combat burst losses in the wireless channel, this paper presents a FEC enhancement scheme using the small‐block interleaving technique to enhance cross‐packet FEC with the decreased delay and improved good‐put. Specifically, adopting short block size is effective in reducing FEC processing delay, whereas the corresponding effect of lower burst‐error correction capacity can be compensated by deliberately controlling the interleaving degree. The main features include (i) the proposed scheme that operates in the post‐processing manner to be compatible with the existing FEC control schemes and (ii) to maximize the data good‐put in lossy networks; an analytical FEC model is built on the interleaved Gilbert‐Elliott channel to determine the optimal FEC parameters. The simulation results show that the small‐block interleaved FEC scheme significantly improves the video streaming quality in lossy channels for delay‐sensitive video. Copyright © 2013 John Wiley & Sons, Ltd.
Identification of (2‐aminopropyl)indole positional isomers in forensic samples
Authors: Scott Kenneth R. , Power John D. , McDermott Seán D. , O'Brien John E. , Talbot Brian N. , Barry Michael G. , Kavanagh Pierce V.
Published: July 2013

In 2012, 5‐(2‐aminopropyl)indole (5‐API, 5‐IT) was reported by Norwegian authorities to the European Monitoring Centre for Drugs and Drug Addiction (EMCDDA) via the Early Warning System (EWS). The 3‐ isomer, 3‐(2‐aminopropyl)indole (3‐API, AMT, alpha‐methyltryptamine), has been available on the recreational drugs market for a somewhat longer time, having first been reported to the EMCDDA by Finnish authorities in 2001. Both isomers are available from online vendors of ‘legal highs’. Recently, three forensic drug cases (two tablets and one powder) were presented for routine analysis and the active constituent was tentatively identified as an API isomer. The six positional isomers (2‐, 3‐, 4‐, 5‐, 6‐ and 7‐(2‐aminopropyl)indoles) were synthesized and analyses by a combination gas chromatography–mass spectrometry (GC‐MS), and liquid chromatography‐mass spectrometry (LC‐MS) showed that these could be readily discriminated thus facilitating the identification of 3‐API in the tablets and 5‐API in the powder. With exception of 5‐ and 6‐APIs, which co‐eluted, it was found possible to separate the isomers by GC without derivatization. LC separation also proved to be a feasible method for the discrimination of the isomers. Although the 2‐ and 7‐ isomers were not fully resolved by LC, it was found possible to distinguish them using their product ion spectra as the 2‐ isomer produced the m/z 132 fragment ion formed by loss of vinylamine, whereas the 7‐ isomer formed m/z 158 through loss of methylamine. In the synthesis 2‐API, a novel tricyclic by‐product was formed in an annulation reaction where the reaction solvent, tetrahydrofuran, was incorporated into the molecule. Copyright © 2013 John Wiley & Sons, Ltd.
Direct Synthesis of 2,5‐Bis(dodecanoxy)phenyleneethynylene‐Butadiynes by Sonogashira Coupling Reaction
Authors: Arias Eduardo , Moggio Ivana , Torres Román , Ziolo Ronald F. , Maldonado José‐Luis , Green Kirk , Cooper Thomas M. , Wicks Geoffrey , Rebane Aleksander , Drobizhev Mikhail , Makarov Nikolay S. , Ottonelli Massimo , Dellepiane Giovanna
Published: July 2013

The synthesis of a 2,5‐bis(dodecanoxy)phenyleneethynylene‐butadiyne series with 2, 4, 6 and 8 phenyl rings is reported. Sonogashira coupling reaction, rather than the Glaser/Eglinton/Hay reactions classically used for butadiyne formation was applied. The molecular structures of all compounds were confirmed by 1H, DEPT‐135, APT 13C, MALDI‐TOF, FTIR and FT‐Raman analyses. The linear and nonlinear optical properties were studied in solution by UV/Vis, static and time‐resolved fluorescence, and by two‐photon absorption (2PA) spectroscopy. With the exception of the dimer, for which intersystem crossing is very favoured due to the low energy gap between the singlet and triplet states as theoretically predicted, the other oligomers present high fluorescence quantum yields (0.77–0.82) and large cross‐sections (up to 5000 GM for the octamer) that could be applied in multiphoton microscopy or nonlinear optics.