bluuebunny/crossref_metadata_2025_split huggingface dataset:
Matrix metalloproteinase 9 is decreased in natalizumab‐treated multiple sclerosis patients at risk for progressive multifocal leukoencephalopathy
Authors: Fissolo Nicolas , Pignolet Béatrice , Matute‐Blanch Clara , Triviño Juan Carlos , Miró Berta , Mota Miriam , Perez‐Hoyos Santiago , Sanchez Alex , Vermersch Patrick , Ruet Aurélie , de Sèze Jérôme , Labauge Pierre , Vukusic Sandra , Papeix Caroline , Almoyna Laurent , Tourbah Ayman , Clavelou Pierre , Moreau Thibault , Pelletier Jean , Lebrun‐Frenay Christine , Montalban Xavier , Brassat David , Comabella Manuel ,   on behalf of Biomarkers and Response to Natalizumab for Multiple Sclerosis Treatment (BIONAT), Best EScalation Treatment in Multiple Sclerosis (BEST‐MS), and the Société Francophone de la Sclérose En Plaques (SFSEP) Network
Published: July 2017

ObjectiveTo identify biomarkers associated with the development of progressive multifocal leukoencephalopathy (PML) in multiple sclerosis (MS) patients treated with natalizumab (NTZ).MethodsRelapsing–remitting MS patients who developed PML under NTZ therapy (pre‐PML) and non‐PML NTZ‐treated patients (NTZ‐ctr) were included in the study. Cryopreserved peripheral blood mononuclear cells and serum samples collected at baseline, at 1‐ and 2‐year treated time points, and during PML were analyzed for gene expression by RNA sequencing and for serum protein levels by Luminex and enzyme‐linked immunosorbent assays, respectively.ResultsAmong top differentially expressed genes in the RNA sequencing between pre‐PML and NTZ‐ctr patients, pathway analysis revealed a high representation of genes belonging to the following categories: proangiogenic factors (MMP9, VEGFA), chemokines (CXCL1, CXCL5, IL8, CCL2), cytokines (IL1B, IFNG), and plasminogen‐ and coagulation‐related molecules (SERPINB2, PLAU, PLAUR, TFPI, THBD). Serum protein levels for these candidates were measured in a 2‐step manner in a screening cohort and a validation cohort of pre‐PML and NTZ‐ctr patients. Only matrix metalloproteinase 9 (MMP9) was validated; in pre‐PML patients, MMP9 protein levels were significantly reduced at baseline compared with NTZ‐ctr patients, and levels remained lower at later time points during NTZ treatment.InterpretationThe results from this study suggest that the proangiogenic factor MMP9 may play a role as a biomarker associated with the development of PML in MS patients treated with NTZ. Ann Neurol 2017;82:186–195.
Vermeiden von Selbstvergiftung – ein Schlüsselaspekt für die hohe Aktivität von Au/Mg(OH)2‐Katalysatoren in der kontinuierlichen Niedertemperatur‐CO‐Oxidation
Authors: Wang Yuchen , Widmann Daniel , Lehnert Felix , Gu Dong , Schüth Ferdi , Behm R. Jürgen 
Published: July 2017

AbstractNach neueren Berichten sind Au/Mg(OH)2‐Katalysatoren bei niedrigen Temperaturen, unterhalb Raumtemperatur, weitaus aktiver in der katalytischen CO‐Oxidation als die häufig untersuchten Au/TiO2‐Katalysatoren. Mithilfe kinetischer und in‐situ‐IR‐spektroskopischer (DRIFTS‐)Messungen wird gezeigt, dass die vergleichsweise schwache Wechselwirkung von Au/Mg(OH)2 mit in der Reaktion gebildetem CO2 der hauptsächliche Grund für die höhere Aktivität dieser Katalysatoren bei niedrigen Reaktionstemperaturen ist. Dies ermöglicht die schnelle Desorption des Reaktionsprodukts CO2 und damit eine effiziente kontinuierliche Oxidation von CO bei Temperaturen deutlich unterhalb 0 °C. Bei diesen Temperaturen katalysiert Au/TiO2 zwar auch die Bildung von CO2, hier ist aber kaum CO2‐Desorption möglich, und dies führt zu einer Selbstvergiftung des Katalysators. Bei höheren Temperaturen (oberhalb 0 °C) ist dagegen die Bildung von CO2 geschwindigkeitsbestimmend, was in einer deutlich höheren Aktivität von Au/TiO2‐Katalysatoren unter diesen Bedingungen resultiert.
Diketopyrrolopyrrole Columnar Liquid‐Crystalline Assembly Directed by Quadruple Hydrogen Bonds
Authors: Soberats Bartolome , Hecht Markus , Würthner Frank 
Published: July 2017

