bluuebunny/crossref_metadata_2025_split huggingface dataset:
Climatic Influences on Southern Makassar Strait Salinity Over the Past Century
Authors: Murty S. A. , Goodkin N. F. , Halide H. , Natawidjaja D. , Suwargadi B. , Suprihanto I. , Prayudi D. , Switzer A. D. , Gordon A. L. 
Published: October 2017

AbstractThe Indonesian Throughflow (ITF) is a globally important ocean current that fuels heat and buoyancy fluxes throughout the Indo‐Pacific and is known to covary in strength with the El Niño Southern Oscillation at interannual time scales. A climate system with a less well‐quantified impact on the ITF is the East Asian Winter Monsoon (EAWM), which drives less saline surface waters from the South China Sea (SCS) into the Makassar Strait, obstructing surface ITF flow. We present a subannually resolved record of sea surface salinity (SSS) from 1927 to 2011 based on coral δ18O from the Makassar Strait that reveals variability in the relative contributions of different source waters to the surface waters of the Makassar Strait during the boreal winter monsoon. We find that the EAWM (January–March) strongly influences interannual SSS variability during boreal winter over the twentieth century (r = 0.54, p << 0.0001), impacting surface water circulation in the SCS and Indonesian Seas.
Electrostatic Potential Radiated by a Pulsating Charge in a Two‐Electron Temperature Plasma
Authors: Gilet N. , Henri P. , Wattieaux G. , Cilibrasi M. , Béghin C. 
Published: October 2017

AbstractMutual impedance experiments have been developed to constrain the plasma bulk properties, such as density and temperature, of ionospheric and later space plasmas, through the electric coupling between an emitter and a receiver electric antennas. So far, the analytical modeling of such instruments has enabled to treat ionospheric plasmas, where charged particles are usually well characterized by Maxwellian electron distributions. With the growth of planetary exploration, mutual impedance experiments are or will be used to constrain space plasma bulk properties. Space plasmas are usually out of local thermodynamic equilibrium; therefore, new methods to calibrate and analyze mutual impedance experiments are now required in such non‐Maxwellian plasmas. To this purpose, this work aims at modeling the electric potential generated in a two‐electron temperature plasma by a pulsating point charge. A numerical method is developed for the computation of the electrostatic potential in a sum of Maxwellian plasmas. After validating the method, the results are used to build synthetic mutual impedance spectra and quantify the effect of a warm electron population on mutual impedance experiments, in order to illustrate how the method could be applied for recent and future planetary space missions, such as Rosetta, BepiColombo, and JUICE. In particular, we show how it enables to separate the densities and temperatures of two different electron populations using in situ measurements from the RPC‐MIP mutual impedance experiment on board Rosetta.
Prediction of foamability of polyethylene terephthalate using viscous and elastic parameters
Authors: Yang Zhaoping , Xin Chunling , Mughal Waqas , Wang Zeming , Bai Xue , He Yadong 
Published: October 2017

AbstractRheological behavior and foamability of polyethylene terephthalate (PET) with different molecular structures were investigated. The aim of this study was to find out the viscous and elastic parameters which can predict the foaming properties of PET. It is found that the foams of strain hardening PET have high expansion ratios and fine cell morphologies. This is correlated with the contribution of strain hardening to the improvement of melt strength and failure strain during elongational experiments. Basing on the fact that foamability of a material is governed by its strain hardening (a pure elastic behavior), a viscous parameter (complex viscosity), and an elastic parameter (loss tangent) obtained from dynamic shear rheology are well linked to the expansion ratios of foams. These two parameters formed an optimized viscoelastic window, which is suitable for foaming. This means the foamability of PET can be determined by viscous and elastic parameters without consideration of molecular constitution.
Unlocking the Potential of Poly(Ortho Ester)s: A General Catalytic Approach to the Synthesis of Surface‐Erodible Materials
Authors: Tschan Mathieu J.‐L. , Ieong Nga Sze , Todd Richard , Everson Jack , Dove Andrew P. 
Published: October 2017

