bluuebunny/crossref_metadata_2025_split huggingface dataset:
n‐Channel Organic Semiconductors Derived from Air‐Stable Four‐Coordinate Boron Complexes of Substituted Thienylthiazoles
Authors: Hecht Reinhard , Kade Juliane , Schmidt David , Nowak‐Król Agnieszka 
Published: June 2017

AbstractThree acceptor‐π‐bridge‐acceptor (A‐π‐A) molecules derived from 2‐(3‐boryl‐2‐thienyl)thiazole have been synthesized and thoroughly characterized. Incorporation of a B−N unit into thienylthiazole and attachment of suitable acceptor moieties allowed to obtain ambient‐stable A‐π‐A molecules with low‐lying LUMO levels. Their potential for applications in organic electronics was tested in vacuum‐deposited organic thin film transistors (OTFT). The OTFT device based on boryl‐thienylthiazole and 1,1‐dicyanomethylene‐3‐indanone (DCIND) acceptor moieties showed an electron mobility of ≈1.4×10−2 cm2 V−1 s−1 in air, which is the highest electron mobility reported to date for organoboron small molecules. Conversely, the device employing the malononitrile (MAL) derivative as an active layer did not show any charge transport behavior. As suggested by single crystal X‐ray analysis of indandione (IND) and MAL derivatives, the enhanced mobility of IND (and DCIND) in comparison to the MAL molecule can be attributed to the effective two‐dimensional π‐stacking in the solid state imparted by the acceptor moieties with an extended π‐surface.
Self‐Assembled Polymeric Ionic Liquid‐Functionalized Cellulose Nano‐crystals: Constructing 3D Ion‐conducting Channels Within Ionic Liquid‐based Composite Polymer Electrolytes
Authors: Shi Qing Xuan , Xia Qing , Xiang Xiao , Ye Yun Sheng , Peng Hai Yan , Xue Zhi Gang , Xie Xiao Lin , Mai Yiu‐Wing 
Published: June 2017

AbstractComposite polymeric and ionic liquid (IL) electrolytes are some of the most promising electrolyte systems for safer battery technology. Although much effort has been directed towards enhancing the transport properties of polymer electrolytes (PEs) through nanoscopic modification by incorporating nano‐fillers, it is still difficult to construct ideal ion conducting networks. Here, a novel class of three‐dimensional self‐assembled polymeric ionic liquid (PIL)‐functionalized cellulose nano‐crystals (CNC) confining ILs in surface‐grafted PIL polymer chains, able to form colloidal crystal polymer electrolytes (CCPE), is reported. The high‐strength CNC nano‐fibers, decorated with PIL polymer chains, can spontaneously form three‐dimensional interpenetrating nano‐network scaffolds capable of supporting electrolytes with continuously connected ion conducting networks with IL being concentrated in conducting domains. These new CCPE have exceptional ionic conductivities, low activation energies (close to bulk IL electrolyte with dissolved Li salt), high Li+ transport numbers, low interface resistances and improved interface compatibilities. Furthermore, the CCPE displays good electrochemical properties and a good battery performance. This approach offers a route to leak‐free, non‐flammable and high ionic conductivity solid‐state PE in energy conversion devices.
A Multiply Bonded Trigonal‐Planar Bismuth(III) Complex: Prodigious Lewis Acidity, Solvatochromism, Etherification, and Semiconducting Characteristics
Authors: Shieh Minghuey , Yu Chia‐Chi , Hsing Kai‐Jieah , Chang Wei‐Jie 
Published: June 2017

AbstractThe formation of a hitherto unknown 4‐center, 6π–conjugated trigonal‐planar complex, [Bi{Cr(CO)5}3]−(1), is reported, in which the oxidation state of the Bi atom is +3, as evidenced by XAS, XPS, and DFT calculations. The BiIIIatom in1has dual donor and acceptor properties in its bonding mode. In contrast to the mild Lewis acidity of BiIII, the central Bi in1functions as a prodigious Lewis acid site to exhibit strong affinity toward F−ions, unique solvatochromic properties, intriguing etherification through the C−O bond cleavage of alcohols, and surprising semiconducting characteristics with an ultra‐narrow optical band gap of 1.02 eV, which can be attributed to the intermolecular Bi⋅⋅⋅O and O⋅⋅⋅O interactions in the solid state. The tetrahedral Fe(CO)4‐adduct [{Fe(CO)4}Bi{Cr(CO)5}3]3−(1‐Fe) allowed the selective demetallation to afford the isoelectronic multiply bonded BiCr3‐complex1and the BiCr2Fe‐complex, [Bi{Cr(CO)5}2{Fe(CO)4}]−(2), which may open a novel pathway for the design of the heterometal‐incorporated trigonal‐planar Bi‐Cr complexes.
Investigations on Gold‐Catalyzed Thioalkyne Activation Toward Facile Synthesis of Ketene Dithioacetals
Authors: Ye Xiaohan , Wang Jin , Ding Shengtao , Hosseyni Seyedmorteza , Wojtas Lukasz , Akhmedov Novruz G. , Shi Xiaodong 
Published: June 2017

