bluuebunny/crossref_metadata_2025_split huggingface dataset:
Enantioselective Intramolecular Hydroacylation of Unactivated Alkenes: An NHC‐Catalyzed Robust and Versatile Formation of Cyclic Chiral Ketones
Authors: Janssen‐Müller Daniel , Schedler Michael , Fleige Mirco , Daniliuc Constantin G. , Glorius Frank 
Published: March 2015

AbstractA highly enantioselective intramolecular N‐heterocyclic carbene (NHC)‐catalyzed hydroacylation reaction gives access to a range of cyclic ketones from unactivated olefin‐substituted aldehydes (up to 99 % ee). Remarkably, aliphatic aldehydes were also transformed efficiently in an NHC‐catalyzed hydroacylation reaction for the first time.
Bioorthogonal Deprotection on the Dendritic Cell Surface for Chemical Control of Antigen Cross‐Presentation
Authors: Pawlak Joanna B. , Gential Geoffroy P. P. , Ruckwardt Tracy J. , Bremmers Jessica S. , Meeuwenoord Nico J. , Ossendorp Ferry A. , Overkleeft Herman S. , Filippov Dmitri V. , van Kasteren Sander I. 
Published: March 2015

AbstractThe activation of CD8+ T‐cells requires the uptake of exogenous polypeptide antigens and proteolytic processing of these antigens to octamer or nonamer peptides, which are loaded on MHC‐I complexes and presented to the T‐cell. By using an azide as a bioorthogonal protecting group rather than as a ligation handle, masked antigens were generated—antigens that are not recognized by their cognate T‐cell unless they are deprotected on the cell using a Staudinger reduction.
Macromolecular Surface Design: Photopatterning of Functional Stable Nitrile Oxides
Authors: Altintas Ozcan , Glassner Mathias , Rodriguez‐Emmenegger Cesar , Welle Alexander , Trouillet Vanessa , Barner‐Kowollik Christopher 
Published: March 2015

AbstractThe efficient trapping of photogenerated thioaldehydes with functional shelf‐stable nitrile oxides in a 1,3‐dipolar cycloaddition is a novel and versatile photochemical strategy for polymer end‐group functionalization and surface modification under mild and equimolar conditions. The modular ligation in solution was followed in detail by electrospray ionization mass spectrometry (ESI‐MS). X‐ray photoelectron spectroscopy (XPS) was employed to analyze the functionalized surfaces, whereas time‐of‐flight secondary‐ion mass spectrometry (ToF‐SIMS) confirmed the spatial control of the surface functionalization using a micropatterned shadow mask. Polymer brushes were grown from the surface in a spatially confined regime by surface‐initiated atom transfer radical polymerization (SI‐ATRP) as confirmed by TOF‐SIMS, XPS as well as ellipsometry.
Synthesis of Ultrathin Face‐Centered‐Cubic Au@Pt and Au@Pd Core–Shell Nanoplates from Hexagonal‐Close‐Packed Au Square Sheets
Authors: Fan Zhanxi , Zhu Yihan , Huang Xiao , Han Yu , Wang Qingxiao , Liu Qing , Huang Ying , Gan Chee Lip , Zhang Hua 
Published: March 2015

AbstractThe synthesis of ultrathin face‐centered‐cubic (fcc) Au@Pt rhombic nanoplates is reported through the epitaxial growth of Pt on hexagonal‐close‐packed (hcp) Au square sheets (AuSSs). The Pt‐layer growth results in a hcp‐to‐fcc phase transformation of the AuSSs under ambient conditions. Interestingly, the obtained fcc Au@Pt rhombic nanoplates demonstrate a unique (101)f orientation with the same atomic arrangement extending from the Au core to the Pt shell. Importantly, this method can be extended to the epitaxial growth of Pd on hcp AuSSs, resulting in the unprecedented formation of fcc Au@Pd rhombic nanoplates with (101)f orientation. Additionally, a small amount of fcc (100)f‐oriented Au@Pt and Au@Pd square nanoplates are obtained with the Au@Pt and Au@Pd rhombic nanoplates, respectively. We believe that these findings will shed new light on the synthesis of novel noble bimetallic nanostructures.
Improving the Electrochemical Performance of the Li4Ti5O12 Electrode in a Rechargeable Magnesium Battery by Lithium–Magnesium Co‐Intercalation
Authors: Wu Na , Yang Zhen‐Zhong , Yao Hu‐Rong , Yin Ya‐Xia , Gu Lin , Guo Yu‐Guo 
Published: March 2015

