bluuebunny/crossref_metadata_2025_split huggingface dataset:
Binder Effects in SiO2‐ and Al2O3‐Bound Zeolite ZSM‐5‐Based Extrudates as Studied by Microspectroscopy
Authors: Whiting Gareth T. , Meirer Florian , Mertens Machteld M. , Bons Anton‐Jan , Weiss Brian M. , Stevens Paul A. , de Smit Emiel , Weckhuysen Bert M. 
Published: January 2015

AbstractMicrospectroscopic methods were explored to investigate binder effects occurring in ZSM‐5‐containing SiO2‐ and Al2O3‐bound millimetre‐sized extrudates. Using thiophene as a selective probe for Brønsted acidity, coupled with time‐resolved in situ UV/Vis and confocal fluorescence microspectroscopy, variations in reactivity and selectivity between the two distinct binder types were established. It was found that aluminium migration occurs in ZSM‐5‐containing Al2O3‐bound extrudates, forming additional Brønsted acid sites. These sites strongly influence the oligomer selectivity, favouring the formation of thiol‐like species (i.e., ring‐opened species) in contrast to higher oligomers, predominantly formed on SiO2‐bound ZSM‐5‐containing extrudates. Not only were the location and distribution of these oligomers visualised by 3 D analysis, it was also observed that more conjugated species appeared to grow off the surface of the zeolite ZSM‐5 crystals (containing less conjugated species) into the surrounding binder material. Furthermore, a higher binder content resulted in an increasing overall reactivity owing to the greater number of stored thiophene monomers available per Brønsted acid site.
Efficient Organocatalyst Supported on a Simple Ionic Liquid as a Recoverable System for the Asymmetric Diels–Alder Reaction in the Presence of Water
Authors: De Nino Antonio , Maiuolo Loredana , Merino Pedro , Nardi Monica , Procopio Antonio , Roca‐López David , Russo Beatrice , Algieri Vincenzo 
Published: January 2015

AbstractThe synthesis, characterization, and evaluation of a new highly efficient organocatalyst, namely, (5S)‐2,2,3‐trimethyl‐5‐thiobenzylmethyl‐4‐imidazolidinone hydrochloride, has been achieved. The catalyst possesses important structural features that should increase the catalytic efficiency and solubility in polar media. The application of the ionic‐liquid‐supported imidazolidinone catalyst in enantioselective Diels–Alder reactions was investigated. The Diels–Alder reactions of several dienes and dienophiles proceeded efficiently in the presence of the catalyst to provide the desired products in moderate to good yields and from good to excellent enantioselectivities. The conformation study confirms that in the transition state the Re face is shielded completely by the phenyl ring and an approach on the less hindered Si face is preferred. Particularly remarkable is the fact that the entire ionic liquid/HCl 0.01 M/catalyst system can be recovered and reused in up to six runs without an appreciable loss of catalytic activity.
Solvent‐Dependent Structure of the I3− Ion Derived from Photoelectron Spectroscopy and Ab Initio Molecular Dynamics Simulations
Authors: Jena Naresh K. , Josefsson Ida , Eriksson Susanna K. , Hagfeldt Anders , Siegbahn Hans , Björneholm Olle , Rensmo Håkan , Odelius Michael 
Published: January 2015

AbstractAb initio molecular dynamics (MD) simulations of the solvation of LiI3 in four different solvents (water, methanol, ethanol, and acetonitrile) are employed to investigate the molecular and electronic structure of the I3− ion in relation to X‐ray photoelectron spectroscopy (XPS). Simulations show that hydrogen‐bond rearrangement in the solvation shell is coupled to intramolecular bond‐length asymmetry in the I3− ion. By a combination of charge analysis and I 4 d core‐level XPS measurements, the mechanism of the solvent‐induced distortions has been studied, and it has been concluded that charge localization mediates intermolecular interactions and intramolecular distortion. The approach involving a synergistic combination of theory and experiment probes the solvent‐dependent structure of the I3− ion, and the geometric structure has been correlated with the electronic structure.
Chemical Synthesis of Burkholderia Lipid A Modified with Glycosyl Phosphodiester‐Linked 4‐Amino‐4‐deoxy‐β‐L‐arabinose and Its Immunomodulatory Potential
Authors: Hollaus Ralph , Ittig Simon , Hofinger Andreas , Haegman Mira , Beyaert Rudi , Kosma Paul , Zamyatina Alla 
Published: January 2015

