bluuebunny/crossref_metadata_2025_split huggingface dataset:
Turning Perspective in Photoelectrocatalytic Cells for Solar Fuels
Authors: Perathoner Siglinda , Centi Gabriele , Su Dangsheng 
Published: December 2015

AbstractThe development of new devices for the use and storage of solar energy is a key step to enable a new sustainable energy scenario. The route for direct solar‐to‐chemical energy transformation, especially to produce liquid fuels, represents a necessary element to realize transition from the actual energy infrastructure. Photoelectrocatalytic (PECa) devices for the production of solar fuels are a key element to enable this sustainable scenario. The development of PECa devices and related materials is of increasing scientific and applied interest. This concept paper introduces the need to turn the viewpoint of research in terms of PECa cell design and related materials with respect to mainstream activities in the field of artificial photosynthesis and leaves. As an example of a new possible direction, the concept of electrolyte‐less cell design for PECa cells to produce solar fuels by reduction of CO2 is presented. The fundamental and applied development of new materials and electrodes for these cells should proceed fully integrated with PECa cell design and systematic analysis. A new possible approach to develop semiconductors with improved performances by using visible light is also shortly presented.
Theoretical Insight into the Trends that Guide the Electrochemical Reduction of Carbon Dioxide to Formic Acid
Authors: Yoo Jong Suk , Christensen Rune , Vegge Tejs , Nørskov Jens K. , Studt Felix 
Published: December 2015

AbstractThe electrochemical reduction (electroreduction) of CO2 to formic acid (HCOOH) and its competing reactions, that is, the electroreduction of CO2 to CO and the hydrogen evolution reaction (HER), on twenty‐seven different metal surfaces have been investigated using density functional theory (DFT) calculations. Owing to a strong linear correlation between the free energies of COOH* and H*, it seems highly unlikely that the electroreduction of CO2 to HCOOH via the COOH* intermediate occurs without a large fraction of the current going to HER. On the other hand, the selective electroreduction of CO2 to HCOOH seems plausible if the reaction occurs via the HCOO* intermediate, as there is little correlation between the free energies of HCOO* and H*. Lead and silver surfaces are found to be the most promising monometallic catalysts showing high faradaic efficiencies for the electroreduction of CO2 to HCOOH with small overpotentials. Our methodology is widely applicable, not only to metal surfaces, but also to other classes of materials enabling the computational search for electrocatalysts for CO2 reduction to HCOOH.
BMP7‐induced dendritic growth in sympathetic neurons requires p75NTR signaling
Authors: Courter Lauren A. , Shaffo Frances C. , Ghogha Atefeh , Parrish Diana J. , Lorentz Christina U. , Habecker Beth A. , Lein Pamela J. 
Published: December 2015

ABSTRACTDendritic morphology is a critical determinant of neuronal connectivity, and in postganglionic sympathetic neurons, tonic activity correlates directly with the size of the dendritic arbor. Thus, identifying signaling mechanisms that regulate dendritic arborization of sympathetic neurons is important to understanding how functional neural circuitry is established and maintained in the sympathetic nervous system. Bone morphogenetic proteins (BMPs) promote dendritic growth in sympathetic neurons; however, downstream signaling events that link BMP receptor activation to dendritic growth are poorly characterized. We previously reported that BMP7 upregulates p75NTR mRNA in cultured sympathetic neurons. This receptor is implicated in controlling dendritic growth in central neurons but whether p75NTR regulates dendritic growth in peripheral neurons is not known. Here, we demonstrate that BMP7 increases p75NTR protein in cultured sympathetic neurons, and this effect is blocked by pharmacologic inhibition of signaling via BMP type I receptor. BMP7 does not trigger dendritic growth in sympathetic neurons dissociated from superior cervical ganglia (SCG) of p75NTR nullizygous mice, and overexpression of p75NTR in p75NTR−/− neurons is sufficient to cause dendritic growth even in the absence of BMP7. Morphometric analyses of SCG from wild‐type versus p75NTR nullizygous mice at 3, 6, and 12 to 16 weeks of age indicated that genetic deletion of p75NTR does not prevent dendritic growth but does stunt dendritic maturation in sympathetic neurons. These data support the hypotheses that p75NTR is involved in downstream signaling events that mediate BMP7‐induced dendritic growth in sympathetic neurons, and suggest that p75NTR signaling positively modulates dendritic complexity in sympathetic neurons in vivo. © 2016 Wiley Periodicals, Inc. Develop Neurobiol 76: 1003–1013, 2016
Population genetics of the olive‐winged bulbul (Pycnonotus plumosus) in a tropical urban‐fragmented landscape
Authors: Tang Grace S. Y. , Sadanandan Keren R. , Rheindt Frank E. 
Published: December 2015

