bluuebunny/crossref_metadata_2025_split huggingface dataset:
Discovery, Characterization, and Analogue Synthesis of Bohemamine Dimers Generated by Non‐enzymatic Biosynthesis
Authors: Fu Peng , Legako Aaron , La Scott , MacMillan John B. 
Published: February 2016

AbstractDibohemamines A–C (5–7), three new dimeric bohemamine analogues dimerized through a methylene group, were isolated from a marine‐derived Streptomyces spinoverrucosus. The structures determined by spectroscopic analysis were confirmed through the semi‐synthetic derivatization of monomeric bohemamines and formaldehyde. These reactions, which could occur under mild conditions, together with the detection of formaldehyde in the culture, revealed that this dimerization is a non‐enzymatic process. In addition to the unique dimerization of the dibohemamines, dibohemamines B and C were found to have nm cytotoxicity against the non‐small cell‐lung cancer cell line A549. In view of the potent cytotoxicity of compounds 6 and 7, a small library of bohemamine analogues was generated for biological evaluation by utilizing a series of aryl and alkyl aldehydes.
Direct Catalytic Asymmetric Mannich‐type Reaction of α,β‐Unsaturated γ‐Butyrolactam with Ketimines
Authors: Lin Shaoquan , Kumagai Naoya , Shibasaki Masakatsu 
Published: February 2016

AbstractWe report a direct catalytic asymmetric Mannich‐type addition of α,β‐unsaturated γ‐butyrolactam to α‐ethoxycarbonyl ketimines promoted by a soft Lewis acid/Brønsted base cooperative catalyst. A thiophosphinoyl group on the nitrogen of ketimines was crucial for both electrophilic activation and α‐addition of γ‐butyrolactams. The obtained aza‐Morita–Baylis–Hillman‐type products bear an α‐amino acid architecture with a tetra‐substituted stereogenic center.
N‐Heterocyclic Carbene Ligand‐Enabled C(sp3)−H Arylation of Piperidine and Tetrahydropyran Derivatives
Authors: Ye Shengqing , Yang Weibo , Coon Timothy , Fanning Dewey , Neubert Tim , Stamos Dean , Yu Jin‐Quan 
Published: February 2016

AbstractPdII‐catalyzed C(sp3)−H arylation of saturated heterocycles with a wide range of aryl iodides is enabled by an N‐heterocyclic carbene (NHC) ligand. A C(sp3)−H insertion step by the PdII/NHC complex in the absence of ArI is demonstrated experimentally for the first time. Experimental data suggests that the previously established NHC‐mediated Pd0/PdII catalytic manifold does not operate in this reaction. This transformation provides a new approach for diversifying pharmaceutically relevant piperidine and tetrahydropyran ring systems.
Entwicklung eines Messgeräts zur Kopplung von kalorimetrischen und volumetrischen Sorptionsmessungen
Authors: Bläker Christian , Luckas Michael , Pasel Christoph , Dreisbach Frieder , Bathen Dieter 
Published: February 2016

AbstractZur simultanen Messung von Adsorptionsenthalpie und Beladung wurde eine neue Messmethodik entwickelt. Ein volumetrisches Adsorptionsmessgerät wird durch eine kalorimetrische Messanordnung erweitert, in der die Druckdifferenz zwischen zwei identischen Sensorgasvolumina gemessen wird, die eine Messzelle und eine Referenzzelle umschließen. Bei der Adsorption tritt infolge der Sorptionswärme ein Druckanstieg im Gasvolumen um die Messzelle auf. Aus dem zeitlichen Verlauf lässt sich nach einer Kalibrierung die Sorptionswärme berechnen. Erste Ergebnisse der Adsorptionsenthalpie von CO2 an einem 13X‐Zeolithen werden gezeigt.
Professor Dr. Lothar Jaenicke
Authors: Offermanns Heribert 
Published: February 2016

AbstractAm 29. 12. 2015 verstarb in gesegnetem Alter der emeritierte Professor der Biochemie der Universität Köln, Lothar Jaenicke, ein herausragender akademischer Lehrer und Forscher, ein bemerkenswerter Biograph, ein bedeutender Übersetzer und Rezensent, ein geschätzter Autor der ChiuZ, dem es auch immer ein Anliegen war, dass in der Wissenschaft “Unverständlichkeit nicht zu Unverständnis führt!”. Noch im Jahr seines Todes schrieb er Beiträge für die ChiuZ (Ligninver”wert”ung und Die Ammoniak‐Brennstoffzelle wird Reaktor).
Grünes Rot: chlorfreie Pyrotechnik
Authors: Nowack Ricardo 
Published: February 2016

