bluuebunny/crossref_metadata_2025_split huggingface dataset:
Growth of the atrial septum after amplatzer device closure of atrial septal defects in young children
Authors: Gossett Jeffrey G. , Mansfield Laura , Acevedo Jennifer , Lay Amy S. , Rychlik Karen , Wax David F. 
Published: May 2015

BackgroundTrans‐catheter closure of atrial septal defects (ASD) with the Amplatzer Septal Occluder (ASO) device is safe and effective, but concern over erosions has increased. Devices are placed in growing children but septal growth after ASOs is ill‐defined. Understanding the device relationship to cardiac structures as a child grows may help us understand erosions. Objective: To define (1) how preprocedural septal measurements change after ASO and (2) the effect of somatic growth on these dimensions. Methods: Data were collected retrospectively. Echocardiograms were reviewed and rims measured prior to ASO, immediately after ASO, and at follow‐up. Demographic, procedural and device data were collected. Results: Thirty‐three patients were enrolled; mean age 5.2 ± 3.2 years with 4.0 ± 2.2 years follow‐up. All septal measurements decreased after ASO. Thirty‐one of 33 devices (94%) contacted the aortic root after ASO; all remained in contact at follow‐up with only the IVC rim growing significantly over time. Change in BSA predicted an asymmetric septal growth with increases in superior (P = 0.01) and IVC (P = 0.005) rims and no increase in aortic or AVV rims. No episodes of erosion occurred. Conclusions: ASDs in young children are not central in the septum, but proximate to the aorta. After ASO, the device remains in close proximity to the aorta. With somatic growth, the septum grows asymmetrically, and device position relative to the aorta is constant. Our study was not powered to detect rare serious adverse events such as erosion, but aortic rims were consistently zero and yet no events occurred. © 2015 Wiley Periodicals, Inc.
Highly Active Bimetallic Nickel–Palladium Alloy Nanoparticle Catalyzed Suzuki–Miyaura Reactions
Authors: Rai Rohit Kumar , Gupta Kavita , Behrens Silke , Li Jun , Xu Qiang , Singh Sanjay Kumar 
Published: May 2015

AbstractA bimetallic Ni–Pd alloy nanoparticle catalyst with a low palladium content (Ni0.90Pd0.10 nanocatalyst) was prepared and its catalytic performance in Suzuki–Miyaura reactions was evaluated along with that of other Ni–Pd nanocatalysts (with varying Ni/Pd molar ratios in the range of ≈0.25–0.75) and the corresponding monometallic, Ni and Pd, analogues. Notably, the bimetallic Ni0.90Pd0.10 alloy nanocatalyst performed exceptionally well for the synthesis of biaryls by employing a wide range of substituted aryl halides and arylboronic acids having electron‐donating and electron‐withdrawing groups, and they exhibited high recyclability in water/ethanol solution at moderate reaction temperatures. Catalyst poisoning tests and leaching experiments inferred the heterogeneous nature of the Ni0.90Pd0.10 nanocatalysts. The significant synergistic interactions between Ni and Pd account for the observed high catalytic efficacy of the Ni0.90Pd0.10 nanocatalyst.
TiO2 with “Fluorine‐Occupied” Surface Oxygen Vacancies and Its Stably Enhanced Photocatalytic Performance
Authors: Xu Liming , Ming Lufei , Chen Feng 
Published: May 2015

AbstractOxygen vacancies have a positive effect on the photocatalytic performance of TiO2, but their benefits are deeply limited owing to their inherent lability. To avoid this disadvantage, fluorine atoms were used to “occupy” the surface oxygen vacancies (O vacancies) of TiO2. The “fluorine‐occupied” surface O vacancies maintain the intrinsic nature of the O vacancies, but they are stable under ambient and photocatalytic conditions. TiO2 with “fluorine‐occupied” surface O vacancies give enhanced performance in terms of both photodegradation and photocurrent conversion. The “occupied” strategy used herein holds promise to be a common method for developing O vacancy‐related photocatalysts.
A Solvate Ionic Liquid as the Anolyte for Aqueous Rechargeable Li–O2 Batteries
Authors: Wang Hui , Sunahiro Shogo , Matsui Masaki , Zhang Peng , Takeda Yasuo , Yamamoto Osamu , Imanishi Nobuyuki 
Published: May 2015

