bluuebunny/crossref_metadata_2025_split huggingface dataset:
Regiospecific ortho‐C−H Allylation of Benzoic Acids
Authors: Trita A. Stefania , Biafora Agostino , Pichette Drapeau Martin , Weber Philip , Gooßen Lukas J. 
Published: February 2018

AbstractA carboxylate‐directed ortho‐C−H functionalization has been developed and it allows the regiospecific introduction of allyl residues to benzoic acids. In the presence of a [Ru(p‐cymene)Cl2]2 and K3PO4, benzoic acids react with allyl acetates at only 50 °C to give the corresponding ortho‐allylbenzoic acids. The protocol is generally applicable to both electron‐rich and electron‐poor benzoic acids in combination with linear and branched allyl acetates. The products can be further functionalized in situ, for example, by double‐bond migration, lactonization, or decarboxylation.
Achieving Simultaneous CO2 and H2S Conversion via a Coupled Solar‐Driven Electrochemical Approach on Non‐Precious‐Metal Catalysts
Authors: Ma Weiguang , Wang Hong , Yu Wei , Wang Xiaomei , Xu Zhiqiang , Zong Xu , Li Can 
Published: February 2018

AbstractCarbon dioxide (CO2) and hydrogen sulfide (H2S) are generally concomitant with methane (CH4) in natural gas and traditionally deemed useless or even harmful. Developing strategies that can simultaneously convert both CO2 and H2S into value‐added products is attractive; however it has not received enough attention. A solar‐driven electrochemical process is demonstrated using graphene‐encapsulated zinc oxide catalyst for CO2 reduction and graphene catalyst for H2S oxidation mediated by EDTA‐Fe2+/EDTA‐Fe3+ redox couples. The as‐prepared solar‐driven electrochemical system can realize the simultaneous conversion of CO2 and H2S into carbon monoxide and elemental sulfur at near neutral conditions with high stability and selectivity. This conceptually provides an alternative avenue for the purification of natural gas with added economic and environmental benefits.
Reversible Clustering of Gold Nanoparticles under Confinement
Authors: Sánchez‐Iglesias Ana , Claes Nathalie , Solís Diego M. , Taboada Jose M. , Bals Sara , Liz‐Marzán Luis M. , Grzelczak Marek 
Published: February 2018

AbstractA limiting factor of solvent‐induced nanoparticle self‐assembly is the need for constant sample dilution in assembly/disassembly cycles. Changes in the nanoparticle concentration alter the kinetics of the subsequent assembly process, limiting optical signal recovery. Herein, we show that upon confining hydrophobic nanoparticles in permeable silica nanocapsules, the number of nanoparticles participating in cyclic aggregation remains constant despite bulk changes in solution, leading to highly reproducible plasmon band shifts at different solvent compositions.
Synthesis of a hypercrosslinked, ionic, mesoporous polymer monolith and its application in deep oxidative desulfurization
Authors: Jiang Bin , Sun Zhaoning , Zhang Luhong , Sun Yongli , Zhang Hongjie , Yang Huawei 
Published: February 2018

ABSTRACTIn this study, we used a facile and scalable strategy to produce a hypercrosslinked, ionic, mesoporous polymer monolith (HCIMPM). On the basis of structure‐directing polymeric crosslinking, the interconnected nanonetwork was formed through the in situ crosslinking of the homopolymer poly(vinyl imidazole) via a quaternization reaction, and its textural properties could be effectively adjusted by the block copolymer poly(ethylene oxide)‐block‐poly(propylene oxide)‐block‐poly(ethylene oxide)(PEO20PPO70PEO20). The maximum specific surface area and pore volume were 212 m2/g and 1.08 cm3/g, respectively. Furthermore, the synthetic framework could be functionalized via the loading of PW12
through ion exchange. The obtained HCIMPM with PW12O403− (PW‐HCIMPM) was applied in the oxidative desulfurization, and approximately 100% sulfur removal could be achieved in the model oil with hydrogen peroxide (30 wt %) as an oxidant. Moreover, the solid catalyst could be recovered readily and recycled at least six times without a significant decrease in the desulfurization efficiency. As for real diesel, we also observed that almost all of the original sulfur compounds could be converted in 120 min. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 46280.
Tuning the properties of segmented polyurea by regulating soft‐segment length
Authors: Iqbal Nahid , Tripathi Manorama , Parthasarathy Surekha , Kumar Devendra , Roy Prasun Kumar 
Published: February 2018

