bluuebunny/crossref_metadata_2025_split huggingface dataset:
The Mechanism of CO and CO2 Hydrogenation to Methanol over Cu‐Based Catalysts
Authors: Studt Felix , Behrens Malte , Kunkes Edward L. , Thomas Nygil , Zander Stefan , Tarasov Andrey , Schumann Julia , Frei Elias , Varley Joel B. , Abild‐Pedersen Frank , Nørskov Jens K. , Schlögl Robert 
Published: March 2015

AbstractMethanol, an important chemical, fuel additive, and precursor for clean fuels, is produced by hydrogenation of carbon oxides over Cu‐based catalysts. Despite the technological maturity of this process, the understanding of this apparently simple reaction is still incomplete with regard to the reaction mechanism and the active sites. Regarding the latter, recent progress has shown that stepped and ZnOx‐decorated Cu surfaces are crucial for the performance of industrial catalysts. Herein, we integrate this insight with additional experiments into a full microkinetic description of methanol synthesis. In particular, we show how the presence or absence of the Zn promoter dramatically changes not only the activity, but unexpectedly the reaction mechanism itself. The Janus‐faced character of Cu with two different sites for methanol synthesis, Zn‐promoted and unpromoted, resolves the long‐standing controversy regarding the Cu/Zn synergy and adds methanol synthesis to the few major industrial catalytic processes that are described on an atomic level.
Irreversible endo‐Selective Diels–Alder Reactions of Substituted Alkoxyfurans: A General Synthesis of endo‐Cantharimides
Authors: Foster Robert W. , Benhamou Laure , Porter Michael J. , Bučar Dejan‐Krešimir , Hailes Helen C. , Tame Christopher J. , Sheppard Tom D. 
Published: March 2015

AbstractThe [4+2] cycloaddition of 3‐alkoxyfurans with N‐substituted maleimides provides the first general route for preparing endo‐cantharimides. Unlike the corresponding reaction with 3H furans, the reaction can tolerate a broad range of 2‐substitued furans including alkyl, aromatic, and heteroaromatic groups. The cycloaddition products were converted into a range of cantharimide products with promising lead‐like properties for medicinal chemistry programs. Furthermore, the electron‐rich furans are shown to react with a variety of alternative dienophiles to generate 7‐oxabicyclo[2.2.1]heptane derivatives under mild conditions. DFT calculations have been performed to rationalize the activation effect of the 3‐alkoxy group on a furan Diels–Alder reaction.
Hexametaphosphate‐Capped Silica Mesoporous Nanoparticles Containing CuII Complexes for the Selective and Sensitive Optical Detection of Hydrogen Sulfide in Water
Authors: El Sayed Sameh , Milani Michele , Licchelli Maurizio , Martínez‐Máñez Ramón , Sancenón Félix 
Published: March 2015

AbstractCuII‐macrocycle functionalized hexametaphosphate‐capped silica mesoporous nanoparticles have been prepared and used for the selective and sensitive detection of hydrogen sulfide in aqueous environments. The possibility of using different metal complexes combined with different capping anions and choice of different dyes or other sensing molecules as indicators makes this new protocol highly appealing for the preparation of new sensing systems for sulfide detection in different environments.
Solvent‐Free Ball‐Milling Subcomponent Synthesis of Metallosupramolecular Complexes
Authors: Giri Chandan , Sahoo Prasit Kumar , Puttreddy Rakesh , Rissanen Kari , Mal Prasenjit 
Published: March 2015

AbstractSubcomponent self‐assembly from components A, B, C, D, and Fe2+ under solvent‐free conditions by self‐sorting leads to the construction of three structurally different metallosupramolecular iron(II) complexes. Under carefully selected ball‐milling conditions, tetranuclear [Fe4(AD2)6]4− 22‐component cage 1, dinuclear [Fe2(BD2)3]2− 11‐component helicate 2, and 5‐component mononuclear [Fe(CD3)]2+ complex 3 were prepared simultaneously in a one‐pot reaction from 38 components. Through subcomponent substitution reaction by adding subcomponent B, the [Fe4(AD2)6]4− cage converts quantitatively to the [Fe2(BD2)3]2− helicate, which, in turn, upon addition of subcomponent C, transforms to [Fe(CD3)]2+, following the hierarchical preference based on the thermodynamic stability of the complexes.
Bioreaktionstechnik in mikrofluidischen Reaktoren
Authors: Peterat Gena , Lladó Maldonado Susanna , Edlich Astrid , Rasch Detlev , Dietzel Andreas , Krull Rainer 
Published: March 2015

