bluuebunny/crossref_metadata_2025_split huggingface dataset:
High‐Performance Organic Solar Cells Based on a Non‐Fullerene Acceptor with a Spiro Core
Authors: Sun Hua , Sun Po , Zhang Cong , Yang Yingguo , Gao Xingyu , Chen Fei , Xu Zongxiang , Chen Zhi‐Kuan , Huang Wei 
Published: January 2017

AbstractDerived from perylenediimide (PDI) building blocks, 3D PDI molecules are considered as a type of promising structure to overcome molecular aggregation, thus improving the performance of organic solar cells. Herein, we report a novel PDI‐based derivative, SCPDT‐PDI4, with four PDI units connected to a unique spiro core. Attributed to this novel molecular design, SCPDT‐PDI4 exhibits a rigid 3D structure, in which the aggregation tendency of PDI chromophores could be effectively attenuated. Additionally, strong intramolecular charge transfer and high charge mobility are achieved due to the well‐conjugated structure and electron‐rich property of SCPDT. Therefore, fullerene‐free organic solar cells based on SCPDT‐PDI4 and PTB7‐Th achieve a remarkable high efficiency of 7.11 %. Such an excellent result demonstrates the opportunity of SCPDT to be a promising building block for non‐fullerene acceptors.
Sustainable design of biorefinery processes: existing practices and new methodology
Authors: Julio Remi , Albet Joël , Vialle Claire , Vaca‐Garcia Carlos , Sablayrolles Caroline 
Published: January 2017

AbstractNowadays, eco‐designing products is increasingly practiced. The next challenge for sustainability is to optimize production processes. Biorefineries are particularly concerned with this improvement, because they use renewable resources. To identify the contribution of transformation processes to the overall environmental impacts, Life Cycle Assessment (LCA) appears as the adequate method. A literature review highlights that LCA is mainly performed on biorefineries to compare biomass feedstocks between them and to a fossil reference. Another part of environmental LCA compares the impacts of different processing routes. Nevertheless, these evaluations concern already designed processes. Generally, processes are considered as a unique operation in assessments. However, some criteria like operating can notably modify environmental burdens. The eco‐design of biorefinery processes can be guided by coupling process simulation to LCA. This method has been emerging in the chemical sector in recent years. Consequently, this paper proposes a new methodological approach to assessing the complete sustainability of biorefinery processes, since its first design stages. In addition to coupling process simulation and environmental LCA, the other pillars of sustainability will be assessed. Indeed, Life Cycle Costing and Social Life Cycle Assessment can be performed to obtain an integrated methodological framework. The simultaneous optimization of the environmental, economic, and social performances of the process can lead to antagonist ways of improving. Consequently, compromises should be realized. Thereby, the multi‐objective optimization can be accomplished by a metaheuristic method supported by a decision‐making tool. Finally, the main limits of this method and some perspectives and ways for improving are discussed. © 2017 Society of Chemical Industry and John Wiley & Sons, Ltd
Measurement analysis of two radials with a common‐origin point and its application
Authors: Liu Zhenyao , Yang Jidong , Zhu Weiwei , Zhou Shang , Tan Xuanping 
Published: January 2017

AbstractIn spectral analysis, a chemical component is usually identified by its characteristic spectra, especially the peaks. If two components have overlapping spectral peaks, they are generally considered to be indiscriminate in current analytical chemistry textbooks and related literature. However, if the intensities of the overlapping major spectral peaks are additive, and have different rates of change with respect to variations in the concentration of the individual components, a simple method, named the ‘common‐origin ray’, for the simultaneous determination of two components can be established. Several case studies highlighting its applications are presented.
Peptide Paratope Mimics of the Broadly Neutralizing HIV‐1 Antibody b12
Authors: Haußner Christina , Damm Dominik , Nirschl Sandra , Rohrhofer Anette , Schmidt Barbara , Eichler Jutta 
Published: January 2017

AbstractThe broadly neutralizing HIV‐1 antibody b12 recognizes the CD4 binding site of the HIV‐1 envelope glycoprotein gp120 and efficiently neutralizes HIV‐1 infections in vitro and in vivo. Based on the 3D structure of a b12⋅gp120 complex, we have designed an assembled peptide (b12‐M) that presents the parts of the three heavy‐chain complementarity‐determining regions (CDRs) of b12, which contain the contact sites of the antibody for gp120. This b12‐mimetic peptide, as well as a truncated peptide presenting only two of the three heavy‐chain CDRs of b12, were shown to recognize gp120 in a similar manner to b12, as well as to inhibit HIV‐1 infection, demonstrating functional mimicry of b12 by the paratope mimetic peptides.
Slowly progressive invasive rhino‐orbito‐cerebral aspergillosis: case report and literature review
Authors: de Martin Truzzi Giselle , Furlan Pauna Henrique , Moreira Hazboun Igor , Benedick Coimbra Igor , Sakuma Emerson Taro Inoue , Barreto Icléia Siqueira , Chone Carlos Takahiro , Sakano Eulalia 
Published: January 2017