AbstractWith increasing urbanization, urban‐fragmented landscapes are becoming more and more prevalent worldwide. Such fragmentation may lead to small, isolated populations that face great threats from genetic factors that affect even avian species with high dispersal propensities. Yet few studies have investigated the population genetics of species living within urban‐fragmented landscapes in the Old World tropics, in spite of the high levels of deforestation and fragmentation within this region. We investigated the evolutionary history and population genetics of the olive‐winged bulbul (Pycnonotus plumosus) in Singapore, a highly urbanized island which retains <5% of its original forest cover in fragments. Combining our own collected and sequenced samples with those from the literature, we conducted phylogenetic and population genetic analyses. We revealed high genetic diversity, evidence for population expansion, and potential presence of pronounced gene flow across the population in Singapore. This suggests increased chances of long‐term persistence for the olive‐winged bulbul and the ecosystem services it provides within this landscape.
Environmental controls on the distribution and diversity of lentic Chironomidae (Insecta: Diptera) across an altitudinal gradient in tropical South America
Authors: Matthews‐Bird Frazer , Gosling William D. , Coe Angela L. , Bush Mark , Mayle Francis E. , Axford Yarrow , Brooks Stephen J. 
Published: December 2015

AbstractTo predict the response of aquatic ecosystems to future global climate change, data on the ecology and distribution of keystone groups in freshwater ecosystems are needed. In contrast to mid‐ and high‐latitude zones, such data are scarce across tropical South America (Neotropics). We present the distribution and diversity of chironomid species using surface sediments of 59 lakes from the Andes to the Amazon (0.1–17°S and 64–78°W) within the Neotropics. We assess the spatial variation in community assemblages and identify the key variables influencing the distributional patterns. The relationships between environmental variables (pH, conductivity, depth, and sediment organic content), climatic data, and chironomid assemblages were assessed using multivariate statistics (detrended correspondence analysis and canonical correspondence analysis). Climatic parameters (temperature and precipitation) were most significant in describing the variance in chironomid assemblages. Temperature and precipitation are both predicted to change under future climate change scenarios in the tropical Andes. Our findings suggest taxa of Orthocladiinae, which show a preference to cold high‐elevation oligotrophic lakes, will likely see range contraction under future anthropogenic‐induced climate change. Taxa abundant in areas of high precipitation, such as Micropsectra and Phaenopsectra, will likely become restricted to the inner tropical Andes, as the outer tropical Andes become drier. The sensitivity of chironomids to climate parameters makes them important bio‐indicators of regional climate change in the Neotropics. Furthermore, the distribution of chironomid taxa presented here is a vital first step toward providing urgently needed autecological data for interpreting fossil chironomid records of past ecological and climate change from the tropical Andes.
A Push–Pull PdII Complex with a Ternary Pd–P–C+ Accepting End and a Key N‐Heterocyclic Carbene–Imid­azoliophosphine Ligand
Authors: Dubrulle Laurent , Poidevin Corentin , Maaliki Carine , Canac Yves , Lepetit Christine , Duhayon Carine , Chauvin Remi 
Published: December 2015

