bluuebunny/crossref_metadata_2025_split huggingface dataset:
The horizontal heat advection in the Middle Atlantic Bight and the cross‐spectral interactions within the heat advection
Authors: Sha Jin , Yan Xiao‐Hai , Li Xiaoming 
Published: June 2017

AbstractThe upper ocean horizontal heat advection over the middle and outer shelf of the Middle Atlantic Bight (MAB) is investigated using satellite and in situ observations. In the upper mixed layer, the heat advection is mostly positive indicating that it decreases the shelf heat content by bringing cold water from upstream. The domain‐averaged heat advection driven by the barotropic geostrophic current is one‐order larger relative to the density‐driven geostrophic shear and the wind‐driven current. The barotropic geostrophic advection components in the alongshore and offshore direction are of the same order. To investigate the temporal properties of the heat advection, the temperature and currents are decomposed into different time scales using Fast Multidimensional Ensemble Empirical Decomposition (FMEEMD). The cross‐spectral interactions within the advection are quantitatively evaluated with major components identified. Due to the cross‐spectral interaction, energy within the heat advection is found to be redistributed through different time scales, with at least 46.5% variation retained within the original band for the barotropic geostrophic advection. Our results help to better understand the temporal variability of the heat advection, provide a baseline of the nonlinear energy transfer framework within different time scales in the heat advection, and imply the possibility of interplays between short and long‐term oceanic phenomena.
Antarctic boundary layer parametrization in a general circulation model: 1‐D simulations facing summer observations at Dome C
Authors: Vignon Etienne , Hourdin Frédéric , Genthon Christophe , Gallée Hubert , Bazile Eric , Lefebvre Marie‐Pierre , Madeleine Jean‐Baptiste , Van de Wiel Bas J. H. 
Published: June 2017

AbstractThe parametrization of the atmospheric boundary layer (ABL) is critical over the Antarctic Plateau for climate modelling since it affects the climatological temperature inversion and the negatively buoyant near‐surface flow over the ice‐sheet. This study challenges state‐of‐the‐art parametrizations used in general circulation models to represent the clear‐sky summertime diurnal cycle of the ABL at Dome C, Antarctic Plateau. The Laboratoire de Météorologie Dynamique‐Zoom model is run in a 1‐D configuration on the fourth Global Energy and Water Cycle Exchanges Project Atmospheric Boundary Layers Study case. Simulations are analyzed and compared to observations, giving insights into the sensitivity of one model that participates to the intercomparison exercise. Snow albedo and thermal inertia are calibrated leading to better surface temperatures. Using the so‐called “thermal plume model” improves the momentum mixing in the diurnal ABL. In stable conditions, four turbulence schemes are tested. Best simulations are those in which the turbulence cuts off above 35 m in the middle of the night, highlighting the contribution of the longwave radiation in the ABL heat budget. However, the nocturnal surface layer is not stable enough to distinguish between surface fluxes computed with different stability functions. The absence of subsidence in the forcings and an underestimation of downward longwave radiation are identified to be likely responsible for a cold bias in the nocturnal ABL. Apart from model‐specific improvements, the paper clarifies on which are the critical aspects to improve in general circulation models to correctly represent the summertime ABL over the Antarctic Plateau.
Mechanical, thermal and accelerated weathering studies of bio‐based polyurethane/clay nanocomposites coatings
Authors: Kalita Hemjyoti , Kamila Rashmirekha , Mohanty Smita , Nayak Sanjay Kumar 
Published: June 2017