ABSTRACTPolyurea is being widely advocated as a “retrofit” coating on structures, which mandate protection against blast. The physical properties of polyurea can be tuned by judicious choice of reactants, and the processing methodology employed for its preparation. The purpose of this study is to establish the dependence of material properties on the soft segment length in polyurea. Polyurea formulations were prepared by reaction of commercially available isocyanate prepolymer with poly(propylene oxide) based amines of varying molecular weights (230–2000 g/mol). The effect of increasing the soft segment length on the mechanical properties of polyurea under both quasi‐static as well as dynamic conditions was determined. Ductility was found to increase proportionally with increasing soft segment length, with a concomitant decrease in the tensile strength. All the compositions exhibited sub‐ambient glass transition temperature, which was found to reduce with increasing soft‐segment length. Time–temperature superposition principle was used to arrive at master curves for all compositions. The frequency essential to initiate the process of dynamic “rubber to glass” transition was found to be directly proportional to the soft segment length. All the formulations were found to be capable of exhibiting an elastomeric response even under high frequencies typical of blast loadings. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 46284.
Effect of dispersed phase on the morphology of in situ microfibrils and the viscoelastic properties of its composite via direct extrusion
Authors: Li Xiaogang , Xin Chunling , Huang Ying , Kang Kai , He Yadong 
Published: February 2018

ABSTRACTA triangle arrayed triple‐screw extruder was used to prepare in situ polypropylene (PP) microfibrillar composites (MFCs) by direct extrusion, in which polyamide 6,6 (PA66) and poly(butylene terephthalate) (PBT) were used as dispersed phases while PP as matrix phase. The morphological evolution of the dispersed phase were investigated by SEM through taking samples along the extruder from different positions. The results showed that the fibrillating mechanism of PA66 was entirely different from that of PBT. Dynamic oscillatory shear rheological properties were used to analyze the effect of different types of in situ microfibrils on the rheological properties of MFCs. The obtained results showed that the storage modulus and complex viscosity of both PP/PA66 and PP/PBT MFCs were improved with increasing fibrillar aspect ratios. The loss tangent tan δ at low frequencies decreased with the increase of fibrillar aspect ratio. Moreover, the gel point concentration of PP/PA66 composite was lower than that of PP/PBT composite. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 46286.
Solid state 13C‐NMR study of a plasticized PLA/PHB polymer blend
Authors: Baran Anton , Vrábel Peter , Olčák Dušan , Chodák Ivan 
Published: February 2018

ABSTRACTHigh‐resolution solid‐state 13C nuclear magnetic resonance spectra and 13C spin–lattice relaxation times T1(13C) are used to characterize the structure of a polymer blend prepared from poly(lactic acid) (85 wt %) and poly(3‐hydroxybutyrate) (15 wt %) and the effect of the plasticizer triacetine on the structure and molecular dynamics of the blend. Single‐pulse and cross‐polarization magic angle spinning 13C nuclear magnetic resonance spectra indicate that the nonplasticized polymer blend consists of semicrystalline poly(3‐hydroxybutyrate) domains built into an amorphous poly(lactic acid) matrix. Triacetine supports formation of the crystalline regions within both polymer components in the blend. Spin–lattice relaxation times of carbonyl carbons indicate that the nonplasticized polymer blend consists of noninteracting chains of blended polymers and plasticization of the polymer blend increases the relaxation rate. The glass transition, cold crystallization, and melting processes of the nonplasticized and plasticized blends were also studied using differential scanning calorimetry methods. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 46296.
Muscle sympathetic nerve activity‐coupled changes in brain activity during sustained muscle pain
Authors: Kobuch Sophie , Fazalbhoy Azharuddin , Brown Rachael , Macefield Vaughan G. , Henderson Luke A. 
Published: February 2018