Key Clinical MessageThis is a report of a patient with aspergillosis infection, which was thought to be a tumoral lesion during its investigation. This is not a common disease in Western countries, and this report should increase our awareness for differential diagnosis of nasal masses. Early diagnosis is desired in order to increase the survival rates.
Ring‐Opening Reaction of Furfural and Tetrahydrofurfuryl Alcohol on Hydrogen‐Predosed Iridium(1 1 1) and Cobalt/Iridium(1 1 1) Surfaces
Authors: Wan Weiming , Jenness Glen R. , Xiong Ke , Vlachos Dionisios G. , Chen Jingguang G. 
Published: January 2017

AbstractThe ring‐opening of furfural is crucial for its conversion into value‐added chemicals such as 1,5‐pentanediol (1,5‐PeD), an important polymer precursor. Ir‐based catalysts have shown activity in ring‐opening reactions, and the use of an oxophilic metal additive is reported to be beneficial. To better understand the effect of an oxophilic metal on Ir for the opening of the furan ring, a combination of DFT calculations and experimental surface science studies were performed to investigate the ring‐opening of furfural and tetrahydrofurfuryl alcohol. The experimental results suggest that Co/Ir(1 1 1) has a higher ring‐opening activity for an unsaturated furan ring, however, the difference in activities between Ir and Co/Ir(1 1 1) is insignificant for a saturated furan ring. The DFT results reveal that Co/Ir(1 1 1) has a stronger interaction with an unsaturated furan ring than Ir(1 1 1); both surfaces show a weaker interaction with the saturated furan ring, which causes the lower ring‐opening activity than that of furfural.
Reactive Template Synthesis of Inorganic/Organic VO2@Polyaniline Coaxial Nanobelts for High‐Performance Supercapacitors
Authors: Nie Guangdi , Lu Xiaofeng , Zhu Yun , Chi Maoqiang , Gao Mu , Chen Sihui , Wang Ce 
Published: January 2017

AbstractConducting polyaniline (PANi) is deposited in situ as a homogeneous shell on the monocrystalline VO2 nanobelts by using a simple and facile reactive template strategy without the assistance of any surfactant for supercapacitor electrodes. The as‐prepared VO2@PANi coaxial heterostructures show larger specific capacitance, better rate capability than the bare VO2 nanobelts, and higher cycling stability than the HCl‐doped PANi nanofibers in neutral electrolyte, owing to the synergetic contributions of the unique configuration and composition. These intriguing results can be extended to the synthesis of core/yolk‐shell or hollow inorganic/organic functional nanostructures with various shapes by tuning the pH or reaction time, which have potential applications in energy storage, optoelectronic devices, environmental governance, and catalysis.
Fluoroacetamide Moieties as NMR Spectroscopy Probes for the Molecular Recognition of GlcNAc‐Containing Sugars: Modulation of the CH–π Stacking Interactions by Different Fluorination Patterns
Authors: Unione Luca , Alcalá Maria , Echeverria Begoña , Serna Sonia , Ardá Ana , Franconetti Antonio , Cañada F. Javier , Diercks Tammo , Reichardt Niels , Jiménez‐Barbero Jesús 
Published: January 2017

AbstractWe herein propose the use of fluoroacetamide and difluoroacetamide moieties as sensitive tags for the detection of sugar–protein interactions by simple 1H and/or 19F NMR spectroscopy methods. In this process, we have chosen the binding of N,N′‐diacetyl chitobiose, a ubiquitous disaccharide fragment in glycoproteins, by wheat‐germ agglutinin (WGA), a model lectin. By using saturation‐transfer difference (STD)‐NMR spectroscopy, we experimentally demonstrate that, under solution conditions, the molecule that contained the CHF2CONH‐ moiety is the stronger aromatic binder, followed by the analogue with the CH2FCONH‐ group and the natural molecule (with the CH3CONH‐ fragment). In contrast, the molecule with the CF3CONH‐ isoster displayed the weakest intermolecular interaction (one order of magnitude weaker). Because sugar–aromatic CH–π interactions are at the origin of these observations, these results further contribute to the characterization and exploration of these forces and offer an opportunity to use them to unravel complex recognition processes.
Fine‐Tuning the Properties of Doped Multifunctional Materials by Controlled Reduction of Dopants
Authors: Barroux Hugo , Jiang Tengfei , Paul Camille , Massuyeau Florian , Génois Romain , Gordon Elijah E. , Whangbo Myung‐Hwan , Jobic Stéphane , Gautier Romain 
Published: January 2017