AbstractRote Pyrotechnik ist jedem Fan von Feuerwerkskunst bekannt: Wenn es knallt und Farbblitze den Himmel erhellen, sind Explosivstoffe im Spiel [1]. Doch auch in der Schifffahrt als Notsignal oder im Militär als Signalleuchte kommen rote Leuchtsätze zum Einsatz. Allerdings ist ihre Verwendung unabhängig vom Einsatzgebiet problematisch, weil sie unter Verdacht stehen, dass sie gesundheitsgefährdend sind. Eine Gruppe von Explosivstoffforschern schlägt daher alternative Chemikalienmischungen vor, die ebenso brillant und lichtintensiv sind, aber gesundheitlich unbedenklich.
Multiferroicity Broken by Commensurate Magnetic Ordering in Terbium Orthomanganite
Authors: Zhang Hao , Flacau Roxana , Du Xin , Manuel Pascal , Cong Junzhuang , Sun Young , Sun Junliang , Yang Sihai , Li Guobao , Liao Fuhui , Lin Jianhua 
Published: February 2016

AbstractTbMnO3 is an important multiferroic material with strong coupling between magnetic and ferroelectric orderings. Incommensurate magnetic ordering is suggested to be vital for this coupling in TbMnO3, which can be modified by doping at the site of Tb and/or Mn. Our study shows that a self‐doped solid solution Tb1−xMnyMnO3 (y≤x) can be formed with Mn doped into the site of Tb of TbMnO3. When y is small Tb1−xMnyMnO3 shows both ferroelectric and incommensurate magnetic orders at low temperature, which is similar to TbMnO3. However, if y is large enough, a commensurate antiferromagnetic ordering appears along with the incommensurate magnetic ordering to prevent the appearance of multiferroicity in Tb1−xMnyMnO3. That is to say, the magnetoeletric coupling can be broken by the co‐existence of a commensurate antiferromagnetic ordering. This finding may be useful to the study of TbMnO3.
Coupling Electrochemistry with Probe Electrospray Ionization Mass Spectrometry
Authors: Cai Yi , Liu Pengyuan , Held Michael A. , Dewald Howard D. , Chen Hao 
Published: February 2016

AbstractA new coupling of electrochemistry with mass spectrometry (MS) using probe electrospray ionization (PESI) is presented. Due to the high salt tolerance of PESI, the detection of electrochemical reaction products in room‐temperature ionic liquids (RTILs) is realized for the first time. Furthermore, PESI‐MS allows the analysis of electrochemical reaction products on different or multiple electrode surfaces. In addition, peptides and proteins fractionated through isoelectric focusing (IEF) in the presence of an external electric field can also be directly analyzed by using PESI‐MS, suggesting a new and rapid characterization means for the IEF technique. This study reveals the versatility of EC/PESI‐MS, which could have an impact in electrochemistry and bioanalysis fields.
Copper‐Based Catalysts Supported on Highly Porous Silica for the Water Gas Shift Reaction
Authors: Marras Claudia , Loche Danilo , Carta Daniela , Casula Maria Francesca , Schirru Manuela , Cutrufello Maria Giorgia , Corrias Anna 
Published: February 2016

AbstractCopper‐based nanoparticles, supported on either a silica aerogel or cubic mesostructured silicas obtained by using two different synthetic protocols, were used as catalysts for the water gas shift reaction. The obtained nanocomposites were thoroughly characterised before and after catalysis through nitrogen adsorption–desorption measurements at −196 °C, TEM, and wide‐ and low‐angle XRD. The samples before catalysis contained nanoparticles of copper oxides (either CuO or Cu2O), whereas the formation of metallic copper nanoparticles, constituting the active catalytic phase, was observed either by using pre‐treatment in a reducing atmosphere or directly during the catalytic reaction owing to the presence of carbon monoxide. A key role in determining the catalytic performances of the samples is played by the ability of different matrices to promote a high dispersion of copper metal nanoparticles. The best catalytic performances are obtained with the aerogel sample, which also exhibits constant carbon monoxide conversion values at constant temperature and reproducible behaviour after subsequent catalytic runs. On the other hand, in the catalysts based on cubic mesostructured silica, the detrimental effects related to sintering of copper nanoparticles are avoided only on the silica support, which is able to produce a reasonable dispersion of the copper nanophase.
Nitrogen and Phosphorous Co‐Doped Graphene Monolith for Supercapacitors
Authors: Wen Yangyang , Rufford Thomas E. , Hulicova‐Jurcakova Denisa , Wang Lianzhou 
Published: February 2016