AbstractNucleophilic addition to thioalkynes was investigated under various catalytic conditions with gold(I) complexes being identified as the optimal catalysts. Structural evaluation of the product revealed an unexpected cis‐addition, arising from a gold‐associated thioketene intermediate. Based on this interesting mechanistic insight, a gold(I)‐catalyzed thioether addition to thioalkynes was developed as a novel approach to prepare ketene dithioacetals with good yields and high efficiency.
ESC sudden‐death risk model in hypertrophic cardiomyopathy: Incremental value of quantitative contrast‐enhanced CMR in intermediate‐risk patients
Authors: Hinojar Rocio , Zamorano José Luis , Gonzalez Gómez Ariana , Plaza Martin Maria , Esteban Amparo , Rincón Luis Miguel , Portugal Juan Carlos , Jimenez Nácher José Julio , Fernández‐Golfín Covadonga 
Published: June 2017

BackgroundHypertrophic cardiomyopathy (HCM) remains the most common cause of sudden cardiac death (SCD) in the young; however, current strategies do not identify all HCM patients at risk. A novel validated algorithm was proposed by the last European Society of Cardiology guidelines to guide implantable cardioverter‐defibrillator (ICD) therapy. Recently, extensive myocardial fibrosis was independently associated with increased risk of SCD events. This study aimed to establish the relation between myocardial fibrosis (late gadolinium enhancement [LGE] extension) and the novel SCD risk‐prediction model in a real population of HCM to evaluate its potential additional value in the different risk groups.HypothesisThere is a significant association between LGE extension and the novel SCD risk calculator that may help conflicting ICD decisions.MethodsSeventy‐seven patients with HCM underwent routine clinical evaluation, echocardiography, and cardiac magnetic resonance study. Their SCD risk at 5 years was calculated using the new model.ResultsExtension of LGE positively correlated with SCD risk prediction (r = 0.7, P < 0.001). Low‐, intermediate‐, and high‐risk groups according to the model showed significantly different extent of LGE (5% ± 6% vs 18% ± 9% vs 17% ± 4%; P < 0.001). Four patients (6%) in the low‐risk group and 5 (62%) in the intermediate‐risk group showed extensive areas of LGE. All patients except 1 (86%) at highest risk (n = 6) showed extensive areas of LGE.Conclusions
LGE extension is concordant with the novel SCD‐risk model defining low‐ and high‐risk groups; it may provide additional information, allowing better discrimination to support implantable cardioverter‐defibrillator decision. LGE quantification holds promise for SCD stratification in HCM.
Long‐Time Asymptotics for the Focusing Nonlinear Schrödinger Equation with Nonzero Boundary Conditions at Infinity and Asymptotic Stage of Modulational Instability
Authors: Biondini Gino , Mantzavinos Dionyssios 
Published: June 2017

AbstractWe characterize the long‐time asymptotic behavior of the focusing nonlinear Schrödinger (NLS) equation on the line with symmetric, nonzero boundary conditions at infinity by using a variant of the recently developed inverse scattering transform (IST) for such problems and by employing the nonlinear steepest‐descent method of Deift and Zhou for oscillatory Riemann‐Hilbert problems. First, we formulate the IST over a single sheet of the complex plane without introducing the uniformization variable that was used by Biondini and Kovačič in 2014. The solution of the focusing NLS equation with nonzero boundary conditions is thereby associated with a matrix Riemann‐Hilbert problem whose jumps grow exponentially with time for certain portions of the continuous spectrum. This growth is the signature of the well‐known modulational instability within the context of the IST. We then eliminate this growth by performing suitable deformations of the Riemann‐Hilbert problem in the complex spectral plane. The results demonstrate that the solution of the focusing NLS equation with nonzero boundary conditions remains bounded at all times. Moreover, we show that, asymptotically in time, the xt‐plane decomposes into two types of regions: a left far‐field region and a right far‐field region, where the solution equals the condition at infinity to leading order up to a phase shift, and a central region in which the asymptotic behavior is described by slowly modulated periodic oscillations. Finally, we show how, in the latter region, the modulus of the leading‐order solution, initially obtained as a ratio of Jacobi theta functions, can be reduced to the well‐known elliptic solutions of the focusing NLS equation. These results provide the first characterization of the long‐time behavior of generic perturbations of a constant background in a modulationally unstable medium. © 2017 Wiley Periodicals, Inc.
Optimizing update scheduling parameters for distributed virtual environments supporting operational test
Authors: Millar Jeremy Robert , Hodson Douglas , Peterson Gilbert , Ahner Darryl 
Published: June 2017

