bluuebunny/crossref_metadata_2025_split huggingface dataset:
Newborn screening: A disease‐changing intervention for glutaric aciduria type 1
Authors: Boy Nikolas , Mengler Katharina , Thimm Eva , Schiergens Katharina A. , Marquardt Thorsten , Weinhold Natalie , Marquardt Iris , Das Anibh M. , Freisinger Peter , Grünert Sarah C. , Vossbeck Judith , Steinfeld Robert , Baumgartner Matthias R. , Beblo Skadi , Dieckmann Andrea , Näke Andrea , Lindner Martin , Heringer Jana , Hoffmann Georg F. , Mühlhausen Chris , Maier Esther M. , Ensenauer Regina , Garbade Sven F. , Kölker Stefan 
Published: April 2018

ObjectiveUntreated individuals with glutaric aciduria type 1 (GA1) commonly present with a complex, predominantly dystonic movement disorder (MD) following acute or insidious onset striatal damage. Implementation of GA1 into newborn screening (NBS) programs has improved the short‐term outcome. It remains unclear, however, whether NBS changes the long‐term outcome and which variables are predictive.MethodsThis prospective, observational, multicenter study includes 87 patients identified by NBS, 4 patients missed by NBS, and 3 women with GA1 identified by positive NBS results of their unaffected children.ResultsThe study population comprises 98.3% of individuals with GA1 identified by NBS in Germany during 1999–2016. Overall, cumulative sensitivity of NBS is 95.6%, but it is lower (84%) for patients with low excreter phenotype. The neurologic outcome of patients missed by NBS is as poor as in the pre‐NBS era, and the clinical phenotype of diagnosed patients depends on the quality of therapeutic interventions rather than noninterventional variables. Presymptomatic start of treatment according to current guideline recommendations clearly improves the neurologic outcome (MD: 7% of patients), whereas delayed emergency treatment results in acute onset MD (100%), and deviations from maintenance treatment increase the risk of insidious onset MD (50%). Independent of the neurologic phenotype, kidney function tends to decline with age, a nonneurologic manifestation not predicted by any variable included in this study.InterpretationNBS is a beneficial, disease‐changing intervention for GA1. However, improved neurologic outcome critically depends on adherence to recommended therapy, whereas kidney dysfunction does not appear to be impacted by recommended therapy. Ann Neurol 2018;83:970–979
Engineering von Proteinen an Oberflächen: Von komplementärer Charakterisierung zu Materialoberflächen mit maßgeschneiderten Funktionen
Authors: Morsbach Svenja , Gonella Grazia , Mailänder Volker , Wegner Seraphine , Wu Si , Weidner Tobias , Berger Rüdiger , Koynov Kaloian , Vollmer Doris , Encinas Noemí , Kuan Seah Ling , Bereau Tristan , Kremer Kurt , Weil Tanja , Bonn Mischa , Butt Hans‐Jürgen , Landfester Katharina 
Published: April 2018

AbstractSobald Materialien mit einer biologischen Flüssigkeit, die Proteine enthält, in Kontakt kommen, werden Proteine im Allgemeinen – ob gewünscht oder nicht – von der Oberfläche des Materials angezogen und adsorbieren darauf. Das Ziel dieses Aufsatzes ist es, einen Überblick über die am häufigsten verwendeten Charakterisierungsmethoden zu geben, um ein besseres Verständnis der Adsorptionsprozesse auf planaren oder gekrümmten Oberflächen zu erhalten. Wir zeigen weiterhin den Vorteil der Kombination verschiedener Methoden, um auf unterschiedliche Oberflächengeometrien des Materials zuzugreifen. Die so erhaltenen Erkenntnisse ebnen idealerweise den Weg für die Entwicklung funktioneller Materialien, die in einer vorbestimmten Weise mit Proteinen interagieren.
Gewinnung reaktiver Fullerene aus Ruß durch exohedrale Derivatisierung
Authors: Yamada Michio , Akasaka Takeshi , Nagase Shigeru 
Published: April 2018