AbstractThe physical properties of doped multifunctional compounds are commonly tuned by controlling the amount of dopants, but this control is limited because all the properties are influenced simultaneously by this single parameter. Here, we present a strategy that enables the fine‐tuning of a specific combination of properties by controlling the reduction of dopants. The feasibility of this approach was demonstrated by optimizing the near‐IR photoluminescence of strontium titanate SrTiO3:Ni for potential applications in biomedicine for a range of absorbance in the visible/near‐IR region. We discussed how material properties, such as luminescence, conductivity, or photocatalytic properties can be designed by carefully controlling the ratio of dopants in different oxidation states.
Dibenzobarrelene‐Based Azaacenes: Emitters in Organic Light‐Emitting Diodes
Authors: Ganschow Michael , Koser Silke , Hahn Sebastian , Rominger Frank , Freudenberg Jan , Bunz Uwe H. F. 
Published: January 2017

AbstractThe synthesis of soluble dibenzobarrelene‐substituted azaacenes either by condensation reactions in solution or, more effectively, in the solid state by using a ball mill is reported herein. We relate their optical properties in thin films to their packing in the solid state. The targets are characterized by cyclic voltammetry, X‐ray crystallography and UV/Vis and fluorescence analysis. Three highly fluorescent, amorphous azaacenes were processed into organic light‐emitting diodes, and their improved performance (luminance, efficiency and efficacy) was compared with that of structurally related iptycene‐based azaacenes.
Hydroaminoalkylation of Allylsilanes and a One‐Pot Procedure for the Synthesis of 1,5‐Benzoazasilepines
Authors: Lühning Lars H. , Strehl Julia , Schmidtmann Marc , Doye Sven 
Published: January 2017

AbstractAllylsilanes undergo highly regioselective intermolecular alkene hydroaminoalkylation with secondary amines in the presence of a titanium mono(formamidinate) catalyst. Corresponding reactions of a suitable allyl(2‐bromophenyl)silane which exclusively deliver the branched hydroaminoalkylation products combined with a subsequent Buchwald–Hartwig amination result in the development of an elegant one‐pot procedure for the synthesis of literature‐unknown silicon analogues of 1,5‐benzodiazepines, the so‐called 1,5‐benzoazasilepines.
Effects of Chlorination on the Tautomeric Equilibrium of 2‐Hydroxypyridine: Experiment and Theory
Authors: Calabrese Camilla , Maris Assimo , Uriarte Iciar , Cocinero Emilio J. , Melandri Sonia 
Published: January 2017

AbstractInvited for the cover of this issue are the groups of Emilio J. Cocinero and Sonia Melandri at the University of País Vasco and the University of Bologna. The image depicts different possibilities that this tautomeric equilibrium can take according to the different positions of the chlorine atom, which, in many cases, are difficult to predict a priori. Read the full text of the article at 10.1002/chem.201604891.
Inhibitor Selectivity for Cyclin‐Dependent Kinase 7: A Structural, Thermodynamic, and Modelling Study
Authors: Hazel Pascale , Kroll Sebastian H. B. , Bondke Alexander , Barbazanges Marion , Patel Hetal , Fuchter Matthew J. , Coombes R Charles , Ali Simak , Barrett Anthony G. M. , Freemont Paul S. 
Published: January 2017

