bluuebunny/crossref_metadata_2025_split huggingface dataset:
Service user involvement in risk assessment and management: The Transition Inventory
Authors: Kroner Daryl G. 
Published: February 2012

ABSTRACTBackgroundDrawing on self‐prediction theory and the positive benefits of increasing health service user participation in risk assessments, the Transition Inventory (TI) was developed. It is an aid to the assessment of areas that people anticipate will be of difficulty in the next stage of transition, for example from open hospital to the community.AimsThe aim of this paper is to determine reliability and convergent/discriminant validity data for the TI and its subscales, including behavioral impulsivity, social pressure, substance misuse, financial/employment, leisure, negative affect, interpersonal and family concerns and social alienation.MethodsEighty‐eight male offenders coming towards the end of a period of imprisonment were asked to complete the TI. Their results were compared with the staff‐rated Measures of Criminal Attitudes and Associates (MCAA) scale, alcohol blame and causation of crime items. Comparisons with the MCAA's antisocial intent scale, which is a future‐orientated scale, and the associates scale allowed for convergent/discriminant validity to be examined with TI scales. With a community offender sample, TI results were used to predict researcher ratings.ResultsThe TI scales demonstrated adequate internal consistency. Overall, the MCAA's antisocial intent scale had higher correlations with the TI than with a nonfuture‐orientated scale. TI scales also demonstrated convergent validity with other measures and preliminary predictive validity with researcher ratings.Conclusions/implications for practiceThe TI provides a way to increase service user involvement in the assessments that determine when and how they transfer to settings where they will have more independence. Copyright © 2012 John Wiley & Sons, Ltd.
Coclustering—a useful tool for chemometrics
Authors: Bro Rasmus , Papalexakis Evangelos E. , Acar Evrim , Sidiropoulos Nicholas D. 
Published: February 2012

Nowadays, chemometric applications in biology can readily deal with tens of thousands of variables, for instance, in omics and environmental analysis. Other areas of chemometrics also deal with distilling relevant information in highly information‐rich data sets. Traditional tools such as the principal component analysis or hierarchical clustering are often not optimal for providing succinct and accurate information from high rank data sets. A relatively little known approach that has shown significant potential in other areas of research iscoclustering, where a data matrix is simultaneously clustered in its rows and columns (objects and variables usually).Coclustering is the tool of choice when only a subset of variables is related to a specific grouping among objects. Hence, coclustering allows aselectnumber of objects to share a particular behavior on aselectnumber of variables.In this paper, we describe the basics of coclustering and use three different example data sets to show the advantages and shortcomings of coclustering. Copyright © 2012 John Wiley & Sons, Ltd.
Facile Carbon–Fluorine Bond Activation and Subsequent Functionalisation of 1,1‐Difluoroethylene and Tetrafluoroethylene Promoted by Adjacent Metal Centres
Authors: Slaney Michael E. , Anderson D. Jason , Ristic‐Petrovic Dusan , McDonald Robert , Cowie Martin 
Published: February 2012

AbstractThe bridging fluoroolefin ligands in the complexes [Ir2(CH3)(CO)2(μ‐olefin)(dppm)2][OTf] (olefin=tetrafluoroethylene, 1,1‐difluoroethylene; dppm=μ‐Ph2PCH2PPh2; OTf−=CF3SO3−) are susceptible to facile fluoride ion abstraction. Both fluoroolefin complexes react with trimethylsilyltriflate (Me3SiOTf) to give the corresponding fluorovinyl products by abstraction of a single fluoride ion. Although the trifluorovinyl ligand is bound to one metal, the monofluorovinyl group is bridging, bound to one metal through carbon and to the other metal through a dative bond from fluorine. Addition of two equivalents of Me3SiOTf to the tetrafluoroethylene‐bridged species gives the difluorovinylidene‐bridged product [Ir2(CH3)(OTf)(CO)2(μ‐OTf)(μ‐CCF2)(dppm)2][OTf]. The 1,1‐difluoroethylene species is exceedingly reactive, reacting with water to give 2‐fluoropropene and [Ir2(CO)2(μ‐OH)(dppm)2][OTf] and with carbon monoxide to give [Ir2(CO)3(μ‐κ1:η2‐CCCH3)(dppm)2][OTf] together with two equivalents of HF. The trifluorovinyl product [Ir2(κ1‐C2F3)(OTf)(CO)2(μ‐H)(μ‐CH2)(dppm)2][OTf], obtained through single CF bond activation of the tetrafluoroethylene‐bridged complex, reacts with H2 to form trifluoroethylene, allowing the facile replacement of one fluorine in C2F4 with hydrogen.
Size‐Dependent Surface Activity of Rutile and Anatase TiO2 Nanocrystals: Facile Surface Modification and Enhanced Photocatalytic Performance
Authors: Xiang Guolei , Wang Yang‐Gang , Wu Di , Li Tianyang , He Jie , Li Jun , Wang Xun 
Published: February 2012

