bluuebunny/crossref_metadata_2025_split huggingface dataset:
Spatial correlations in bed load transport: Evidence, importance, and modeling
Authors: Heyman J. , Ma H. B. , Mettra F. , Ancey C. 
Published: July 2014

AbstractThis article examines the spatial dynamics of bed load particles in water. We focus particularly on the fluctuations of particle activity, which is defined as the number of moving particles per unit bed length. Based on a stochastic model recently proposed by Ancey and Heyman (2014), we derive the second moment of particle activity analytically, that is, the spatial correlation functions of particle activity. From these expressions, we show that large moving particle clusters can develop spatially. Also, we provide evidence that fluctuations of particle activity are scale dependent. Two characteristic lengths emerge from the model: a saturation length ℓsat describing the length needed for a perturbation in particle activity to relax to the homogeneous solution and a correlation length ℓc describing the typical size of moving particle clusters. A dimensionless Péclet number can also be defined according to the transport model. Three different experimental data sets are used to test the theoretical results. We show that the stochastic model describes spatial patterns of particle activity well at all scales. In particular, we show that ℓc and ℓsat may be relatively large compared to typical scales encountered in bed load experiments (grain diameter, water depth, bed form wavelength, flume length, etc.) suggesting that the spatial fluctuations of particle activity have a nonnegligible impact on the average transport process.
Observations of plasma waves in the colliding jet region of a magnetic flux rope flanked by two active X lines at the subsolar magnetopause
Authors: Øieroset M. , Sundkvist D. , Chaston C. C. , Phan T. D. , Mozer F. S. , McFadden J. P. , Angelopoulos V. , Andersson L. , Eastwood J. P. 
Published: July 2014

AbstractWe have performed a detailed analysis of plasma and wave observations in a magnetic flux rope encountered by the THEMIS‐D spacecraft at the subsolar magnetopause. The extent of the flux rope was ∼270 ion skin depths in the outflow direction, and it was flanked by two active X lines producing colliding plasma jets in the flux rope core where ion heating and suprathermal electrons were observed. The colliding jet region was highly dynamic and characterized by enhanced wave power in a broad frequency range. High‐frequency waves, including ion acoustic‐like waves, electron holes, and whistler mode waves, were observed in a limited spatial region near the flux rope center and did not appear to be associated with the observed large‐scale heating and energization. Low‐frequency kinetic Alfvén waves, on the other hand, were enhanced in the entire flux rope core, suggesting a possible link with the observed ion heating.
Approximate Bayesian Computation using Markov Chain Monte Carlo simulation: DREAM(ABC)
Authors: Sadegh Mojtaba , Vrugt Jasper A. 
Published: July 2014

AbstractThe quest for a more powerful method for model evaluation has inspired Vrugt and Sadegh (2013) to introduce “likelihood‐free” inference as vehicle for diagnostic model evaluation. This class of methods is also referred to as Approximate Bayesian Computation (ABC) and relaxes the need for a residual‐based likelihood function in favor of one or multiple different summary statistics that exhibit superior diagnostic power. Here we propose several methodological improvements over commonly used ABC sampling methods to permit inference of complex system models. Our methodology entitled DREAM(ABC)uses the DiffeRential Evolution Adaptive Metropolis algorithm as its main building block and takes advantage of a continuous fitness function to efficiently explore the behavioral model space. Three case studies demonstrate that DREAM(ABC)is at least an order of magnitude more efficient than commonly used ABC sampling methods for more complex models. DREAM(ABC)is also more amenable to distributed, multi‐processor, implementation, a prerequisite to diagnostic inference of CPU‐intensive system models.
Assessing the value of seasonal climate forecast information through an end‐to‐end forecasting framework: Application to U.S. 2012 drought in central Illinois
Authors: Shafiee‐Jood Majid , Cai Ximing , Chen Ligang , Liang Xin‐Zhong , Kumar Praveen 
Published: July 2014