AbstractDeregulation of the cell cycle by mechanisms that lead to elevated activities of cyclin‐dependent kinases (CDK) is a feature of many human diseases, cancer in particular. We identified small‐molecule inhibitors that selectively inhibit CDK7, the kinase that phosphorylates cell‐cycle CDKs to promote their activities. To investigate the selectivity of these inhibitors we used a combination of structural, biophysical, and modelling approaches. We determined the crystal structures of the CDK7‐selective compounds ICEC0942 and ICEC0943 bound to CDK2, and used these to build models of inhibitor binding to CDK7. Molecular dynamics (MD) simulations of inhibitors bound to CDK2 and CDK7 generated possible models of inhibitor binding. To experimentally validate these models, we gathered isothermal titration calorimetry (ITC) binding data for recombinant wild‐type and binding site mutants of CDK7 and CDK2. We identified specific residues of CDK7, notably Asp155, that are involved in determining inhibitor selectivity. Our MD simulations also show that the flexibility of the G‐rich and activation loops of CDK7 is likely an important determinant of inhibitor specificity similar to CDK2.
Scalable SDN architecture with distributed placement of controllers for WAN
Authors: Zhao Zhipeng , Wu Bin 
Published: January 2017

SummaryBy separating control plane from data plane, software‐defined network (SDN) adopts centralized controllers to manage data flows in the network. Nevertheless, the rapid growth of network service traffic requires a large number of controllers, reducing network performance due to the scalability constraint. Therefore, we consider distributed placement of controllers in wide‐area network to construct a scalable SDN architecture, by taking service traffics, traffic propagation delay, and load balancing into account. Specifically, we first partition the network into several small sections (named SDN domains) and then place the least amount of controllers to a proper node in each domain. The architecture provides a control channel to deliver requested messages for each SDN domain, so it reduces the link delay (which is assumed to be proportional to the physical length of the link) between switches and SDN controllers. Unfortunately, it also introduces extra latency among controller sets at different SDN domain. Accordingly, we formulate an integer linear program to optimize network cost and performance by considering all those conflicting factors and propose an efficient heuristic algorithm called distributed SDN placement to solve the problem. Simulation results confirm that our proposed heuristic distributed SDN placement can achieve suboptimal solutions as compared with the integer linear program results.
Interplay among Electrostatic, Dispersion, and Steric Interactions: Spectroscopy and Quantum Chemical Calculations of π‐Hydrogen Bonded Complexes
Authors: Kumar Sumit , Singh Santosh K. , Vaishnav Jamuna K. , Hill J. Grant , Das Aloke 
Published: January 2017

Abstractπ‐Hydrogen bonding interactions are ubiquitous in both materials and biology. Despite their relatively weak nature, great progress has been made in their investigation by experimental and theoretical methods, but this becomes significantly more complicated when secondary intermolecular interactions are present. In this study, the effect of successive methyl substitution on the supramolecular structure and interaction energy of indole⋅⋅⋅methylated benzene (ind⋅⋅⋅n‐mb, n=1–6) complexes is probed through a combination of supersonic jet experiments and benchmark‐quality quantum chemical calculations. It is demonstrated that additional secondary interactions introduce a subtle interplay among electrostatic and dispersion forces, as well as steric repulsion, which fine‐tunes the overall structural motif. Resonant two‐photon ionization and IR–UV double‐resonance spectroscopy techniques are used to probe jet‐cooled ind⋅⋅⋅n‐mb (n=2, 3, 6) complexes, with redshifting of the N−H IR stretching frequency showing that increasing the degree of methyl substitution increases the strength of the primary N−H⋅⋅⋅π interaction. Ab initio harmonic frequency and binding energy calculations confirm this trend for all six complexes. Electronic spectra of the three dimers are broad and structureless, with quantum chemical calculations revealing that this is likely to be due to multiple tilted conformations of each dimer possessing similar stabilization energies.
A proposed model of psychodynamic psychotherapy linked to Erik Erikson's eight stages of psychosocial development
Authors: Knight Zelda Gillian 
Published: January 2017

Just as Freud used stages of psychosexual development to ground his model of psychoanalysis, it is possible to do the same with Erik Erikson's stages of development with regards to a model of psychodynamic psychotherapy. This paper proposes an eight‐stage model of psychodynamic psychotherapy linked to Erik Erikson's eight stages of psychosocial development. Various suggestions are offered. One such suggestion is that as each of Erikson's developmental stages is triggered by a crisis, in therapy it is triggered by the client's search. The resolution of the search often leads to the development of another search, which implies that the therapy process comprises a series of searches. This idea of a series of searches and resolutions leads to the understanding that identity is developmental and therapy is a space in which a new sense of identity may emerge. The notion of hope is linked to Erikson's stage of Basic Trust and the proposed model of therapy views hope and trust as essential for the therapy process. Two clinical vignettes are offered to illustrate these ideas.Key Practitioner Message