AbstractThe size‐dependent surface activity of titania was illustrated through the formation of ultrafine nanocrystals with clean surfaces. It was demonstrated that, when the size of the nanocrystals was small enough, their surface activity could be significantly enhanced, as evidenced by the formation of transparent macroassemblies, their increased dispersity in various solvents, the facile modification of their surface by organic molecules at room temperature, their strong visible‐light absorption through coordination with peroxide, and highly enhanced photocatalytic performance.
Charged Behaviour from Neutral Ligands: Synthesis and Properties of N‐Heterocyclic Pseudo‐amides
Authors: Thatcher Robert J. , Johnson David G. , Slattery John M. , Douthwaite Richard E. 
Published: February 2012

AbstractDeprotonation of the 1‐isopropyl‐3‐(phenylamino)pyridin‐1‐ium iodide gives the corresponding neutral betaine, which is formalised as a pyridinium‐amido ligand when coordinated to a metal. Spectroscopic, structural and theoretical methods have been used to investigate the metal–ligand bonding, ligand dynamics and electron distribution. Collectively, the data show that the ligand can be characterised as a pseudo‐amide and is a strong donor akin to alkyl phosphines and N‐heterocyclic carbenes. Furthermore, rotation about both N substituent CN bonds occurs, which is in contrast to the two alternative pyridinium positional isomers that exhibit neutral resonance structures. For comparison, compounds and complexes derived from norharman were prepared, which contain an additional CC bond supporting conjugation and the accessibility of a neutral resonance structure. Notwithstanding the formal neutral structure, norharman‐derived ligands are comparably strong donors, and have the additional advantage of exhibiting stability to dioxygen and water.
Synthesis and Characterization of a Singlet Delocalized 2,4‐Diimino‐1,3‐disilacyclobutanediyl and a Silylenylsilaimine
Authors: Zhang Shu‐Hua , Xi Hong‐Wei , Lim Kok Hwa , Meng Qingyong , Huang Ming‐Bao , So Cheuk‐Wai 
Published: February 2012

AbstractThe synthesis and characterization of a singlet delocalized 2,4‐diimino‐1,3‐disilacyclobutanediyl, [LSi(μ‐CNAr)2SiL] (2, L: PhC(NtBu)2, Ar: 2,6‐iPr2C6H3), and a silylenylsilaimine, [LSi(NAr)SiL] (3), are described. The reaction of three equivalents of the disilylene [LSiSiL] (1) with two equivalents of ArNCNAr in toluene at room temperature for 12 h afforded [LSi(μ‐CNAr)2SiL] (2) and [LSi(NAr)SiL] (3) in a ratio of 1:2. Compounds 2 and 3 have been characterized by NMR spectroscopy and X‐ray crystallography. Compound 2 was also investigated by theoretical studies. The results show that compound 2 possesses singlet biradicaloid character with an extensive electronic delocalization throughout the Si2C2 four‐membered ring and exocyclic CN bonds. Compound 3 is the first example of a silylenylsilaimine, which contains a low‐valent silicon center and a silaimine substituent. A mechanism for the formation of 2 and 3 is also proposed.
A Non‐damaging Method to Analyze the Configuration and Dynamics of Nitrotyrosines in Proteins
Authors: Díaz‐Moreno Irene , Nieto Pedro M. , Del Conte Rebecca , Gairí Margarida , García‐Heredia José M. , De la Rosa Miguel A. , Díaz‐Quintana Antonio 
Published: February 2012