AbstractDie bemerkenswerte Allotropie von Kohlenstoff liefert zahlreiche topologisch mögliche Käfigstrukturen von molekularem Kohlenstoff. Dazu gehören auch die sogenannten endohedralen Metallofullerene, bei denen ein Metallatom im Käfig eingeschlossen ist. Stabile und lösliche leere Fullerene und endohedrale Metallofullerene in reiner Form sind in makroskopischen Mengen durch Erzeugung im Kohlenstofflichtbogen oder andere physikalische Prozesse mit anschließender Extraktion und chromatographischer Trennung verfügbar. Jedoch bleiben viele andere, nicht identifizierte Fulleren‐Spezies, die in ihrer reinen Form offenbar reaktiv und unlöslich sind, im Ruß zurück. Solche “fehlenden” Spezies müssen extrem kleine HOMO‐LUMO‐Aufspaltungen aufweisen und könnten unkonventionelle Käfigstrukturen zeigen. Jüngste Fortschritte in diesem Bereich haben gezeigt, dass sich reaktive Fullerene unter Verwendung einer exohedralen Derivatisierung gewinnen lassen, durch die die reaktiven Kohlenstoffkäfige stabilisiert werden können. Dieses Konzept bietet ein Mittel zur Produktion von makroskopischen Mengen unkonventioneller Fullerene.
Spectral Imaging and Archival Data in Analysing Madonna of the Rabbit Paintings by Manet and Titian
Authors: Striova Jana , Ruberto Chiara , Barucci Marco , Blažek Jan , Kunzelman Diane , Dal Fovo Alice , Pampaloni Enrico , Fontana Raffaella 
Published: April 2018

AbstractA concise insight into the outputs provided by the latest prototype of visible‐near infrared (Vis‐NIR) multispectral scanner (National Research Council‐National Institute of Optics, CNR‐INO, Italy) is presented. The analytical data acquired on an oil painting Madonna of the Rabbit by É. Manet are described. In this work, the Vis‐NIR was complemented with X‐ray fluorescence (XRF) mapping for the chemical and spatial characterization of several pigments. The spatially registered Vis‐NIR data facilitated their processing by spectral correlation mapping (SCM) and artificial neural network (ANN) algorithm, respectively, for pigment mapping and improved visibility of pentimenti and of underdrawing style. The data provided several key elements for the comparison with a homonymous original work by Titian studied within the ARCHive LABoratory (ARCHLAB) transnational access project.
Wasserbildung unter dünnen Silika‐Filmen: Echtzeitbeobachtung einer chemischen Reaktion in einem physikalisch eingegrenzten Raum
Authors: Prieto Mauricio J. , Klemm Hagen W. , Xiong Feng , Gottlob Daniel M. , Menzel Dietrich , Schmidt Thomas , Freund Hans‐Joachim 
Published: April 2018

AbstractMit niederenergetischer Elektronenmikroskopie und lokaler Fotoelektronenspektroskopie wurde die Bildung von Wasser aus absorbierten O und H2 auf einer Ru(0001)‐Oberfläche untersucht, die mit einer glasartigen SiO2‐Bilage (BL) bedeckt war, und mit der gleichen Reaktion auf der reinen Ru(0001)‐Oberfläche verglichen. In beiden Fällen tritt eine fortschreitende Reaktionsfront auf. Der Grund hierfür kann mit der Anforderung zusammenhängen, dass die O‐Adatome Platz freigeben müssen, damit weiterer H2 dissoziativ adsorbiert. Wir finden scheinbare Aktivierungsenergien (
) für die Frontbewegung von 0.59 eV ohne Deckschicht und 0.27 eV mit Deckschicht. Wir schlagen vor, dass bei der SiO2‐BL‐bedeckten Ru(0001)‐Oberfläche die geringere Aktivierungsenergie aber höhere Reaktionstemperatur durch eine Änderung des geschwindigkeitsbestimmenden Schritts verursacht wird. Weitere mögliche Auswirkungen der Deckschicht werden diskutiert. Unsere Resultate ergeben die ersten Werte für
im eingegrenzten Raum (“confinement”).
Fluor‐NMR‐Spektroskopie rekalibriert
Authors: Rosenau Carl Philipp , Jelier Benson J. , Gossert Alvar D. , Togni Antonio 
Published: April 2018