AbstractBiobased polymer has taken tremendous attention in recent times. In the present study bio‐based polyurethane have been synthesized from the vegetable oil i.e., dehydrated castor oil, 1,4‐butanediol and isophorone diisocyanate in presence of a catalyst by solution polymerization method. Then polyurethane nanocomposites were synthesized using different amount of nanoclay (C30B) (1, 3 and 5 wt%). The synthesis of polyurethane and its nanocomposites were confirmed by FTIR and XRD analysis. The mechanical properties such as tensile strength (2.2–4.5 MPa), elongation at break (299%–435%) hardness (46–70) and abrasion resistance (351–201 mg/1,000 cycles) increased with the increase of nanoclay content. The initial thermal degradation temperature found to increase from (220 to 290°C) with the increase of nanoclay content in the nanocomposites. The nanoclay was interacted with the hard segment of the matrix polymer as reflected from the atomic force microscopy studies. Weathering study revealed that nanocomposites have higher weather resistance capacity than pristine polyurethane. It can be concluded that the prepared nanocomposites might be good outdoor topcoat materials.
The Importance of Confined Sulfur Nanodomains and Adjoining Electron Conductive Pathways in Subreaction Regimes of Li‐S Batteries
Authors: Park Jungjin , Kim Eui Tae , Kim Chunjoong , Pyun Jeffrey , Jang Hyung‐Seok , Shin Jaeho , Choi Jang Wook , Char Kookheon , Sung Yung‐Eun 
Published: June 2017

AbstractPolysulfide dissolution into the electrolyte and poor electric conductivity of elemental sulfur are well‐known origins for capacity fading in lithium–sulfur batteries. Various smart electrode designs have lately been introduced to avoid these fading mechanisms, most of which demonstrate significantly improved cycle life. Nevertheless, an in‐depth understanding on the effect of sulfur microstructure and nanoscale electron transport near sulfur is currently lacking. In this study, the authors report an organized nanocomposite comprising linear sulfur chains and oleylamine‐functionalized reduced graphene oxide (O‐rGO) to achieve robust cycling performance (81.7% retention after 500 cycles) as well as to investigate the reaction mechanism in different regimes, i.e., S8 dissolution, polysulfide conversion, and Li2S formation. In the nanocomposite, linear sulfur chains terminate with 1,3‐diisopropylbenzene are covalently linked to O‐rGO. The comparison with control samples that do not contain either the capping of sulfur chains or O‐rGO reveals the synergistic interplay between both treatments, simultaneously unveiling the distinct roles of confined sulfur nanodomains and their adjoining electron pathways in different reaction regimes.
Oxidation State Dichotomy in Copper‐Catalyzed Intramolecular Cyclization of α‐Diazoanilides: An Integrated Synthetic Platform for Oxindoles and Isatins Enabled by Oxygenase‐Type Reactivity
Authors: Garg Parul , Jadhav Santosh D. , Singh Anand 
Published: June 2017

AbstractA ligand‐free, copper‐catalyzed divergent route toward oxindoles and isatins from a common α‐diazoanilide precursor is reported. The reaction offers a broad scope, provides an efficient catalytic synthesis protocol that is mild, involves only oxygen as an oxidant, and unique in its ability to provide either oxindoles or isatins by exploiting oxygenase‐type reactivity that does not require peroxide additives or sacrificial aldehydes. The versatility of this reaction manifold has been demonstrated by synthesizing an analog of sunitinib, an FDA approved drug for renal cell carcinoma and imatinib‐resistant gastrointestinal stromal tumor.
The Late Neandertal permanent lower left third premolar from Walou Cave (Trooz, Belgium) and its context
Authors: Toussaint Michel , Verna Christine , Le Cabec Adeline , Gómez‐Robles Aida , Draily Christelle , Richards Michael P. , Pirson Stéphane 
Published: June 2017

AbstractObjectivesWe describe a hominin permanent lower left third premolar unearthed in 1997 at Walou Cave (Belgium), found in direct association with a Mousterian lithic industry, in a layer directly dated to 40–38,000 years BP.Materials and methodsThe taxonomical attribution of the tooth is addressed through comparative morphometric analyses, and stable isotope analyses aimed at determining the diet of the individual.ResultsThe Walou P3 plots within the Neandertal range of variation and is significantly different from recent modern humans in all morphometric assessments. The isotope data showed that like other Neandertals, the Walou individual acquired its dietary proteins primarily from terrestrial food sources.DiscussionWe discuss the implications of the existence of a clearly Neandertal premolar dating to the period of the Middle to Upper Paleolithic transition in the Meuse river basin.
Inorganic‐Macroion‐Induced Formation of Bicontinuous Block Copolymer Nanocomposites with Enhanced Conductivity and Modulus
Authors: Zhang Liying , Cui Tingting , Cao Xiao , Zhao Chengji , Chen Quan , Wu Lixin , Li Haolong 
Published: June 2017