AbstractNeutral and cationic PdCl2 complexes based on the neutral frame of a cis‐chelating N‐heterocyclic carbene (NHC)–imidazolophosphine ligand involving an o‐phenylene bridge have been devised for comparison of their relative push–pull character. Both target complexes, which are globally isosteric in the Pd coordination sphere, have been prepared in 58–68 % yield by direct coordination of the corresponding cis‐chelating NHC‐imidazol(i)ophosphine “free ligand”, or by extrusion of a Ph2P+ phosphenium moiety from (imidazoliophosphine)PdII complex precursors. The cationic complex has also been obtained in 64 % yield by selective N‐methylation of the neutral counterpart. The charge transfer from the NHC donating end (LD) to the imidazol(i)ophosphine accepting end (LA) has been investigated by electronic spectroscopy and by calculations of the first excited states at the time‐dependent (TD)‐DFT level. Although all the excitations involving the LD and LA ends of the neutral complex converge to the Pd center, the excited states |S7> (305 nm) and |S8> (303 nm) of the cationic complex exhibit a net LD[M]LA charge‐tranfer (CT) character, which is clearly visualized by particle–hole density analysis. The push–pull complex involving a Pd–P–C+ π‐accepting end is regarded as a “ternary” counterpart of “binary” phosphine–borane complexes involving two‐center Pd–B σ‐accepting ends.
The Relationship between Structure and Properties in ZnII Complexes of Bulky N,N′‐Diarylformamidinate N‐Oxides
Authors: Cibian Mihaela , Langis‐Barsetti Sophie , Ferreira Janaina G. , Hanan Garry S. 
Published: December 2015

AbstractHomoleptic zinc(II) complexes (3a–3d) of the bulky N,N′‐diarylformamidinate N‐oxide ligands N‐hydroxy‐N,N′‐bis(2,6‐diisopropylphenyl)formamidine (2a), N‐hydroxy‐N,N′‐bis(2,6‐dimethylphenyl)formamidine (2b), N‐hydroxy‐N,N′‐bis(2‐isopropylphenyl)formamidine (2c) and N‐hydroxy‐N,N′‐bis(2‐biphenyl)formamidine (2d) were synthesized and characterized. Their solid‐state structures are presented together with their solution properties, as examined by NMR and UV/Vis spectroscopy, and cyclic voltammetry. Theoretical calculations [DFT and time‐dependent DFT (TD‐DFT)] were performed to assess and to rationalize the influence of ligand modification on the properties of the complexes: the highest occupied molecular orbital (HOMO), localized on the NCNO moiety, is less influenced by the substitution pattern, whereas the lowest unoccupied molecular orbital (LUMO), localized on the aryl ring with the O–N moiety, is directly affected; therefore, the optical band gap can be fine‐tuned for potential applications.
High‐Yielding Synthesis and Full Spectroscopic Characterization of 5,6:11,12‐Di‐o‐phenylenetetracene and Its Synthesis Intermediates
Authors: Wombacher Tobias , Foro Sabine , Schneider Jörg J. 
Published: December 2015

AbstractHerein we present a synthetic gram‐scale route to 5,6:11,12‐di‐o‐phenylenetetracene (DOPT, 8), which is a member of the class of cyclopenta‐fused polycyclic aromatic hydrocarbons (CP‐PAHs). Full analytical characterization of the title compound was carried out by IR, Raman, UV/Vis, and high‐field 1H NMR spectroscopy, as well as by mass spectrometry. A unique double‐elimination of phenylide moieties, as the key reaction step, gave DOPT for the first time in high purity and in an isolated yield of >70 %. Re‐aromatization of the annulated π‐ring system occurred following the reductive elimination of the two phenyl groups from the DOPT precursor. Two alternative reaction pathways for this process are discussed. The synthetic method described herein may allow development of the chemistry of the title compound further, for example, to investigate the organometallic chemistry of DOPT as well as its semiconducting behavior in organic electronics.
Improved Enzymatic Procedure for the Synthesis of Anandamide and N‐Fatty Acylalkanolamine Analogues: A Combination Strategy to Antitumor Activity
Authors: Quintana Paula G. , García Liñares Guadalupe , Chanquia Santiago N. , Gorojod Roxana M. , Kotler Mónica L. , Baldessari Alicia 
Published: December 2015