AbstractRechargeable magnesium batteries have attracted recent research attention because of abundant raw materials and their relatively low‐price and high‐safety characteristics. However, the sluggish kinetics of the intercalated Mg2+ ions in the electrode materials originates from the high polarizing ability of the Mg2+ ion and hinders its electrochemical properties. Here we report a facile approach to improve the electrochemical energy storage capability of the Li4Ti5O12 electrode in a Mg battery system by the synergy between Mg2+ and Li+ ions. By tuning the hybrid electrolyte of Mg2+ and Li+ ions, both the reversible capacity and the kinetic properties of large Li4Ti5O12 nanoparticles attain remarkable improvement.
Preparation of artificial wood films with controlled biodegradability
Authors: Kim Sung Hee , Kim Min Hoo , Kim Ji Hyun , Park Saerom , Kim Hyungsup , Won Keehoon , Lee Sang Hyun 
Published: March 2015

ABSTRACTArtificial wood films containing cellulose, xylan, and lignin were easily prepared by the dissolution of wood components in 1‐ethyl‐3‐methylimidazolium acetate followed by reconstitution with distilled water. The composition and characteristics of wood films were highly controllable and predictable through the variation of the concentration of each component in the wood solution. The water vapor solubility of the wood films was increased when the xylan content was increased and the content of lignin was decreased. The biodegradability of the artificial wood films was investigated with cellulase from Trichoderma viride. The relative degradability of the wood film prepared with 5% cellulose and 5% lignin was 42%, whereas that of the wood film made with 5% cellulose and 5% xylan was 189%. The biodegradability of cellulose in the wood films correlated well with the content of xylan and lignin, and it was enhanced when the xylan content was increased and the content of lignin was decreased. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 42109.
Photodynamic antifungal activities of nanostructured fabrics grafted with rose bengal and phloxine B against Aspergillus fumigatus
Authors: Kim Joo Ran , Michielsen Stephen 
Published: March 2015

ABSTRACTThis study demonstrates that nanostructured fabrics grafted with rose bengal (RB) and phloxine B (PB) have photodynamic antifungal effects on Aspergillus fumigatus. RB and PB were attached to vinyl benzyl chloride, and, subsequently, this was polymerized with acrylic acid and styrene sulfonic acid to produce long, water‐soluble polymers to attach to the fabric surface. This gave high grafting yield and photodynamic antifungal activity against A. fumigatus. In RB and PB microdilution tests, there was no visible turbidity at 63 µmol/L. When polymerized RB and PB were incorporated into fabrics, the actions of polymerized RB and PB resulted in less hyphal growth and germination of conidia on A. fumigatus than the free RB and PB dyes. Nanostructured fabrics created by bonding RB‐ or PB‐containing polymers to electrospun nylon mats exhibited higher concentrations of the dyes, equivalent to 86 µmol/L. The microstructured fabrics created by bonding RB‐ or PB‐containing polymers to spunbonded nylon nonwoven fabrics only exhibited the equivalent of 32 µmol/L of the dyes. The nanostructured fabrics had a specific surface area of 28.1 m2/g, whereas the microfabric had 1.5 m2/g. Thus, the nanostructured fabrics increased the surface area 18.7× and the reflectance percent 16.2× when compared with the microstructured fabrics. This resulted in much higher photodynamic antifungal activity against A. fumigatus. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 42114.
Colorimetric and Fluorescent Bimodal Ratiometric Probes for pH Sensing of Living Cells
Authors: Liu Yuan‐Yuan , Wu Ming , Zhu Li‐Na , Feng Xi‐Zeng , Kong De‐Ming 
Published: March 2015

AbstractpH measurement is widely used in many fields. Ratiometric pH sensing is an important way to improve the detection accuracy. Herein, five water‐soluble cationic porphyrin derivatives were synthesized and their optical property changes with pH value were investigated. Their pH‐dependent assembly/disassembly behaviors caused significant changes in both absorption and fluorescence spectra, thus making them promising bimodal ratiometric probes for both colorimetric and fluorescent pH sensing. Different substituent identity and position confer these probes with different sensitive pH‐sensing ranges, and the substituent position gives a larger effect. By selecting different porphyrins, different signal intensity ratios and different fluorescence excitation wavelengths, sensitive pH sensing can be achieved in the range of 2.1–8.0. Having demonstrated the excellent reversibility, good accuracy and low cytotoxicity of the probes, they were successfully applied in pH sensing inside living cells.
Aromaticity Switching in Porphyrinoids
Authors: Pawlicki Miłosz , Latos‐Grażyński Lechosław 
Published: March 2015