AbstractA diketopyrrolopyrrole (DPP) dye self‐assembles via a unique hydrogen‐bonding motif into an unprecedented columnar liquid‐crystalline (LC) structure. X‐ray and polarized FTIR experiments reveal that the DPPs organize into a one‐dimensional assembly with the chromophores oriented parallel to the columnar axis. This columnar structure is composed of two π–π‐stacked DPP dimers with mirror‐image configurations that stack alternately through quadruple hydrogen bonding by 90° rotation. This exotic packing is dictated by the complementarity between H‐bonds and the steric demands of the wedge‐shaped groups attached at the core. This novel LC supramolecular material opens a new avenue of research on DPP dye assemblies with photofunctional properties tailored by H‐bonding networks.
Zirconium/Nickel‐Mediated One‐Pot Ketone Synthesis
Authors: Ai Yanran , Ye Ning , Wang Qiaoyi , Yahata Kenzo , Kishi Yoshito 
Published: July 2017

AbstractA zirconium/nickel‐mediated one‐pot synthesis of ketones is reported. In the presence of Zn or Mn, Cp2ZrCl2 was found to dramatically accelerate the coupling and suppress side product formation via an I→SPy displacement at the same time. Unlike Zn/Pd‐ and Fe/Cu‐mediated one‐pot ketone syntheses, the new method is effective for nucleophiles bearing OR or equivalent functional groups at the α‐position. A mechanism comprising a nickel catalytic cycle, a zirconium catalytic cycle, and Zr→Ni transmetalation is proposed, and Cp2ZrCl2 and/or low‐valent Zr species are suggested to play crucial dual roles.
A Water‐Bridged H‐Bonding Network Contributes to the Catalysis of the SAM‐Dependent C‐Methyltransferase HcgC
Authors: Bai Liping , Wagner Tristan , Xu Tao , Hu Xile , Ermler Ulrich , Shima Seigo 
Published: July 2017

Abstract[Fe]‐hydrogenase hosts an iron‐guanylylpyridinol (FeGP) cofactor. The FeGP cofactor contains a pyridinol ring substituted with GMP, two methyl groups, and an acylmethyl group. HcgC, an enzyme involved in FeGP biosynthesis, catalyzes methyl transfer from S‐adenosylmethionine (SAM) to C3 of 6‐carboxymethyl‐5‐methyl‐4‐hydroxy‐2‐pyridinol (2). We report on the ternary structure of HcgC/S‐adenosylhomocysteine (SAH, the demethylated product of SAM) and 2 at 1.7 Å resolution. The proximity of C3 of substrate 2 and the S atom of SAH indicates a catalytically productive geometry. The hydroxy and carboxy groups of substrate 2 are hydrogen‐bonded with I115 and T179, as well as through a series of water molecules linked with polar and a few protonatable groups. These interactions stabilize the deprotonated state of the hydroxy groups and a keto form of substrate 2, through which the nucleophilicity of C3 is increased by resonance effects. Complemented by mutational analysis, a structure‐based catalytic mechanism was proposed.
Validation of Molecular Simulation: An Overview of Issues
Authors: van Gunsteren Wilfred F. , Daura Xavier , Hansen Niels , Mark Alan E. , Oostenbrink Chris , Riniker Sereina , Smith Lorna J. 
Published: July 2017