AbstractA facile and electrostatically driven approach has been developed to prepare bicontinuous polymer nanocomposites that is based on the polyoxometalate (POM) macroion induced phase transition of PS‐b‐P2VP from an initial lamellar phase to a stable bicontinuous phase. The multi‐charged POMs can electrostatically cross‐link P2VP blocks and give rise to bicontinuous phases in which the POM hybrid conductive domains occupy a large volume fraction of more than 50 %. Furthermore, the POMs can give rise to high proton conductivity and serve as nanoenhancers, endowing the bicontinuous nanocomposites with a conductivity of 0.1 mS cm−1 and a Young's modulus of 7.4 GPa at room temperature; these values are greater than those of pristine PS‐b‐P2VP by two orders of magnitude and a factor of 1.8, respectively. This approach can provide a new concept based on electrostatic control to design functional bicontinuous polymer materials.
Ringöffnende 1‐Amino‐3‐aminomethylierung von Donor‐Akzeptor‐substituierten Cyclopropanen über 1,3‐Diazepane
Authors: Garve Lennart K. B. , Jones Peter G. , Werz Daniel B. 
Published: June 2017

AbstractDie erste Ringöffnungsreaktion von Donor‐Akzeptor‐Cyclopropanen zu Diaminen wird beschrieben. Die entwickelte 1,3‐Difunktionalisierung nutzt Cyclopropane und Triazinane sowie Sc(OTf)3 als Katalysator, gefolgt von einer anschließenden Umsetzung mit Säure. Die Reaktion verläuft unter sehr milden Bedingungen und toleriert eine Vielzahl an funktionellen Gruppen. Darüber hinaus konnte eine Bibliothek an verschiedenen 1,3‐Diazepanen synthetisiert werden, die als Intermediat bei der Aza‐[4+3]‐Cycloaddition mit Donor‐Akzeptor‐Cyclopropanen auftreten.
Quanteninterferenzexperimente für die Vermessung von Vitaminen in der Gasphase
Authors: Mairhofer Lukas , Eibenberger Sandra , Cotter Joseph P. , Romirer Marion , Shayeghi Armin , Arndt Markus 
Published: June 2017

AbstractExperimente der letzten Jahre haben gezeigt, dass die Materiewelleninterferometrie dazu verwendet werden kann, einem freien Molekülstrahl eine periodische Struktur aufzuprägen und so auch noch einen Strahlversatz auf der Skala von Nanometern messbar zu machen. Im vorliegenden Beitrag nutzen wir diese Idee, um elektronische Eigenschaften der (Pro)Vitamine A, E und K1 im Flug zu bestimmen. Die elektrische Suszeptibilität und das zeitgemittelte dynamische elektrische Dipolmoment können dabei aus dem Versatz des Interferenzmusters in einem kontrollierten elektrischen Feld ermittelt werden. Die Abhängigkeit des Interferenzmusters von der Intensität eines zentralen optischen Beugungsgitters erlaubt schließlich die Bestimmung einer optischen Polarisierbarkeit. Durch den Vergleich der experimentellen Daten mit Molekulardynamiksimulationen kombiniert mit Dichtefunktionaltheorie erhalten wir Einblick in die elektronische Struktur und Dynamik der isolierten Biomoleküle. Dabei stellt β‐Carotin aufgrund seiner ausgedehnt konjugierten Bindungen einen interessanten Spezialfall in der Reihe der hier untersuchten (Pro)Vitamine dar.
Addition of a Cyclophosphine to Nitriles: An Inorganic Click Reaction Featuring Protio, Organo, and Main‐Group Catalysis
Authors: Chitnis Saurabh S. , Sparkes Hazel A. , Annibale Vincent T. , Pridmore Natalie E. , Oliver Alex M. , Manners Ian 
Published: June 2017

