bluuebunny/crossref_metadata_2025_split huggingface dataset:
Electrochemical and Resonance Raman Spectroscopic Studies of Water‐Oxidizing Ruthenium Terpyridyl–Bipyridyl Complexes
Authors: Keidel Anke , López Isidoro , Staffa Jana , Kuhlmann Uwe , Bozoglian Fernando , Gimbert‐Suriñach Carolina , Benet‐Buchholz Jordi , Hildebrandt Peter , Llobet Antoni 
Published: November 2016

AbstractThe irreversible conversion of single‐site water‐oxidation catalysts (WOC) into more rugged catalysts structurally related to [(trpy)(5,5′‐X2‐bpy)RuIV(μ‐O)RuIV(trpy)(O)(H2O)]4+ (X=H, 1‐dn4+; X=F, 2‐dn4+; bpy=2,2′‐bipyridine; trpy=2,2′:6′,2“‐terpyridine) represents a critical issue in the development of active and durable WOCs. In this work, the electrochemical and acid–base properties of 1‐dn4+ and 2‐dn4+ were evaluated. In situ resonance Raman spectroscopy was employed to characterize the species formed upon the stoichiometric oxidation of the single‐site catalysts and demonstrated the formation of high‐oxidation‐state mononuclear Ru=O and RuO−O complexes. Under turnover conditions, the dinuclear intermediates, 1‐dn4+ and 2‐dn4+ as well as the previously proposed [RuVI(trpy)(O)2(H2O)]2+ complex (32+) are formed. Complex 32+ is a pivotal intermediate that provides access to the formation of dinuclear species. Single‐crystal X‐ray diffraction analysis of the isolated complex [RuIV(O)(trpy)(5,5′‐F2‐bpy)]2+ reveals a clear elongation of the Ru−N bond trans to the oxido ligand that documents the weakness of this bond, which promotes the release of the bpy ligand and the subsequent formation of 32+.
Foot of the Wave Analysis for Mechanistic Elucidation and Benchmarking Applications in Molecular Water Oxidation Catalysis
Authors: Matheu Roc , Neudeck Sven , Meyer Franc , Sala Xavier , Llobet Antoni 
Published: November 2016

AbstractThe description of the foot of the wave analysis (FOWA) applied to the electrocatalytic oxidation of water to dioxygen is reported for cases where the rate determining step is first order and second order with regard to catalyst concentration, coinciding mechanistically with the so‐called water nucleophilic attack (WNA) and the interaction of two M−O units (I2M, where M represents the metal center of the catalyst), respectively. The newly adapted equations are applied to a range of relevant molecular catalysts, both in homogeneous and heterogeneous phase, and the kinetic parameters are determined, including apparent rate constants and turnover frequencies. In this respect, the application of FOWA at different catalyst concentrations allows elucidation of the reaction mechanism that operates in each case. In addition, catalytic Tafel plots are used for assessing the performance of several molecular water oxidation catalysts (WOCs) as a function of overpotential under analogous conditions, and thus can be used for benchmarking purposes. This analysis was carried out earlier for oxide‐based WOCs; however, this is the first report using molecular WOCs.
Kinetics of Levoglucosenone Isomerization
Authors: Krishna Siddarth H. , Walker Theodore W. , Dumesic James A. , Huber George W. 
Published: November 2016

AbstractWe studied the acid‐catalyzed isomerization of levoglucosenone (LGO) to 5‐hydroxymethylfurfural (HMF) and developed a reaction kinetics model that describes the experimental data across a range of conditions (100–150 °C, 50–100 mm H2SO4, 50–150 mm LGO). LGO and its hydrated derivative exist in equilibrium under these reaction conditions. Thermal and catalytic degradation of HMF are the major sources of carbon loss. Within the range of conditions studied, higher temperatures and shorter reaction times favor the production of HMF. The yields of HMF and levulinic acid decrease monotonically as tetrahydrofuran is added to the aqueous solvent system, indicating that water plays a role in the LGO isomerization reaction. Initial‐rate analyses show that HMF is produced solely from LGO rather than from the hydrated derivative of LGO. The results of this study are consistent with a mechanism for LGO isomerization that proceeds through hydration of the anhydro bridge, followed by ring rearrangement analogous to the isomerization of glucose to fructose.
Impact of Oxygen Deficiency on the Electrochemical Performance of K2NiF4‐Type (La1−xSrx)2NiO4−δ Oxygen Electrodes
Authors: Kravchenko Ekaterina , Zakharchuk Kiryl , Viskup Alexander , Grins Jekabs , Svensson Gunnar , Pankov Vladimir , Yaremchenko Aleksey 
Published: November 2016