AbstractOften, deregulation of protein activity and turnover by tyrosine nitration drives cells toward pathogenesis. Hence, understanding how the nitration of a protein affects both its function and stability is of outstanding interest. Nowadays, most of the in vitro analyses of nitrated proteins rely on chemical treatment of native proteins with an excess of a chemical reagent. One such reagent, peroxynitrite, stands out for its biological relevance. However, given the excess of the nitrating reagent, the resulting in vitro modification could differ from the physiological nitration. Here, we determine unequivocally the configuration of distinct nitrated‐tyrosine rings in single‐tyrosine mutants of cytochrome c. We aimed to confirm the nitration position by a non‐destructive method. Thus, we have resorted to 1H‐15N heteronuclear single quantum coherence(HSQC) spectra to identify the 3J(NH) correlation between a 15N‐tagged nitro group and the adjacent aromatic proton. Once the chemical shift of this proton was determined, we compared the 1H‐13C HSQC spectra of untreated and nitrated samples. All tyrosines were nitrated at ε positions, in agreement to previous analysis by indirect techniques. Notably, the various nitrotyrosine residues show a different dynamic behaviour that is consistent with molecular dynamics computations.
Regulation of π‐Stacked Anthracene Arrangement for Fluorescence Modulation of Organic Solid from Monomer to Excited Oligomer Emission
Authors: Hinoue Tomoaki , Shigenoi Yuta , Sugino Misa , Mizobe Yuji , Hisaki Ichiro , Miyata Mikiji , Tohnai Norimitsu 
Published: February 2012

AbstractThe construction and precise control of the face‐to‐face π‐stacked arrangements of anthracene fluorophores in the crystalline state led to a remarkable red shift in the fluorescence spectrum due to unprecedented excited oligomer formation. The arrangements were regulated by using organic salts including anthracene‐1,5‐disulfonic acid (1,5‐ADS) and a variety of aliphatic amines. Because of the smaller number of hydrogen atoms at the edge positions and the steric effect of the sulfonate groups, 1,5‐ADS should prefer face‐to‐face π‐stacked arrangements over the usual edge‐to‐face herringbone arrangement. Indeed, as the alkyl substituents were lengthened, the organic salts altered their anthracene arrangement to give two‐dimensional (2D) edge‐to‐face and end‐to‐face herringbone arrangements, one‐dimensional (1D) face‐to‐face zigzag and slipped stacking arrangements, a lateral 1D face‐to‐face arrangement like part of a brick wall, and a discrete monomer arrangement. The monomer arrangement behaved as a dilute solution even in the close‐packed solid state to emit deep blue light. The 1D face‐to‐face zigzag and slipped stacking of the anthracene fluorophores caused a red shift of 30–40 nm in the fluorescence emission with respect to the discrete arrangement, probably owing to ground‐state associations. On the other hand, the 2D end‐to‐face stacking induced a larger red shift of 60 nm, which is attributed to the excimer fluorescence. Surprisingly, the brick‐like lateral face‐to‐face arrangement afforded a remarkable red shift of 150 nm to give yellow fluorescence. This anomalous red shift is probably due to excited oligomer formation in such a lateral 1D arrangement according to the long fluorescence lifetime and little shift in the excitation spectrum. The regulation of the π‐stacked arrangement of anthracene fluorophores enabled the wide modulation of the fluorescence and a detailed investigation of the relationships between the photophysical properties and the arrangements.
Highly Chemoselective Calcium‐Catalyzed Propargylic Deoxygenation
Authors: Meyer Vera J. , Niggemann Meike 
Published: February 2012