AbstractComputer simulation of molecular systems enables structure–energy–function relationships of molecular processes to be described at the sub‐atomic, atomic, supra‐atomic, or supra‐molecular level. To interpret results of such simulations appropriately, the quality of the calculated properties must be evaluated. This depends on the way the simulations are performed and on the way they are validated by comparison to values Qexp of experimentally observable quantities Q. One must consider 1) the accuracy of Qexp, 2) the accuracy of the function Q(rN) used to calculate a Q‐value based on a molecular configuration rN of N particles, 3) the sensitivity of the function Q(rN) to the configuration rN, 4) the relative time scales of the simulation and experiment, 5) the degree to which the calculated and experimental properties are equivalent, and 6) the degree to which the system simulated matches the experimental conditions. Experimental data is limited in scope and generally corresponds to averages over both time and space. A critical analysis of the various factors influencing the apparent degree of (dis)agreement between simulations and experiment is presented and illustrated using examples from the literature. What can be done to enhance the validation of molecular simulation is also discussed.
Unified, Efficient, and Scalable Synthesis of Halichondrins: Zirconium/Nickel‐Mediated One‐Pot Ketone Synthesis as the Final Coupling Reaction
Authors: Yahata Kenzo , Ye Ning , Ai Yanran , Iso Kentaro , Kishi Yoshito 
Published: July 2017

AbstractUnified, efficient, and scalable syntheses of the halichondrin natural products are reported. A newly developed Zr/Ni‐mediated one‐pot ketone synthesis was used to couple the two halves of the final product at a late stage in the synthesis. With the use of a slight excess of the left halves, the desired ketones were isolated in yields of 80–90 %. The halichondrins were obtained from these ketones in two steps, namely desilylation and [5,5]‐spiroketal formation. The new synthetic route was effective for the total synthesis of all members in the homohalichondrin subgroup. The scalability of this process was demonstrated with halichondrin B; 150 mg of halichondrin B (68 % overall yield) were obtained from 200 mg of the right‐half precursor.
Codeposition of catechol–polyethyleneimine followed by interfacial polymerization for nanofiltration membranes with enhanced stability
Authors: Qiu Wen‐Ze , Du Yong , Lv Yan , Yang Hao‐Cheng , Xu Zhi‐Kang 
Published: July 2017

ABSTRACTThin‐film composite (TFC) nanofiltration (NF) membranes were fabricated via the codeposition of catechol (CCh) and polyethyleneimine (PEI) followed by subsequent interfacial polymerization with trimesoyl chloride (TMC) on the surface of polysulfone ultrafiltration substrates. The detailed structures and surface properties were characterized by X‐ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, scanning electron microscopy, ζ potential analysis, and water contact angle measurement. The surface properties, including the roughness, hydrophilicity, surface potential, and NF performances, were facilely tuned through variation of the codeposition time of CCh–PEI for the prepared TFC membranes. The optimized membrane achieved a high rejection (ca. 93%) of MgCl2 with a flux of around 31 L m−2 h−1 under 0.7 MPa. The results also reveal that the codeposition process endowed the final membranes with much better structural stability in alcohol and improved chlorine resistance compared to commonly interfacial polymerized ones with PEI and TMC. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 45422.
Dual‐bonding structured ternary composite film of poly(vinyl alcohol)–boric acid–nanodiamond
Authors: Li Yina , Xu Xiangyang , Zhao Hongye , Wei Shanshan , Lu Qinghua , Dai Lei , Yang Lin 
Published: July 2017

ABSTRACTTernary composite films of poly(vinyl alcohol) (PVA), boric acid (BA), and detonation nanodiamond (DND) were prepared by aqueous solution method. Because of its excellent mechanical/thermal properties and low friction coefficient, DND is expected to offer PVA film superior performance if the puzzles of particle agglomeration in polymer matrix and fragile interface reaction between DND and PVA can be settled. BA was used as a crosslinking agent to form a strong network structure between DND and PVA. Investigation on microstructure of PVA/BA/DND films and bonding mechanisms therein shows that BA, DND, and PVA may crosslink by oxo‐bridges owing to the interaction of hydroxyl groups. The Young's modulus (E) of composite films was enhanced by nearly 3.3 times with only 0.8 wt % DND loading, and the antiwear, thermal stability, and waterproof properties can be significantly improved after the crosslinking. Meanwhile, the transparency of composite films can be well preserved even with large DND content. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 45449.
Distribution of Calretinin Immunoreactivity in the Lateral Nucleus of the Bottlenose Dolphin (Tursiops truncatus) Amygdala
Authors: Rambaldi A.M. , Cozzi B. , Grandis A. , Canova M. , Mazzoni M. , Bombardi C. 
Published: July 2017