AbstractIm letzten Jahrzehnt hat die Mikrobioreaktor (MBR)‐Technologie rasche Fortschritte in der biotechnologischen Prozessentwicklung und der Untersuchung biologischer Systeme von der industriellen Biotechnologie bis hin zur Pharmabioverfahrenstechnik erzielt. Zahlreiche MBR‐Systeme werden in der Literatur vorgestellt, die als automatisierte, parallele Bioreaktoren für den Laboreinsatz entwickelt wurden, um einen sinnvollen Scale‐up/‐down konventioneller biotechnologischer Pilotanwendungen und industrieller Prozesse zu ermöglichen. Die MBR‐Technologie bietet die Möglichkeit, die Kultivierung mit einer hohen Datendichte von Prozessvariablen in‐situ durchzuführen und quantitative Daten aus dem Mikro‐Volumen in Echtzeit zu erhalten. Der Beitrag gibt einen Überblick von mikrotechnisch hergestellten MBR, über ihre Gestaltung, Vorteile bei biotechnologischen Applikationen sowie Grenzen und zukünftige potentielle Herausforderungen.
P2‐Quinazolinones and Bis‐Macrocycles as New Templates for Next‐Generation Hepatitis C Virus NS3/4a Protease Inhibitors: Discovery of MK‐2748 and MK‐6325
Authors: Rudd Michael T. , Butcher John W. , Nguyen Kevin T. , McIntyre Charles J. , Romano Joseph J. , Gilbert Kevin F. , Bush Kimberly J. , Liverton Nigel J. , Holloway M. Katharine , Harper Steven , Ferrara Marco , DiFilippo Marcello , Summa Vincenzo , Swestock John , Fritzen Jeff , Carroll Steven S. , Burlein Christine , DiMuzio Jillian M. , Gates Adam , Graham Donald J. , Huang Qian , McClain Stephanie , McHale Carolyn , Stahlhut Mark W. , Black Stuart , Chase Robert , Soriano Aileen , Fandozzi Christine M. , Taylor Anne , Trainor Nicole , Olsen David B. , Coleman Paul J. , Ludmerer Steven W. , McCauley John A. 
Published: March 2015

AbstractWith the goal of identifying inhibitors of hepatitis C virus (HCV) NS3/4a protease that are potent against a wide range of genotypes and clinically relevant mutant viruses, several subseries of macrocycles were investigated based on observations made during the discovery of MK‐5172. Quinazolinone‐containing macrocycles were identified as promising leads, and optimization for superior cross‐genotype and mutant enzyme potency as well as rat liver and plasma concentrations following oral dosing, led to the development of MK‐2748. Additional investigation of a series of bis‐macrocycles containing a fused 18‐ and 15‐membered ring system were also optimized for the same properties, leading to the discovery of MK‐6325. Both compounds display the broad genotype and mutant potency necessary for clinical development as next‐generation HCV NS3/4a protease inhibitors.
Aromatase inhibitors, tamoxifen, and endometrial cancer in breast cancer survivors
Authors: Chlebowski Rowan T. , Schottinger Joanne E. , Shi Jiaxiao , Chung Joanie , Haque Reina 
Published: March 2015

BACKGROUNDThe risks of both endometrial cancer and postmenopausal breast cancer are increased by obesity and higher endogenous estrogen levels. Although aromatase inhibitors reduce breast cancer incidence, their influence on endometrial cancer is uncertain.METHODSThe authors investigated this issue in a cohort of 17,064 women who were diagnosed with hormone receptor‐positive breast cancer in an integrated group practice health plan. Information on demographics, comorbidities, and the receipt of adjuvant endocrine therapy was available from electronic medical records and pharmacy records, respectively. Endometrial cancer information was obtained from the health plan's Surveillance, Epidemiology, and End Results‐affiliated tumor registry, and rates were compared across endocrine therapy groups (aromatase inhibitor, n = 5303; tamoxifen, n = 5155; switchers: both [n = 3787] or none [n = 2819]) using multivariable adjusted Cox proportional‐hazards models.RESULTSEndometrial cancer incidence was a statistically significant 48% lower in the aromatase inhibitor group versus the tamoxifen group (hazard ratio, 0.52; 95% confidence interval, 0.31‐0.87; P = .01). Endometrial cancer incidence was 29% lower in the aromatase inhibitor group versus the no endocrine therapy group (hazard ratio, 0.71; 95% confidence interval, 0.37‐1.35; P = .30) and 33% lower in the aromatase inhibitor group versus the tamoxifen group (hazard ratio, 0.67; 95% confidence interval, 0.42‐1.06; P = .08), but neither difference was statistically significant. Associations were stronger among those with good drug adherence.CONCLUSIONSIn a community‐based, integrated health plan setting, endometrial cancer incidence was lower in women who were receiving an aromatase inhibitor compared with those who were receiving tamoxifen. In addition, aromatase inhibitors may mitigate the incidence of tamoxifen‐associated endometrial cancer. Although there were somewhat fewer endometrial cancers in the aromatase inhibitor group versus the no endocrine therapy group, further studies are needed for the definitive assessment of this potential association. Cancer 2015;121:2147–2155. © 2015 American Cancer Society.
Factors Affecting the Branching Ratio of Photodissociation: Thiophenol Studied through Quantum Wavepacket Dynamics
Authors: An Heesun , Choi Heechol , Lee Yoon Sup , Baeck Kyoung Koo 
Published: March 2015