AbstractA calcium‐catalyzed direct reduction of propargylic alcohols and ethers has been accomplished by using triethylsilane as a nucleophilic hydride source. At room temperature a variety of secondary propargylic alcohols was deoxygenated to the corresponding hydrocarbons in excellent yields. Furthermore, for the first time, a catalytic deoxygenation of tertiary propargylic alcohols was generally applicable. The same protocol was suitable for an efficient reduction of secondary as well as tertiary propargylic methyl, benzyl and allyl ethers. Substrates containing an additional keto‐, ester or secondary hydroxyl function were reduced with exceptional chemoselectivity at the propargylic position.
Photooxygenation of a Microbial Arene Oxidation Product and Regioselective Kornblum–DeLaMare Rearrangement: Total Synthesis of Zeylenols and Zeylenones
Authors: Palframan Matthew J. , Kociok‐Köhn Gabriele , Lewis Simon E. 
Published: February 2012

AbstractWe report the enantioselective total syntheses of zeylenol (+)‐1, as well as its congeners (−)‐7 and 16, and of 3‐O‐debenzoylzeylenone 28. To this end, a new variant of the Kornblum–DeLaMare rearrangement, which utilises neighbouring‐group participation to impart regioselectivity, has been developed. The approach employs photooxygenation of building blocks derived from a microbial arene oxidation product.
CFD Simulation and LDA Measurement of the Fluid Flow in Fluid Phase Resonance Mixing
Authors: Schmalfuß Silvio , Säuberlich Ralph , Sommerfeld Martin 
Published: February 2012

AbstractBeim Fluidphasenresonanzmischen wird eine flüssige Phase in einem Behälter über ein Gaspolster mit harmonisch schwingendem Wechseldruck beaufschlagt und so zu Schwingungen angeregt. Dieses Verfahren wird als instationäre Strömung zweier getrennter Phasen mit der CFD‐Software OpenFOAM simuliert und die Ergebnisse werden durch Messungen mit einem Einkomponenten‐Laser‐Doppler‐Anemometer verifiziert.
Xanthan Sulfuric Acid: An Efficient Bio‐supported and Recyclable Solid Acid Catalyst for the Synthesis of 2‐Aryl Thiadiazolo Benzimidazoles
Authors: Kuarm B. Suresh , Janardan B. , Crooks Peter A. , Rajitha B. 
Published: February 2012

AbstractXanthan sulfuric acid is an efficient solid acid catalyst for the preparation of 2‐aryl benzimidazoles in excellent yields. This method is applicable for the reaction of benzo[c][1,2,5]thiadiazole‐4,5‐diamine with aldehydes by simple physical grinding at room temperature. The salient features of the present methodology is cheaper process, easy synthesis of stable catalyst and the catalyst can be easily recycled without significant loss of activity.
Synthesis, Photophysical Properties and Near Infrared Electroluminescence of 1(4),8(11),15(18),22(25)‐Tetra‐(methoxy‐phenoxy)phthalocyanine
Authors: Bai Qinglong , Zhang Chunhua , Cheng Chuanhui , Li Wancheng , Wang Jin , Du Guotong 
Published: February 2012

AbstractA new soluble phthalocyaine 1(4),8(11),15(18),22(25)‐tetra‐(methoxy‐phenoxy)phthalocyanine (MPPc) was synthesized and verified by mass spectrum (MS), 1H NMR, IR and elemental analysis. The methoxy‐phenoxy groups were introduced in order to enhance the solubility of the phthalocyanine. The photophysical and electroluminescent properties were investigated. The organic light‐emitting diodes (OLEDs) with the structure of ITO/PVK:MPPc(40 nm)/BCP(20 nm)/Alq3(30 nm)/Al were fabricated. Room‐temperature near infrared (NIR) electroluminescence (EL) was observed near 891 nm that effectively covered the ?rst optical communication window near 850 nm.
One Pot Synthesis of Medicinally Important cis‐2‐Methyl‐4‐amino substituted‐1,2,3,4‐tetrahydroquinolines
Authors: Kiran Kumar H. C. , Mahadevan K. M. , Prabhakara Varma P. , Srinivasa A. 
Published: February 2012