SummaryDistributed virtual environments provide a shared sense of time and space to geographically distributed users. They depend on a limited ability to ensure system nodes at different locations maintain consistent state data. This paper presents system models and algorithms designed to find optimal update scheduling parameters that minimize the effects of inconsistent simulation state data. The first model is concerned with ensuring distributed virtual environments that present a fair experience to all users while simultaneously providing adequate levels of system performance. In the second model, we introduce the concept of plausibility limits and address their use in ensuring all participants in an interaction to see the same result.
Photo‐Switchable Self‐Assemblies Based on Thymine‐Containing Bolaamphiphiles
Authors: Al‐Shereiqi Ahmed S. , Boyd Ben J. , Saito Kei 
Published: June 2017

AbstractThe photoswitching of photosensitive bolaamphiphiles based on thymine was investigated. Topochemical principles were applied to create light‐responsive supra‐amphiphiles by the utilisation of dynamic covalent bonds created by the photo‐dimerisation of a DNA base, thymine. In order to induce the photo‐dimerisation of thymine, two bolaamphiphilic molecules were designed and synthesised to meet the required [2 π+2 π] photo‐cycloaddition conditions. The amphiphiles were synthesised with different spacers and their photo‐reversibility and morphologies were studied by using UV/Vis, NMR and infrared spectroscopy, rheometry, dynamic light scattering and transmission electron microscopy.
Enhanced Interfacial Charge Transfer on a Tungsten Trioxide Photoanode with Immobilized Molecular Iridium Catalyst
Authors: Tong Haili , Jiang Yi , Zhang Qian , Li Jialing , Jiang Wenchao , Zhang Donghui , Li Na , Xia Lixin 
Published: June 2017

AbstractThe rational design of active photoanodes for photoelectrochemical (PEC) water splitting is crucial for future applications in sustainable energy conversion. A combination of catalysts with photoelectrodes is generally required to improve surface kinetics and suppress surface recombination. In this study, we present WO3 photoanode modified with the iridium complex [(H4dphbpy)IrIII(Cp*)Cl]Cl (Ir‐PO3H2; H4dphbpy=2,2′‐bipyridine‐4,4′‐bisphosphonic acid, Cp*=pentamethylcyclopentadiene (WO3+Ir‐PO3H2)‐ for PEC water oxidation. When Ir‐PO3H2 is anchored to a WO3 electrode, the photoanode shows a significant improvement in both photocurrent and faradaic efficiency compared to the bare WO3 photoanode. Under simulated sunlight illumination (AM 1.5G, 100 mW cm−2) with an applied bias of 1.23 V (vs. reversible hydrogen electrode), the photoanode exhibits a photocurrent of 1.16 mA cm−2 in acidic conditions, which is double that of the bare WO3 photoanode. The faradaic efficiency is promoted from 56 % to 95 %. Kinetic studies reveal that Ir‐PO3H2 exhibits a different interfacial charge‐transfer mechanism on the WO3 photoanode for PEC water oxidation compared to iridium oxide. Ir‐PO3H2, as a water‐oxidation catalyst, can accelerate the surface charge transfer through rapid surface kinetics.
Copper‐Catalyzed Oxidative Dehydrogenative C(sp3)−H Bond Amination of (Cyclo)Alkanes using NH‐Heterocycles as Amine Sources
Authors: Wang Chang‐Sheng , Wu Xiao‐Feng , Dixneuf Pierre H. , Soulé Jean‐François 
Published: June 2017

AbstractA copper‐catalyzed oxidative C(sp3)−H/N−H coupling of NH‐heterocycles with affordable (cyclo)alkanes has been developed. This procedure involves C(sp3)−N bond formation through a radical pathway generated by homolytic cleavage of di‐tert‐butyl peroxide and trapping of the radical(s) by copper catalysts. The reaction tolerates a series of functional groups, such as bromo, fluoro, ester, ketone, nitrile, methyl, and methoxy. free‐NH‐containing indoles, pyrroles, pyrazoles, indazoles, and benzotriazoles are successfully N‐alkylated.
Mechanochemical Ring‐Opening Polymerization of Lactide: Liquid‐Assisted Grinding for the Green Synthesis of Poly(lactic acid) with High Molecular Weight
Authors: Ohn Nuri , Shin Jihoon , Kim Sung Sik , Kim Jeung Gon 
Published: June 2017