AbstractA reversible high‐areal‐capacity metallic lithium anode is pivotal to develop high specific‐energy‐density lithium‐metal‐based batteries. A novel solvate ionic liquid has been prepared by mixing tetraethylene glycol dimethyl ether (G4) and lithium bis(fluorosulfonyl)imide (LiFSI). Raman measurements revealed that the solvent was completely complexed by lithium cations to form a solvate ionic liquid (SIL) when the molar ratio of solvent to lithium cations was lower than 2. A symmetrical Li/LiFSI‐2G4/Li cell showed no short circuit for 41.2 h, until the capacity of the loaded lithium anode at 1 mA cm−2 and 60 °C was reached. A metallic lithium anode could deliver a high areal capacity of 12 mAh cm−2 for 40 cycles in the SIL of LiFSI‐2G4 with a current density as high as 6 mA cm−2 at 60 °C. This novel SIL of LiFSI‐2G4 as an anolyte coupled with lithium metal allows favorable cyclability for a high specific‐energy‐density aqueous lithium–O2 cell.
Quinone‐Decorated Onion‐Like Carbon/Carbon Fiber Hybrid Electrodes for High‐Rate Supercapacitor Applications
Authors: Zeiger Marco , Weingarth Daniel , Presser Volker 
Published: May 2015

AbstractThe energy performance of carbon onions can be significantly enhanced by introducing pseudocapacitive materials, but this is commonly at the cost of power handling. In this study, a novel synergistic electrode preparation method was developed by using carbon‐fiber substrates loaded with quinone‐decorated carbon onions. The electrodes are free standing, binder free, extremely conductive, and the interfiber space filling overcomes the severely low apparent density commonly found for electrospun fibers. Electrochemical measurements were performed in organic and aqueous electrolytes. For both systems, a high electrochemical stability after 10 000 cycles was measured, as well as a long‐term voltage floating test for the organic electrolyte. The capacitance in 1 M H2SO4 was 288 F g−1 for the highest loading of quinones, which is similar to literature values, but with a very high power handling, showing more than 100 F g−1 at a scan rate of 2 Vs−1.
Combining Noble Metals and Enzymes for Relay Cascade Electrocatalysis of Nitrate Reduction to Ammonia at Neutral pH
Authors: Duca Matteo , Weeks Justin R. , Fedor Justin G. , Weiner Joel H. , Vincent Kylie A. 
Published: May 2015

AbstractElectrocatalytic reduction of nitrate at noble metals is particularly sluggish at neutral pH, while nitrate reductase enzymes are highly active for selective reduction of nitrate to nitrite under these conditions. However, noble metal electrodes can effectively reduce nitrite, even at millimolar concentrations in neutral media. In this study, we demonstrate tandem electrochemical reduction of nitrate to ammonia by combining Escherichia (E.) coli nitrate reductase (NarGHI) on an electrode with Pt or Rh nanoparticles. Under potential control, the enzyme first reduces nitrate to nitrite, which is further reduced by the metal at a slightly more negative potential. This creates a novel electrocatalytic relay cascade where the enzyme overcomes an inherent limitation of the metal. This proof‐of‐concept study, using biological and metal catalysts supported on commercial carbon beads, demonstrates a simple approach to the assembly of ‘hybrid’ electrocatalysts.
Photobiocatalysis: The Power of Combining Photocatalysis and Enzymes
Authors: Maciá‐Agulló Juan Antonio , Corma Avelino , Garcia Hermenegildo 
Published: May 2015