AbstractFluorchemie nimmt eine zentrale Rolle bei der Entdeckung chemischer Reaktionen, in der Wirkstoffentwicklung und in der Chemischen Biologie ein. NMR‐Spektroskopie, die wohl meistbenutzte und wichtigste analytische Methode für fluorierte Verbindungen, weist weitverbreitete Missstände auf, die durch inkonsistentes Referenzieren chemischer Verschiebungen zustande kommen und Abweichungen von über 1 ppm verursachen können. In dieser Zuschrift beschreiben wir neuartige, eindeutige Belege, die zeigen, wie es – unbeabsichtigt – zur weitverbreiteten Streuung von 19F‐NMR‐chemischen‐Verschiebungen gekommen ist. Dies betrifft sowohl die Konzipierung der Spektrometer als auch das gegenwärtige Unified Scale System, das typischerweise als Grundlage für die Kalibrierung von heteronuklearen NMR‐Spektren dient. Wir zeigen, dass internes Referenzieren als robuste, pragmatische und reproduzierbare Methode die Abweichung chemischer Verschiebungen, die an mehreren verschiedenen Instituten gemessen wurden, auf weniger als 30 ppb minimiert. Schließlich wird eine umfassende Tabelle mit entsprechend kalibrierten Referenzverbindungen zur Verfügung gestellt, die es Nutzern ermöglicht, 19F‐NMR‐Spektren künftig korrekt zu kalibrieren.
Wrapping Nanocellulose Nets around Graphene Oxide Sheets
Authors: Xiong Rui , Kim Ho Shin , Zhang Lijuan , Korolovych Volodymyr F. , Zhang Shuaidi , Yingling Yaroslava G. , Tsukruk Vladimir V. 
Published: April 2018

AbstractConstructing advanced functional nanomaterials with pre‐designed organized morphologies from low‐dimension synthetic and biological components is challenging. Herein, we report an efficient and universal amphiphilicity‐driven assembly strategy to construct “hairy” flexible hybrid nanosheets with a 1D cellulose nanofibers (CNFs) net conformally wrapped around 2D graphene oxide (GO) monolayers. This interface‐driven bio‐synthetic assembly is facilitated by tailoring the surface chemistry of flexible GO sheets, resulting in individual sheets tightly surrounded by dense conformal nanocellulose network. The mechanical stability of the products far exceeds the compressive instability limits of both individual components. Additionally, the CNF network significantly enhances the wetting ability of initial hydrophobic reduced GO nanosheets, allowing fast water transport combined with high filtration efficiency.
Von einer Helix zu einem kleinen Ring: Metadynamik‐inspirierte, selektive Liganden für αvβ6‐Integrin
Authors: Di Leva Francesco Saverio , Tomassi Stefano , Di Maro Salvatore , Reichart Florian , Notni Johannes , Dangi Abha , Marelli Udaya Kiran , Brancaccio Diego , Merlino Francesco , Wester Hans‐Jürgen , Novellino Ettore , Kessler Horst , Marinelli Luciana 
Published: April 2018

AbstractDas RGD‐erkennende Integrin αvβ6 trat in jüngster Zeit als vielbeachtete Zielstruktur für die Diagnostik und Therapie von Krebserkrankungen in Erscheinung. Infolgedessen besteht derzeit ein dringender Bedarf an niedermolekularen Liganden für diesen Rezeptor. Ein auf Metadynamik beruhender Ansatz ermöglichte die erfolgreiche Konvertierung eines helikalen Nonapeptids in ein zyklisches Pentapeptid (6) mit bemerkenswerter Affinität und Spezifität für αvβ6‐Integrin. Die Gründe hierfür konnten mittels NMR‐ und Docking‐Untersuchungen aufgeklärt werden und bilden einen Ausgangspunkt für die zielgerichtete Konzeption neuer αvβ6‐spezifischer Peptide oder sogar Peptidomimetika. Des Weiteren wurde die Möglichkeit einer medizinischen Anwendung von 6 mittels PET‐Bildgebungsexperimenten im lebenden Organismus veranschaulicht.
Divergent Coupling of Anilines and Enones by Integration of C−H Activation and Transfer Hydrogenation
Authors: Zhou Xukai , Xia Jintao , Zheng Guangfan , Kong Lingheng , Li Xingwei 
Published: April 2018