ABSTRACTThe amgdaloid complex consists of different nuclei, each with unique cytoarchitectonic, chemoarchitectonic and connectional characteristics. Most of the inputs coming from cortical and subcortical areas enter the amygdala via the lateral nucleus, which makes it the main receiving structure of the complex. The activity of its neurons is coordinated and modulated by different inhibitory, GABAergic‐interneurons, which can be classified for their expression of various calcium‐binding proteins, as well as by morphological characteristics. This research based on the analysis of the amygdala of three bottlenose dolphins, provides the first description of the topography, cytoarchitecture and distribution of calretinin immunoreactivity of the lateral nucleus. Our observations on the bottlenose dolphin confirmed the general topography of the mammalian amygdala and of the lateral nucleus. Notably, we identified six subdivision of the nucleus, more than those reported until now in the rat, monkey and human lateral nucleus. This could reveal an outstanding capability of integration and elaboration of external stimuli. In addition, we observed a strong presence of CR‐immunoreactive (‐ir) neurons and fibres. CR‐ir neurons were mainly non‐pyramidal inhibitory neurons; in particular, 80% of IR‐cells were represented by large and small polygonal neurons. In the lateral nucleus of the human amygdala, CR‐ir neurons form inhibitory synapses on calbindin‐D28k‐IR inhibitory interneurons. Since calbindin‐D28k‐ir interneurons make inhibitory synapses on the pyramidal cells, the final goal of the CR‐ir interneurons could be the synchronization of cells activity, thus playing an important role in the control of information flow in the lateral amygdalar nucleus. Anat Rec, 2017. © 2017 Wiley Periodicals, Inc. Anat Rec, 300:2008–2016, 2017. © 2017 Wiley Periodicals, Inc.
A Novel Method for Observation of the Mandibular Foramen: Application to a Better Understanding of Dental Anatomy
Authors: Iwanaga Joe , Watanabe Koichi , Saga Tsuyoshi , Tubbs R. Shane , Tanaka Kengo , Kikuta Shogo , Tabira Yoko , Fisahn Christian , Kamura Yasuhiko , Kusukawa Jingo , Yamaki Koh‐Ichi 
Published: July 2017

ABSTRACTCone‐beam computed tomography gives us much useful morphological information about the mandibular bone. Many studies of the mandible include findings from this technique. However, there have been no endoscopic studies of the mandible. Sixteen sides of eight dry mandibles resected from cadavers (age range 38–83 years) were examined by endoscopy. The head of the endoscope was 2.0 mm in diameter. We examined the mandibular foramen, lingula, mylohyoid groove, and mandibular canal. The mylohyoid grooves showed variations such as double grooves and canals. The mandibular lingula was located superior or medial to the the mandibular foramen. In a single case, the medial wall inside the mandibular canal showed a porous surface. The retromolar canal was observed in three sides. None of the images in the present study have been seen in other studies. Observation of the retromolar canal from the mandibular canal in particular can help dental students as well as oral and maxillofacial surgeons to understand its morphology. Anat Rec, 2017. © 2017 Wiley Periodicals, Inc. Anat Rec, 300:1875–1880, 2017. © 2017 Wiley Periodicals, Inc.
Greenhouse gas emissions of electricity and biomethane produced using the Biogasdoneright™ system: four case studies from Italy
Authors: Valli Laura , Rossi Lorella , Fabbri Claudio , Sibilla Fabrizio , Gattoni Piero , Dale Bruce E. , Kim Seungdo , Ong Rebecca Garlock , Bozzetto Stefano 
Published: July 2017