AbstractPhotobiocatalysts are constituted by a semiconductor with or without a light harvester that activates an enzyme. A logical source of inspiration for the development of photobiocatalysts has been natural photosynthetic centers. In photobiocatalysis, the coupling of the semiconductor and the enzyme frequently requires a natural cofactor and a relay transferring charge carriers from the semiconductor. The most widely studied photobiocatalysts so far make use of conduction band electrons of excited semiconductors to promote enzymatic reductions mediated by NAD+/NADH and an electron relay. The present review presents the state of the art in the field and has been organized based on the semiconductor and the reaction type including oxidations, hydrogen generation, and CO2 reduction. The possibility of direct enzyme activation by the semiconductor and the influence of the nature of mediator are also discussed as well as the use of mimics of the enzyme active center in combination with the semiconductor. The final section summarizes the state of the art of photobiocatalysis and comments on our view on future developments of the field.
Donor/Acceptor Dihydroindeno[1,2‐a]fluorene and Dihydroindeno[2,1‐b]fluorene: Towards New Families of Organic Semiconductors
Authors: Romain Maxime , Tondelier Denis , Geffroy Bernard , Jeannin Olivier , Jacques Emmanuel , Rault‐Berthelot Joëlle , Poriel Cyril 
Published: May 2015

AbstractNew families of donor/acceptor semiconductors based on dihydroindeno[1,2‐a]fluorene and dihydroindeno[2,1‐b]fluorene are reported. Due to the spiro bridges, this new generation of dihydroindenofluorenes allows a spatial separation of HOMO and LUMO, which retains the high ET value of the dihydroindenofluorene backbone and excellent physical properties. This control of the electronic and physical properties has allowed a second generation of dihydroindeno[1,2‐a]fluorene to be obtained with strongly enhanced performance in green and sky‐blue phosphorescent organic light‐emitting diodes (PhOLEDs) relative to the first generation of materials. To date, this is the highest performance ever reported for a blue PhOLED by using a dihydroindenofluorene derivative. Through this structure–property relationship study, a remarkable difference of performance between syn and anti isomers has also been highlighted. This surprising behaviour has been attributed to the different symmetry of the two molecules, and highlights the importance of the geometry profiles in the design of host materials for PhOLEDs.
Centromeric Alpha‐Satellite DNA Adopts Dimeric i‐Motif Structures Capped by AT Hoogsteen Base Pairs
Authors: Garavís Miguel , Escaja Núria , Gabelica Valérie , Villasante Alfredo , González Carlos 
Published: May 2015

AbstractHuman centromeric alpha‐satellite DNA is composed of tandem arrays of two types of 171 bp monomers; type A and type B. The differences between these types are concentrated in a 17 bp region of the monomer called the A/B box. Here, we have determined the solution structure of the C‐rich strand of the two main variants of the human alpha‐satellite A box. We show that, under acidic conditions, the C‐rich strands of two A boxes self‐recognize and form a head‐to‐tail dimeric i‐motif stabilized by four intercalated hemi‐protonated C:C+ base pairs. Interestingly, the stack of C:C+ base pairs is capped by T:T and Hoogsteen A:T base pairs. The two main variants of the A box adopt a similar three‐dimensional structure, although the residues involved in the formation of the i‐motif core are different in each case. Together with previous studies showing that the B box (known as the CENP‐B box) also forms dimeric i‐motif structures, our finding of this non‐canonical structure in the A box shows that centromeric alpha satellites in all human chromosomes are able to form i‐motifs, which consequently raises the possibility that these structures may play a role in the structural organization of the centromere.
Ligand Symmetry Modulation for Designing a Mesoporous Metal–Organic Framework: Dual Reactivity to Transition and Lanthanide Metals for Enhanced Functionalization
Authors: Du Miao , Wang Xi , Chen Min , Li Cheng‐Peng , Tian Jia‐Yue , Wang Zhuo‐Wei , Liu Chun‐Sen 
Published: May 2015