AbstractPerovskite‐related (La1−xSrx)2NiO4−δ (x=0.5–0.8) phases were explored for possible use as oxygen electrodes in solid electrolyte cells with a main focus on the effect of oxygen deficiency on the electrocatalytic activity. (La1−xSrx)2NiO4−δ solid solutions were demonstrated to preserve the K2NiF4‐type tetragonal structure under oxidizing conditions. Acceptor‐type substitution by Sr is compensated by the formation of oxygen vacancies and electron holes and progressively increases high‐temperature oxygen nonstoichiometry, which reaches as high as δ=0.40 for x=0.8 at 950 °C in air. The electrical conductivity of (La1−xSrx)2NiO4−δ ceramics at 500–1000 °C and p(O2)≥10−3 atm is p‐type metallic‐like. The highest conductivity, 300 S cm−1 at 800 °C in air, is observed for x=0.6. The average thermal expansion coefficients, (14.0–15.4)×10−6 K−1 at 25–900 °C in air, are sufficiently low to ensure the thermomechanical compatibility with common solid electrolytes. The polarization resistance of porous (La1−xSrx)2NiO4−δ electrodes applied on a Ce0.9Gd0.1O2−δ solid electrolyte decreases with increasing Sr concentration in correlation with the concentration of oxygen vacancies in the nickelate lattice and the anticipated level of mixed ionic–electronic conduction. However, this is accompanied by increasing reactivity between the cell components and necessitates the microstructural optimization of the electrode materials to reduce the electrode fabrication temperature.
Selective Hydrogenolysis of Glycerol to 1,3‐Propanediol: Manipulating the Frustrated Lewis Pairs by Introducing Gold to Pt/WOx
Authors: Zhao Xiaochen , Wang Jia , Yang Man , Lei Nian , Li Lin , Hou Baolin , Miao Shu , Pan Xiaoli , Wang Aiqin , Zhang Tao 
Published: November 2016

AbstractA highly dispersed Au and Pt catalyst supported on WOx was developed for high performance in the selective hydrogenolysis of glycerol to 1,3‐propanediol (1,3‐PD) under very mild reaction conditions (81.4 % glycerol conversion, 51.6 % 1,3‐PD selectivity at 413 K, 1 MPa H2). The highly dispersed Au decreased the original surface Lewis‐acid sites on Pt/WOx but greatly increased its in situ generated Brønsted‐acid sites with the assistance of H2 through the formation of frustrated Lewis pairs. These in situ formed and spatially separated pairs of H+ and H− function as the active sites in glycerol conversion to 1,3‐PD.
An 11‐μ W, 9‐bit fully differential, cyclic/algorithmic ADC in 0.13 μm CMOS
Authors: Bako Niko , Fricke Kyle , Sobot Robert , Baric Adrijan 
Published: November 2016

SummaryThis paper describes a fully differential, cyclic, analogue‐to‐digital converter (ADC). It utilizes a 4‐bit binary weighted capacitor array to obtain 9‐bit resolution. The ADC uses an operational amplifier to suppress supply voltage variations. The operational amplifier with the slew‐rate detection is used to increase the speed of the ADC. The ADC is fabricated in IBM 0.13 μm CMOS process and occupies 650 × 850μm2 active area. At 10 kS/s sampling rate, the ADC consumes 11 μW. In order to test immunity of the ADC on the supply voltage variations, static and dynamic performance of the ADC is measured with triangular supply voltage (VDC = 1.5 V, VAC = 200mVpp, f = 1 kHz). The measured peak of differential nonlinearity and integral nonlinearity is + 0.26/ − 0.67 and + 0.65/ − 0.59, respectively. At 250 Hz, effective number of bit is 8.4 bits, SFDR = 66.7 dB and SNDR = 52.6 dB. Copyright © 2016 John Wiley & Sons, Ltd.
A configurable 2‐Gbps LVDS transceiver in 150‐nm CMOS with pre‐emphasis, equalization, and slew rate control
Authors: Jawed Syed Arsalan , Asghar Ali , Khan Khubaib , Abbasi Shahbaz , Naveed Muhammad , Siddiqi Yasir , Siddiqi Waqas 
Published: November 2016

