bluuebunny/crossref_metadata_2025_split huggingface dataset:
Reducing the Cost and Preserving the Reactivity in Noble‐Metal‐Based Catalysts: Oxidation of CO by Pt and Al–Pt Alloy Clusters Supported on Graphene
Authors: Koizumi Kenichi , Nobusada Katsuyuki , Boero Mauro 
Published: February 2016

AbstractThe oxidation mechanisms of CO to CO2 on graphene‐supported Pt and Pt‐Al alloy clusters are elucidated by reactive dynamical simulations. The general mechanism evidenced is a Langmuir–Hinshelwood (LH) pathway in which O2 is adsorbed on the cluster prior to the CO oxidation. The adsorbed O2 dissociates into two atomic oxygen atoms thus promoting the CO oxidation. Auxiliary simulations on alloy clusters in which other metals (Al, Co, Cr, Cu, Fe, Ni) replace a Pt atom have pointed to the aluminum doped cluster as a special case. In the nanoalloy, the reaction mechanism for CO oxidation is still a LH pathway with an activation barrier sufficiently low to be overcome at room temperature, thus preserving the catalyst efficiency. This provides a generalizable strategy for the design of efficient, yet sustainable, Pt‐based catalysts at reduced cost.
From Umpolung to Alternation: Modified Reactivity of Donor–Acceptor Cyclopropanes Towards Nucleophiles in Reaction with Nitroalkanes
Authors: Budynina Ekaterina M. , Ivanov Konstantin L. , Chagarovskiy Alexey O. , Rybakov Victor B. , Trushkov Igor V. , Melnikov Mikhail Ya. 
Published: February 2016

AbstractA conceptually new type of donor–acceptor cyclopropane reactivity towards nucleophiles has been disclosed. An essential characteristic of the process is an unusual nucleophilic attack on the C(3)‐position of a cyclopropane, combined with typical small ring‐opening by cleavage of the C(1)−C(2) bond between the acceptor and the donor. Based on this new reaction between cyclopropane‐1,1‐diesters and nitroalkanes, we developed a convenient approach to γ‐nitroesters that can be efficiently transformed to the substituted pyrrolidones, structural analogues of racetame family drugs (rolipram, phenylpiracetam, etc.).
Can Cyclen Bind Alkali Metal Azides? A DFT Study as a Precursor to Synthesis
Authors: Bhakhoa Hanusha , Rhyman Lydia , Lee Edmond P. F. , Ramasami Ponnadurai , Dyke John M. 
Published: February 2016

AbstractCan cyclen (1,4,7,10‐tetraazacyclododecane) bind alkali metal azides? This question is addressed by studying the geometric and electronic structures of the alkali metal azide‐cyclen [M(cyclen)N3] complexes using density functional theory (DFT). The effects of adding a second cyclen ring to form the sandwich alkali metal azide‐cyclen [M(cyclen)2N3] complexes are also investigated. N3− is found to bind to a M+(cyclen) template to give both end‐on and side‐on structures. In the end‐on structures, the terminal nitrogen atom of the azide group (N1) bonds to the metal as well as to a hydrogen atom of the cyclen ring through a hydrogen bond in an end‐on configuration to the cyclen ring. In the side‐on structures, the N3 unit is bonded (in a side‐on configuration to the cyclen ring) to the metal through the terminal nitrogen atom of the azide group (N1), and through the other terminal nitrogen atom (N3) of the azide group by a hydrogen bond to a hydrogen atom of the cyclen ring. For all the alkali metals, the N3‐side‐on structure is lowest in energy. Addition of a second cyclen unit to [M(cyclen)N3] to form the sandwich compounds [M(cyclen)2N3] causes the bond strength between the metal and the N3 unit to decrease. It is hoped that this computational study will be a precursor to the synthesis and experimental study of these new macrocyclic compounds; structural parameters and infrared spectra were computed, which will assist future experimental work.
Photochemical Hydrogen Generation Initiated by Oxidative Quenching of the Excited Ru(bpy)32+* by a Bio‐Inspired [2Fe2S] Complex
Authors: Na Yong , Wei Peicheng , Zhou Li 
Published: February 2016