AbstractIntroductionLong‐lasting experimental muscle pain elicits divergent muscle sympathetic responses, with some individuals exhibiting a persistent increase in muscle sympathetic nerve activity (MSNA), and others a decrease. These divergent responses are thought to result from sustained functional changes in specific brain regions that modulate the cardiovascular responses to pain.AimThe aim of this study was to investigate brain regions that are functionally coupled to the generation of an MSNA burst at rest and to determine their behavior during tonic muscle pain.MethodsFunctional magnetic resonance imaging of the brain was performed concurrently with microelectrode recording of MSNA from the common peroneal nerve during a 40 min infusion of hypertonic saline into the ipsilateral tibialis anterior muscle of 37 healthy human subjects.ResultsAt rest, blood oxygen level‐dependent signal intensity coupled to bursts of MSNA increased in the rostral ventrolateral medulla, insula, dorsolateral prefrontal cortex, posterior cingulate cortex, and precuneus and decreased in the region of the midbrain periaqueductal gray. During pain, MSNA‐coupled signal intensity was greater in the region of the nucleus tractus solitarius, midbrain periaqueductal gray, dorsolateral prefrontal, medial prefrontal, and anterior cingulate cortices, than at rest. Conversely, MSNA‐coupled signal intensity decreased during pain in parts of the prefrontal cortex.ConclusionsThese results suggest that multiple brain regions are recruited in a burst‐to‐burst manner, and the magnitude of these signal changes is correlated to the overall change in MSNA amplitude during tonic muscle pain.
The impact of cognitive remediation on cerebral activity in schizophrenia: Systematic review of the literature
Authors: Bon Laura , Franck Nicolas 
Published: February 2018

AbstractContextcognitive remediation involves either intensive training of impaired functions or implementing strategies to compensate for these impairments. In cases of schizophrenia, both methods have demonstrated benefits in terms of behavior and cerebral activity. However, despite the major differences between these two approaches, their impact has not yet been compared.MethodWe searched the PsychInfo, Pubmed, and ScienceDirect databases using the key words “cognitive remediation,” “schizophrenia,” “cerebral activity,” and “magnetic resonance imaging,” in order to select studies investigating the effects of cognitive remediation on patients with schizophrenia. The studies selected had to present their approach in detail and measure its impact in terms of both cerebral activity and cognitive function, both before and after therapy. We divided the studies into two groups, those using the strategy method and those using the training method.ResultsEight studies were included in the review, four for the strategy method (88 patients, 44 of whom underwent remediation) and 4 for the training method (87 patients, 43 of whom underwent remediation). The analysis of the results of this study indicates that the training method is capable of activating more the targeted brain areas than the strategy method. However, the latter appears to encourage more extensive activation of the cerebral networks.DiscussionThe studies used for this review vary widely in terms of the imaging methods and protocol. However, differences were found between the two methods and lead us to suggest that further studies, with proper bias control, should be conducted to systematically compare the two approaches.
Practices of Third Wave Coffee: A Burundian Producer's Perspective
Authors: Rosenberg Lauren , Swilling Mark , Vermeulen Walter J V 
Published: February 2018

AbstractThe relationship between coffee quality and sustainability is typically analysed using symbolic quality attributes, not material quality. This article provides a bottom‐up perspective of Burundi's current competitive advantage in the global coffee market: material quality. The research agenda was embedded within the operations of a Burundian coffee washing station and describes critical business practices for producing and selling high material quality coffee. We argue that these business practices represent quality governance mechanisms that are significantly different from the exogenous and fixed criteria of sustainability certifications and labels. Such quality governance mechanisms are an important trading trend to recognize and understand in a producing country such as Burundi that is unable to effectively compete in the certified coffee market because of the small size and irregularity of its supply. Copyright © 2018 John Wiley & Sons, Ltd and ERP Environment
Interdisciplinary flipped learning for engineering classrooms in higher education: Students’ motivational regulation and design achievement
Authors: Park Sanghoon , Kaplan Howard , Schlaf Rudy 
Published: February 2018

AbstractAn interdisciplinary approach can improve both functional and aesthetic design skills for undergraduate engineering students. In this paper, we designed and compared two flipped engineering classrooms, one involving only engineering students who worked on individual design tasks, and the other including groups of an engineering student and an art major student that performed design tasks collaboratively. Fifty‐one engineering students, 29 from the individual flipped classroom and 22 from the interdisciplinary flipped classroom participated in the study. During the semester, all students studied pre‐recorded video lectures and homework before the class and then participated in weekly engineering design activities either individually or in a group. Students’ motivational experiences and engineering design achievement were assessed at the end of the semester. The results showed that students’ preferences in employing motivational regulation between the two flipped classrooms were different. Also, the students participated in the interdisciplinary flipped classroom exhibited higher aesthetic design achievement.
Is shock impedance value alone to be considered a good predictor for shock efficacy in subcutaneous implantable cardioverter defibrillator?
Authors: Di Girolamo Enrico , Furia Nanda , Faustino Massimiliano , Appignani Marianna , Arcari Giampiero , Angelini Alessandro , Spadoni Loris 
Published: February 2018