AbstractThis study proposes an end‐to‐end forecasting framework to incorporate operational seasonal climate forecasts to help farmers improve their decisions prior to the crop growth season, which are vulnerable to unanticipated drought conditions. The framework couples a crop growth model with a decision‐making model for rainfed agriculture and translates probabilistic seasonal forecasts into more user‐related information that can be used to support farmers' decisions on crop type and some market choices (e.g., contracts with ethanol refinery). The regional Climate‐Weather Research and Forecasting model (CWRF) driven by two operational general circulation models (GCMs) is used to provide the seasonal forecasts of weather parameters. To better assess the developed framework, CWRF is also driven by observational reanalysis data, which theoretically can be considered as the best seasonal forecast. The proposed framework is applied to the Salt Creek watershed in Illinois that experienced an extreme drought event during 2012 crop growth season. The results show that the forecasts cannot capture the 2012 drought condition in Salt Creek and therefore the suggested decisions can make farmers worse off if the suggestions are adopted. Alternatively, the optimal decisions based on reanalysis‐based CWRF forecasts, which can capture the 2012 drought conditions, make farmers better off by suggesting “no‐contract” with ethanol refineries. This study suggests that the conventional metric used for ex ante value assessment is not capable of providing meaningful information in the case of extreme drought. Also, it is observed that institutional interventions (e.g., crop insurance) highly influences farmers' decisions and, thereby, the assessment of forecast value.
In Vitro Bacterial Screening and Degradation Kinetics of a Terpolymer Ligand and Its Transition Metal Complexes
Authors: Ahamed Mohamed A. Riswan , Azarudeen Raja S. , Prabu N. , Burkanudeen Abdul R. 
Published: July 2014

ABSTRACTA novel terpolymer ligand involving 2‐amino‐6‐nitro‐benzothiazole–semicarbazide–formaldehyde was synthesized in a 1:1:2 mole ratio with a dimethylformamide reaction medium at 150 ± 2°C for 6 h. The synthesized ligand was used to prepare various metal complexes with Cu2+, Ni2+, and Zn2+ metal ions. The structure of the terpolymer ligand and its complexes were confirmed based on elemental analysis, molecular weight measurements, molar conductivity, magnetic susceptibilities, Fourier transform infrared, electronic, electron spin resonance, and 1H and 13C nuclear magnetic resonance spectroscopy. Scanning electronic microscopy and X‐ray diffraction method were used to analyze the morphological features of the terpolymer and its metal complexes. The thermal stabilities of the terpolymer and its metal complexes were determined using thermogravimetric analysis. Kinetic parameters such as activation energy (Ea) and order of reaction (n), thermodynamic parameters, viz. entropy change (ΔS), free energy change (ΔF), apparent entropy (S*), and frequency factor (Z) were calculated using Sharp–Wentworth and Freeman–Carroll methods. The thermal degradation mechanism was also proposed for both the terpolymer ligand and its complexes using the Phadnis–Deshpande method. The terpolymer ligand and its complexes were screened for antibacterial activities against selected microorganisms such as Shigella sonnei, Escherichia coli, Klebsiella species, Staphylococcus aureus, Bacillus subtilis, and Salmonella typhimurium.
One‐Pot Copper‐Catalyzed Aerobic Decarboxylative Coupling of Phenylacetic Acids with o‐Aminobenzenes and Dioxygen as the Oxidant Leading to Benzoxazoles and Benzothiazoles
Authors: Yang Daoshan , Yan Kelu , Wei Wei , Tian Laijin , Shuai Yuanyuan , Li Ruixia , You Jinmao , Wang Hua 
Published: July 2014

AbstractA simple and practical copper‐catalyzed one‐pot method for the synthesis of benzoxazole and benzothiazole derivatives has been developed. The protocol uses inexpensive CuSO4 as the catalyst, readily available substituted phenylacetic acids and o‐aminobenzenes as the starting materials, and dioxygen as the sole oxidant. The corresponding benzoxazoles and benzothiazoles were obtained in moderate to good yields. The procedure is based on sequential copper‐catalyzed decarboxylation and aerobic cyclization reactions. This method should provide a useful strategy for the construction of heterocycles.
Local Transient Unfolding of Native State PAI‐1 Associated with Serpin Metastability
Authors: Trelle Morten B. , Madsen Jeppe B. , Andreasen Peter A. , Jørgensen Thomas J. D. 
Published: July 2014