AbstractA promising alternative strategy for designing mesoporous metal–organic frameworks (MOFs) has been proposed, by modifying the symmetry rather than expanding the length of organic linkers. By means of this approach, a unique MOF material based on the target [Zn8(ad)4] (ad=adeninate) clusters and C3‐symmetric organic linkers can be obtained, with trigonal microporous (ca., 0.8 nm) and hexagonal mesoporous (ca., 3.0 nm) 1D channels. Moreover, the resulting 446‐MOF shows distinct reactivity to transition and lanthanide metal ions. Significantly, the transmetalation of CoII or NiII on the ZnII centers in 446‐MOF can enhance the sorption capacities of CO2 and CH4 (16–21 %), whereas the impregnation of EuIII and TbIII in the channels of 446‐MOF will result in adjustable light‐emitting behaviors.
Conformational Tuning of the Intramolecular Electronic Coupling in Molecular‐Wire Biruthenium Complexes Bridged by Biphenyl Derivatives
Authors: Kong Dan‐Dan , Xue Lu‐Sha , Jang Rui , Liu Bin , Meng Xiang‐Gao , Jin Shan , Ou Ya‐Ping , Hao Xiao , Liu Sheng‐Hua 
Published: May 2015

AbstractThe synthesis and characterization of a series of biphenyl‐derived binuclear ruthenium complexes with terminal {RuCl(CO)(PMe3)3} moieties and different structural arrangements of the phenyl rings are reported. Electrochemical studies revealed that the two metal centers of the binuclear ruthenium complexes interact with each other through the biphenyl bridge, and the redox splittings ΔE1/2 show a strong linear correlation with cos2 ϕ, where ϕ is the torsion angle between the two phenyl rings. A combination of electrochemical, UV/Vis/NIR, and in situ IR differential spectroelectrochemical analysis clearly showed that: 1) the intramolecular electronic couplings in the binuclear ruthenium complexes could be modulated by changing ϕ; 2) the electronic ground state of the mixed‐valent cations changes from delocalized to localized through the biphenyl bridge with increasing torsion angle ϕ, that is, the redox processes of these complexes change from significant involvement of the bridging ligand to an oxidation behavior with less participation of the bridge.
From the N‐Heterocyclic Carbene‐Catalyzed Conjugate Addition of Alcohols to the Controlled Polymerization of (Meth)acrylates
Authors: Ottou Winnie Nzahou , Bourichon Damien , Vignolle Joan , Wirotius Anne‐Laure , Robert Fredéric , Landais Yannick , Sotiropoulos Jean‐Marc , Miqueu Karinne , Taton Daniel 
Published: May 2015

AbstractAmong various N‐heterocyclic carbenes (NHCs) tested, only 1,3‐bis(tert‐butyl)imidazol‐2‐ylidene (NHCtBu) proved to selectively promote the catalytic conjugate addition of alcohols onto (meth)acrylate substrates. This rather rare example of NHC‐catalyzed 1,4‐addition of alcohols was investigated as a simple means to trigger the polymerization of both methyl methacrylate and methyl acrylate (MMA and MA, respectively). Well‐defined α‐alkoxy poly(methyl (meth)acrylate) (PM(M)A) chains, the molar masses of which could be controlled by the initial [(meth)acrylate]0/[ROH]0 molar ratio, were ultimately obtained in N,N‐dimethylformamide at 25 °C. A hydroxyl‐terminated poly(ethylene oxide) (PEO‐OH) macro‐initiator was also employed to directly access PEO‐b‐PMMA amphiphilic block copolymers. Investigations into the reaction mechanism by DFT calculations revealed the occurrence of two competitive concerted pathways, involving either the activation of the alcohol or that of the monomer by NHCtBu.
Probing the Catalytic Activity of Reduced Graphene Oxide Decorated with Au Nanoparticles Triggered by Visible Light
Authors: Wang Jiale , Trindade Fabiane J. , de Aquino Caroline B. , Pieretti Joana C. , Domingues Sergio H. , Ando Romulo A. , Camargo Pedro H. C. 
Published: May 2015