AbstractModification of the Lipid A phosphates by positively charged appendages is a part of the survival strategy of numerous opportunistic Gram‐negative bacteria. The phosphate groups of the cystic fibrosis adapted Burkholderia Lipid A are abundantly esterified by 4‐amino‐4‐deoxy‐β‐L‐arabinose (β‐L‐Ara4N), which imposes resistance to antibiotic treatment and contributes to bacterial virulence. To establish structural features accounting for the unique pro‐inflammatory activity of Burkholderia LPS we have synthesised Lipid A substituted by β‐L‐Ara4N at the anomeric phosphate and its Ara4N‐free counterpart. The double glycosyl phosphodiester was assembled by triazolyl‐tris‐(pyrrolidinyl)phosphonium‐assisted coupling of the β‐L‐Ara4N H‐phosphonate to α‐lactol of β(1→6) diglucosamine, pentaacylated with (R)‐(3)‐acyloxyacyl‐ and Alloc‐protected (R)‐(3)‐hydroxyacyl residues. The intermediate 1,1′‐glycosyl‐H‐phosphonate diester was oxidised in anhydrous conditions to provide, after total deprotection, β‐L‐Ara4N‐substituted Burkholderia Lipid A. The β‐L‐Ara4N modification significantly enhanced the pro‐inflammatory innate immune signaling of otherwise non‐endotoxic Burkholderia Lipid A.
Internal Dynamics in Halogen‐Bonded Adducts: A Rotational Study of Chlorotrifluoromethane–Formaldehyde
Authors: Gou Qian , Feng Gang , Evangelisti Luca , Vallejo‐López Montserrat , Spada Lorenzo , Lesarri Alberto , Cocinero Emilio J. , Caminati Walther 
Published: January 2015

AbstractThe rotational spectra of two isotopologues of the 1:1 complex between chlorotrifluoromethane and formaldehyde have been recorded and analyzed by using Fourier‐transform microwave spectroscopy. Only one rotamer was detected, with the two constituent molecules held together through a Cl⋅⋅⋅O halogen bond (RCl⋅⋅⋅O=3.048 Å). The dimer displays two simultaneous large‐amplitude intramolecular motions. The internal rotation of formaldehyde around its symmetry axis (V2=28(5) cm−1) splits all the rotational transitions into two component lines with a relative intensity ratio of 1:3. On the other hand, the almost free internal rotation (V3≈2.5 cm−1) of the CF3 symmetric top increases the “rigid” value of the rotational constant A by almost one order of magnitude. In addition, all the transitions display a hyperfine structure due to the 35Cl (or 37Cl) nucleus quadrupole effects.
Evaluation of tert‐Butyl Isosteres: Case Studies of Physicochemical and Pharmacokinetic Properties, Efficacies, and Activities
Authors: Westphal Matthias V. , Wolfstädter Bernd T. , Plancher Jean‐Marc , Gatfield John , Carreira Erick M. 
Published: January 2015

AbstractThe tert‐butyl group is a common motif in medicinal chemistry. Its incorporation into bioactive compounds is often accompanied by unwanted property modulation, such as increased lipophilicity and decreased metabolic stability. Several alternative substituents are available for the drug discovery process. Herein, physicochemical data of two series of drug analogues of bosentan and vercirnon are documented as part of a comparative study of tert‐butyl, pentafluorosulfanyl, trifluoromethyl, bicyclo[1.1.1]pentanyl, and cyclopropyl‐trifluoromethyl substituents.
Hemodynamic analysis of patient‐specific coronary artery tree
Authors: Zhang Jun‐Mei , Luo Tong , Tan Swee Yaw , Lomarda Aileen Mae , Wong Aaron Sung Lung , Keng Felix Yung Jih , Allen John Carson , Huo Yunlong , Su Boyang , Zhao Xiaodan , Wan Min , Kassab Ghassan S. , Tan Ru San , Zhong Liang 
Published: January 2015

SummaryLocal hemodynamic parameters, such as wall shear stress (WSS), oscillatory shear index and relative resident time (RRT), have been linked to coronary plaque initiation and progression. In this study, a left coronary artery tree model was reconstructed from computed tomography angiography images of a patient with multiple stenoses. The geometry of the coronary artery tree model was virtually restored by eliminating the lesions, essentially re‐creating the virtually healthy artery anatomy. Using numerical simulations, flow characteristics and hemodynamic parameter distributions in the stenosed and virtually healthy models were investigated. In the virtually healthy artery model, disturbed flows were found at four locations, prone to initialization of plaque formation. Low WSS and high RRT were exhibited in three of the four locations, and high WSS and low RRT were exhibited in the fourth. These findings suggest that coronary plaque is more likely to form in locations with disturbed flow conditions characterized by low WSS and high RRT or high WSS and low RRT. In addition, clinical index of fractional flow reserve was found to significantly correlate with blood flow rate, rather than anatomic parameters, such as diameter stenosis, which implied the importance of hemodynamic environment in stenosis formation. Copyright © 2015 John Wiley & Sons, Ltd.
A quantitative index for measuring the development of supercomputing
Authors: Hu Yonghong , Chi Xuebin , Chen Debbi , Kahaner David K. , Yuen David A. 
Published: January 2015