AbstractThe metastability of the native fold makes serpin (serine protease inhibitor) proteins prone to pathological conformational change, often by insertion of an extra β‐strand into the central β‐sheet A. How this insertion is made possible is a hitherto unresolved question. By the use of advanced hydrogen/deuterium‐exchange mass spectrometry (HDX‐MS) it is shown that the serpin plasminogen activator inhibitor 1 (PAI‐1) transiently unfolds under native condition, on a second‐to‐minute time scale. The unfolding regions comprise β‐strand 5A as well as the underlying hydrophobic core, including β‐strand 6B and parts of helices A, B, and C. Based thereon, a mechanism is proposed by which PAI‐1 makes transitions through progressively more unfolded states along the reaction coordinate to the inactive, so‐called latent form. Our results highlight the profound utility of HDX‐MS in detecting sparsely populated, transiently unfolded protein states.
Asymmetric Hydroxylative Phenol Dearomatization Promoted by Chiral Binaphthylic and Biphenylic Iodanes
Authors: Bosset Cyril , Coffinier Romain , Peixoto Philippe A. , El Assal Mourad , Miqueu Karinne , Sotiropoulos Jean‐Marc , Pouységu Laurent , Quideau Stéphane 
Published: July 2014

AbstractThe long‐standing quest for chiral hypervalent organoiodine compounds (i.e., iodanes) as metal‐free reagents for asymmetric synthesis continues. Although remarkable progress has recently been made in organoiodine‐catalyzed reactions using a terminal oxidant in stoichiometric amounts, there is still a significant need for “flaskable” chiral iodane reagents. Herein, we describe the synthesis of new iodobinaphthyls and iodobiphenyls, their successful and selective DMDO‐mediated oxidation into either λ3‐ or λ5‐iodanes, and the evaluation of their capacity to promote asymmetric hydroxylative phenol dearomatization (HPD) reactions. Most notably, a C2‐symmetrical biphenylic λ5‐iodane promoted the HPD‐induced conversion of the monoterpene thymol into the corresponding ortho‐quinol‐based [4+2] cyclodimer (i.e., bis(thymol)) with enantiomeric excesses of up to 94 %.
A Fast Deposition‐Crystallization Procedure for Highly Efficient Lead Iodide Perovskite Thin‐Film Solar Cells
Authors: Xiao Manda , Huang Fuzhi , Huang Wenchao , Dkhissi Yasmina , Zhu Ye , Etheridge Joanne , Gray‐Weale Angus , Bach Udo , Cheng Yi‐Bing , Spiccia Leone 
Published: July 2014

AbstractThin‐film photovoltaics based on alkylammonium lead iodide perovskite light absorbers have recently emerged as a promising low‐cost solar energy harvesting technology. To date, the perovskite layer in these efficient solar cells has generally been fabricated by either vapor deposition or a two‐step sequential deposition process. We report that flat, uniform thin films of this material can be deposited by a one‐step, solvent‐induced, fast crystallization method involving spin‐coating of a DMF solution of CH3NH3PbI3 followed immediately by exposure to chlorobenzene to induce crystallization. Analysis of the devices and films revealed that the perovskite films consist of large crystalline grains with sizes up to microns. Planar heterojunction solar cells constructed with these solution‐processed thin films yielded an average power conversion efficiency of 13.9±0.7 % and a steady state efficiency of 13 % under standard AM 1.5 conditions.
Catalytic 1,4‐Rhodium(III) Migration Enables 1,3‐Enynes to Function as One‐Carbon Oxidative Annulation Partners in CH Functionalizations
Authors: Burns David J. , Lam Hon Wai 
Published: July 2014