AbstractThe photodissociation dynamics of thiophenol (PhSH) excited to the 11ππ* state was investigated by time‐dependent quantum wavepacket propagation within two‐dimensional (2D) space consisting of the SH bond and SH torsion. We systematically studied the dependence of the branching ratio ${\left( {{{{\rm{\tilde A}}} \mathord{\left/ {\vphantom {{{\rm{\tilde A}}} {{\rm{\tilde X}}}}} \right. \kern-\nulldelimiterspace} {{\rm{\tilde X}}}}} \right)}$ between the two electronic states of the phenylthiyl radical (PhS.) on several factors of the 2D potential energy surfaces (PESs). The effect of a reduced initial barrier to the first ππ*/πσ* conical intersection (CI) was found to be marginal, whereas the effects of a reduced torsional barrier of SH on the excited ππ* state and the mitigated slope of the πσ* PES between the first (ππ*/πσ*) and the second (πσ*/S0) CIs were noticeable. The effect of the slope on the branching ratio has never been previously noticed. It was shown that the branching ratio can be sufficiently above unity without pre‐excitation of the torsion mode of SH, which has been assumed so far.
A waveform generator circuit for extra low‐frequency CMOS micro‐power applications
Authors: Abbas Al‐Darkazly Ibtisam A. , Hasan S. M. Rezaul 
Published: March 2015

SummaryThis paper presents a novel low‐power CMOS extra low‐frequency (ELF) waveform generator based on an operational trans‐conductance amplifier (OTA). The generator has been designed and fabricated using 2.5‐V devices available in 130‐nm IBM CMOS technology with a ±1.2‐V voltage supply. Using the same topology, two sets of device dimensions and circuit components are designed and fabricated for comparing relative performance, silicon area and power dissipation. The first design consumes 691 μW, while the second design consumes 943 μW using the same voltage supply. This low‐power performance enables the circuit to be used in many micro‐power applications. ELF oscillation is achieved for the two designs being around 3.95 Hz and 3.90 Hz, respectively, with negligible waveform distortion. The measured frequencies agree well with the simulation results. The first design is found to provide overall optimal performance compared to the second design at the expense of higher silicon area. Copyright © 2015 John Wiley & Sons, Ltd.
Fault‐block rotation controlling the distribution of fluvial sediments; a quantitative test on a Lower Pennsylvanian (Carboniferous) cyclothem succession
Authors: van den Belt Frank J. G. , de Boer Poppe L. , van Bergen Frank 
Published: March 2015

AbstractDepositional models of axial fluvial systems in half‐grabens predict that the fluvial‐sandstone percentage increases towards the downthrown side of a fault, because channel systems tend to migrate to the area of maximum subsidence. This migration is at the expense of mudstone, but floodplain deposition occurs near faults occasionally. The models assume gradual, transverse tilting and no external base‐level change, and their applicability to cases involving tectonics and/or sea‐level change may therefore be restricted. Here, a quantitative analysis is presented on a subsurface data set from a Lower Pennsylvanian cyclothem succession, which formed under conditions of differential subsidence and fluctuating sea‐level. The studied interval is wedge‐shaped and shows a systematic thickness increase from 165 to 245 m, controlled by syndepositional fault‐block tilting. It comprises three depositional units, bounded by coal groups. These units display an upward change from wedge‐shaped (75 to 120 m) to tabular (42 to 55 m). Despite their variable thickness, the units contain almost equal amounts of ca 45 m of floodplain deposits, plus ca 5 m of encased channel sandstones, in all boreholes. Where units are thicker, the remaining thickness comprises fluvial‐braidplain sandstone. This arrangement indicates that the units represent equal time periods, during which background subsidence allowed the deposition of thin channel sands and overbank mud on a level floodplain. Occasional tilting produced additional accommodation space, which was completely filled by sand‐dominated braided systems. The temporary cessation of floodplain‐mud deposition suggests that aggradation of the river system could not keep up with floodplain tilting. In addition, bypass of floodplain fines may have been promoted by a basin parallel tilting component. It is shown that (i) cases in which the standard models fully apply, and (ii) cases in which differential subsidence is too strong or too abrupt, can be distinguished by analysing cross‐plots of cumulative‐sandstone and cumulative‐mudstone thickness.
International REgistry to assess medical Practice with lOngitudinal obseRvation for Treatment of Heart Failure (REPORT‐HF): rationale for and design of a global registry
Authors: Filippatos Gerasimos , Khan Sadiya Sana , Ambrosy Andrew P. , Cleland John G.F. , Collins Sean P. , Lam Carolyn S.P. , Angermann Christiane E. , Ertl Georg , Dahlström Ulf , Hu Dayi , Dickstein Kenneth , Perrone Sergio V. , Ghadanfar Mathieu , Bermann Georgina , Noe Adele , Schweizer Anja , Maier Thomas , Gheorghiade Mihai 
Published: March 2015