Psychotherapy can be approached as an eight‐stage process and linked to Erikson's eight stages model of development.
Psychotherapy may be viewed as a series of searches and thus as a developmental stage resolution process, which leads to the understanding that identity is ongoing throughout the life span.
High Redox Capacity of Al‐Doped La1−xSrxMnO3−δ Perovskites for Splitting CO2 and H2O at Mn‐Enriched Surfaces
Authors: Ezbiri M. , Becattini V. , Hoes M. , Michalsky R. , Steinfeld A. 
Published: January 2017

AbstractPerovskites are attractive candidates for the solar‐driven thermochemical redox splitting of CO2 and H2O into CO and H2 (syngas) and O2. This work investigates the surface activity of La1−xSrxMn1−yAlyO3−δ (0≤x≤1, 0≤y≤1) and La0.6Ca0.4Mn0.6Al0.4O3−δ. At 1623 K and 15 mbar O2, the oxygen non‐stoichiometry of La0.2Sr0.8Mn0.8Al0.2O3−δ increases with the strontium content and reaches a maximum of δ=0.351. X‐ray photoelectron spectroscopy analysis indicates that manganese is the only redox‐active metal at the surface. All La1−xSrxMn1−yAlyO3−δ compositions exhibit surfaces enriched in manganese and depleted in strontium. We discuss how these compositional differences of the surface from the bulk lead to the beneficially higher reduction extents and lower strontium carbonate concentrations at the aluminum‐doped surfaces. Using first principles calculations, we validate the experimental reduction trends and elucidate the mechanism of the partial electronic charge redistribution upon perovskite reduction.
Lignin‐Derived Thioacidolysis Dimers: Reevaluation, New Products, Authentication, and Quantification
Authors: Yue Fengxia , Lu Fachuang , Regner Matt , Sun Runcang , Ralph John 
Published: January 2017

AbstractLignin structural studies play an essential role both in understanding the development of plant cell walls and for valorizing lignocellulosics as renewable biomaterials. Dimeric products released by selectively cleaving β–aryl ether linkages between lignin units reflect the distribution of recalcitrant lignin units, but have been neither absolutely defined nor quantitatively determined. Here, 12 guaiacyl‐type thioacidolysis dimers were identified and quantified using newly synthesized standards. One product previously attributed to deriving from β–1‐coupled units was established as resulting from β–5 units, correcting an analytical quandary. Another longstanding dilemma, that no β–β dimers were recognized in thioacidolysis products from gymnosperms, was resolved with the discovery of two such authenticated compounds. Individual GC response factors for each standard compound allowed rigorous quantification of dimeric products released from softwood lignins, affording insight into the various interunit‐linkage distributions in lignins and thereby guiding the valorization of lignocellulosics.
VIM‐1 carbapenemase‐producing Escherichia coli in gulls from southern France
Authors: Vittecoq Marion , Laurens Chrislène , Brazier Lionel , Durand Patrick , Elguero Eric , Arnal Audrey , Thomas Frédéric , Aberkane Salim , Renaud Nicolas , Prugnolle Franck , Solassol Jérôme , Jean‐Pierre Hélène , Godreuil Sylvain , Renaud François 
Published: January 2017

AbstractAcquired carbapenemases currently pose one of the most worrying public health threats related to antimicrobial resistance. A NDM‐1‐producing Salmonella Corvallis was reported in 2013 in a wild raptor. Further research was needed to understand the role of wild birds in the transmission of bacteria resistant to carbapenems. Our aim was to investigate the presence of carbapenem‐resistant Escherichia coli in gulls from southern France. In 2012, we collected 158 cloacal swabs samples from two gull species: yellow‐legged gulls (Larus michahellis) that live in close contact with humans and slender‐billed gulls (Chroicocephalus genei) that feed at sea. We molecularly compared the carbapenem‐resistant bacteria we isolated through culture on selective media with the carbapenem‐susceptible strains sampled from both gull species and from stool samples of humans hospitalized in the study area. The genes coding for carbapenemases were tested by multiplex PCR. We isolated 22 carbapenem‐resistant E. coli strains from yellow‐legged gulls while none were isolated from slender‐billed gulls. All carbapenem‐resistant isolates were positive for blaVIM‐1 gene. VIM‐1‐producing E. coli were closely related to carbapenem‐susceptible strains isolated from the two gull species but also to human strains. Our results are alarming enough to make it urgently necessary to determine the contamination source of the bacteria we identified. More generally, our work highlights the need to develop more bridges between studies focusing on wildlife and humans in order to improve our knowledge of resistant bacteria transmission routes.