SummaryCurrent assessments of supercomputing (high‐performance computing) primarily focus on system performance. Quantitative methods to measure the impact of supercomputing in a broad context have not been well developed. In this paper, the basic meaning of supercomputing development is analyzed. An evaluation index system for assessing the development status of supercomputing is constructed innovatively, and the SuperComputing Development Index (SCDI) is proposed to measure supercomputing development status. SCDI is a composite index combining various indicators into one benchmark measure that monitors and compares supercomputing development in the past years. This appears to be the first attempt to quantitatively measure the supercomputing ecosystem. As an example, the SCDI of the Chinese Academy of Sciences is obtained, which is based on the data collected from 130 research groups about and covers the period from 2006 to 2012. The results have demonstrated that the proposed evaluation index system is objectively reasonable. The constructed SCDI provides a scientific method to quantitatively evaluate the development status of supercomputing for institutions or organizations.
A congestion control scheme based on probabilistic packet acceptance and drop in delay‐tolerant networks
Authors: An Ying , Luo Xi , Liu Yao , Huang Jiawei , Min Geyong , Wang Jianxin 
Published: January 2015

SummaryMessage replication is often used to improve the delivery ratio in delay‐tolerant networks because of the short‐lived wireless connectivity environment. However, packet replication may easily incur large resource consumption and finally result in network congestion. This paper proposes a probabilistic packet acceptance and drop algorithm (PAD), which adaptively controls congestion for delay‐tolerant networks. In PAD algorithm, the queue length and the input/output rate are combined to detect congestion. Based on the congestion state, each node determines the probability of accepting or dropping packets to obtain a good trade‐off between high delivery ratio and low overhead. Furthermore, based on the birth–death model, we construct the continuous‐time Markov chain to analyze the delivery ratio of a packet. Theory analysis and simulation results show that PAD increases the delivery ratio by more than 130% with least overhead. Meanwhile, it also achieves the shortest average end‐to‐end delay when the buffer of a node is severely limited. Copyright © 2015 John Wiley & Sons, Ltd.
Resilient gossip algorithms for collecting online management information in exascale clusters
Authors: Barak Amnon , Drezner Zvi , Levy Ely , Lieber Matthias , Shiloh Amnon 
Published: January 2015

SummaryManagement of forthcoming exascale clusters requires frequent collection of run‐time information about the nodes and the running applications. This paper presents a new paradigm for providing online information to the management system of scalable clusters, consisting of a large number of nodes and one or more masters that manage these nodes. We describe the details of resilient gossip algorithms for sharing local information within subsets of nodes and for sending global information to a master, which holds information on all the nodes. The presented algorithms are decentralized, scalable and resilient, working well even when some nodes fail, without needing any recovery protocol. The paper gives formal expressions for approximating the average ages of the local information at each node and the information collected by the master. It then shows that these results closely match the results of simulations and measurements on a real cluster. The paper also investigates the resilience of the algorithms and the impact on the average age when nodes or masters fail. The main outcome of this paper is that partitioning of large clusters can improve the quality of information available to the management system without increasing the number of messages per node. Copyright © 2015 John Wiley & Sons, Ltd.
Raman and FTIR Spectroscopic Studies of 1‐Ethyl‐3‐methylimidazolium Trifluoromethylsulfonate, its Mixtures with Water and the Solvation of Zinc Ions
Authors: Liu Zhen , El Abedin Sherif Zein , Endres Frank 
Published: January 2015