Key Clinical MessageSubcutaneous implantable cardioverter defibrillator (S‐ICD) is easy to implant, with poor risks of the patient. However, fat is a poor current conductor and increases defibrillation threshold. As shock impedance alone should not be considered a good efficacy predictor of an S‐ICD system, an X‐ray latero‐lateral view for lead position should be achieved.
Color Changes of a Full‐Color Emissive ESIPT Fluorophore in Response to Recognition of Certain Acids and Their Conjugate Base Anions
Authors: Tsuchiya Saki , Sakai Ken‐ichi , Kawano Keiichi , Nakane Yuta , Kikuchi Takemitsu , Akutagawa Tomoyuki 
Published: February 2018

Abstract2‐(1,3‐Benzothiazol‐2‐yl)‐4‐methoxy‐6‐(1,4,5‐triphenyl‐1H‐imidazol‐2‐yl)phenol (BTImP) is an excited‐state intramolecular proton transfer (ESIPT) fluorophore, containing an acid‐stimuli‐responsive intramolecular hydrogen bond (H‐bond) that can switch from the central phenolic proton to the imidazole (Im) or benzothiazole (BT) nitrogen atoms. Here, we demonstrate that BTImP shows full‐color (red, green, blue, and white) emission upon the addition of different concentrations of HClO4 or, with time, after the addition of HBF4. It also shows thermally dependent color changes from pink through white to blue in a narrow temperature range of 25–60 °C. 1H and 15N NMR measurements suggest that, after the green fluorescent BTImP is protonated at its Im nitrogen atom, a conjugate base anion coordinates to the imidazolium (HIm+) proton, forming two types of complexes with different coordination states. One state shows a significantly Stokes‐shifted red emission resulting from ESIPT at the BT side, whereas the other shows a typical Stokes‐shifted blue emission, probably caused by interaction of the anion with the phenolic proton, which breaks the H‐bond on the BT side. BF4− and ClO4− are effective in forming such a blue emitter, whereas Cl− and PF6− are not; this behavior depends on whether the anion can fit into the bidentate binding site consisting of HIm+ and the phenolic hydroxy group.
Zinc‐Containing Radical Anions via Single Electron Transfer to Donor–Acceptor Adducts
Authors: Cao Levy L. , Bamford Karlee L. , Liu Liu Leo , Stephan Douglas W. 
Published: February 2018

AbstractReactions of [Cp*2Fe] with the Lewis acid [Zn(C6F5)2] in the presence of [(PhC(S)S)2], 9,10‐phenanthrenedione or 4,5‐pyrenedione yield the salt [Cp*2Fe][(PhC(S)S)Zn(C6F5)2] 1, [Cp*2Fe][((C14H8O2)Zn(C6F5)2)⋅] 4, and [Cp*2Fe][((C16H8O2)Zn(C6F5)2)⋅] 5, respectively. The latter two species represent the first examples of isolable zinc‐containing radical anions. While [(PhC(S)S)2] binds weakly to [Zn(C6F5)2], the diones afford the isolable adducts [(C14H8O2)Zn(C6F5)2] 2 and [(C16H8O2)Zn(C6F5)2] 3. Cyclic voltammetry and computational studies support the view that 4 and 5 are formed via single electron transfer (SET) to the donor–acceptor adducts, 2 and 3, respectively. Subsequent treatment of 4 and 5 with [NC5H4NMe2] affords [Zn(C6F5)2(NC5H4NMe2)2] with liberation of the dione, and regeneration of [Cp*2Fe].
Influence of Filtration on the Agglomeration Degree of Two Crystalline Amino Acids
Authors: Löbnitz Lisa , Böser Marius , Nirschl Hermann 
Published: February 2018

AbstractSeparating crystalline material from the mother liquor is often performed by filtration, whereas different options to generate the driving force are possible to use. However, the separation process can affect the structure of crystalline material, either by breakage events or agglomeration. In this work, a method of automated image analysis was used to evaluate the agglomeration degree of two crystalline amino acids after a pressure or vacuum filtration. The information resulting from this consideration enables to adjust the crystal structure depending on the individual filtration type.
Numerical Analysis of the Die Filling Process Within a Pharmaceutical Tableting Machine
Authors: Hildebrandt Claudia , Gopireddy Srikanth R. , Scherließ Regina , Urbanetz Nora 
Published: February 2018