AbstractA diiron dithiolate complex 1 containing 1,8‐naphthalic anhydride bridge was prepared, which possessed the lowest reduction potential for the synthetic diiron complexes modeled on the active site of [FeFe] hydrogenase reported so far. For the first time, oxidative quenching of the excited Ru(bpy)32+* through electron transfer to a bio‐inspired [2Fe2S] complex was corroborated. Hydrogen evolution, driven by visible light, was successfully observed for a three‐component system, consisting of Ru(bpy)32+, complex 1, and EDTA as electron donor in aqueous/organic media. These results provide a basis and also opportunity to develop a photo water splitting system employing Fe‐based catalysts without sacrificial electron donors.
Impact of Awareness and Patterns of Nonhospitalized Atrial Fibrillation on the Risk of Mortality: The Reasons for Geographic And Racial Differences in Stroke (REGARDS) Study
Authors: O'Neal Wesley T. , Efird Jimmy T. , Judd Suzanne E. , McClure Leslie A. , Howard Virginia J. , Howard George , Soliman Elsayed Z. 
Published: February 2016

ABSTRACTBackgroundAlthough mortality associated with atrial fibrillation (AF) has been reported to decrease over prior decades, the mortality risk of asymptomatic, nonhospitalized AF has not been examined.HypothesisAsymptomatic, nonhospitalized AF is associated with an increased risk of death.MethodsThis analysis included 25 976 participants (mean age, 65 ± 9.4 years; 55% female; 38% black) from the Reasons for Geographic And Racial Differences (REGARDS) study. Atrial fibrillation was detected on the baseline electrocardiogram (ECG AF) or by self‐reported history. Atrial fibrillation unawareness was defined as present if ECG evidence of the arrhythmia was detected but no self‐reported history was reported. All‐cause mortality was confirmed during follow‐up through March 31, 2014.ResultsA total of 2208 (8.5%) participants had AF at baseline (ECG: n = 371/17%; self‐reported: n = 1837/83%). Over a median follow‐up of 7.6 years, 3481 deaths occurred. In a multivariable Cox regression model, AF was associated with a 32% increased risk of mortality (95% confidence interval [CI]: 1.19‐1.46). Risk of death was higher among those with ECG AF (hazard ratio: 1.71, 95% CI: 1.42‐2.07) compared with self‐reported cases (hazard ratio: 1.15, 95% CI: 1.03‐1.29). Those who were unaware of their AF diagnosis had a 94% increased risk of death (95% CI: 1.50‐2.52) compared with AF participants who were aware of their diagnosis.ConclusionsAsymptomatic, nonhospitalized AF is associated with an increased risk of mortality in the general population. Mortality is higher in those with ECG‐confirmed cases and among those who are unaware of their diagnosis.
Outlier Eigenvalues for Deformed I.I.D. Random Matrices
Authors: Bordenave Charles , Capitaine Mireille 
Published: February 2016

AbstractWe consider a square random matrix of size N of the form A + Y where A is deterministic and Y has i.i.d. entries with variance 1/N. Under mild assumptions, as N grows the empirical distribution of the eigenvalues of A + Y converges weakly to a limit probability measure β on the complex plane. This work is devoted to the study of the outlier eigenvalues, i.e., eigenvalues in the complement of the support of β. Even in the simplest cases, a variety of interesting phenomena can occur. As in earlier works, we give a sufficient condition to guarantee that outliers are stable and provide examples where their fluctuations vary with the particular distribution of the entries of Y or the Jordan decomposition of A. We also exhibit concrete examples where the outlier eigenvalues converge in distribution to the zeros of a Gaussian analytic function. © 2016 Wiley Periodicals, Inc.
CdS Nanowires Decorated with Ultrathin MoS2 Nanosheets as an Efficient Photocatalyst for Hydrogen Evolution
Authors: He Jie , Chen Lang , Wang Fu , Liu Ying , Chen Peng , Au Chak‐Tong , Yin Shuang‐Feng 
Published: February 2016

AbstractCdS nanowires decorated with ultrathin MoS2 nanosheets were synthesized for the first time by ultrasonic exfoliation by using dimethylformamide as the dispersing agent. An excellent hydrogen evolution rate of 1914 μmol h−1 (20 mg catalyst) under visible‐light irradiation (λ≥400 nm, ≈154 mW cm−1) and an apparent quantum yield of 46.9 % at λ=420 nm were achieved over the MoS2/CdS composite. The presence of ultrathin MoS2 nanosheets (rich in active edge sites) on the CdS surface promotes the separation of photogenerated charge carriers and facilitates the surface processes of photocatalytic hydrogen evolution.
A New 1,3,4‐Oxadiazole‐Based Hole‐Transport Material for Efficient CH3NH3PbBr3 Perovskite Solar Cells
Authors: Carli Stefano , Baena Juan Pablo Correa , Marianetti Giulia , Marchetti Nicola , Lessi Marco , Abate Antonio , Caramori Stefano , Grätzel Michael , Bellina Fabio , Bignozzi Carlo Alberto , Hagfeldt Anders 
Published: February 2016