AbstractThe aromaticity of porphyrinoids can be substantially altered by reversible modification of their original electronic structures. Well‐defined modulators can be used as a means to initiate these modifications, including redox processes, acid–base chemistry, and conformational phenomena. This Focus Review emphasizes the situation for which a single macrocyclic frame alternatively adopts diatropic and paratropic features and both situations are readily and mutually exchangeable. Eventually, such a porphyrinoid transformation can be explored as a suitable element to construct switchable optoelectronic materials.
Continuous precipitation of IgG from CHO cell culture supernatant in a tubular reactor
Authors: Hammerschmidt Nikolaus , Hintersteiner Beate , Lingg Nico , Jungbauer Alois 
Published: March 2015

AbstractWe successfully transferred a two‐stage batch precipitation‐based antibody capture step to continuous mode using continuous tubular reactors. The precipitation process solely employs a cheap mineral salt (CaCl2) and an organic solvent (ethanol) and could replace the costly protein A capture step in the purification of recombinant antibodies from cell culture supernatant. The time from startup untill attaining steady state conditions was reached in less than 15 minutes and both reactors were operated for several hours at steady state without manual intervention, delivering antibody at a constant yield and purity. An overall yield of > 90 percent, with a host cell protein reduction from 42 777 to 9000 ppm and a DNA reduction from 359 ppm to 7 ppm, could be achieved for the antibody investigated. The precipitated antibody can be dissolved at very high concentrations (> 40 g/L) in numerous buffer systems of various pH and high and low ionic strength, thereby rendering a subsequent concentration or buffer exchange step redundant. This system enables cell culture supernatants with low or high antibody titer to be processed with constant reactor size and without changing any parameters or increasing precipitant consumption. Aggregate levels were below 1% under all conditions tested. Purification by precipitation did not affect binding to CD16a or the isoform distribution of the antibody.
Intraoperative radiotherapy in early breast cancer
Authors: Esposito E , Anninga B , Harris S , Capasso I , D'Aiuto M , Rinaldo M , Douek M 
Published: March 2015

Abstract

Background
Intraoperative radiotherapy (IORT) constitutes a paradigm shift from the conventional 3–5 weeks of whole-breast external beam radiotherapy (EBRT). IORT enables delivery of radiation at the time of excision of the breast tumour, targeting the area at highest risk of recurrence, while minimizing excessive radiation exposure to healthy breast tissue. The rationale for IORT is based on the observation that over 90 per cent of local recurrences after breast-conserving surgery occur at or near the original operation site.

Methods
This article reviews trials of IORT delivered with different techniques and devices.

Results
IORT is a very attractive option for delivering radiotherapy, reducing the traditional fractionated treatment to a single fraction administered at the time of surgery. IORT has been shown to be associated with reduced toxicity and has several potential benefits over EBRT. Only two randomized clinical trials have been published to date. The TARGIT-A and ELIOT trials have demonstrated that IORT is associated with a low rate of local recurrence, although higher than that after EBRT (TARGIT-A: 3·3 versus 1·3 per cent respectively, P = 0·042; ELIOT: 4·4 versus 0·4 per cent, P &lt; 0·001). However, the local recurrence rate for IORT fell within the predefined 2·5 per cent non-inferiority margin in TARGIT-A, and the 7·5 per cent equivalence margin in ELIOT.

Conclusion
Longer follow-up data from existing trials, optimization of patient criteria and cost-effectiveness analyses are needed. Based on the current evidence, IORT can be offered as an alternative to EBRT to selected patients within agreed protocols, and outcomes should be monitored within national registries.
‘I Miss My Little One A Lot’: How Father Love Motivates Change in Men Who Have Used Violence
Authors: Broady Timothy R. , Gray Rebecca , Gaffney Irene , Lewis Pamela 
Published: March 2015

This paper presents selected findings from a research‐based evaluation of a men's domestic violence intervention programme, which aims to assist men to develop alternative ways of relating to their partners, children and others. The qualitative component of this evaluation involved conducting interviews with 21 group participants after their completion of the course. These interviews investigated several issues, including participants' perceptions of their relationships with their children. The main theme underpinning all discussions of children was an expression of love, in that love for their children served as a motivation to stop using violence and to develop alternative ways of relating to all family members. The paper concludes by discussing the potential of men's relationships with their children as powerful contexts, or points of leverage, through which the impact of their violent behaviour can be realised and confronted. By realising the impact that violent behaviour can have on children's wellbeing and fathers' interpersonal relationships with them, it is argued that intervention programmes can support men to develop more appropriate ways of relating to their children, and thus safeguard children from potential long‐term consequences of domestic abuse. Copyright © 2015 John Wiley & Sons, Ltd.‘The main theme underpinning all discussions of children was an expression of love’Key Practitioner Messages