SummaryA configurable full‐duplex low‐voltage differential signaling transceiver is presented, which can be configured to operate either for smaller differential channels (a few inches of striplines) or for longer channels (10 m of twisted pair cables). The configurability is embedded in the form of functionalities like pre‐emphasis, equalization, and slew rate control within the transceiver. The transmitter employs a hybrid voltage–current‐mode driver, which due to replica action, achieves a high‐impedance current‐mode signal dispatch and at the same time provides a matched impedance at the near end for improved intersymbol interference. The transmitter achieves slew rate control through a band‐limited pre‐driver, while the pre‐emphasis is achieved through a capacitive feed‐forward. The receiver employs a large‐input common‐mode first stage enclosed in a common‐mode control loop that enables its first stage to also act like a domain shifter (VDDIO‐to‐VDDCORE) reducing the overall power consumption. The equalization in the receiver is implemented by using carefully sized active inductive loads inside the receiver. The transceiver is designed and fabricated in 150‐nm complementary metal–oxide–semiconductor, sharing the space with a larger die, occupying an area of 400 × 400μm. The measurement results demonstrate that the transceiver is operating at 2 Gbps both for a 4‐in microstrip and a 10‐m twisted pair CAT6 cable with 30 and 180 ps of total jitter, respectively. The built‐in impedance calibrator minimizes the spread in the on‐die termination at the near end provided by the transmitter‐minimizing bit error rate across process, voltage, and temperature corners. The transmitter consumes a total power of 17 mW operating at 2 Gbps, that is, 8.5 pJ/bit of energy consumption; the receiver consumes a total power of 3.5 mW while driving a load of 5 pF at 2 Gbps. Copyright © 2016 John Wiley & Sons, Ltd.
A three‐vector‐based direct power control strategy for three‐phase voltage source PWM converters
Authors: Wang Meng , Shi Yanyan , Qi Mingyan , Shen Minghui 
Published: November 2016

SummaryFor traditional direct power control strategy, there exist high steady‐state power ripples and large current harmonics. To solve this problem, this work proposes a novel three‐vector‐based direct power control strategy for three‐phase voltage source pulse‐width‐modulated (PWM) converters. Different from traditional predictive direct power control strategy, an improved vector table is presented and three voltage vectors are selected, which considers the impact of voltage vectors on the active and reactive power simultaneously. The performance of the three‐phase voltage source PWM converters with the proposed control strategy is investigated and compared with the predictive deadbeat direct power control strategy. Furthermore, the three‐phase voltage source PWM converters have also been tested in the condition of different loads and when voltage unbalance occurs. Simulation and experimental work are conducted. The results conclude that the proposed strategy is of simple structure and fast dynamic response. Besides, it can effectively reduce steady‐state power ripples and current harmonics, improving the performance of the three‐phase PWM converters. Copyright © 2016 John Wiley & Sons, Ltd.
Disturbance‐mediated heterogeneity drives pollinator diversity in boreal managed forest ecosystems
Authors: Rodríguez Antonio , Kouki Jari 
Published: November 2016