AbstractThe co‐doping of heteroatoms has been regarded as a promising approach to improve the energy‐storage performance of graphene‐based materials because of the synergetic effect of the heteroatom dopants. In this work, a single precursor melamine phosphate was used for the first time to synthesise nitrogen/phosphorus co‐doped graphene (N/P‐G) monoliths by a facile hydrothermal method. The nitrogen contents of 4.27–6.58 at % and phosphorus levels of 1.03–3.00 at % could be controlled by tuning the mass ratio of melamine phosphate to graphene oxide in the precursors. The N/P‐G monoliths exhibited excellent electrochemical performances as electrodes for supercapacitors with a high specific capacitance of 183 F g−1 at a current density of 0.05 A g−1, good rate performance and excellent cycling performance. Additionally, the N/P‐G electrode was stable at 1.6 V in 1 m H2SO4 aqueous electrolyte and delivered a high energy density of 11.33 Wh kg−1 at 1.6 V.
Catalytic Hydrotreatment of Humins in Mixtures of Formic Acid/2‐Propanol with Supported Ruthenium Catalysts
Authors: Wang Yuehu , Agarwal Shilpa , Kloekhorst Arjan , Heeres Hero Jan 
Published: February 2016

AbstractThe catalytic hydrotreatment of humins, which are the solid byproducts from the conversion of C6 sugars (glucose, fructose) into 5‐hydroxymethylfurfural (HMF) and levulinic acid (LA), by using supported ruthenium catalysts has been investigated. Reactions were carried out in a batch setup at elevated temperatures (400 °C) by using a hydrogen donor (formic acid (FA) in isopropanol (IPA) or hydrogen gas), with humins obtained from d‐glucose. Humin conversions of up to 69 % were achieved with Ru/C and FA, whereas the performance for Ru on alumina was slightly poorer (59 % humin conversion). Humin oils were characterized by using a range of analytical techniques (GC, GC–MS, GCxGC, gel permeation chromatography) and were shown to consist of monomers, mainly alkyl phenolics (>45 % based on compounds detectable by GC) and higher oligomers. A reaction network for the reaction is proposed based on structural proposals for humins and the main reaction products.
Hierarchical Zeolites with Amine‐Functionalized Mesoporous Domains for Carbon Dioxide Capture
Authors: Nguyen Tien Hoa , Kim Sungjune , Yoon Minyoung , Bae Tae‐Hyun 
Published: February 2016

AbstractTo prepare materials with high CO2 adsorption, a series of hierarchical LTA zeolites possessing various mesopore spaces that are decorated with alkylamines was designed and synthesized. The highest CO2 uptake capacity was achieved when (3‐aminopropyl)trimethoxysilane (APTMS) was grafted onto the hierarchical LTA zeolite having the largest mesopores. Owing to the contributions of both alkylamine groups grafted onto the mesopore surfaces and active sites in the LTA zeolites, the amount of CO2 that can be taken up on these materials is much higher than for conventional aminosilicas such SBA‐15 and MCM‐41. Furthermore, the adsorbent shows good CO2 uptake capacity and recyclability in dynamic flow conditions.
Homogenizing effects of cities on North American winter bird diversity
Authors: Murthy Adeline C. , Fristoe Trevor S. , Burger Joseph R. 
Published: February 2016