AbstractThe addition of a cyclotriphosphine to a broad range of nitriles gives access to the first examples of free 1‐aza‐2,3,4‐triphospholenes in a rapid, ambient temperature, one‐pot, high‐yield protocol. The reaction produces electron‐rich heterocycles (four lone pairs) and features homoatomic σ‐bond heterolysis, thereby combining the key features of the 1,3‐dipolar cycloaddition chemistry of azides and cyclopropanes. Also reported is the first catalytic addition of P−P bonds to the C≡N bond. The coordination chemistry of the new heterocycles is explored.
Tight Molecular Recognition of Benzo[a]pyrene by a High‐Affinity Antibody
Authors: Eichinger Andreas , Neumaier Irmgard , Pschenitza Michael , Niessner Reinhard , Knopp Dietmar , Skerra Arne 
Published: June 2017

AbstractBenzo[a]pyrene, which is produced during the incomplete combustion of organic material, is an abundant noxious pollutant because of its carcinogenic metabolic degradation products. The high‐affinity (KD≈3 nm) monoclonal antibody 22F12 allows facile bioanalytical quantification of benzo[a]pyrene even in complex matrices. We report the functional and X‐ray crystallographic analysis of 22F12 in complex with 3‐hydroxybenzo[a]pyrene after cloning of the V‐genes and production as a recombinant Fab fragment. The polycyclic aromatic hydrocarbon is bound in a deep pocket between the light and heavy chains, surrounded mainly by aromatic and aliphatic amino acid side chains. Interestingly, the hapten–antibody interface is less densely packed than expected and reveals polar, H‐bond‐like interactions with the polycyclic aromatic π‐electron system, which may allow the antibody to maintain a large, predominantly hydrophobic binding site in an aqueous environment while providing sufficient complementarity to its ligand.
Ring‐Opening 1‐Amino‐3‐aminomethylation of Donor–Acceptor Cyclopropanes via 1,3‐Diazepanes
Authors: Garve Lennart K. B. , Jones Peter G. , Werz Daniel B. 
Published: June 2017

AbstractThe first ring‐opening reaction of donor–acceptor cyclopropanes to give diamines is reported. For this reaction, a 1,3‐bisfunctionalization was developed using cyclopropanes, triazinanes, and Sc(OTf)3 as the catalyst, followed by treatment with acid. The reaction proceeds under very mild conditions and tolerates many functional groups. Moreover, a library of various 1,3‐diazepanes, which arise as intermediates of the first formal aza‐[4+3]‐cycloaddition reaction with donor–acceptor cyclopropanes, was synthesized.
Stereoretentive Olefin Metathesis: An Avenue to Kinetic Selectivity
Authors: Montgomery T. Patrick , Ahmed Tonia S. , Grubbs Robert H. 
Published: June 2017

AbstractOlefin metathesis is an incredibly valuable transformation that has gained widespread use in both academic and industrial settings. Lately, stereoretentive olefin metathesis has garnered much attention as a method for the selective generation of both E‐ and Z‐olefins. Early studies employing ill‐defined catalysts showed evidence for retention of the stereochemistry of the starting olefins at low conversion. However, thermodynamic ratios E/Z were reached as the reaction proceeded to equilibrium. Recent studies in olefin metathesis have focused on the synthesis of catalysts that can overcome the inherent thermodynamic preference of an olefin, providing synthetically useful quantities of a kinetically favored olefin isomer. These reports have led to the development of stereoretentive catalysts that not only generate Z‐olefins selectively, but also kinetically produce E‐olefins, a previously unmet challenge in olefin metathesis. Advancements in stereoretentive olefin metathesis using tungsten, ruthenium, and molybdenum catalysts are presented.
Methylenecyclopropane Annulation by Manganese(I)‐Catalyzed Stereoselective C−H/C−C Activation
Authors: Liang Yu‐Feng , Müller Valentin , Liu Weiping , Münch Annika , Stalke Dietmar , Ackermann Lutz 
Published: June 2017