AbstractWe reported previously on the Biogasdoneright™ system for on‐farm biogas production. This innovative system employs sequential (year‐round) cropping to produce both food and energy from agricultural biomass, primarily cellulosic materials. This paper uses a marginal analysis approach to estimate the life cycle greenhouse gas emissions (GHGs) of electricity and biomethane produced by four currently operating Italian biogas plants that process various agricultural feedstocks, residues, and by‐products. The biogas is burned on‐farm to generate electricity that is then exported to the grid. The marginal lifecycle GHGs of this farm‐produced electricity range from ‐335 to 25 grams CO2 per kilowatt hour (kWh). By comparison, the marginal GHGs of electricity generated by fossil fuels in the European Union (EU) is 752 grams CO2 per kWh. The biogas might also be upgraded to produce pipeline‐quality biomethane, a direct substitute for natural gas. The marginal lifecycle GHGs of biomethane potentially produced from the Biogasdoneright™ plants range from 10 to ‐36 grams CO2 per megajoule (MJ) while the corresponding figure for a conventional biogas plant is 27 grams CO2 per MJ. Natural gas in the EU produces 72 grams CO2 per MJ and marginal fossil fuel in the EU generates 115 grams CO2 per MJ. Negative GHG emissions arise largely from avoided emissions of agricultural effluents and residues. © 2017 Society of Chemical Industry and John Wiley & Sons, Ltd
The luminescence properties of Sr2–1.5x−1.5yP2O7:xDy3+,yCe3+ phosphor for near‐UV‐based white LEDs synthesized by a chemical co‐precipitation method
Authors: Liu Sha‐Sha , Zhu Da‐Chuan , Wang Jin‐Shan , Zhao Cong , Han Tao 
Published: July 2017

AbstractA series of Sr2P2O7:Dy3+, Sr2P2O7:Ce3+ and Sr2P2O7:Dy3+,Ce3+ phosphors was synthesized via the one‐step calcination process for the precursors prepared by co‐precipitation methods. The phases, morphology, quantum efficiency and photoluminescence properties of the obtained phosphors were characterized systematically. These results show that the near‐spherical particles prepared through calcining the precursors by means of ammonium dibasic phosphate co‐precipitation (method 3) have the smallest particle size and strongest emission intensity among the three methods in the paper. With Dy3+ concentration increasing in Sr2P2O7:Dy3+ phosphors, the luminescence intensity first increases, reaches maximum, and then decreases. A similar trend was followed by Sr2P2O7:Ce3+ with Ce3+concentration increasing. A successful attempt was made to initiate the energy transfer mechanism from Ce3+ to Dy3+ in the host lattice and an overlap between the emission band of Ce3+ and the excitation band of Dy3+ indicated that the Ce3+ → Dy3+ energy transfer may indeed exist. It is clear that the photoluminescence intensity of Dy3+ as well as the quantum efficiency of the phosphor can be enhanced markedly by co‐doping Ce3+. Sr2P2O7:Dy3+,Ce3+ has its (CIE) chromaticity coordinates in the bluish‐white‐light region, near the standard illuminant D65. The CIE 1913 chromaticity coordinates of Sr2P2O7:Dy3+ phosphors fall in the white‐light region, and are adjacent to the ideal white‐light coordinates. In addition, the colour temperature and colour tone of Sr2P2O7:Dy3+ could be adjusted by changing the relative concentration of Dy3+. In short, Sr2P2O7:Dy3+ can be a promising single‐phased white‐light emitting phosphor for near‐UV (NUV) w‐LEDs.
Enhanced green emissions of Er3+/Yb3+ co‐doped Gd2(MoO4)3 by co‐excited up‐conversion processes
Authors: Hao Haoyue , Lu Hongyu , Ao Guanghong , Song Yinglin , Wang Yuxiao , Zhang Xueru 
Published: July 2017