AbstractIntensive forest management, together with fire suppression, have decreased structural complexity and altered dynamics of boreal forests profoundly. Such management threatens forest biodiversity and can reduce the provision of ecosystem services. Although the importance of ecosystem services is widely acknowledged, conservation strategies are hindered by poor knowledge about diversity patterns of service provider species as well as on mechanisms affecting these assemblages at different spatial and temporal scales. In this study, we assessed the effect of disturbance management on forest pollinator communities. To do so, we used a large‐scale ecological experiment conducted in the year 2000, where forest complexity was manipulated with different harvest regimes and prescribed fire. Results were consistent with a positive response of pollinators to increasing habitat heterogeneity driven by past disturbances. Harvested sites harbored a diverse pollinator community, and showed higher spatial and temporal turnover in species richness. Conversely, old‐growth forest communities were a nested subset of harvested sites and contained half of their total diversity. Variation in community composition (β diversity) was primarily affected by species temporal turnover. Throughout the season, β diversity was controlled by fire and harvesting legacies, which provide environmental heterogeneity in the form of flowering and nesting resources over space and time. Conservation strategies may undervalue ecosystem services in dynamic, naturally disturbance‐driven, landscapes when relying solely on undisturbed forests areas. However, maintaining natural dynamics in early successional forests, by emulating natural disturbances at harvesting, hold promise for the conservation of both biodiversity and ecosystem services in boreal forests.
Direct and indirect costs among patients with binge‐eating disorder in the United States
Authors: Ling You‐Li , Rascati Karen L. , Pawaskar Manjiri 
Published: November 2016

ABSTRACTObjectiveTo quantify the economic burden of binge‐eating disorder (BED) in terms of work productivity loss, healthcare resource utilization, and healthcare costs.MethodsRespondents of the US National Health and Wellness Survey 2013 were invited to participate in a follow‐up internet survey to identify adults with BED using DSM‐5 criteria. Work productivity loss, healthcare resource utilization, and direct and indirect costs were assessed for BED respondents and matched non‐BED respondents using generalized linear models or two‐part models as appropriate.ResultsA total of 1,720 people were included in our analysis (N = 344 with BED; N= 1,376 without BED). BED respondents had higher levels of activity impairment than non‐BED respondents (41.29% vs. 23.18%, p < .001). Employed BED respondents (N = 178) had a greater level of work impairment than employed non‐BED respondents (N = 686) (36.83% vs. 14.41%, p = .009). Higher healthcare resource utilization in the past 6 months among BED respondents was reported than matched non‐BED respondents: numbers of surgeries (0.23 vs. 0.13, p = .021), ER visits (0.26 vs. 0.15, p = .016), and physician visits (6.09 vs. 4.56, p = .002). BED respondents reported higher total direct costs than matched non‐BED respondents ($20,194 vs. $14,465, p = .005). The indirect costs among employed BED respondents were also higher than those without BED ($19,327 vs. $9,032, p < .001).DiscussionIndividuals with BED reported significantly greater economic burden with respect to work productivity loss, level of healthcare resource utilization, and costs compared to non‐BED respondents. © 2016 Wiley Periodicals, Inc.(Int J Eat Disord 2017; 50:523–532)
Predictors of dropout in face‐to‐face and internet‐based cognitive‐behavioral therapy for bulimia nervosa in a randomized controlled trial
Authors: Watson Hunna J. , Levine Michele D. , Zerwas Stephanie C. , Hamer Robert M. , Crosby Ross D. , Sprecher Caroline S. , O'Brien Amy , Zimmer Benjamin , Hofmeier Sara M. , Kordy Hans , Moessner Markus , Peat Christine M. , Runfola Cristin D. , Marcus Marsha D. , Bulik Cynthia M. 
Published: November 2016

ABSTRACTObjectiveWe sought to identify predictors and moderators of failure to engage (i.e., pretreatment attrition) and dropout in both Internet‐based and traditional face‐to‐face cognitive‐behavioral therapy (CBT) for bulimia nervosa. We also sought to determine if Internet‐based treatment reduced failure to engage and dropout.MethodParticipants (N = 191, 98% female) were randomized to Internet‐based CBT (CBT4BN) or traditional face‐to‐face group CBT (CBTF2F). Sociodemographics, clinical history, eating disorder severity, comorbid psychopathology, health status and quality of life, personality and temperament, and treatment‐related factors were investigated as predictors.ResultsFailure to engage was associated with lower perceived treatment credibility and expectancy (odds ratio [OR] = 0.91, 95% CI: 0.82, 0.97) and body mass index (BMI) (OR = 1.10; 95% CI: 1.03, 1.18). Dropout was predicted by not having a college degree (hazard ratio [HR] = 0.55; 95% CI: 0.37, 0.81), novelty seeking (HR = 1.02; 95% CI: 1.01, 1.03), previous CBT experience (HR = 1.77; 95% CI: 1.16, 2.71), and randomization to the individual's nonpreferred treatment format (HR = 1.95, 95% CI: 1.28, 2.96).DiscussionThose most at risk of failure to engage had a higher BMI and perceived treatment as less credible and less likely to succeed. Dropout was associated with less education, higher novelty seeking, previous CBT experience, and a mismatch between preferred and assigned treatment. Contrary to expectations, Internet‐based CBT did not reduce failure to engage or dropout. © 2016 Wiley Periodicals, Inc.(Int J Eat Disord 2017; 50:569–577)
Soil phosphorus heterogeneity promotes tree species diversity and phylogenetic clustering in a tropical seasonal rainforest
Authors: Xu Wumei , Ci Xiuqin , Song Caiyun , He Tianhua , Zhang Wenfu , Li Qiaoming , Li Jie 
Published: November 2016