AbstractMechanochemical polymerization of lactide is carried out by using ball milling. Mechanical energy from collisions between the balls and the vessel efficiently promotes an organic‐base‐mediated metal‐ and solvent‐free solid‐state polymerization. Investigation of the parameters of the ball‐milling synthesis revealed that the degree of lactide ring‐opening polymerization could be modulated by the ball‐milling time, vibration frequency, mass of the ball media, and liquid‐assisted grinding. Liquid‐assisted grinding was found to be an especially important factor for achieving a high degree of mechanochemical polymerization. Although polymer‐chain scission from the strong collision energy prevented mechanical‐force‐driven high‐molecular‐weight polymer synthesis, the addition of only a small amount of liquid enabled sufficient energy dissipation and poly(lactic acid) was thereby obtained with a molecular weight of over 1×105 g mol−1.
Autonomy support and autonomous motivation in the outpatient treatment of adults with an eating disorder
Authors: Steiger Howard , Sansfaçon Jeanne , Thaler Lea , Leonard Niamh , Cottier Danaëlle , Kahan Esther , Fletcher Emilie , Rossi Erika , Israel Mimi , Gauvin Lise 
Published: June 2017

AbstractObjectiveAcross diverse clinical problems, therapists’ autonomy support has been found to increase patients’ autonomous motivation for change. Being self‐motivated has, in turn, been linked to superior treatment response. In people undergoing outpatient eating disorder (ED) treatment, we examined associations among ratings of autonomy support received from therapists and other carers, self‐reported engagement in therapy, and clinical outcomes.MethodNinety‐seven women with anorexia nervosa, bulimia nervosa, or a related ED provided measures of motivational status and clinical symptoms at the beginning and end of time‐limited (12–16 weeks) segments of specialized treatment. At mid‐treatment, patients also rated the extent to which they perceived their individual therapists, group therapists, group‐therapy peers, family members, friends, and romantic partners as being autonomy supportive.ResultsOverall, multiple regression analyses indicated autonomy support to moderate (rather than mediate) the link between initial autonomous motivation and later change in autonomous motivation—with results indicating that, independently of ED diagnosis or treatment intensity, greater perceived autonomy support (from therapists and nontherapists alike) coincided with larger increases in autonomous motivation over the course of therapy. In turn, higher autonomous motivation at end‐of‐therapy coincided with larger reductions in eating symptoms.DiscussionFindings suggest that the experience of autonomy support (from therapists and nontherapists) is associated with increasing motivation in people undergoing ED treatment, and that becoming self‐motivated is linked to better outcomes. Such results indicate that support from therapists, relatives, and peers can favorably influence personal engagement in individuals undergoing ED treatment.
The Roles of Residents in Climate Adaptation: A systematic review in the case of the Netherlands
Authors: Hegger Dries L.T. , Mees Heleen L.P. , Driessen Peter P.J. , Runhaar Hens A.C. 
Published: June 2017

AbstractClimate adaptation literature has hitherto devoted limited attention to the roles of residents. Yet their role is crucial in addressing non‐ or maladaptation, as their initiative or consent is often necessary to take adaptation measures in or around the house. To address this knowledge gap, this paper explores mainstream and additional roles for residents through a literature review. Mainstream roles are those roles that residents usually take, while additional roles are more specific and local in nature. The latter may, however, provide the seeds for wider change. To structure the results, we made a distinction between three forms of residents' commitment to adaptation: as (1) citizens falling under the jurisdiction of various governmental levels; (2) consumers (including home owners) in the market; and (3) civil society members/partners. While this is an established categorization in other domains of environmental governance, it has not yet been systematically applied to the adaptation domain. The paper's empirical focus regarding mainstream and additional roles is on the Dutch adaptation domains of flood risk management, stormwater management and dealing with heat stress. We found scope for additional roles for residents, especially as consumers in the market and civil society members. The findings are of significance for the global debate on residents' roles in climate adaptation and suggest that addressing all three forms of commitment may enhance the implementation of measures as well as their legitimacy, residents' awareness and societies' potential to innovate. Copyright © 2017 John Wiley & Sons, Ltd and ERP Environment
Partial coalescence in double (W1/O/W2) emulsions prepared with skimmed milk, polyglycerol polyricinoleate, and different fats
Authors: Pérez María P. , Wagner Jorge R. , Márquez Andrés L. 
Published: June 2017