Abstract1,3‐Enynes containing allylic hydrogens cis to the alkyne are shown to act as one‐carbon partners, rather than two‐carbon partners, in various rhodium‐catalyzed oxidative annulations. The mechanism of these unexpected transformations is proposed to occur through double CH activation, involving a hitherto rare example of the 1,4‐migration of a RhIII species. This phenomenon is general across a variety of substrates, and provides a diverse range of heterocyclic products.
Breath figure templated semifluorinated block copolymers with tunable surface properties and binding capabilities
Authors: Valtola Lauri , Karesoja Mikko , Tenhu Heikki , Ihalainen Petri , Sarfraz Jawad , Peltonen Jouko , Malinen Melina , Urtti Arto , Hietala Sami 
Published: July 2014

ABSTRACTPatterning of functionalized polymeric surfaces enables the adjustment of their characteristics and use in novel applications. We prepared breath figure (BF) films from three semifluorinated diblock copolymers, which all are composed of a polystyrene block and a semifluorinated one to compare their surface properties. “Click” chemistry was employed to one of the polymers, containing a poly(pentafluorostyrene) block to incorporate hydrophilic sugar or carboxylic acid moieties. The structure of the polymer alters the obtained porous morphology of the films. Contact angle (CA) analyses of the BF films reveals that the surface porosity increases water CAs compared with solvent cast films, and, in the case of hydrophobic polymers, leads to significant increase in the CAs of dodecane. The hydrophobicity of the BF films is further amplified by the removal of the topmost layer which leads in some cases to superhydrophobic surfaces. BF films containing glucose units are hydrophilic exhibiting water CAs below 90°. These glycosylated porous surfaces are shown to bind lectin Con A‐FITC or can be labelled with isothiocyanate marker. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 41225.
Hydrogenation of Imines Catalyzed by Trisphosphine‐Substituted Molybdenum and Tungsten Nitrosyl Hydrides and Co‐Catalytic Acid
Authors: Chakraborty Subrata , Blacque Olivier , Fox Thomas , Berke Heinz 
Published: July 2014

AbstractHydride complexes Mo,W(CO)(NO)H(mer‐etpip) (iPr2PCH2CH2)2PPh=etpip) (2 a,b(syn), syn and anti of NO and Ph(etpip) orientions) were prepared and probed in imine hydrogenations together with co‐catalytic [H(Et2O)2][B(C6F5)4] (140 °C, 60 bar H2). 2 a,b(syn) were obtained via reduction of syn/anti‐Mo,W(NO)Cl3(mer‐etpip) and syn,anti‐Mo,W(NO)(CO)Cl(mer‐etpip). [H(Et2O)2][B(C6F5)4] in THF converted the hydrides into THF complexes syn‐[Mo,W(NO)(CO)(etpip)(THF)][B(C6F5)4]. Combinations of the p‐substituents of aryl imines p‐R1C6H4CH=N‐p‐C6H4R2 (R1,R2=H,F,Cl,OMe,α‐Np) were hydrogenated to amines (maximum initial TOFs of 1960 h−1 (2 a(syn)) and 740 h−1 (2 b(syn)) for N‐(4‐methoxybenzylidene)aniline). An ‘ionic hydrogenation’ mechanism based on linear Hammett plots (ρ=−10.5, p‐substitution on the C‐side and ρ=0.86, p‐substitution on the N‐side), iminium intermediates, linear P(H2) dependence, and DKIE=1.38 is proposed. Heterolytic splitting of H2 followed by ‘proton before hydride’ transfers are the steps in the ionic mechanism where H2 ligand addition is rate limiting.
Feasibility of reirradiation in the treatment of locally recurrent rectal cancer
Authors: Bosman S J , Holman F A , Nieuwenhuijzen G A P , Martijn H , Creemers G-J , Rutten H J T 
Published: July 2014

Abstract

Background
Many patients with locally recurrent rectal cancer receive radiotherapy for the treatment of the primary tumour. It is unclear whether reirradiation is safe and effective when a local recurrence develops. The aim of this study was to evaluate the toxicity and oncological outcome of reirradiation in patients with locally recurrent rectal carcinoma.