Men attending domestic violence intervention programmes demonstrate a wide range of attitudes towards their partners and former partners, but unanimously report a desire to maintain meaningful relationships with their children.
Men who have used violence in their family relationships can be challenged and motivated to change through realising the impact of their behaviour on their children's wellbeing and their father‐child relationships.
‘Unanimously report a desire to maintain meaningful relationships with their children’
Tunable Photochromism in the Robust Dithienylethene‐Containing Phospholes: Design, Synthesis, Characterization, Electrochemistry, Photophysics, and Photochromic Studies
Authors: Chan Jacky Chi‐Hung , Wong Hok‐Lai , Wong Wing‐Tak , Yam Vivian Wing‐Wah 
Published: March 2015

AbstractA series of dithienylethene‐containing phosphole derivatives has been designed, synthesized and characterized. One of the compounds has been characterized by X‐ray crystallography. Upon photoexcitation, the compounds exhibit drastic color changes, ascribed to the reversible photochromic behavior. Their photochromic, photophysical and electrochemical properties have been studied. They show photochromic reactivities with high photocyclization quantum yields. Their photophysical and photochromic properties are found to be facilely tuned in this system by substitution at the phosphole backbone, as well as variation on the extent of π‐conjugation of the phosphole backbone. Some selected compounds have been demonstrated to exhibit photochromic properties in polymethylmethacrylate (PMMA) films.
Twist versus Linkage Mode: Which One is Better for the Construction of Blue Luminogens with AIE Properties?
Authors: Yang Jie , Huang Jing , Sun Ning , Peng Qian , Li Qianqian , Ma Dongge , Li Zhen 
Published: March 2015

AbstractTwo new blue luminogens, Py‐4MethylTPE and Py‐4mTPE, constructed with a pyrene core and tetraphenylethene peripheries, have been successfully obtained. These two luminogens show AIE and AEE effects, respectively, as a result of minor differences in their structures. An OLED device based on Py‐4mTPE exhibits a good performance (ηC,max=4.02 cd A−1, λEL,max=436 nm) and reveals the powerful effect of a different linkage mode for the construction of blue AIE luminogens.
Synthesis of One‐Dimensional Schiff Base Polymers that Contain an Oligothiophene Building Block on the Graphite Surface
Authors: Sun Xiu‐Ling , Fan Li‐Xia , Yang Yong‐Jing , Guo Zongxia , Tian Wei Quan , Lei Shengbin 
Published: March 2015

AbstractSurface‐mediated Schiff base coupling reactions between oligothiophenes equipped with an aldehyde group and aromatic diamines were investigated on highly oriented pyrolytic graphite (HOPG) by means of scanning tunneling microscopy (STM) under ambient conditions. To investigate the evolution process from monomers to resultant polymers and the mechanism of reactions, we controlled the ratio of precursors and the reactive temperature, and we obtained high‐resolution STM images of different stages of the surface reaction. The results suggest that preferential adsorption of one kind of monomer has a great influence on the on‐ surface Schiff base reaction.
Square Tiling by Square Macrocycles at the Liquid/Solid Interface: Co‐crystallisation with One‐ or Two‐Dimensional Order
Authors: Tahara Kazukuni , Gotoda Jun , Carroll Calden N. , Hirose Keiji , De Feyter Steven , Tobe Yoshito 
Published: March 2015

AbstractWe have systematically investigated the self‐assembled monolayers of seven bimolecular mixtures of square‐shaped pyridinophanes and cyclophanes bearing alkoxy or alkoxycarbonyl substituents in the presence of the tropylium ion as a marker of pyridinophanes at liquid/graphite interfaces by means of scanning tunnelling microscopy (STM). The purpose of this work was to elucidate the mixing behaviour of these macrocycles highlighting the formation of one‐ or two‐dimensionally ordered square tilings consisting of alternating alignments of different macrocycles as a result of attractive dipole–dipole or hydrogen‐bonding interactions; four co‐crystals differing in the dimensionality of the ordering of pyridinophane and cyclophane were observed. The different modes of interaction between the functional groups (ether or carbonyl group) in the side‐chains of the pyridinophanes and cyclophanes lead to the formation of co‐crystals with dimensionally different orderings of the two macrocycles. These observations revealed that a slight modification of the molecular structure may dramatically change the mixing behaviour and structures of the co‐crystals.
Cooperative Dehydrogenation of N‐Heterocycles Using a Carbon Nanotube–Rhodium Nanohybrid
Authors: Jawale Dhanaji V. , Gravel Edmond , Shah Nimesh , Dauvois Vincent , Li Haiyan , Namboothiri Irishi N. N. , Doris Eric 
Published: March 2015