AbstractUrbanization is widespread throughout the United States and Canada. Studies at different scales have shown mixed consequences of urban areas for ecological communities and biodiversity. Here, we use geographic data on urban extent and survey data from the Christmas Bird Count to investigate the influence of urbanization on winter bird diversity over a continental scale. We compared the alpha (local richness) and beta diversity (turnover with distance) of 42 urban bird communities to nearby non‐urban communities. We investigated the processes underlying beta diversity between non‐urban and urban sites by comparing the frequency of occurrence in species and variability in relative abundances across sites. Alpha diversity was statistically indistinguishable between urban and non‐urban sites when controlling for latitude. Community similarity decreased less rapidly over distance in urban compared to non‐urban sites, indicating that spatial homogenization from urbanization results in lower beta diversity. Eighteen species of non‐native or native generalists occurred across all urban sites, whereas no species occurred in all non‐urban sites. Mean‐variance scaling of relative abundance shows that species in urban sites maintained similar levels of community dominance across space compared to non‐urban sites. The widespread presence of urban species is likely due to similarity in habitats among cities compared to nearby non‐urban sites. The decreased variability in relative abundance of urban species is possibly due to urban resource subsidies (e.g., bird feeders, garbage, and irrigation) and shelter (e.g., landscaping, buildings, and microclimates). The increased occurrence of widespread species in cities and less variation in relative abundances across urban sites contribute to the homogenizing effect of cities on avian communities.
Mimicry of the 2‐His‐1‐Carboxylate Facial Triad Using Bulky N,N,O‐Ligands: Non‐Heme Iron Complexes Featuring a Single Facial Ligand and Easily Exchangeable Co‐Ligands
Authors: Folkertsma Emma , de Waard Esther F. , Korpershoek Gerda , van Schaik Arnoldus J. , Solozabal Mirón Naiara , Borrmann Mandy , Nijsse Sjoerd , Moelands Marcel A. H. , Lutz Martin , Otte Matthias , Moret Marc‐Etienne , Klein Gebbink Robertus J. M. 
Published: February 2016

AbstractMononuclear iron(II) complexes with facially coordinating N,N,O‐ligands were synthesized as accurate structural mimics of the 2‐His‐1‐carboxylate facial triad found in mononuclear non‐heme iron enzymes. Mimicking of the facial triad is achieved by designing sterically demanding ligands providing two histidine‐like benzimidazole moieties and a coordinating carboxylate or ester moiety. The new methyl‐substituted analogue of the bis(benzimidazolyl)propionate ligand, BMBMeIP and its ester analogue, BMBMeIPnPr are designed to prevent the formation of previously reported coordinatively saturated FeL2 type complexes. The crystal structure of [Fe(BMBMeIPnPr)(OTf)2] shows a facial N,N,O‐coordination that is very similar to the structure of the enzyme active sites. Both [Fe(BMBMeIPnPr)(OTf)2] and [Fe(BMBMeIP)(OTf)(MeCN)n] catalyze the epoxidation of olefins using H2O2, reaching turnover numbers up to 5.8 per iron. These results represent the first examples of iron complexes bearing a single facial and rigid N,N,O‐coordinating ligand and three readily available coordination sites showing catalytic activity in oxidation reactions.
Morphology, structure and kinematics of a rainfall controlled slow‐moving Andean landslide, Peru
Authors: Zerathe Swann , Lacroix Pascal , Jongmans Denis , Marino Jersy , Taipe Edu , Wathelet Marc , Pari Walter , Smoll Lionel Fidel , Norabuena Edmundo , Guillier Bertrand , Tatard Lucile 
Published: February 2016

AbstractThe large slow‐moving landslide of Maca is located in the upper Colca valley (southern Peru), a region characterized by a well pronounced rainy period, and intense and recurrent sustained seismicity. The landslide, developed in deep lacustrine deposits, has recently accelerated, threatening the Maca village. This work aims at understanding the rupture mechanism and the causes of the recent landslide reactivation/acceleration. We present a multidisciplinary characterization of the Maca landslide that includes: (i) geological and morphological mapping in the field; (ii) remote sensing analysis using an historical aerial photograph of 1955 and the Pléiades satellite images (2013); (iii) global positioning system (GPS) including time‐series of surveys over 13 years, and continuous measurements over 14 months; (iv) a geophysical campaign with deep electrical resistivity tomography profiles acquired across the landslide mass. Our study shows that this 60 Mm3 landslide, which can be classified as a clay/silt compound landslide, moved by 15 m between 2001 and 2014 with a large inter‐annual velocity variation (up to a factor of 500) depending on the rainfall intensity. We suggest that these dramatic changes in velocity are the result of the combination of a threshold mechanism and the short intense rainy season in Peru. This study reveals three main driving factors acting at different timescales: (i) over several decades, the river course has significantly changed, causing the Maca landslide reactivation in the 1980s due to the erosion of its toe; (ii) at the year scale, a minimum amount of rainfall is required to trigger the motion and this amount controls the landslide velocity; (iii) transient changes in slide velocity may occur anytime due to earthquakes. This study particularly highlights the non‐linear behaviour of the motion with rainfall. Copyright © 2016 John Wiley & Sons, Ltd.
IOFI recommended practice for the use of predicted relative‐response factors for the rapid quantification of volatile flavouring compounds by GC‐FID
Authors: Cachet T. , Brevard H. , Chaintreau A. , Demyttenaere J. , French L. , Gassenmeier K. , Joulain D. , Koenig T. , Leijs H. , Liddle P. , Loesing G. , Marchant M. , Merle Ph. , Saito K. , Schippa C. , Sekiya F. , Smith T. 
Published: February 2016