AbstractIn this paper we report on the interactions of the ionic liquid 1‐ethyl‐3‐methylimidazolium trifluoromethylsulfonate ([EMIm]TfO) with water and the solvation of zinc ions in neat [EMIm]TfO and [EMIm]TfO–water mixtures investigated by FTIR and Raman spectroscopy. The structures and physicochemical properties of the [EMIm]TfO–water mixtures are strongly dependent on the interaction between cations, anions, and water. The structure was changed from ionic‐liquid‐like to water‐like solutions upon addition of water. In addition, zinc salts can precipitate in 0.2 M Zn(TfO)2/[EMIm]TfO upon addition of 10 % (v/v) water, presumably as a result of polarity change of the solution. The average coordination number of TfO− per zinc ion calculated from Raman spectra is 3.8 in neat [EMIm]TfO, indicating that [Zn(TfO)4]2−, and [Zn(TfO)3]− complexes are present in the solution. However, in the presence of water, water interacts preferentially with the zinc ions, leading to aqueous zinc species. The solvation of zinc ions in 1‐butyl‐1‐methylpyrrolidinium trifluoromethylsulfonate ([Py1,4]TfO) was also investigated. In [Py1,4]TfO, there are, on average, 4.5 TfO− anions coordinating each zinc ion, corresponding to the weak interaction between [Py1,4]+ cations and TfO− anions. The species present in [Py1,4]TfO are likely a mixture of [Zn(TfO)4]2− and [Zn(TfO)5]3−.
Quantifying sapwood width for three Australian native species using electrical resistivity tomography
Authors: Wang Hailong , Guan Huade , Guyot Adrien , Simmons Craig T. , Lockington David A. 
Published: January 2015

AbstractSap flow measurement techniques have been successfully applied in ecohydrological studies as they can be used to estimate watershed transpiration. Sapwood area (As) is one of the most important tree parameters for estimating transpiration from point sap flow measurements. Accurate and efficient determination of As and the relationship between As and other tree parameters (e.g. diameter at 130 cm, DBH) is essential for the practical upscaling of sap flow data. The conventional methods for determining sapwood area are accurate (although coring can damage the trees) but prohibitive when a large number of trees need to be sampled. Electrical resistivity tomography (ERT) is a non‐destructive geophysical method, which detects the moisture or electrolyte concentration difference in wood tissue to identify sapwood–heartwood boundaries. In this study, a rigorous method for quantifying sapwood width and area using ERT is detailed using measurements on 30 trees of three Australian native species (drooping sheoak and two eucalypts). Results show that sapwood widths estimated by ERT were in good agreement with those obtained from wood core analyses for the three species. A strong linear relationship was observed between As and DBH and between heartwood radius and DBH. The As–DBH relationship extends the synthesis for eucalypts species in previous studies. Sapwood width was overestimated for trees under wet conditions, which indicates that the ERT technique for sapwood width quantification is limited under such conditions. Copyright © 2015 John Wiley & Sons, Ltd.
Effects of a ‘natural’ flood event on the riparian ecosystem of a regulated large‐river system: the 2011 flood on the Missouri River, USA
Authors: Dixon Mark D. , Boever Christopher J. , Danzeisen Victoria L. , Merkord Christopher L. , Munes Eszter C. , Scott Michael L. , Johnson W. Carter , Cowman Tim C. 
Published: January 2015

AbstractFlow regulation has significantly altered hydrological, geomorphic, and ecological processes on the Missouri River. Cumulative effects are evident in declines in cottonwood (Populus deltoides) recruitment and in altered forest age structure and composition. Record runoff in 2011 exceeded reservoir capacity on the Upper and Middle Missouri, leading to a 500‐year recurrence interval flood in terms of volume, with the highest peak discharge in 59 years and flood durations of up to 3 months. We assessed the effects of this ‘large infrequent disturbance’ by comparing pre‐flood (2006–2009) to post‐flood (2012) changes in riparian forests along two unchannelized segments of the Missouri River. Live shrub and tree density declined sharply within young forest stands (<30 years). Higher proportions of non‐native (Elaeagnus angustifolia) and upland (Juniperus virginiana) trees showed evidence of recent mortality than did the native cottonwood. Sandbar area increased sharply from 2006 to 2012 and area of young forests declined, with particularly sharp declines in sapling stands that had established following the previous post‐dam record flow releases in 1997. Cottonwood recruitment was widespread in 2012, but nearly all seedling patches occurred on sandbars in the active channel rather than on overbank sites, with moderately high (61–77%) seedling mortality over 2012–2013. Physical and operational constraints within the regulated Missouri River limited the restorative effects of the 2011 flood and will likely limit future forest recovery. Process‐based riparian restoration would require restoring flow and sediment regimes that more closely mimic historical conditions, as well as overcoming the physical legacies of decades of flow regulation. Copyright © 2015 John Wiley & Sons, Ltd.
Meta‐analysis of Genome‐Wide Association Studies Identifies Novel Loci Associated With Optic Disc Morphology
Authors: Springelkamp Henriët , Mishra Aniket , Hysi Pirro G. , Gharahkhani Puya , Höhn René , Khor Chiea‐Chuen , Cooke Bailey Jessica N. , Luo Xiaoyan , Ramdas Wishal D. , Vithana Eranga , Koh Victor , Yazar Seyhan , Xu Liang , Forward Hannah , Kearns Lisa S. , Amin Najaf , Iglesias Adriana I. , Sim Kar‐Seng , van Leeuwen Elisabeth M. , Demirkan Ayse , van der Lee Sven , Loon Seng‐Chee , Rivadeneira Fernando , Nag Abhishek , Sanfilippo Paul G. , Schillert Arne , de Jong Paulus T. V. M. , Oostra Ben A. , Uitterlinden André G. , Hofman Albert ,   NEIGHBORHOOD Consortium, Zhou Tiger , Burdon Kathryn P. , Spector Timothy D. , Lackner Karl J. , Saw Seang‐Mei , Vingerling Johannes R. , Teo Yik‐Ying , Pasquale Louis R. , Wolfs Roger C. W. , Lemij Hans G. , Tai E‐Shyong , Jonas Jost B. , Cheng Ching‐Yu , Aung Tin , Jansonius Nomdo M. , Klaver Caroline C. W. , Craig Jamie E. , Young Terri L. , Haines Jonathan L. , MacGregor Stuart , Mackey David A. , Pfeiffer Norbert , Wong Tien‐Yin , Wiggs Janey L. , Hewitt Alex W. , van Duijn Cornelia M. , Hammond Christopher J. 
Published: January 2015