AbstractImproving the emission from rare earth ions doped materials is of great importance to broaden their application in bio‐imaging, photovoltaics and temperature sensing. The green emissions of Gd2(MoO4)3:Er3+/Yb3+ powder upon co‐excitation with 980 and 808 nm lasers were investigated in this paper. Distinct enhancement of green emissions was observed compared with single laser excitation. Based on the energy level structure of Er3+, the enhancement mechanism was discussed. Moreover, the result of temperature‐dependent enhancement revealed that the enhancement factor reached its maximum (2.5) as the sample heated to 120°C, which is due to the competition of two major thermal effects acting in the co‐excited up‐conversion processes. In addition, the same enhancement of green emissions was also observed in Gd2(MoO4)3:Er3+ powder and NaYF4:Er3+/Yb3+ powder.
An LC–MS/MS method for quantitation of cyanidin‐3‐O‐glucoside in rat plasma: Application to a comparative pharmacokinetic study in normal and streptozotocin‐induced diabetic rats
Authors: Yang Chunxia , Wang Qiuhua , Yang Shenbao , Yang Qiong , Wei Ying 
Published: July 2017

AbstractA sensitive and reliable liquid chromatography tandem mass spectrometry (LC–MS/MS) method was developed to determine cyanidin‐3‐O‐glucoside (Cy‐3G) in normal and streptozotocin‐induced diabetic rat plasma. Chromatographic separation was carried out on a Zorbax SB‐C18 (50 × 4.6 mm, 5 μm) column and mass spectrometric analysis was performed using a Thermo Finnigan TSQ Quantum Ultra triple‐quadrupole mass spectrometer coupled with an ESI source in the negative ion mode. Selected reaction monitoring mode was applied for quantification using target fragment ions m/z 447.3 → 285.2 for Cy‐3G and m/z 463.0 → 300.1 for quercetin‐3‐O‐glucoside (internal standard). The calibration curve was linear over the range 3.00–2700 ng/mL (r2 ≥ 0.99) with the lower limit of quantitation at 3.00 ng/mL. Intra‐ and inter‐day precision was <14.5% and mean accuracy was from −11.5 to 13.6%. Stability testing showed that Cy‐3G remained stable during the whole analytical procedure. After validation, the assay was successfully used to support a preclinical pharmacokinetic comparison of Cy‐3G between normal and diabetic rats. Results indicated that diabetes mellitus significantly altered the in vivo pharmacokinetic characteristics of Cy‐3G after oral administration in rats.
New Fluorescent Nanoparticles for Ultrasensitive Detection of Nucleic Acids by Optical Methods
Authors: Westergaard Mulberg Mads , Taskova Maria , Thomsen Rasmus P. , Okholm Anders H. , Kjems Jørgen , Astakhova Kira 
Published: July 2017

AbstractFor decades the detection of nucleic acids and their interactions at low abundances has been a challenging task that has thus far been solved by enzymatic target amplification. In this work we aimed at developing efficient tools for amplification‐free nucleic acid detection, which resulted in the synthesis of new fluorescent nanoparticles. Here, the fluorescent nanoparticles were made by simple and inexpensive radical emulsion polymerization of butyl acrylate in the presence of fluorescent dyes and additional functionalization reagents. This provided ultra‐bright macrofluorophores of 9–84 nm mean diameter, modified with additional alkyne and amino groups for bioconjugation. By using click and NHS chemistries, the new nanoparticles were attached to target‐specific DNA probes that were used in fluorimetry and fluorescence microscopy. Overall, these fluorescent nanoparticles and their oligonucleotide derivatives have higher photostability, brighter fluorescence and hence dramatically lower limits of target detection than the individual organic dyes. These properties make them useful in approaches directed towards ultrasensitive detection of nucleic acids, in particular for imaging and in vitro diagnostics of DNA.
Asymmetrical Microchannel Emulsification Plates for Production of Small‐Sized Monodispersed Emulsion Droplets
Authors: Khalid Nauman , Kobayashi Isao , Uemura Kunihiko , Nakajima Mitsutoshi 
Published: July 2017

AbstractMonodispersed emulsion droplets have promising advantages in food, pharmaceutical, and chemical industries. Previous microchannel emulsification (MCE) plates having the capacity of generating small‐sized droplets exhibited very low droplet productivity since these plates operate at a low dispersed‐phase flow rate and with a relatively small number of microchannels. An innovative MCE plate with 176 176 circular asymmetric through‐holes was manufactured, which is comprised of a series of discrete outlets on each microchannel line with an effective cross‐sectional area of 1 cm2. The newly fabricated MCE plate is capable to produce monodispersed emulsion droplets with small Sauter mean diameters.