AimsThe clinical characteristics, initial presentation, management, and outcomes of patients hospitalized with new‐onset (first diagnosis) heart failure (HF) or decompensation of chronic HF are poorly understood worldwide. REPORT‐HF (International REgistry to assess medical Practice with lOngitudinal obseRvation for Treatment of Heart Failure) is a global, prospective, and observational study designed to characterize patient trajectories longitudinally during and following an index hospitalization for HF.MethodsData collection for the registry will be conducted at ∼300 sites located in ∼40 countries. Comprehensive data including demographics, clinical presentation, co‐morbidities, treatment patterns, quality of life, in‐hospital and post‐discharge outcomes, and health utilization and costs will be collected. Enrolment of ∼20 000 adult patients hospitalized with new‐onset (first diagnosis) HF or decompensation of chronic HF over a 3‐year period is planned with subsequent 3 years follow‐up.PerspectiveThe REPORT‐HF registry will explore the clinical characteristics, management, and outcomes of HF worldwide. This global research programme may have implications for the formulation of public health policy and the design and conduct of international clinical trials.
Substrate stiffness regulates B‐cell activation, proliferation, class switch, and T‐cell‐independent antibody responses in vivo
Authors: Zeng Yingyue , Yi Junyang , Wan Zhengpeng , Liu Kai , Song Ping , Chau Alicia , Wang Fei , Chang Zai , Han Weidong , Zheng Wenjie , Chen Ying‐Hua , Xiong Chunyang , Liu Wanli 
Published: March 2015

B cells use B‐cell receptors (BCRs) to sense antigens that are usually presented on substrates with different stiffness. However, it is not known how substrate stiffness affects B‐cell proliferation, class switch, and in vivo antibody responses. We addressed these questions using polydimethylsiloxane (PDMS) substrates with different stiffness (20 or 1100 kPa). Live cell imaging experiments suggested that antigens on stiffer substrates more efficiently trigger the synaptic accumulation of BCR and phospho‐Syk molecules compared with antigens on softer substrates. In vitro expansion of mouse primary B cells shows different preferences for substrate stiffness when stimulated by different expansion stimuli. LPS equally drives B‐cell proliferation on stiffer or softer substrates. Anti‐CD40 antibodies enhance B‐cell proliferation on stiffer substrates, while antigens enhance B‐cell proliferation on softer substrates through a mechanism involving the enhanced phosphorylation of PI3K, Akt, and FoxO1. In vitro class switch differentiation of B cells prefers softer substrates. Lastly, NP67‐Ficoll on softer substrates accounted for an enhanced antibody response in vivo. Thus, substrate stiffness regulates B‐cell activation, proliferation, class switch, and T cell independent antibody responses in vivo, suggesting its broad application in manipulating the fate of B cells in vitro and in vivo.
Self‐regulation of time management: Mental contrasting with implementation intentions
Authors: Oettingen Gabriele , Kappes Heather Barry , Guttenberg Katie B. , Gollwitzer Peter M. 
Published: March 2015