AbstractA new hole‐transport material (HTM) based on the 1,3,4‐oxadiazole moiety (H1) was prepared through a single‐step synthetic pathway starting from commercially available products. Thanks to a deep HOMO level, H1 was used as HTM in CH3NH3PbBr3 perovskite solar cells yielding an efficiency of 5.8 %. The reference HTM (Spiro‐OMeTAD), under the same testing conditions, furnished a lower efficiency of 5.1 %. Steady‐state and time‐resolved photoluminescence of the thin films showed good charge‐extraction dynamics for H1 devices. In addition, H1 shows a large thermal stability and completely amorphous behavior (as evaluated by thermal gravimetric analysis and differential scanning calorimetry).
Structure and function of gene regulatory networks associated with worker sterility in honeybees
Authors: Sobotka Julia A. , Daley Mark , Chandrasekaran Sriram , Rubin Benjamin D. , Thompson Graham J. 
Published: February 2016

AbstractA characteristic of eusocial bees is a reproductive division of labor in which one or a few queens monopolize reproduction, while her worker daughters take on reproductively altruistic roles within the colony. The evolution of worker reproductive altruism involves indirect selection for the coordinated expression of genes that regulate personal reproduction, but evidence for this type of selection remains elusive. In this study, we tested whether genes coexpressed under queen‐induced worker sterility show evidence of adaptive organization within a model brain transcriptional regulatory network (TRN). If so, this structured pattern would imply that indirect selection on nonreproductive workers has influenced the functional organization of genes within the network, specifically to regulate the expression of sterility. We found that literature‐curated sets of candidate genes for sterility, ranging in size from 18 to 267, show strong evidence of clustering within the three‐dimensional space of the TRN. This finding suggests that our candidate sets of genes for sterility form functional modules within the living bee brain's TRN. Moreover, these same gene sets colocate to a single, albeit large, region of the TRN's topology. This spatially organized and convergent pattern contrasts with a null expectation for functionally unrelated genes to be haphazardly distributed throughout the network. Our meta‐genomic analysis therefore provides first evidence for a truly “social transcriptome” that may regulate the conditional expression of honeybee worker sterility.
The fate of the Arctic seaweed Fucus distichus under climate change: an ecological niche modeling approach
Authors: Jueterbock Alexander , Smolina Irina , Coyer James A. , Hoarau Galice 
Published: February 2016

AbstractRising temperatures are predicted to melt all perennial ice cover in the Arctic by the end of this century, thus opening up suitable habitat for temperate and subarctic species. Canopy‐forming seaweeds provide an ideal system to predict the potential impact of climate‐change on rocky‐shore ecosystems, given their direct dependence on temperature and their key role in the ecological system. Our primary objective was to predict the climate‐change induced range‐shift of Fucus distichus, the dominant canopy‐forming macroalga in the Arctic and subarctic rocky intertidal. More specifically, we asked: which Arctic/subarctic and cold‐temperate shores of the northern hemisphere will display the greatest distributional change of F. distichus and how will this affect niche overlap with seaweeds from temperate regions? We used the program MAXENT to develop correlative ecological niche models with dominant range‐limiting factors and 169 occurrence records. Using three climate‐change scenarios, we projected habitat suitability of F. distichus – and its niche overlap with three dominant temperate macroalgae – until year 2200. Maximum sea surface temperature was identified as the most important factor in limiting the fundamental niche of F. distichus. Rising temperatures were predicted to have low impact on the species' southern distribution limits, but to shift its northern distribution limits poleward into the high Arctic. In cold‐temperate to subarctic regions, new areas of niche overlap were predicted between F. distichus and intertidal macroalgae immigrating from the south. While climate‐change threatens intertidal seaweeds in warm‐temperate regions, seaweed meadows will likely flourish in the Arctic intertidal. Although this enriches biodiversity and opens up new seaweed‐harvesting grounds, it will also trigger unpredictable changes in the structure and functioning of the Arctic intertidal ecosystem.
Compact AC/DC Susceptometer Using a High‐Temperature Superconducting Quantum Interference Device
Authors: TAKAGI RYUKI , SAARI MOHD MAWARDI , SAKAI KENJI , KIWA TOSHIHIKO , TSUKADA KEIJI 
Published: February 2016