AbstractA simple synthesis of medicinally important cis‐2‐methyl‐4‐azapan‐2‐one‐1,2,3,4‐tetrahydroquinolines/cis‐9‐(2‐methyl‐1,2,3,4‐tetrahydroquinolin‐4‐yl)‐9H‐carbazole was reported. Multicomponent one pot synthesis with anilines and N‐vinylcaprolactam/N‐vinyl carbazole via imino Diels‐Alder reaction by using antimony trichloride as catalyst and acetonitrile as solvent was employed. NMR technique (2D) was used to study the regio‐ and stereo‐chemistry of newly synthesized compounds. The cis diastereo‐selectivity of the products was predicted by COSY and NOESY studies.
Synthesis, Structure and Thermodynamic Property of a New Lithium Borate: Li4[B8O13(OH)2]&middot;3H2O
Authors: Li Ping , Liu Zhihong 
Published: February 2012

AbstractA new hydrated lithium borate, Li4[B8O13(OH)2]&middot;3H2O, has been hydrothermally synthesized and characterized by single crystal X‐ray diffraction, FT‐IR spectroscopy, simultaneous TGA‐DTA and chemical analysis. It crystallizes in the triclinic, space group $ P {\bar 1} $, a=8.4578(5) Å, b=8.7877(5) Å, c=10.8058(7) Å, α=87.740(3)°, β=71.819(3)°, γ=61.569(3)°, Z=2, V=665.26(7) Å3, Dc=2.043 g/cm3. Its crystal structure features polyborate anionic layers with the larger odd 13‐membered boron rings constructed by [B8O13(OH)2]4− FBBs. Through designing the thermochemical cycle, the standard molar enthalpy of formation of this borate was determined to be −(7953.8±6.6) kJ&middot;mol−1 by using a heat conduction microcalorimeter.
Environmentally Benign Synthesis of Sugar Orthoesters Promoted by Anhydrous Sodium Acetate and Ultrasound
Authors: Zhao Jinzhong , Wei Shanqiao , Yue Aiqin , Shao Huawu 
Published: February 2012

AbstractA convenient and alternative procedure for the synthesis of sugar orthoesters from glycosyl bromides with anhydrous sodium acetate as base under ultrasound irradiation is described. Various sugar and sugar‐sugar orthoesters were prepared in 70&percnt;–91&percnt; isolated yields.
Fluorescent Properties of the Amidinophenylporphyrins Interacting with DNA
Authors: Wang Kai , Li Tian , Yu Faquan , Zheng Yunman , Wong Wai‐Kwok , Kwong Daniel W. J. , Li Zaoying 
Published: February 2012

Abstract5,10,15,20‐Tetrakis(4‐amidinolphenyl)porphyrin, its Zn complex and amidinolphenyl bispophyrin interacting with calf thymus DNA were investigated by fluorescence emission spectra and fluorescence life time measurements were also shown. The binding modes of these compounds were recorded and lifetimes of luminescence were measured as a function of the nature to understand the interaction with DNA. The results suggest those amidinoporphyrins are promising new photodynamic therapeutic agents.
Synthesis of Small Molecules Targeting Multiple DNA Structures using Click Chemistry
Authors: Howell Lesley A. , Bowater Richard A. , O'Connell Maria A. , Reszka Anthony P. , Neidle Stephen , Searcey Mark 
Published: February 2012