Methods
From March 1994 until December 2013, data on patients with locally recurrent rectal cancer (without distant metastasis) were entered into a database. Patients were reirradiated with a reduced dose of 30 Gy and received an intraoperative electron radiotherapy boost during surgery. Morbidity associated with radiotherapy, postoperative complications and oncological outcome were evaluated.

Results
Clear margins (R0) were obtained in 75 (55·6 per cent) of the 135 patients who were reirradiated. Forty-six patients developed serious postoperative complications and the 30-day mortality rate was 4·6 per cent. Multivariable analysis showed that margin status was the main factor influencing oncological outcome (hazard ratio for overall survival 2·51 for R1 and 3·19 for R2versus R0 resection; both P &lt; 0·001). There was no significant difference in survival between the reirradiated group and a group of 113 patients who had full-course irradiation (5-year overall survival rate 34·1 and 39·1 per cent respectively; P = 0·278). Both reirradiation and full-course irradiation were associated with better survival than no irradiation in a historical control group of 24 patients (5-year overall survival rate 23 per cent; P = 0·225 and P = 0·062).

Conclusion
Reirradiation (with concomitant chemotherapy) has few side-effects and complements radical resection of recurrent rectal cancer.
Co‐culture of bone marrow‐derived mesenchymal stem cells overexpressing lipocalin 2 with HK‐2 and HEK293 cells protects the kidney cells against cisplatin‐induced injury
Authors: Halabian Raheleh , Roudkenar Mehryar Habibi , Jahanian‐Najafabadi Ali , Hosseini Kamran Mousavi , Tehrani Hossein Abdul 
Published: July 2014

AbstractConditioned medium of mesenchymal stem cells (MSCs) is now being used for its cytoprotective effects, especially when the cells are equipped with cytoprotective factors to strengthen them against unfavorable microenvironments. Overexpression of Lcn2 in MSCs mimics in vivo kidney injury. Hence, unraveling how Lcn2‐engineered MSCs affect kidney cells has been investigated. Cisplatin treated HK‐2 or HEK293 kidney cells were co‐cultivated with Lcn2 overexpressing MSCs in upper and lower chambers of transwell plates. Proliferation, apoptosis, and expression of growth factors and cytokines were assessed in the kidney cells. Co‐cultivation with the MSCs‐Lcn2 not only inhibited cisplatin‐induced cytotoxicity in the HK‐2 and HEK293 cells, but increased proliferation rate, prevented cisplatin‐induced apoptosis, and increased expression of growth factors and the amount of antioxidants in the kidney cells. Thus Lcn2‐engineered MSCs can ameliorate and repair injured kidney cells in vitro, which strongly suggests there are beneficial effects of the MSCs‐Lcn2 in cell therapy of kidney injury.
Abnormal Anti‐Quenching and Controllable Multi‐Transitions of Bi3+ Luminescence by Temperature in a Yellow‐Emitting LuVO4:Bi3+ Phosphor for UV‐Converted White LEDs
Authors: Kang Fengwen , Peng Mingying , Zhang Qinyuan , Qiu Jianrong 
Published: July 2014