SUMMARYWe developed a compact susceptometer employing a high‐temperature superconductor (HTS) superconducting quantum interference device (SQUID) that can measure the M–H characteristics and the harmonic components induced in the ac magnetic field response from a sample. In the dc function for measuring M–H characteristics, the sample was vibrated in a dc magnetic field, and the secondary magnetic field generated from the sample was detected by a dc pickup coil. In the ac function for measuring harmonic components, the sample placed in an ac magnetic field, and the ac response was detected by an ac pickup coil. The pickup coil is connected in series with the input coil, which is inductively connected to the HTS‐SQUID. A signal from the HTS‐SQUID was transmitted to a lock‐in amplifier and was analyzed as the intensity and phase of the measured magnetic field. In order to clarify the basic properties of the system, we measured the ac magnetic field response from a sample while varying the relative positions of the sample and the pickup coil, and the M–H characteristics while varying the dc bias magnetic field intensity. Furthermore, by analyzing the harmonic components of the ac/dc magnetic field response, the proposed system can measure magnetic field properties with high sensitivity and at high speed.
Magnetoencephalographic Correlates of Apparent Motion Illusion of Beta Movement
Authors: IMAI AKIRA , TAKASE HIROKI , TANAKA KEITA , UCHIKAWA YOSHINORI 
Published: February 2016

SUMMARYWe examined the underlying mechanisms of the apparent motion illusion of beta movement by obtaining neuromagnetic responses of event‐related fields (ERFs). A simple setting for visual stimulation of two circles, presented 10° apart horizontally, was used in experiment 1. The first circle, with a duration of 16.7 ms, was followed by the second with three conditions of stimulus‐onset‐asynchrony: (a) 16.7 ms, the two circles seen almost simultaneously, (b) 83.3 ms, perceived optimally as beta movement, and (c) 549.8 ms occurring isolatedly. In experiment 2, three conditions of real motion for visual stimulation were set: (a) six circles presented successively for one animation, (b) 14 circles for one animation, and (c) 34 circles for one animation. We applied minimum current estimates (MCEs) to obtain the source activity of the ERFs for beta movement, then calculated an average amplitude for each five 100‐ms epoch after the second stimulus onset in experiment 1, and after the first stimulus onset in experiment 2. As the results, the optimal condition showed maximum activities in the first 100‐ms epoch at the parietal region in experiment 1, suggesting that the motion components of the MCEs were emerging from this epoch. In experiment 2, three conditions of real motion evoked prolonged MCE activities for the temporal and central areas, suggesting that these components were changed with the “speed” of motion perception. The neuromagnetic activities of beta movement and motion perception may originate from parietal areas within 100 ms after the perception of movement.
Valorization of soursop flowers (Annona muricata L.) as potent source of natural antioxidants for stabilization of palm olein during accelerated storage
Authors: Womeni Hilaire Macaire , Tonfack Djikeng Fabrice , Iruku Naga Satya Surya Prabhakar , Karuna Mallampalli Sri Lakshmi , Prasad Rachapudi Badari Narayana , Linder Michel 
Published: February 2016

AbstractThis study investigates the effect of soursop flowers methanolic extract on the physicochemical characteristics of palm olein during accelerated storage. After analysis of the extract by determining its total phenolic content by colorimetry and identification of some of its phenolic antioxidants by HPLC‐DAD(Diode Array Detector), preliminary antioxidants tests have been done. After that, the extract was added in palm olein at concentrations 200–1800 ppm. BHT, at 200 ppm served as standard besides the Control. Induction time, peroxide, p‐anisidine, Total oxidation (TOTOX), thiobarbituric acid and iodine values, as well as changes in linoleic acid profile Gas Chromatography/Flamme Ionization Detector (GC/FID) of oil during the storage were evaluated. Results showed soursop flower extract to be rich in phenolic antioxidants and to be efficient, at all concentrations, in delaying palm olein oxidation on Rancimat and accelerated Schaal oven test of 30 days at 70°C. Soursop flowers might be used as potent source of antioxidants for the stabilization of palm olein.
Anaplastic thyroid carcinoma: Failure of conventional therapy but hope of targeted therapy
Authors: Lennon Paul , Deady Sandra , Healy Maire L. , Toner Mary , Kinsella John , Timon Conrad I. , O'Neill James P. 
Published: February 2016

AbstractBackgroundAnaplastic thyroid cancer has a median survival between 1.2 and 10 months. The purpose of our study was to evaluate the outcomes of patients with anaplastic thyroid cancer in Ireland.MethodsWe carried out a retrospective analysis of the Irish National Cancer Database for patients with anaplastic thyroid cancer between 2000 and 2010.ResultsOf a total of 64 patients (40 women, 24 men), the median age was 69 years, and 29.7% of the patients had distant metastases. The overall median survival was 2.3 months and the 1, 2, and 5‐year survival was 12.5%, 6.25%, and 4.69%, respectively. On univariate analysis age, sex, metastases at diagnosis, and multimodality treatment were statistically significant indicators of prognosis, and metastases at diagnosis remained statistically significant on multivariate analysis.ConclusionThese results correlate with the American Thyroid Association (ATA) guidelines, in which, when possible, multimodality therapy offers a survival advantage to a select group of patients. Novel therapies may offer the greatest hope for these patients. © 2016 Wiley Periodicals, Inc. Head Neck 38: E1122–E1129, 2016
Collocation of hydrological and biological attenuation of nitrate in an urban stream
Authors: Klein Trevor , Toran Laura 
Published: February 2016