AbstractThe niche theory predicts that environmental heterogeneity and species diversity are positively correlated in tropical forests, whereas the neutral theory suggests that stochastic processes are more important in determining species diversity. This study sought to investigate the effects of soil nutrient (nitrogen and phosphorus) heterogeneity on tree species diversity in the Xishuangbanna tropical seasonal rainforest in southwestern China. Thirty‐nine plots of 400 m2 (20 × 20 m) were randomly located in the Xishuangbanna tropical seasonal rainforest. Within each plot, soil nutrient (nitrogen and phosphorus) availability and heterogeneity, tree species diversity, and community phylogenetic structure were measured. Soil phosphorus heterogeneity and tree species diversity in each plot were positively correlated, while phosphorus availability and tree species diversity were not. The trees in plots with low soil phosphorus heterogeneity were phylogenetically overdispersed, while the phylogenetic structure of trees within the plots became clustered as heterogeneity increased. Neither nitrogen availability nor its heterogeneity was correlated to tree species diversity or the phylogenetic structure of trees within the plots. The interspecific competition in the forest plots with low soil phosphorus heterogeneity could lead to an overdispersed community. However, as heterogeneity increase, more closely related species may be able to coexist together and lead to a clustered community. Our results indicate that soil phosphorus heterogeneity significantly affects tree diversity in the Xishuangbanna tropical seasonal rainforest, suggesting that deterministic processes are dominant in this tropical forest assembly.
Cellular and humoral immunity in a wild mammal: Variation with age & sex and association with overwinter survival
Authors: Watson Rebecca L. , McNeilly Tom N. , Watt Kathryn A. , Pemberton Josephine M. , Pilkington Jill G. , Waterfall Martin , Hopper Phoebe R.T. , Cooney Daniel , Zamoyska Rose , Nussey Daniel H. 
Published: November 2016

AbstractImmune defenses are expected to be crucial for survival under the considerable parasite pressures experienced by wild animals. However, our understanding of the association between immunity and fitness in nature remains limited due to both the complexity of the vertebrate immune system and the often‐limited availability of immune reagents in nonmodel organisms. Here, we use methods and reagents developed by veterinary researchers for domestic ungulates on blood samples collected from a wild Soay sheep population, to evaluate an unusually broad panel of immune parameters. Our evaluation included different innate and acquired immune cell types as well as nematode parasite‐specific antibodies of different isotypes. We test how these markers correlate with one another, how they vary with age‐group and sex, and, crucially, whether they predict overwinter survival either within or among demographic groups. We found anticipated patterns of variation in markers with age, associated with immune development, and once these age trends were accounted for, correlations among our 11 immune markers were generally weak. We found that females had higher proportions of naïve T cells and gamma–delta T cells than males, independent of age, while our other markers did not differ between sexes. Only one of our 11 markers predicted overwinter survival: sheep with higher plasma levels of anti‐nematode IgG antibodies were significantly more likely to survive the subsequent high mortality winter, independent of age, sex, or weight. This supports a previous finding from this study system using a different set of samples and shows that circulating antibody levels against ecologically relevant parasites in natural systems represent an important parameter of immune function and may be under strong natural selection. Our data provide rare insights into patterns of variation among age‐ and sex groups in different T‐cell subsets and antibody levels in the wild, and suggest that certain types of immune response—notably those likely to be repeatable within individuals and linked to resistance to ecologically relevant parasites—may be most informative for research into the links between immunity and fitness under natural conditions.