AbstractPoly(ortho ester)s (POEs) are well‐known for their surface‐eroding properties and hence present unique opportunities for controlled‐release and tissue‐engineering applications. Their development and wide‐spread investigation has, however, been severely limited by challenging synthetic requirements that incorporate unstable intermediates and are therefore highly irreproducible. Herein, the first catalytic method for the synthesis of POEs using air‐ and moisture‐stable vinyl acetal precursors is presented. The synthesis of a range of POE structures is demonstrated, including those that are extremely difficult to achieve by other synthetic methods. Furthermore, application of this chemistry permits efficient installation of functional groups through ortho ester linkages on an aliphatic polycarbonate.
Tunable elasticity and thermodynamic parameters of hydroxypropyl methacrylate‐based gels with varying extents of monomer concentration: Statistical mechanics treatments of physical observations
Authors: Orakdogen Nermin , Sanay Berran 
Published: October 2017

ABSTRACTThe present article reports the scaling laws relating the preparation conditions with the equilibrium swelling degree and the crosslinking density of a new family of hydroxyl functional hydrogels (Hgs) prepared by free radical crosslinking polymerization of hydroxypropyl methacrylate (HPMA) in aqueous solution with tetraethylene glycol dimethacrylate (TEGDMA) as crosslinker. For comparison of physical properties, chemical and mechanical stability, HPMA cryogels (Cgs) were also prepared using the cryotropic gelation technique by conducting the gelation reactions at subzero temperatures. The measurements of the equilibrium swelling degree and the elastic properties of poly(hydroxypropyl methacrylate) (PHPMA) gel samples having different initial monomer concentration were treated according to the scaling theory to explain the rubbery behavior of the resulting Hgs. The obtained scaling relation between the reduced modulus and the swelling degreeindicated limiting chain extensibility which is neglected in the Flory–Rehner theory. The effective crosslink density and polymer–solvent interaction parameter of PHPMA Hgs were used to interpret the observed deviation. Results showed that the properties of PHPMA Hgs and Cgs can be controlled by varying the HPMA and TEGDMA content. Increase of total monomer concentrations causes a pronounced decrease in the equilibrium swelling degree, and an increase in the elastic response of PHPMA Hgs and Cgs. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci.2018,135, 45889.
High cycling stability and well printability poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate)/multi‐walled carbon nanotube nanocomposites via in situ polymerization applied on electrochromic display
Authors: Chen Ting , Chen Qifeng , Liu Guhong , Chen Guangxue 
Published: October 2017

ABSTRACTA high cycling stability material and an additive manufacturing method are reported for the fabrication of solid electrochromic devices. The poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate)/multi‐walled carbon nanotube (PEDOT:PSS/MWCNT) nanocomposites were synthesized via in situ polymerization. A carboxymethyl cellulose gel was used as the ink vehicle for screen printing. The electrochromic (EC) performance of films patterned by screen printing was also examined. The results of characterization indicate that strong interfacial interactions occurred between PEDOT:PSS and the MWCNTs and the MWCNTs formed a network in these conducting polymers film, so the composite was more conductive than pure PEDOT:PSS. Devices containing PEDOT:PSS/MWCNTs were more stable after 1000 cycles, exhibited higher rate of ion exchange and faster increases in current. The composite containing 0.3 wt % MWCNTs also had a 23% higher color contrast (ΔE*) than pure PEDOT:PSS at 2.5 V applied voltages. The EC inks with well printability not only can be used to print large area films, but also can print fine lines and pixel‐type dots in displays. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 45943.
Quantitative Analysis of the Self‐Assembly Process of a Pd12L24 Coordination Sphere
Authors: Kai Shumpei , Shigeta Taro , Kojima Tatsuo , Hiraoka Shuichi 
Published: October 2017

AbstractThe self‐assembly process of a Pd12L24 sphere was revealed by a quantitative approach (quantitative analysis of self‐assembly process: QASAP) quantifying all the substrates, the products, and the observable intermediates, indicating that the Pd12L24 sphere is produced through several pathways. Firstly, PdnL2n (n=6, 8, and 9), which are perfectly closed structures smaller than the Pd12L24 sphere, and a mixture of intermediates not observed by NMR (Int) were produced. Next, the sphere was assembled from intra‐/intermolecular reaction of a certain class of Int (path A) and from the coordination of free pyridyl groups in Int to the PdII center of PdnL2n (n=6, 8, and 9) (path B). While capping the free pyridyl groups in Int with PdII ions perfectly inhibited the sphere formation, the addition of free L to Int accelerated the formation of the sphere.
Benziodoxole Triflate as a Versatile Reagent for Iodo(III)cyclization of Alkynes
Authors: Wu Bin , Wu Junliang , Yoshikai Naohiko 
Published: October 2017