AbstractThe ability of small molecules to target DNA forms the basis of many clinically used antitumour agents. This study examines the effects of novel 9‐aminoacridine carboxamides, synthesised by click chemistry based upon the reactions of either 9‐(2‐azidoethyl)amino or 9‐propargylaminoacridine compounds, on various types of DNA tertiary structures. This gave either monomeric or dimeric compounds, the dimeric derivatives being the first unsymmetrical acridine dimers to be described. The compounds were assayed for duplex DNA, quadruplex DNA and four‐way junction DNA binding. Their antiproliferative activity in the Human promyelocytic leukaemia cell line, HL60, was also assessed. Although for some of the compounds, notably the acridine 4‐carboxamides, activity correlated with DNA binding affinity, for others it did not, with the rigidly linked dimers in particular showing a complicated relationship between 3‐ and 4‐carboxamide structure and biological activity. The monomeric 3‐carboxamides were more effective at stabilising G‐quadruplex structures and also gave more hits in the four‐way junction stabilisation assay. There is clear evidence from the binding of the 3‐carboxamides that these compounds destabilise the open X form of the junction at lower concentrations and stabilise the X‐stacked at higher concentrations. This might have implications for the biological activity of these compounds against proteins that bind to the Holliday junction (HJ).
A genetic algorithm tuned optimal controller for glucose regulation in type 1 diabetic subjects
Authors: Ghosh Subhojit , Gude Srihari 
Published: February 2012

SUMMARYAn optimal state feedback controller is designed with the objective of minimizing the elevated glucose levels caused by meal intake in Type 1 diabetic subjects, by the minimal infusion of insulin. The states for the controller based on linear quadratic regulator theory are estimated from noisy data using Kalman filter. The controller designed for a physiological relevant mathematical model is coupled with another model for simulating meal dynamics, which converts meal intake into glucose appearance rate in the plasma. The tuning parameters (weighting matrices) of the controller and the design parameters (noise covariance matrices) of the Kalman filter are optimized using genetic algorithm. The controller based on the combined framework of evolutionary computing and state estimated linear quadratic regulator is found to maintain normoglycemia for meal intakes of varying carbohydrate content. The proposed approach addresses noisy output measurement, modeling error and delay in sensor measurement. Copyright © 2012 John Wiley & Sons, Ltd.
Polarization‐Dependent SERS at Differently Oriented Single Gold Nanorods
Authors: Jiao Jiqing , Wang Xiao , Wackenhut Frank , Horneber Anke , Chen Liuping , Failla Antonio Virgilio , Meixner Alfred J. , Zhang Dai 
Published: February 2012

AbstractWe investigated the influence of the orientation of individual gold nanorods on the polarization‐dependent single‐particle surface‐enhanced Raman spectroscopy (SERS) of adenine. Higher‐order laser beams (radial and azimuthal polarizations) have been used in combination with a parabolic mirror‐assisted confocal optical microscope. Based on the photoluminescence (PL) patterns of the single gold nanorods and the simulated electric‐field distribution in the focus, we distinguished between isolated gold rods and clusters as well as single nanorods with different orientations. We found that for single gold nanorods lying flat on the substrate, the longitudinal particle plasmon resonance (PPR) mode can be excited more efficiently with the in‐plane field component in the focus of an azimuthally polarized laser beam, which enables the observation of stronger enhanced adenine Raman spectra from the single gold nanorods compared to the case of a radially polarized beam.
Li2 Trapped inside Tubiform [n] Boron Nitride Clusters (n=4–8): Structures and First Hyperpolarizability
Authors: Ma Fang , Zhou Zhong‐Jun , Liu Ying‐Tao 
Published: February 2012

AbstractThe geometries and electronic properties of tubiform [n] boron nitride clusters entrapping Li2 (Li2@BN‐cluster(n,0); n=4–8), obtained by doping BN‐cluster(n,0) with Li2 molecules, are investigated by means of DFT. The effects of tube diameter n on the dipole moment μ0, static polarizability α0, and first hyperpolarizability β0 are elucidated. Both the dipole moment and polarizability increase with increasing tube diameter, whereas variation of the static first hyperpolarizability with tube diameter is not monotonic; β0 follows the order 1612 (n=4)<3112 (n=5)<5534 (n=7)<8244 (n=6)<12 282 a.u. (n=8). In addition, the natural bond orbital (NBO) charges show that charge transfer takes place from the Li2 molecule to the BN cluster, except for BN‐cluster(8,0) with larger tube diameter. Since the large‐diameter tubular BN‐cluster(8,0) can trap the excess electrons of the Li2 molecule, Li2@BN‐cluster(8,0) can be considered to be a novel electride compound.