AbstractMental contrasting with implementation intentions (MCII) has been found to improve self‐regulation across many life domains. The present research investigates whether MCII can benefit time management. In Study 1, we asked students to apply MCII to a pressing academic problem and assessed how they scheduled their time for the upcoming week. MCII participants scheduled more time than control participants who in their thoughts either reflected on similar contents using different cognitive procedures (content‐control group) or applied the same cognitive procedures on different contents (format‐control group). In Study 2, students were taught MCII as a metacognitive strategy to be used on any upcoming concerns of the subsequent week. As compared with the week prior to the training, students in the MCII (vs. format control) condition improved in self‐reported time management. In Study 3, MCII (vs. format control) helped working mothers who enrolled in a vocational business program to attend classes more regularly. The findings suggest that performing MCII on one's everyday concerns improves time management. Copyright © 2015 John Wiley & Sons, Ltd.
Comparative analyses of aromas of fresh, naringinase‐treated and resin‐absorbed juices of pummelo by GC‐MS and sensory evaluation
Authors: Ni Hui , Hong Peng , Ji Hai Feng , Sun Hao , Chen Yan Hong , Xiao An Feng , Chen Feng 
Published: March 2015

AbstractResin adsorption and naringinase treatment represent two major methods for debittering naringin in citrus juices, but their effects on the aroma profiles of citrus juices have not been intensively investigated yet. In this study, the volatiles of the fresh, naringinase‐treated and resin‐absorbed juices of pummelo were investigated by gas chromatography coupled with a mass spectrometer (GC‐MS) and sensory evaluation. The fresh juice was analyzed to have 24 volatiles, among which (E)‐3‐hexen‐1‐ol and 1‐hexanol had the highest concentrations. After the naringinase treatment, the juice showed 32 volatiles, among which (Z)‐ and (E)‐linalool oxides were the most dominant in concentration; while the resin adsorption captured most of the volatiles. Principal component analysis (PCA) showed that naringinase treatment led to an increase in some compounds, particularly aldehydes, whereas resin adsorption decreased the amounts of a lot of volatile compounds. The sensory evaluation demonstrated the fresh and naringinase‐treated juices had similar aroma profiles, whereas the resin‐adsorbed juice had a much weaker aroma intensity than its counterparts. These results indicated that the naringinase treatment is more desirable than the resin adsorption for debittering citrus juice because the naringinase treatment could maintain the aroma profile close to the original, fresh juice. Copyright © 2015 John Wiley & Sons, Ltd.
Resistance and resilience to droughts: hydropedological controls on catchment storage and run‐off response
Authors: Geris Josie , Tetzlaff Doerthe , Soulsby Chris 
Published: March 2015

AbstractHydropedological units are of critical importance in modulating catchment response in terms of storage and flux dynamics under changing hydrological conditions. We examined the short‐term impacts of an extreme drought on the storage dynamics and run‐off response in hydropedological units in a headwater catchment in the Scottish Highlands. These included poorly drained histosols in riparian zones and freely draining podzols on steeper hillslopes. To characterize the storage and run‐off dynamics prior to, during and after the drought period, precipitation, soil moisture, shallow ground water levels and consequent run‐off were monitored and stable water isotopes samples collected. Storage changes in the histosols were remarkably small (<40 mm), compared with those in moorland (~100 mm) and forest (~200 mm) covered podzols. Although storage in all soils recovered soon after the drought, this took longest (3–4 months) for the forested podzols. During events, there was consistent threshold behaviour in most hydropedological units and the integrated response at the catchment scale, which was not affected by drying or wetting. The results suggest that during dry periods, large parts of the catchment were disconnected from the river network and run‐off was generated mainly from the wet histosols. However, during events, there was an intermittent connection of the hillslopes that recharged the wetland and stream. This contributed to strong recovery and resilience of the catchment in its run‐off response. Nevertheless, as future climate projections for northern environments suggest that prolonged dry periods are likely to become more frequent, further work is needed on the potential cumulative or carry over effects of consecutive drier periods. Copyright © 2015 John Wiley & Sons, Ltd.
Performance Assessment for Irrigation Water Management: Case Study of the Great Chao Phraya Irrigation Scheme
Authors: Bumbudsanpharoke Wimolpat , Prajamwong Somkiat 
Published: March 2015

AbstractThe objective of this study is to assess the performance of irrigation water management of the Great Chao Phraya Irrigation Scheme consisting of 25 operation and maintenance irrigation projects (OMPs) in the Chao Phraya River Basin, central Thailand. Benchmarking is used to evaluate irrigation performance amongst the schemes. The eight performance indicators are crop yield ratio, output per unit area, operation and maintenance (O&M) cost, total financial viability, efficiency of infrastructure, sufficiency of irrigation staff, irrigation ratio and cropped area ratio. The results provide a feasible mechanism for performance improvement in the irrigation and drainage sector, but need strong support from key stakeholders. Though there are some uncertainties concerning the quality of secondary data, experience and insight gained from this study could provide valuable information for other schemes and will be a good starting point for benchmarking the performance of irrigation in Thailand. Copyright © 2015 John Wiley & Sons, Ltd.