AbstractThe utility of benziodoxole triflate, derived from α,α‐bis(trifluoromethyl)‐2‐iodobenzyl alcohol, as a versatile reagent for iodo(III)cyclization via electrophilic activation of alkyne, is reported herein. The reagent promotes cyclization of alkynes tethered to a variety of nucleophilic moieties, affording benziodoxole‐appended (hetero)arenes such as benzofurans, benzothiophenes, isocoumarins, indoles, and polyaromatics under mild conditions. This unprecedented class of (hetero)aryl‐IIII compounds proved easy to purify, stable, and amenable to various synthetic transformations.
Proteomics analysis of altered proteins in kidney of mice with aristolochic acid nephropathy using the fluorogenic derivatization–liquid chromatography–tandem mass spectrometry method
Authors: Lin Chia‐En , Chang Wen‐Shin , Lee Jen‐Ai , Chang Ting‐Ya , Huang Yu‐Shen , Hirasaki Yoshiro , Chen Hung‐Shing , Imai Kazuhiro , Chen Shih‐Ming 
Published: October 2017

AbstractAristolochic acid (AA) causes interstitial renal fibrosis, called aristolochic acid nephropathy (AAN). There is no specific indicator for diagnosing AAN, so this study aimed to investigate the biomarkers for AAN using a proteomics method. The C3H/He female mice were given ad libitum AA–distilled water (0.5 mg/kg/day) and distilled water for 56 days in the AA and normal groups, respectively. The AA‐induced proteins in the kidney were investigated using a proteomics study, including fluorogenic derivatization with 7‐chloro‐N‐[2‐(dimethylamino)ethyl]‐2,1,3‐benzoxadiazole‐4‐sulfonamide, followed by high‐performance liquid chromatography analysis and liquid chromatography tandem mass spectrometry with a MASCOT database searching system. There were two altered proteins, thrombospondin type 1 (TSP1) and G protein‐coupled receptor 87 (GPR87), in the kidney of AA‐group mice on day 56. GPR87, a tumorigenesis‐related protein, is reported for the first time in the current study. The renal interstitial fibrosis was certainly induced in the AA‐group mice under histological examination. Based on the results of histological examination and the proteomics study, this model might be applied to AAN studies in the future. TSP1 might be a novel biomarker for AAN, and the further role of GPR87 leading to AA‐induced tumorigenesis should be researched in future studies.
Online Measurement of Oxygen‐Dependent Enzyme Reaction Kinetics
Authors: Meissner Murray P. , Nordblad Mathias , Woodley John M. 
Published: October 2017

AbstractAs the application of biocatalysis to complement conventional chemical and catalytic approaches continues to expand, an increasing number of reactions involve poorly water‐soluble substrates. At required industrial concentrations necessary for industrial implementation, this frequently leads to heterogeneous reaction mixtures composed of multiple phases. Such systems are challenging to sample, and therefore, it is problematic to measure representative component concentrations. Herein, an online method for following the progress of oxygen‐dependent reactions through accurate measurement of the oxygen mass balance in the gas phase of a reactor is demonstrated and validated. The method was successfully validated and demonstrated by using two model reactions: firstly, the oxidation of glucose by glucose oxidase and, secondly, the Baeyer–Villiger oxidation of macrocyclic ketones to lactones. Initial reaction rate constants and time‐course progressions calculated from the oxygen mass balance were validated against conventional online methods of dissolved oxygen tension and pH titration measurements. A feasible operating window and the sensitivity to dynamic changes of reaction rates were established by controlling oxygen transfer through the operating parameters of the reactor. Such kinetic data forms the basis for reaction characterisation, from which bottlenecks may be made evident and directed improvement strategies can be identified and implemented.
When high‐volume PCI operators in high‐volume hospitals move to lower volume hospitals—Do they still maintain high volume and quality of outcomes?
Authors: Lu Tsung‐Hsueh , Li Sheng‐Tun , Liang Fu‐Wen , Lee Jo‐Chi , Yin Wei‐Hsian 
Published: October 2017