AbstractTwenty N‐fatty acylamines from linolenic and arachidonic acids, fifteen of them new compounds, were obtained through Candida antarctica B lipase‐catalyzed esterification and aminolysis reactions in very good yields and with high chemoselectivity. The optimal reaction conditions were achieved by studying the reaction parameters (temperature, E/S ratio, alcohol and alkanolamine/fatty acid ratio, time, solvent, free‐solvent system, etc.). To identify ideal enzymatic methods for generating the alkanolamides we evaluated enzyme performance in three procedures: i) aminolysis of ethyl ester, ii) direct condensation between the fatty acid and the alkanolamine, and iii) a one‐pot/two‐step conversion of fatty acids into alkanolamides via in situ formation of the ethyl ester and subsequent aminolysis by the alkanolamine. The advantages noted with the enzymatic methodology, such as mild reaction conditions and low environmental impact, underscore biocatalysis as a convenient way to prepare the reported compounds. The cytotoxic activities of all compounds and mixtures of anandamide and its analogues were evaluated in rat glioma C6 cells. These studies reveal that some anandamide analogues enhance the antitumor effects of anandamide, suggesting their possible application as therapeutic tools in cancer treatment.
Assessing the Practice Impact of Research on Evaluation
Authors: Cousins J. Bradley , Svensson Kateryna , Szijarto Barbara , Pinsent Celine , Andrew Caroline , Sylvestre John 
Published: December 2015

AbstractCalls for more and better research on evaluation (RoE) have been sounded for some 20 years now and the recent appearance of several significant reviews of empirical research suggests that interest in RoE is on the rise. Although many empirical studies on evaluation and syntheses of such studies result in implications for evaluation policy and practice, to date there has been little attention devoted to tracking the practice impact of RoE. The chapter draws on recent work on research and knowledge utilization to develop a conceptual approach to assessing the impact of RoE on evaluation policy and practice. Specifically, a theory of change for RoE is developed as part of a contribution analysis (CA) approach to the problem. Recommendations for moving forward are then considered.
Reflections on the Future of Research on Evaluation
Authors: Azzam Tarek , Jacobson Miriam R. 
Published: December 2015

AbstractThis chapter explores the future of research on evaluation (RoE) and the actions that we can take to help RoE develop and thrive in the coming years. These actions focus on the production of RoE that is specifically usable and relevant to practicing evaluators, the systematic collection and sharing of evaluation practice data, the active development of methods and tools that feasibly and rigorously measure different aspects of evaluation, the use of new technological developments (e.g., crowdsourcing) in RoE, and dissemination through new and existing systems that target other researchers and evaluation professionals. The potential impact of these actions on the future of RoE is discussed throughout this chapter, along with concluding thoughts on the current and future importance of RoE for evaluation theory and practice.
Atypical age‐dependent effects of autism on white matter microstructure in children of 2–7 years
Authors: Ouyang Minhui , Cheng Hua , Mishra Virendra , Gong Gaolang , Mosconi Matthew W. , Sweeney John , Peng Yun , Huang Hao 
Published: December 2015

AbstractAtypical age‐dependent changes of white matter (WM) microstructure play a central role in abnormal brain maturation of the children with autism spectrum disorder (ASD), but their early manifestations have not been systematically characterized. The entire brain core WM voxels were surveyed to detect differences in WM microstructural development between 31 children with ASD of 2–7 years and 19 age‐matched children with typical development (TD), using measurements of fractional anisotropy (FA) and radial diffusivity (RD) from diffusion tensor imaging (DTI). The anatomical locations, distribution, and extent of the core WM voxels with atypical age‐dependent changes in a specific tract or tract group were delineated and evaluated by integrating the skeletonized WM with a digital atlas. Exclusively, unidirectional FA increases and RD decreases in widespread WM tracts were revealed in children with ASD before 4 years, with bi‐directional changes found for children with ASD of 2–7 years. Compared to progressive development that raised FA and lowered RD during 2–7 years in the TD group, flattened curves of WM maturation were found in multiple major WM tracts of all five tract groups, particularly associational and limbic tracts, in the ASD group with trend lines of ASD and TD crossed around 4 years. We found atypical age‐dependent changes of FA and RD widely and heterogeneously distributed in WM tracts of children with ASD. The early higher WM microstructural integrity before 4 years reflects abnormal neural patterning, connectivity, and pruning that may contribute to aberrant behavioral and cognitive development in ASD. Hum Brain Mapp 37:819–832, 2016. © 2015 Wiley Periodicals, Inc.
Shared and distinct contributions of rostrolateral prefrontal cortex to analogical reasoning and episodic memory retrieval
Authors: Westphal Andrew J. , Reggente Nicco , Ito Kaori L. , Rissman Jesse 
Published: December 2015