AbstractCp*RhIII/IrIII complexes are known to play important roles in both C−H activation and transfer hydrogenation (TH). However, these two areas evolved separately. They have been integrated in redox‐ and chemodivergent coupling reactions of N‐pyridylanilines with enones. The iridium‐catalyzed coupling with enones leads to the efficient synthesis of tetrahydroquinolines through TH from iPrOH. Counterintuitively, iPrOH does not serve as the sole hydride source, and the major reaction pathway involves disproportionation of a dihydroquinoline intermediate, followed by the convergent and iterative reduction of quinolinium species.
Polar Fluorooxoborate, NaB4O6F: A Promising Material for Ionic Conduction and Nonlinear Optics
Authors: Zhang Zhizhong , Wang Ying , Zhang Bingbing , Yang Zhihua , Pan Shilie 
Published: April 2018

AbstractThe search of new borates with improved functional properties has attracted considerable attention. Herein, a new polar fluorooxoborate, NaB4O6F (NBF) was prepared by high‐temperature solid‐state reaction. NBF belongs to the AB4O6F family (A=alkali metal or ammonium), a series of compounds that undergoes significant cation‐dependent structural changes. NBF is of particular interest owing to the special cation position. Temperature‐dependent ionic conductivity measurements show that NBF is a solid ionic conductor, and it has the lowest active energy of 32.5 kJ mol−1 of fluorooxoborates. NBF also shows a second‐harmonic generation (SHG) response of 0.9×KH2PO4 and 0.2×β‐BaB2O4, at 1064 and 532 nm, respectively, and it has a short UV cutoff edge below 180 nm. Based on bond valence (BV) concepts, symmetry analysis, and the first principles calculation, the unique [B4O6F]∞ layer can be regarded as the “multifunctional unit”, which is responsible for the observed properties of NBF.
Bottom‐up Construction of π‐Extended Arenes by a Palladium‐Catalyzed Annulative Dimerization of o‐Iodobiaryl Compounds
Authors: Zhu Chendan , Wang Di , Wang Dingyi , Zhao Yue , Sun Wei‐Yin , Shi Zhuangzhi 
Published: April 2018

AbstractA straightforward method was developed for construction of aromatic compounds with a triphenylene core. The method involves Pd‐catalyzed annulative dimerization of o‐iodobiaryl compounds by double C−I and C−H bond cleavage steps. Simple reaction conditions are needed, requiring neither a ligand nor an oxidant, and the reaction tolerates a wide range of coupling partners without compromising efficiency or scalability. Significantly, the tetrachloro‐substituted synthon, 1,6,11‐trichloro‐4‐(4‐chlorophenyl)triphenylene, can be generated and used to prepare a series of fully fused, small graphene nanoribbons by a late‐stage arylation with arylboronic acids and a subsequent Scholl reaction. The synthetic strategy enables bottom‐up access to extended π‐systems in a controlled manner.
Engineering Proteins at Interfaces: From Complementary Characterization to Material Surfaces with Designed Functions
Authors: Morsbach Svenja , Gonella Grazia , Mailänder Volker , Wegner Seraphine , Wu Si , Weidner Tobias , Berger Rüdiger , Koynov Kaloian , Vollmer Doris , Encinas Noemí , Kuan Seah Ling , Bereau Tristan , Kremer Kurt , Weil Tanja , Bonn Mischa , Butt Hans‐Jürgen , Landfester Katharina 
Published: April 2018

AbstractOnce materials come into contact with a biological fluid containing proteins, proteins are generally—whether desired or not—attracted by the material's surface and adsorb onto it. The aim of this Review is to give an overview of the most commonly used characterization methods employed to gain a better understanding of the adsorption processes on either planar or curved surfaces. We continue to illustrate the benefit of combining different methods to different surface geometries of the material. The thus obtained insight ideally paves the way for engineering functional materials that interact with proteins in a predetermined manner.
Salvaging Reactive Fullerenes from Soot by Exohedral Derivatization
Authors: Yamada Michio , Akasaka Takeshi , Nagase Shigeru 
Published: April 2018