AbstractObjectivesThe aim of this quasi‐experimental study was to examine whether high‐volume percutaneous coronary intervention (PCI) operators still maintain high volume and quality of outcomes when they moved to lower volume hospitals.BackgroundSystematic reviews have indicated that high‐volume PCI operators and hospitals have higher quality outcomes. However, little is known on whether high PCI volume and high quality outcomes are mainly due to operator characteristics (i.e., skill and experience) and is portable across organizations or whether it is due to hospital characteristics (i.e., equipment, team, and management system) and is less portable.MethodsWe used Taiwan National Health Insurance claims data 2000–2012 to identify 98 high‐volume PCI operators, 10 of whom moved from one hospital to another during the study period. We compared the PCI volume, risk‐adjusted mortality ratio, and major adverse cardiovascular event (MACE) ratio before and after moving.ResultsOf the 10 high‐volume operators who moved, 6 moved from high‐ to moderate‐ or low‐volume hospitals, with median annual PCI volumes (interquartile range) of 130 (117–165) in prior hospitals and 54 (46–84) in subsequent hospitals (the hospital the operator moved to), and the remaining 4 moved from high to high‐volume hospitals, with median annual PCI volumes (interquartile range) of 151 (133–162) in prior hospitals and 193 (178–239) in subsequent hospitals. No significant differences were observed in the risk‐adjusted mortality ratios and MACE ratios between high‐volume operators and matched controls before and after moving.ConclusionsHigh‐volume operators cannot maintain high volume when they moved from high to moderate or low‐volume hospitals; however, the quality of care is maintained. High PCI volume and high‐quality outcomes are less portable and more hospital bound.
Copper–Palladium Tetrapods with Sharp Tips as a Superior Catalyst for the Oxygen Reduction Reaction
Authors: Zhang Lan , Chen Sheng , Dai Yanmeng , Shen Zeqi , Wei Miaojin , Huang Ruijie , Li Hongliang , Zheng Tingting , Zhang Yunjiao , Zhou Shiming , Zeng Jie 
Published: October 2017

AbstractThe development of superior non‐Pt catalysts for the oxygen reduction reaction (ORR) is highly desirable but still challenging. Herein, we prepared 50‐nm CuPd tetrapods with catalytic performance towards the alkaline ORR that was higher than that of Pd nanoparticles, CuPd nanoparticles, CuPd tetrahedrons, and 7‐nm CuPd tetrapods. The mass activity of 50‐nm CuPd tetrapods was 0.29 A mgPd−1, which was superior to that of commercial Pt/C and most Pd‐based catalysts reported to date. Mechanistic studies revealed that the enhanced performance could be attributed to the synergy of the alloy effect and sharp‐tip effect, both of which enable the accumulation of negative charges on the Pd atoms at the vertices of the tetrapods. The high negative charge density of the Pd atoms at the vertices lowers the Pd d‐band center and, thus, its oxygen adsorption energy. This work provides a pathway to improve the activity of ORR catalysts by modulating their electronic structures, which opens up new sight to design promising non‐Pt catalysts for the ORR.
Single‐Particle Studies to Advance the Characterization of Heterogeneous Biocatalysts
Authors: Benítez‐Mateos Ana I. , Nidetzky Bernd , Bolivar Juan M. , López‐Gallego Fernando 
Published: October 2017

AbstractImmobilized enzymes have been widely exploited because they work as heterogeneous biocatalysts, allowing their recovery and reutilization and easing the downstream processing once the chemical reactions are completed. Unfortunately, we suffer a lack of analytical methods to characterize those heterogeneous biocatalysts at microscopic and molecular levels with spatio‐temporal resolution, which limits their design and optimization. Single‐particle studies are vital to optimize the performance of immobilized enzymes in micro/nanoscopic environments. In this Concept article, we review different analytical techniques that address single‐particle studies to image the spatial distribution of the enzymes across the solid surfaces, the sub‐particle substrate diffusion, the structural integrity and mobility of the immobilized enzymes inside the solid particles, and the pH and O2 internal gradients. From our view, such sub‐particle information elicited from single‐particle analysis is paramount for the design and fabrication of optimal heterogeneous biocatalyst.
Spin‐Forbidden Reactions: Adiabatic Transition States Using Spin–Orbit Coupled Density Functional Theory
Authors: Gaggioli Carlo Alberto , Belpassi Leonardo , Tarantelli Francesco , Harvey Jeremy N. , Belanzoni Paola 
Published: October 2017