AbstractC−H/C−C functionalizations with methylenecyclopropanes (MCPs) were accomplished with a versatile base‐metal catalyst. A robust manganese(I) complex enabled the expedient annulation of MCPs by synthetically meaningful ketimines to deliver, upon one‐pot hydroarylation, densely substituted polycylic anilines in a step‐economical fashion. Mechanistic studies provided strong support for a facile organometallic C−H manganation, while typical cobalt, ruthenium, rhodium, and palladium catalysts were found completely ineffective.
Degradation of phenol by heterogeneous Fenton process in an impinging streams reactor with catalyst bed
Authors: Dinarvand Maryam , Sohrabi Morteza , Royaee Sayed Javid , Zeynali Vahid 
Published: June 2017

AbstractIn the present study, the decomposition of phenol in aqueous solutions was investigated in both impinging system and batch reactor. In impinging reactor, catalyst particles with an average diameter of 1.5 × 103μm were confined in a wired cage located in the middle of the reaction vessel. The catalyst was synthesized by impregnation of iron on clinoptilolite zeolite as the support. The mean residence time of the solution in this reactor was 3 s. Therefore, the number of impingements required for the complete degradation of phenol was assessed to be 8 times. The advantage of performing the impinging reactor over a conventional reaction system has been demonstrated in this study. In the impinging reactor at 55 °C, time needed for degradation of phenol in aqueous media was measured to be as low as 24 s; however, phenol degraded completely in 10 min in batch stirred reactor. The optimum operating conditions for the impinging reactor were found as: catalyst containing 5 wt% iron, pH = 3.25, weight ratio of H2O2/phenol = 20, temperature = 55 °C. © 2017 Curtin University of Technology and John Wiley & Sons, Ltd.
Neuroanatomy of the Pig Cardiac Ventricles. A Stereomicroscopic, Confocal and Electron Microscope Study
Authors: Pauziene Neringa , Rysevaite‐Kyguoliene Kristina , Alaburda Paulius , Pauza Audrys G. , Skukauskaite Monika , Masaityte Aiste , Laucaityte Goda , Saburkina Inga , Inokaitis Hermanas , Plisiene Jurgita , Pauza Dainius H. 
Published: June 2017

ABSTRACTAlthough the pig is a model for heart disease, the neuroanatomy of cardiac ventricles (CV) in this species remains undetailed. We aimed to define the innervation pattern of pig CV, combining histochemistry for acetylcholinesterase, immunofluorescent labeling and electron microscopy. Forty nine examined pig hearts show that the major nerves supplying the ventral side of CV descend from the venous part of the heart hilum. Fewer in number and smaller in size, epicardial nerves supply the dorsal half of the CV. Epicardial nerves on the left ventricle are thicker than those on the right. Ventricular ganglia of various sizes distribute at the basal level of both CV. Averagely, we found 3,848 ventricular neuronal somata per heart. The majority of somata were cholinergic, although ganglionic cells of different neurochemical phenotypes (positive for nNOS, ChAT/nNOS, or ChAT/TH) were also observed. Large and most numerous nerves proceeded within the epicardium. Most of endocardium and myocardium contained a network of nerve bundles and nerve fibers (NFs). But, a large number of thin nerves extended along the bundle of His and its branches. The majority of NFs were adrenergic, while cholinergic NFs were scarce yet more abundant than nitrergic ones. Sensory NFs positive for CGRP were the second most abundant phenotype after adrenergic NFs in all layers of the ventricular wall. Electron microscopy elucidated that ultrastructure of nerves varied between different areas of CV. The described structural organization of CV provides an anatomical basis for further functional and pathophysiological studies in the pig heart. Anat Rec, 2017. © 2017 Wiley Periodicals, Inc. Anat Rec, 300:1756–1780, 2017. © 2017 Wiley Periodicals, Inc.
Lesinurad, a Selective Uric Acid Reabsorption Inhibitor, in Combination With Febuxostat in Patients With Tophaceous Gout: Findings of a Phase III Clinical Trial
Authors: Dalbeth Nicola , Jones Graeme , Terkeltaub Robert , Khanna Dinesh , Kopicko Jeff , Bhakta Nihar , Adler Scott , Fung Maple , Storgard Chris , Baumgartner Scott , Perez‐Ruiz Fernando 
Published: June 2017