ABSTRACTPrimary open‐angle glaucoma is the most common optic neuropathy and an important cause of irreversible blindness worldwide. The optic nerve head or optic disc is divided in two parts: a central cup (without nerve fibers) surrounded by the neuroretinal rim (containing axons of the retinal ganglion cells). The International Glaucoma Genetics Consortium conducted a meta‐analysis of genome‐wide association studies consisting of 17,248 individuals of European ancestry and 6,841 individuals of Asian ancestry. The outcomes of the genome‐wide association studies were disc area and cup area. These specific measurements describe optic nerve morphology in another way than the vertical cup‐disc ratio, which is a clinically used measurement, and may shed light on new glaucoma mechanisms. We identified 10 new loci associated with disc area (CDC42BPA, F5, DIRC3, RARB, ABI3BP, DCAF4L2, ELP4, TMTC2, NR2F2, and HORMAD2) and another 10 new loci associated with cup area (DHRS3, TRIB2, EFEMP1, FLNB, FAM101, DDHD1, ASB7, KPNB1, BCAS3, and TRIOBP). The new genes participate in a number of pathways and future work is likely to identify more functions related to the pathogenesis of glaucoma.
Mean diffusivity of globus pallidus associated with verbal creativity measured by divergent thinking and creativity‐related temperaments in young healthy adults
Authors: Takeuchi Hikaru , Taki Yasuyuki , Sekiguchi Atsushi , Hashizume Hiroshi , Nouchi Rui , Sassa Yuko , Kotozaki Yuka , Miyauchi Carlos Makoto , Yokoyama Ryoichi , Iizuka Kunio , Nakagawa Seishu , Nagase Tomomi , Kunitoki Keiko , Kawashima Ryuta 
Published: January 2015

AbstractRecent investigations revealed mean diffusivity (MD) in gray matter and white matter areas is correlated with individual cognitive differences in healthy subjects and show unique properties and sensitivity that other neuroimaging tools donot have. In this study, we tested the hypothesis that the MD in the dopaminergic system is associated with individual differences in verbal creativity measured by divergent thinking (VCDT) and novelty seeking based on prior studies suggesting associations between these and dopaminergic functions. We examined this issue in a large sample of right‐handed healthy young adults. We used analyses of MD and a psychological measure of VCDT, as well as personality measures of the Temperament and Character Inventory (TCI). Our results revealed associations between higher VCDT and lower MD in the bilateral globus pallidus. Furthermore, not only higher novelty seeking, but also lower harm avoidance, higher self‐directedness, and higher self‐transcendence were robustly associated with lower MD in the right globus pallidus, whereas higher persistence was associated with lower MD in the left globus pallidus. These personality variables were also associated with VCDT. The globus pallidus receives the dopaminergic input from the substantia nigra and plays a key role in motivation which is critically linked to dopamine. These results suggested the MD in the globus pallidus, underlie the association between VCDT and multiple personalities in TCI including novelty seeking. Hum Brain Mapp 36:1808–1827, 2015. © 2015 The Authors Human Brain Mapping Published by Wiley Periodicals, Inc.