AbstractRhodium nanoparticles were anchored on carbon nanotubes and the resulting nanohybrid was studied as co‐catalyst, along with tert‐butylcatechol, for the dehydrogenation of various N‐heterocycles. The co‐catalytic system operates in high yields, under the mildest conditions reported so far, and can be applied to a wide variety of secondary amine‐containing scaffolds.
Bismetal Complexes of 5,20‐Bis(5‐formyl‐2‐pyrrolyl)‐[26]hexaphyrin(1.1.1.1.1.1) Exhibiting Strong Near‐Infrared Region Absorptions
Authors: Mori Hirotaka , Osuka Atsuhiro 
Published: March 2015

Abstract[26]Hexaphyrin(1.1.1.1.1.1) bearing two 5‐formyl‐2‐pyrrolyl groups at the 5‐ and 20‐positions was prepared by cross‐condensation of 5,10‐bis(pentafluorophenyl)‐substituted tripyrrane with 2,5‐diformylpyrrole as an effective binuclear metal‐coordinating ligand, owing to the two hemiporphyrin‐like NNNN pockets. In fact, metalation of this hexaphyrin with ZnII, CuII, and PdII salts proceed smoothly at room temperature to give the corresponding bismetal complexes that displayed remarkably redshifted absorption spectra reaching deep into near infrared region. These redshifted absorption bands are ascribed, through electrochemical investigations and DFT calculations, to two structural motifs: the N‐metalopyrrole substructure that elevates the HOMO level due to the electron‐donating property and the two coordinated metal ions that serve as Lewis acids to lower the LUMO level.
Targeting the Erythrocytic and Liver Stages of Malaria Parasites with s‐Triazine‐Based Hybrids
Authors: Rodrigues Catarina A. B. , Frade Raquel F. M. , Albuquerque Inês S. , Perry Maria J. , Gut Jiri , Machado Marta , Rosenthal Philip J. , Prudêncio Miguel , Afonso Carlos A. M. , Moreira Rui 
Published: March 2015

AbstractA diversity‐oriented library of s‐triazine‐based hybrids was screened for activity against the chloroquine‐resistant Plasmodium falciparum W2 strain. The most striking result was sub‐micromolar activity against cultured erythrocytic‐stage parasites of hybrid molecules containing one or two 8‐aminoquinoline moieties. These compounds were not clearly toxic to human cells. The most effective blood‐schizontocidal s‐triazine derivatives were then screened for activity against the liver stage of malaria parasites. The s‐triazine hybrid containing two 8‐aminoquinoline moieties and one chlorine atom emerged as the most potent against P. berghei liver‐stage infection, active in the low nanomolar region, combined with good metabolic stability in rat liver microsomes. These results indicate that s‐triazine‐8‐aminoquinoline‐based hybrids are excellent starting points for lead optimization as dual‐stage antimalarials.
High spatial resolution proteomic comparison of the brain in humans and chimpanzees
Authors: Bauernfeind Amy L. , Reyzer Michelle L. , Caprioli Richard M. , Ely John J. , Babbitt Courtney C. , Wray Gregory A. , Hof Patrick R. , Sherwood Chet C. 
Published: March 2015

ABSTRACTWe performed high‐throughput mass spectrometry at high spatial resolution from individual regions (anterior cingulate and primary motor, somatosensory, and visual cortices) and layers of the neocortex (layers III, IV, and V) and cerebellum (granule cell layer), as well as the caudate nucleus in humans and chimpanzees. A total of 39 mass spectrometry peaks were matched with probable protein identifications in both species, allowing for comparison in expression. We explored how the pattern of protein expression varies across regions and cortical layers to provide insights into the differences in molecular phenotype of these neural structures between species. The expression of proteins differed principally in a region‐ and layer‐specific pattern, with more subtle differences between species. Specifically, human and chimpanzee brains were similar in their distribution of proteins related to the regulation of transcription and enzyme activity but differed in their expression of proteins supporting aerobic metabolism. Whereas most work assessing molecular expression differences in the brains of primates has been performed on gene transcripts, this dataset extends current understanding of the differential molecular expression that may underlie human cognitive specializations. J. Comp. Neurol. 523:2043–2061, 2015. © 2015 Wiley Periodicals, Inc.