ObjectiveTo investigate the efficacy and safety of lesinurad in combination with febuxostat in a 12‐month phase III trial in patients with tophaceous gout.MethodsPatients with serum urate (UA) ≥8.0 mg/dl (≥6.0 mg/dl with urate‐lowering therapy) and ≥1 measurable target tophus were given febuxostat 80 mg/day for 3 weeks before randomization to receive lesinurad (200 or 400 mg daily) or placebo in addition to the febuxostat. The primary end point was the proportion of patients achieving a serum UA level of <5.0 mg/dl (month 6). The key secondary end point was the proportion of patients with complete resolution of ≥1 target tophus (month 12). Other end points included the percentage change in total target tophi area. Safety assessments included adverse events and laboratory data.ResultsPatients (n = 324) were predominantly male, with a mean age of 54.1 years. Significantly more patients achieved the serum UA target by month 6 with the addition of lesinurad 400 mg (76.1%; P < 0.0001), but not 200 mg (56.6%; P = 0.13), to the febuxostat therapy as compared with febuxostat alone (46.8%). At all other time points, significantly more patients in the lesinurad 200 mg group achieved the serum UA target. The number of patients with complete tophus resolution was not different between groups. Treatment with lesinurad (200 mg and 400 mg) plus febuxostat reduced the total target tophi area as compared with febuxostat alone (50.1% and 52.9% versus 28.3%, respectively; P < 0.05). Safety was generally comparable with that of febuxostat alone, except for higher rates of predominantly reversible elevations in the serum creatinine level, particularly with lesinurad 400 mg.ConclusionTreatment with lesinurad in combination with febuxostat demonstrated superior lowering of serum UA levels as compared with febuxostat alone, with clinically relevant added effects on tophi and an acceptable safety profile with lesinurad 200 mg in patients with tophaceous gout warranting additional therapy.
Doing the Research that Informs Practice: A Retrospective View of One Group's Attempt to Study The Teaching and Learning of Organic Chemistry
Authors: Bodner George M. , Ferguson Rob , Çalimsiz Selçuk 
Published: June 2017

AbstractThe idea that the focus of educational research should be on results that can inform the practice of teaching has been an implicit assumption for so many years that one would be hard‐pressed to trace it back to an individual source. At one time, the people doing such research in STEM disciplines were faculty in schools or colleges of education who focused on K‐12 classrooms and looked for ideas, concepts, and principles that would be valid across a range of STEM disciplines. Eventually, this research was done on college‐ or university‐level students, as well, and there was a shift toward what has been called discipline‐based educational research (DBER) that looks at the problems associated with the teaching and learning of a given discipline, such as chemistry. This paper will discuss the results of research on problem‐solving in chemistry that has been done in our research group, with particular emphasis on the challenges of teaching and learning organic chemistry. The goal of this paper is to show what can happen when one listens carefully to students and begins to appreciate the difference between what we think we have taught and what the students learned. The examples we will use have the potential for convincing those of us who teach chemistry to rethink what we do in our classes to find better ways of helping our students understand the material we are trying to teach. Although this paper will focus on results from the second‐year organic chemistry course, similar results have been observed in both inorganic and physical chemistry, as well as biochemistry courses.