AbstractRostrolateral prefrontal cortex (RLPFC) is widely appreciated to support higher cognitive functions, including analogical reasoning and episodic memory retrieval. However, these tasks have typically been studied in isolation, and thus it is unclear whether they involve common or distinct RLPFC mechanisms. Here, we introduce a novel functional magnetic resonance imaging (fMRI) task paradigm to compare brain activity during reasoning and memory tasks while holding bottom‐up perceptual stimulation and response demands constant. Univariate analyses on fMRI data from twenty participants identified a large swath of left lateral prefrontal cortex, including RLPFC, that showed common engagement on reasoning trials with valid analogies and memory trials with accurately retrieved source details. Despite broadly overlapping recruitment, multi‐voxel activity patterns within left RLPFC reliably differentiated these two trial types, highlighting the presence of at least partially distinct information processing modes. Functional connectivity analyses demonstrated that while left RLPFC showed consistent coupling with the fronto‐parietal control network across tasks, its coupling with other cortical areas varied in a task‐dependent manner. During the memory task, this region strengthened its connectivity with the default mode and memory retrieval networks, whereas during the reasoning task it coupled more strongly with a nearby left prefrontal region (BA 45) associated with semantic processing, as well as with a superior parietal region associated with visuospatial processing. Taken together, these data suggest a domain‐general role for left RLPFC in monitoring and/or integrating task‐relevant knowledge representations and showcase how its function cannot solely be attributed to episodic memory or analogical reasoning computations. Hum Brain Mapp 37:896–912, 2016. © 2015 Wiley Periodicals, Inc.
Presurgical brain mapping of the language network in patients with brain tumors using resting‐state fMRI: Comparison with task fMRI
Authors: Sair Haris I. , Yahyavi‐Firouz‐Abadi Noushin , Calhoun Vince D. , Airan Raag D. , Agarwal Shruti , Intrapiromkul Jarunee , Choe Ann S. , Gujar Sachin K. , Caffo Brian , Lindquist Martin A. , Pillai Jay J. 
Published: December 2015

AbstractPurposeTo compare language networks derived from resting‐state fMRI (rs‐fMRI) with task‐fMRI in patients with brain tumors and investigate variables that affect rs‐fMRI vs task‐fMRI concordance.Materials and MethodsIndependent component analysis (ICA) of rs‐fMRI was performed with 20, 30, 40, and 50 target components (ICA20 to ICA50) and language networks identified for patients presenting for presurgical fMRI mapping between 1/1/2009 and 7/1/2015. 49 patients were analyzed fulfilling criteria for presence of brain tumors, no prior brain surgery, and adequate task‐fMRI performance. Rs‐vs‐task‐fMRI concordance was measured using Dice coefficients across varying fMRI thresholds before and after noise removal. Multi‐thresholded Dice coefficient volume under the surface (DiceVUS) and maximum Dice coefficient (MaxDice) were calculated. One‐way Analysis of Variance (ANOVA) was performed to determine significance of DiceVUS and MaxDice between the four ICA order groups. Age, Sex, Handedness, Tumor Side, Tumor Size, WHO Grade, number of scrubbed volumes, image intensity root mean square (iRMS), and mean framewise displacement (FD) were used as predictors for VUS in a linear regression.ResultsArtificial elevation of rs‐fMRI vs task‐fMRI concordance is seen at low thresholds due to noise. Noise‐removed group‐mean DiceVUS and MaxDice improved as ICA order increased, however ANOVA demonstrated no statistically significant difference between the four groups. Linear regression demonstrated an association between iRMS and DiceVUS for ICA30‐50, and iRMS and MaxDice for ICA50.ConclusionOverall there is moderate group level rs‐vs‐task fMRI language network concordance, however substantial subject‐level variability exists; iRMS may be used to determine reliability of rs‐fMRI derived language networks. Hum Brain Mapp 37:913–923, 2016. © 2015 Wiley Periodicals, Inc.