AbstractPhosphors with an efficient yellow‐emitting color play a crucial role in phosphor‐converted white LEDs (pc‐WLEDs), but popular yellow phosphors such as YAG:Ce or Eu2+‐doped (oxy)nitrides cannot smoothly meet this seemingly simple requirement due to their strong absorptions in the visible range. Herein, we report a novel yellow‐emitting LuVO4:Bi3+ phosphor that can solve this shortcoming. The emission from LuVO4:Bi3+ shows a peak at 576 nm with a quantum efficiency (QE) of up to 68 %, good resistance to thermal quenching (T50 %=573 K), and no severe thermal degradation after heating–cooling cycles upon UV excitation. The yellow emission, as verified by X‐ray photoelectron spectra (XPS), originates from the (3P0,3P1)→1S0 transitions of Bi3+. Increasing the temperature from 10 to 300 K produces a temperature‐dependent energy‐transfer process between VO43− groups and Bi3+, and further heating of the samples to 573 K intensifies the emission. However, it subsequently weakens, accompanied by blueshifts of the emission peaks. This abnormal anti‐thermal quenching can be ascribed to temperature‐dependent energy transfer from VO43− groups to Bi3+, a population redistribution between the excited states of 3P0 and 3P1 upon thermal stimulation, and discharge of electrons trapped in defects with a trap depth of 359 K. Device fabrication with the as‐prepared phosphor LuVO4:Bi3+ has proved that it can act as a good yellow phosphor for pc‐WLEDs.
Palladium Nanoparticles Bonded to Two‐Dimensional Iron Oxide Graphene Nanosheets: A Synergistic and Highly Reusable Catalyst for the Tsuji–Trost Reaction in Water and Air
Authors: Liu Jian , Huo Xing , Li Tianrong , Yang Zhengyin , Xi Pinxian , Wang Zhiyi , Wang Baodui 
Published: July 2014

AbstractLow cost, high activity and selectivity, convenient separation, and increased reusability are the main requirements for noble‐metal‐nanocatalyst‐catalyzed reactions. Despite tremendous efforts, developing noble‐metal nanocatalysts to meet the above requirements remains a significant challenge. Here we present a general strategy for the preparation of strongly coupled Fe3O4 and palladium nanoparticles (PdNPs) to graphene sheets by employing polyethyleneimine as the coupling linker. Transmission electron microscopic images show that Pd and Fe3O4 nanoparticles are highly dispersed on the graphene surface, and the mean particle size of Pd is around 3 nm. This nanocatalyst exhibits synergistic catalysis by Pd nanoparticles supported on reduced graphene oxide (rGO) and a tertiary amine of polyethyleneimine (Pd/Fe3O4/PEI/rGO) for the Tsuji–Trost reaction in water and air. For example, the reaction of ethyl acetoacetate with allyl ethyl carbonate afforded the allylated product in more than 99 % isolated yield, and the turnover frequency reached 2200 h−1. The yield of allylated products was 66 % for Pd/rGO without polyethyleneimine. The catalyst could be readily recycled by a magnet and reused more than 30 times without appreciable loss of activity. In addition, only about 7.5 % of Pd species leached off after 20 cycles, thus rendering this catalyst safer for the environment.
Total Synthesis of Isoquinocyclinone
Authors: Dischmann Mike , Frassetto Timo , Breuning M. André , Koert Ulrich 
Published: July 2014

AbstractThe total synthesis of the heptacyclic natural product isoquinocyclinone has been achieved. A Hauser annulation was used to assemble the anthraquinone core structure. The unique 2,4,5,6‐tetrahydropyrrolo[2,3‐b]pyrrole substructure was prepared by alkyne addition to a lactone intermediate and subsequent Ni0‐mediated cyanide addition, the conversion of an O,O‐ into an N,O‐acetal, and final intramolecular N‐alkylation.
From Double‐Four‐Ring Germanosilicates to New Zeolites: In Silico Investigation
Authors: Trachta Michal , Bludský Ota , Čejka Jiří , Morris Russell E. , Nachtigall Petr 
Published: July 2014

AbstractTo date, the majority of zeolites have been prepared by the solvothermal route using organic structure directing agents. Two new zeolites with structural codes PCR and OKO were recently prepared from UTL germanosilicate by removal of the double‐four ring (D4R) connecting the dense two‐dimensional layers [Nature Chem. 2013, 5, 628]. The corresponding experimental protocol, Assembly–Disassembly–Organization–Reassembly (ADOR), is explored in this contribution with an in silico investigation. The structure and properties of hypothetical zeolites that could be obtained from zeolites with IWW, IWV, IWR, ITR, and ITH topologies using the ADOR protocol are reported based on a computational investigation. A total of 20 new structures are presented together with their characteristics.