Partial coalescence was studied in double (W1/O/W2) emulsions prepared with skimmed milk, polyglycerol polyricinoleate (PGPR) as lipophilic emulsifier, and different fats. Microstructural and rheological analyses were performed. Encapsulation efficiency (as a parameter of inner water retention) and solid fat content were estimated by differential scanning calorimetry. The presence of PGPR in dispersed lipid phase promoted partial coalescence especially at higher concentration. This promotion of partial coalescence may have been produced by the increase of collision frequency due to protein displacement by PGPR at the outer interface and/or the increase of capture efficiency due to the modification of fat crystals by PGPR. Partial coalescence was also favored when inner water droplets were released as a consequence of an osmotic unbalance between inner and outer aqueous phases. Thus, the addition of glucose in dispersed aqueous phase decreased the partial coalescence degree due to the higher encapsulation efficiency given by the balanced osmotic pressures. With respect to the effect of the employed fat on partial coalescence, the obtained data indicate that the phenomenon was favored at higher solid fat content in lipid phase. Results led to the conclusion that inner osmolality, encapsulation efficiency, and inhibition of partial coalescence were correlated.Practical applications: The originality of this work resides on boarding the subject of partial coalescence in W1/O/W2 emulsions. The studied systems are proposed as potential lipid‐reduced substitutes of dairy creams, with the employment of alternative non‐dairy fats such as low trans vegetable fat. The combined analysis of partial coalescence and encapsulation efficiency allowed studying their reciprocal effects and evaluating the potentiality of the systems for the encapsulation of hydrophilic compounds. The variations of relative osmotic pressures in inner and outer aqueous phases, lipophilic emulsifier concentration, and solid fat content may lead to desirable or undesirable rheological properties depending on the required texture of the food emulsion. The findings of this work could be an important step pointing to control the factors leading to partial coalescence in W1/O/W2 emulsions for food applications.The stability against partial coalescence in W1/O/W2 emulsions containing polyglycerol polyricinoleate (PGPR) and solid fat in lipid phase is linked to the retention of inner water droplets or the encapsulation efficiency of the system. The higher the inner osmolality the higher the encapsulation efficiency; and the higher the encapsulation efficiency the lower the partial coalescence degree. This aggregation of fat globules is attributed to the increase of collision frequency due to protein displacement by PGPR at the outer interface and/or the increase of capture efficiency due to the modification of fat crystals by PGPR.
Improving substance information in USEtox®, part 1: Discussion on data and approaches for estimating freshwater ecotoxicity effect factors
Authors: Saouter Erwan , Aschberger Karin , Fantke Peter , Hauschild Michael Z. , Bopp Stephanie K. , Kienzler Aude , Paini Alicia , Pant Rana , Secchi Michela , Sala Serenella 
Published: June 2017

Abstract

The scientific consensus model USEtox® is recommended by the European Commission as the reference model to characterize life cycle chemical emissions in terms of their potential human toxicity and freshwater aquatic ecotoxicity impacts in the context of the International Reference Life Cycle Data System Handbook and the Environmental Footprint pilot phase looking at products (PEF) and organizations (OEF). Consequently, this model has been systematically used within the PEF/OEF pilot phase by 25 European Union industry sectors, which manufacture a wide variety of consumer products. This testing phase has raised some questions regarding the derivation of and the data used for the chemical-specific freshwater ecotoxicity effect factor in USEtox. For calculating the potential freshwater aquatic ecotoxicity impacts, USEtox bases the effect factor on the chronic hazard concentration (HC50) value for a chemical calculated as the arithmetic mean of all logarithmized geometric means of species-specific chronic median lethal (or effect) concentrations (L[E]C50). We investigated the dependency of the USEtox effect factor on the selection of ecotoxicological data source and toxicological endpoints, and we found that both influence the ecotoxicity ranking of chemicals and may hence influence the conclusions of a PEF/OEF study. We furthermore compared the average measure (HC50) with other types of ecotoxicity effect indicators, such as the lowest species EC50 or no-observable-effect concentration, frequently used in regulatory risk assessment, and demonstrated how they may also influence the ecotoxicity ranking of chemicals. We acknowledge that these indicators represent different aspects of a chemical's ecotoxicity potential and discuss their pros and cons for a comparative chemical assessment as performed in life cycle assessment and in particular within the PEF/OEF context. Environ Toxicol Chem 2017;36:3450–3462. © 2017 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals, Inc. on behalf of SETAC.