AbstractA spin‐forbidden chemical reaction involves a change in the total electronic spin state from reactants to products. The mechanistic study is challenging because such a reaction does not occur on a single diabatic potential energy surface (PES), but rather on two (or multiple) spin diabatic PESs. One possible approach is to calculate the so‐called “minimum energy crossing point” (MECP) between the diabatic PESs, which however is not a stationary point. Inclusion of spin–orbit coupling between spin states (SOC approach) allows the reaction to occur on a single adiabatic PES, in which a transition state (TS SOC) as well as activation free energy can be calculated. This Concept article summarizes a previously published application in which, for the first time, the SOC effects, using spin–orbit ZORA Hamiltonian within density functional theory (DFT) framework, are included and account for the mechanism of a spin‐forbidden reaction in gold chemistry. The merits of the MECP and TS SOC approaches and the accuracy of the results are compared, considering both our recent calculations on molecular oxygen addition to gold(I)‐hydride complexes and new calculations for the prototype spin‐forbidden N2O and N2Se dissociation reactions.
Exploring potentialities and limitations of stapled o‐oligo(phenyleneethynylene)s (o‐OPEs) as efficient circularly polarized luminescence emitters
Authors: Reiné Pablo , Justicia José , Morcillo Sara P. , Mazzeo Giuseppe , García‐Fernández Emilio , Rodríguez‐Diéguez Antonio , Álvarez de Cienfuegos Luis , Abbate Sergio , Cuerva Juan M. , Longhi Giovanna , Miguel Delia 
Published: October 2017

AbstractIn this paper, we have studied the chiroptical properties of a family of o‐oligo(phenyleneethynylene) (o‐OPE) derivatives with different steric hindrance. Experimental results show high dissymmetry factors (gabs and glum up to 1.1 × 10−2) and very similar electronic circular dichroism (ECD) and circularly polarized luminescence (CPL) for all the derivatives that make this basic o‐OPE scaffold a robust pure organic emitter. Vibrational circular dichroism spectra are used to characterize conformational properties in solution. Density functional theory and time‐dependent density functional theory calculations support experimental results also proving that ECD and CPL are almost exclusively linked to helical moiety and not to size or conformation of substituents. As chiroptical properties of these emitters are independent of substituents, this OPE scaffold can be used as basic skeleton for the design of sensing probes with high CPL efficiencies.
Physical driving force of actomyosin motility based on the hydration effect
Authors: Suzuki Makoto , Mogami George , Ohsugi Hideyuki , Watanabe Takahiro , Matubayasi Nobuyuki 
Published: October 2017

AbstractWe propose a driving force hypothesis based on previous thermodynamics, kinetics and structural data as well as additional experiments and calculations presented here on water‐related phenomena in the actomyosin systems. Although Szent‐Györgyi pointed out the importance of water in muscle contraction in 1951, few studies have focused on the water science of muscle because of the difficulty of analyzing hydration properties of the muscle proteins, actin, and myosin. The thermodynamics and energetics of muscle contraction are linked to the water‐mediated regulation of protein–ligand and protein–protein interactions along with structural changes in protein molecules. In this study, we assume the following two points: (1) the periodic electric field distribution along an actin filament (F‐actin) is unidirectionally modified upon binding of myosin subfragment 1 (M or myosin S1) with ADP and inorganic phosphate Pi (M.ADP.Pi complex) and (2) the solvation free energy of myosin S1 depends on the external electric field strength and the solvation free energy of myosin S1 in close proximity to F‐actin can become the potential force to drive myosin S1 along F‐actin. The first assumption is supported by integration of experimental reports. The second assumption is supported by model calculations utilizing molecular dynamics (MD) simulation to determine solvation free energies of a small organic molecule and two small proteins. MD simulations utilize the energy representation method (ER) and the roughly proportional relationship between the solvation free energy and the solvent‐accessible surface area (SASA) of the protein. The estimated driving force acting on myosin S1 is as high as several piconewtons (pN), which is consistent with the experimentally observed force.