AbstractThe awesome allotropy of carbon yields innumerable topologically possible cage structures of molecular carbon. This field is also related to endohedral metallofullerenes constructed by metal‐atom encapsulation. Stable and soluble empty fullerenes and endohedral metallofullerenes are available in pure form in macroscopic amounts from carbon arc production or other physical processes followed by extraction and subsequent chromatographic separation. However, many other unidentified fullerene species, which must be reactive and insoluble in their pristine forms, remain in soot. These “missing” species must have extremely small HOMO–LUMO gaps and may have unconventional cage structures. Recent progress in this field has demonstrated that reactive fullerenes can be salvaged by exohedral derivatization, which can stabilize the reactive carbon cages. This concept provides a means of preparing macroscopic amounts of unconventional fullerenes as their derivatives.
Water Formation under Silica Thin Films: Real‐Time Observation of a Chemical Reaction in a Physically Confined Space
Authors: Prieto Mauricio J. , Klemm Hagen W. , Xiong Feng , Gottlob Daniel M. , Menzel Dietrich , Schmidt Thomas , Freund Hans‐Joachim 
Published: April 2018

AbstractUsing low‐energy electron microscopy and local photoelectron spectroscopy, water formation from adsorbed O and H2 on a Ru(0001) surface covered with a vitreous SiO2 bilayer (BL) was investigated and compared to the same reaction on bare Ru(0001). In both cases the reaction is characterized by moving reaction fronts. The reason for this might be related to the requirement of site release by O adatoms for further H2‐dissociative adsorption. Apparent activation energies (
) are found for the front motion of 0.59 eV without cover and 0.27 eV under cover. We suggest that the smaller activation energy but higher reaction temperature for the reaction on the SiO2 BL covered Ru(0001) surface is due to a change of the rate‐determining step. Other possible effects of the cover are discussed. Our results give the first values for
in confined space.
Macrotheranostic Probe with Disease‐Activated Near‐Infrared Fluorescence, Photoacoustic, and Photothermal Signals for Imaging‐Guided Therapy
Authors: Zhen Xu , Zhang Jianjian , Huang Jiaguo , Xie Chen , Miao Qingqing , Pu Kanyi 
Published: April 2018

AbstractTheranostics provides opportunities for precision cancer therapy. However, theranostic probes that simultaneously turn on their diagnostic signal and pharmacological action only in respond to a targeted biomarker have been less exploited. We herein report the synthesis of a macrotheranostic probe that specifically activates its near‐infrared fluorescence (NIRF), photoacoustic (PA), and photothermal signals in the presence of a cancer‐overexpressed enzyme for imaging‐guided cancer therapy. Superior to the small‐molecule counterpart probe, the macrotheranostic probe has ideal biodistribution and renal clearance, permitting passive targeting of tumors, in situ activation of multimodal signals, and effective photothermal ablation. Our study thus provides a macromolecular approach towards activatable multimodal phototheranostics.
Mono‐ and binuclear nickel catalysts for 1‐hexene polymerization
Authors: Dechal Abbas , Khoshsefat Mostafa , Ahmadjo Saeid , Mortazavi Seyed Mohammad Mahdi , Zohuri Gholam Hossein , Abedini Hossein 
Published: April 2018

Polymerization of 1‐hexene was carried out using a mononuclear (MN) catalyst and two binuclear (BN1 and BN2) α‐diimine Ni‐based catalysts synthesized under controlled conditions. Ethylaluminium sesquichloride (EASC) was used as an efficient activator under various polymerization conditions. The highly active BN2 catalyst (2372 g poly(1‐hexene) (PH) mmol−1 cat) in comparison to BN1 (920 g PH mmol−1 cat) and the MN catalyst (819 g PH mmol−1 cat) resulted in the highest viscosity‐average molecular weight (Mv) of polymer. Moreover, the molecular weight distribution (MWD) of PH obtained using BN2/EASC was slightly broader than those obtained using BN1 and MN (2.46 for BN2 versus 2.30 and 1.96 for BN1 and MN, respectively). These results, along with the highest extent of chain walking for BN2, were attributed to steric, nuclearity and electronic effects of the catalyst structures which could control the catalyst behaviour. Differential scanning calorimetry showed that the glass transition temperatures of polymers were in the range − 58 to −81 °C, and broad melting peaks below and above 0 °C were also observed. In addition, longer α‐olefins (1‐octene and 1‐decene) were polymerized and characterized, for which higher yield, conversion and molecular weight were observed with a narrower MWD. The polymerization parameters such as polymerization time and polymerization temperature showed a significant influence on the productivity of the catalysts and Mv of samples.
Sucrose chelated auto combustion synthesis of BiFeO3 nanoparticles: Magnetically recoverable catalyst for the one‐pot synthesis of polyhydroquinoline
Authors: Singh Harminder , Garg Nidhi , Arora Priya , Rajput Jaspreet Kaur , Jigyasa  
Published: April 2018