AbstractThe hydrologic and biogeochemical processes that control nutrient export in urban streams are not well understood. Attenuation can occur by tributary dilution, groundwater discharge, and biological processing both in the water column and the hyporheic zone. A wastewater treatment plant on Pennypack Creek, an urban stream near Philadelphia, PA, provided high nitrate concentrations for analysis of downstream attenuation processes. Longitudinal sampling for an 8‐km reach revealed decreases in nitrate concentration of 2 mg l−1 at high flow and 4.5 mg l−1 during low flow. During high flow, δ15N‐NO3 increased from 9.5 to 10.5‰ and during low flow increased from 10.1 to 11.1‰. Two reaches were sampled at fine spatial intervals (approximately 200 m) to better identify attenuation processes. Mixing analysis indicated that groundwater discharge and biological processing both control nitrate concentration and isotope signatures. However, fine‐scaled sampling did not reveal spatially discrete zones; instead, these processes were occurring simultaneously. While both processes attenuate nitrate, they have opposite isotope signatures, which may have muted changes in δ15N‐NO3. At high flow, a decrease in Cl/NO3 ratios helped distinguish groundwater discharge occurring along both finely sampled reaches. At low flow, biological processing seemed to be occurring more extensively, but the δ15N‐NO3 signature was not consistent with either a single process or a sequential combination of groundwater dilution and biological nitrate attenuation. The collocation of processes makes it more difficult to assess biological processing hot spots and predict how urbanization and subsequent stream restoration influence nitrate attenuation. Copyright © 2016 John Wiley & Sons, Ltd.
Testing the functional assessment of mentation: A mobile application based assessment of mental status
Authors: Hamilton David E. , Press Valerie G. , Twu Nicole M. , Yuen Trevor C. , Azu Crystal N. , Churpek Matthew M. , Edelson Dana P. 
Published: February 2016

BACKGROUNDAltered mental status is a significant predictor of mortality in hospitalized patients and a prerequisite component to the diagnosis of delirium. However, the detection of altered mental status is often incomplete, inaccurate, and resource intensive.OBJECTIVETo identify the clinical utility and feasibility of the Functional Assessment of Mentation (FAMTM), a mobile application for evaluating attention and recall.DESIGNProspective observational pilot study.SETTINGTertiary care medical center.PARTICIPANTSNine hundred thirty‐one adult subjects (612 nonhospitalized and 319 hospitalized).MEASUREMENTSScore distribution and time to FAMTM completion were compared between nonhospitalized and hospitalized subjects (as well as between hospitalized subjects discharged home and those not discharged home). Additionally, in the hospitalized subgroup, FAMTM was compared to the Glasgow Coma Scale (GCS), using the Short Portable Mental Status Questionnaire (SPMSQ) as our criterion standard for altered mental status assessment.RESULTSMedian time to completion of FAMTM was 55 seconds (interquartile range [IQR], 45–67 seconds). Our data identified a graded reduction in score comparing nonhospitalized subjects to hospitalized subjects discharged home and not discharged home (median 5 [IQR 4–7] vs 5 [IQR 3–6] vs 3 [IQR 1–5]; P < 0.001). In the hospitalized subset, FAMTM scores were more highly correlated to SPMSQ (Spearman ρ = 0.27, P < 0.001) compared to GCS (Spearman ρ = 0.05, P = 0.40).CONCLUSIONSFAMTM is a rapid and clinically feasible tool that can identify minor alterations in mental status often missed by GCS. Journal of Hospital Medicine 2016;11:463–466. 2016 Society of Hospital Medicine
Imaging synucleinopathies
Authors: Brooks David J. , Tambasco Nicola 
Published: February 2016

ABSTRACTIn this review the structural and functional imaging changes associated with the synucleinopathies PD, MSA, and dementias associated with Lewy bodies are reviewed. The role of imaging for supporting differential diagnosis, detecting subclinical disease, and following disease progression is discussed and its potential use for monitoring disease progression is debated. © 2016 International Parkinson and Movement Disorder Society