AbstractThis recommended practice enables the quantification of volatile compounds in flavourings to be made by gas chromatography with flame‐ionization detection, without having authentic compounds available, and also in many cases it can avoid time‐consuming calibration procedures. The relative‐response factors (RRF) can be predicted from the molecular formula of the compound, and this approach can be applied to compounds containing the atoms C, H, O, N, S, F, Cl, Br, I, and Si, providing that the molecular formula and number of benzene rings in the analytes are known. The purity of chemically‐defined flavouring substances or chromatographic standards can also be estimated using these predicted RRF, and this procedure can also be used to quantify (poly)hydroxylated compounds, after their derivatization into trimethylsilyl ethers or esters. Copyright © 2016 John Wiley & Sons, Ltd.
The mental health and mortality impact of death of a partner with dementia
Authors: Shah Sunil M. , Carey Iain M. , Harris Tess , DeWilde Stephen , Victor Christina R. , Cook Derek G. 
Published: February 2016

ObjectiveCaring for a partner with dementia and partner bereavement are independently associated with poor health. An understanding of the health effects of living with a partner dying with dementia can help optimise support. We describe health in the year before and after loss of a partner with dementia compared with other bereavements.MethodsIn a UK primary care database, 2624 older individuals whose partner died with dementia during 2005–2012 were matched with 7512 individuals experiencing bereavement where the deceased partner had no dementia recorded.ResultsPrior to bereavement, partners of the deceased with dementia were more likely to be diagnosed with depression (OR 2.31, 1.69–3.14) and receive psychotropic medication (OR 1.34, 1.21–1.49) than partners from bereavements without dementia. In contrast, psychotropic medication initiation two months after dementia bereavement was lower (HR 0.69, 0.56–0.85). Compared with other bereaved individuals, mortality after bereavement was lower in men experiencing a dementia bereavement (HR 0.68, 0.49–0.94) but similar in women (HR 1.02, 0.75–1.38). Prior to bereavement, those who died with dementia were less likely to receive palliative care (OR 0.47, 0.41–0.54).ConclusionIn the year before bereavement, partners of individuals dying with dementia experience poorer mental health than those facing bereavement from other causes, and their partner is less likely to receive palliative care. In the year after, individuals whose partner died with dementia experience some attenuation of the adverse health effects of bereavement. Services need to address the needs of carers for individuals dying with dementia and improve access to palliative care. Copyright © 2016 John Wiley & Sons, Ltd.
The bicaudate index inversely associates with performance in the Montreal Cognitive Assessment (MoCA) in older adults living in rural Ecuador. The Atahualpa project
Authors: Del Brutto Oscar H. , Mera Robertino M. , Del Brutto Victor J. , Sedler Mark J. 
Published: February 2016

ObjectiveAssessment of cognitive impairment in rural areas of developing countries is complicated by illiteracy and cross‐cultural factors. A better way to estimate the usefulness of cognitive screening instruments is to evaluate their correlation with imaging biomarkers. The bicaudate index (a marker of central atrophy) correlates with cognitive performance. We assessed the relationship of the bicaudate index with the MoCA to estimate the usefulness of this test to detect individuals with cognitive decline in these regions.MethodsAtahualpa residents aged ≥60 years identified during door‐to‐door surveys were evaluated with the MoCA and invited to undergo brain MRI. Using generalized linear models, we estimated whether the bicaudate index correlates with MoCA scores, after adjusting for demographics and relevant clinical and neuroimaging confounders.ResultsOut of 385 eligible persons, 290 (75%) were enrolled. Mean bicaudate index was 0.14 ± 0.03, and mean total MoCA score was 19 ± 5 points. Locally weighted scatterplot smoothing showed a nearly linear inverse relationship between the bicaudate index and the total MoCA score. In the fully adjusted generalized linear model, the bicaudate index was inversely associated with the total MoCA score (p < 0.001), which dropped by 5.3% (95% C.I.: 1.7%–8.8%) for every standard deviation of the bicaudate index. In addition, most domain‐specific MoCA scores were inversely associated with the bicaudate index.ConclusionsThe inverse relationship between the bicaudate index and the MoCA score provides evidence that the MoCA is reliable to detect structural brain damage and useful to assess cognitive performance in less educated individuals. Copyright © 2016 John Wiley & Sons, Ltd.