Sucrose chelated Bismuth ferrite (BiFeO3) nanoparticles as a novel heterogeneous catalyst was synthesized by an auto combustion route. Different calcination temperatures (150 °C, 450 °C, 550 °C, 650 °C, 750 °C and 850 °C) have been employed to obtain single phased BiFeO3 nanoparticles. The perovskite structure formation and disappearance of organic phase (sucrose) was obtained by Fourier transform infrared spectroscopy (FT‐IR). Phase determination and structural characterization was carried out by powder X‐ray diffraction (XRD). The magnetic properties were analyzed by vibrating sample magnetometer (VSM) whereas surface area/pore volume was obtained by Brunauer–Emmett–Teller (BET). Transmission electron microscope (TEM) analyzed the particles size and morphology. Thermal stability was investigated by thermogravimetric analysis (TGA) and determination of constituent elements was carried out by X‐ray Photo‐Electron Spectroscopy (XPS). Raman spectroscopy confirmed the perovskite structure of the synthesized materials. The BiFeO3 nanoparticles so obtained were employed as heterogeneous catalyst for the synthesis of polyhydroquinoline derivatives. All the polyhydroquinoline derivatives were characterized by Fourier transform infrared spectroscopy (FT‐IR) and Nuclear magnetic resonance spectroscopy (1H NMR). For the very first time ever we have used BiFeO3 as a recyclable magnetic nanocatalyst in the one‐pot four component cyclization reaction of benzaldehyde, ethylacetoacetate/methylacetoacetate, dimedone/cyclohexane‐1,3‐dione, and ammonium acetate for the synthesis of polyhydroquinoline derivatives without solvent under refluxing conditions to provide excellent yields of products. BiFeO3 nanocatalyst (without any functionalization/surface coatings) shows easy magnetic separation, recyclability, reusability along with excellent yield of polyhydroquinoline derivatives in an economic and benign way.
Triel–hydride triel bond between ZX3 (Z = B and Al; X = H and Me) and THMe3 (T = Si, Ge and Sn)
Authors: Zhang Jingru , Wei Yuanxin , Li Wenzuo , Cheng Jianbo , Li Qingzhong 
Published: April 2018

Complexes between THMe3 (T = Si, Ge and Sn) and ZX3 (Z = B and Al; X = H and Me) have been characterized using MP2/aug‐cc‐pVTZ calculations. These complexes are chiefly stabilized by a triel–hydride triel bond with the T–H bond pointing to the π‐hole on the triel atom. The triel–hydride interaction is mainly attributed to the charge transfer from the T–H bond orbital to the empty p orbital of the triel atom. These complexes are very stable with a large interaction energy (>10 kcal mol−1) excluding THMe3···BMe3 (T = Si and Ge), indicating that the sp2‐hydridized triel atom has a strong affinity for the T–H bond. The formation of THMe3···BH3 results in proton transfer, characterized by conversion of orbital interaction and large charge transfer (ca 0.5e). The large deformation is primarily responsible for the abnormally greater interaction energy in THMe3···BH3 (>30 kcal mol−1) than in the AlH3 analogue. Methyl substitution on the triel atom weakens the triel–hydride interaction and causes a larger interaction energy in THMe3···AlMe3 with respect to its BMe3 counterpart. Most of these interactions possess characteristics of covalent bonds. Polarization makes a contribution to the stability of most complexes nearly equivalent to the electrostatic term.