AbstractOne of the main benefits of numerical simulations is the ability to shed light on the underlying physics in unit operations. This advantage was exploited in this work to study the die filling process in a lab‐scale pharmaceutical rotary tablet press. The die filling process with emphasis on mass holdup, mass flow rate, tablet mass, and API content in the dies is described in detail. Eventually a design of experiments provides a clear picture on the influence of process conditions and material properties on the tablet mass to improve the process understanding.
Use of the 22C3 anti–programmed death‐ligand 1 antibody to determine programmed death‐ligand 1 expression in cytology samples obtained from non–small cell lung cancer patients
Authors: Ilie Marius , Juco Jonathan , Huang Lingkang , Hofman Veronique , Khambata‐Ford Shirin , Hofman Paul 
Published: February 2018

BACKGROUNDPembrolizumab monotherapy is a standard‐of‐care treatment for the first‐ and second‐line treatment of advanced non–small cell lung cancer with programmed death‐ligand 1 (PD‐L1) tumor proportion score (TPS) values ≥ 50% and ≥ 1%, respectively. PD‐L1 testing with the PD‐L1 immunohistochemistry (IHC) 22C3 pharmDx companion assay has been validated on tumor tissue with the Dako Autostainer Link 48 (ASL48). 22C3 anti–PD‐L1 antibody–based laboratory‐developed tests (LDTs) compatible with other autostainers and cytology samples are essential to support pembrolizumab treatment decisions across institutions globally.METHODSASL48 and BenchMark Ultra LDTs were optimized for the evaluation of cytology samples through comparisons with cell lines with known PD‐L1 expression levels (strong, moderate, and negative). The PD‐L1 TPS was then evaluated for 70 paired biopsy and cytology samples (bronchial washes, n = 40; pleural effusions, n = 30) with these LDTs. Biopsy and cytology LDT TPS values were also compared with a subset of biopsy samples (n = 37) evaluated with the PD‐L1 IHC 22C3 pharmDx assay on the ASL48.RESULTSIntraclass correlation coefficients of 0.884 to 0.898 were observed for biopsy samples versus cytology samples with the ASL48 and BenchMark Ultra LDTs. Concordance was high, regardless of the TPS cut point (<1% vs ≥ 1% and <50% vs ≥ 50%), sample type (pleural effusion vs bronchial wash), or tumor histology (adenocarcinoma vs squamous cell carcinoma). Concordance was high for each LDT versus the PD‐L1 IHC 22C3 pharmDx assay.CONCLUSIONSASL48 and BenchMark Ultra 22C3 antibody concentrate–based LDTs have been validated for PD‐L1 testing in cytology samples, and they will support reliable, high‐quality PD‐L1 testing across regions globally. Cancer Cytopathol 2018;126:264‐74. © 2018 American Cancer Society.
5,5′,6,6′‐Tetranitro‐2,2′‐bibenzimidazole: A Thermally Stable and Insensitive Energetic Compound
Authors: Gutowski Łukasz , Trzciński Waldemar , Szala Mateusz 
Published: February 2018

AbstractA new energetic compound, namely a secondary explosive (5,5′,6,6′‐tetranitro‐2,2′‐bibenzimidazole, TNBBI) with high thermal stability is described. TNBBI is synthesized through direct nitration of 2,2′‐bibenzimidazole with nitric acid. TNBBI decomposes exothermically at 394 °C without visible melting. The heat of combustion and the standard enthalpy of formation are determined experimentally. The detonation parameters calculated for the new compound are slightly lower than those for TNT. However, the combination of TNBBI′s high decomposition temperature and low sensitivity make it a promising thermally stable energetic compound. The structure of the new compound is confirmed by NMR and IR spectroscopy.
Piezofluorochromism in Charge‐Transfer Inclusion Crystals: The Influence of High Pressure versus Mechanical Grinding
Authors: Ono Toshikazu , Tsukiyama Yoshifumi , Taema Ai , Sato Hiroyasu , Kiyooka Hidetoshi , Yamaguchi Yuma , Nagahashi Ayumi , Nishiyama Manami , Akahama Yuichi , Ozawa Yoshiki , Abe Masaaki , Hisaeda Yoshio 
Published: February 2018

AbstractThe distinct piezochromic luminescent responses of charge−transfer inclusion crystals, which consist of small aromatic guest molecules with naphthalenediimide derivatives, are reported. Reversible multichromism is observed over the entire visible region in response to high pressure, whereas a weak response to mechanical grinding is evident. High‐pressure single‐crystal X‐ray diffraction analysis and TD‐DFT calculations clearly suggest that high compression induces a closer arrangement with a short interfacial distance between small aromatic guest molecules and naphthalenediimide derivatives, which is proposed as the origin of the drastic luminescent color change.