AbstractHybrid materials in which reduced graphene oxide (rGO) is decorated with Au nanoparticles (rGO–Au NPs) were obtained by the in situ reduction of GO and AuCl4−(aq) by ascorbic acid. On laser excitation, rGO could be oxidized as a result of the surface plasmon resonance (SPR) excitation in the Au NPs, which generates activated O2 through the transfer of SPR‐excited hot electrons to O2 molecules adsorbed from air. The SPR‐mediated catalytic oxidation of p‐aminothiophenol (PATP) to p,p′‐dimercaptoazobenzene (DMAB) was then employed as a model reaction to probe the effect of rGO as a support for Au NPs on their SPR‐mediated catalytic activities. The increased conversion of PATP to DMAB relative to individual Au NPs indicated that charge‐transfer processes from rGO to Au took place and contributed to improved SPR‐mediated activity. Since the transfer of electrons from Au to adsorbed O2 molecules is the crucial step for PATP oxidation, in addition to the SPR‐excited hot electrons of Au NPs, the transfer of electrons from rGO to Au contributed to increasing the electron density of Au above the Fermi level and thus the Au‐to‐O2 charge‐transfer process.
Heteroatom‐Guided, Palladium‐Catalyzed, Site‐Selective CH Arylation of 4H‐Chromenes: Diastereoselective Assembly of the Core Structure of Myristinin B through Dual CH Functionalization
Authors: Pawar Govind Goroba , Tiwari Virendra Kumar , Jena Himanshu Sekhar , Kapur Manmohan 
Published: May 2015

AbstractA highly site‐selective, heteroatom‐guided, palladium‐catalyzed direct arylation of 4H‐chromenes is reported. The CH functionalization is driven not only by the substituents and structure of the substrate but also by the coupling partner being used. The diastereoselective assembly of the core structure of Myristinin B has been achieved by using a dual CH functionalization strategy for regioselective direct arylation.
Phenyl Groups Result in the Highest Benzene Storage and Most Efficient Desulfurization in a Series of Isostructural Metal–Organic Frameworks
Authors: He Wen‐Wen , Yang Guang‐Sheng , Tang Yu‐Jia , Li Shun‐Li , Zhang Shu‐Ran , Su Zhong‐Min , Lan Ya‐Qian 
Published: May 2015

AbstractA series of isoreticular metal–organic frameworks (MOFs; NENU‐511–NENU‐514), which all have high surface areas and strong adsorption capacities, have been successfully constructed by using mixed ligands. NENU‐513 has the highest benzene capacity of 1687 mg g−1at 298 K, which ranks as the top MOF material among those reported up to now. This NENU series has been used for adsorptive desulfurization because of its permanent porosity. The results indicate that this series has a higher adsorptive efficiency in the removal of organosulfur compounds than other MOF materials, especially NENU‐511, which has the highest adsorptive efficiency in the ambient atmosphere. This study proves that the design and synthesis of targeted MOFs with higher surface areas and with functional groups present is an efficient method to enhance benzene‐storage capacity and the adsorption of organosulfur compounds.
Directional Dynamic Covalent Motion of a Carbonyl Walker on a Polyamine Track
Authors: Kovaříček Petr , Lehn Jean‐Marie 
Published: May 2015

AbstractControlled directional displacement of a molecular group has been achieved based on dynamic covalent motions implementing the reactional features of the imine bond.ortho‐Carboxybenzaldehyde derivatives are able to form stable adducts with both primary and secondary amines as imines or as amino lactones, respectively, depending on the acidity of the medium. They may thus perform pH‐driven intramolecular “walking” along a non‐symmetric polyamine chain, in which an imine serves as the terminus under basic conditions on one end of the chain and a lactone formed on a secondary hydroxylamine nitrogen on the other end serves as the terminal site upon addition of acid. The displacement between the termini occurs stochastically through reversible change in valency at the carbon site of the carbonyl group between imine, aminal, iminium and amino lactone form. On the other hand, the directionality results from the stabilisation of the terminal products under given pH conditions. By its ability to undergo interconversion between CN and O‐C‐N moieties, theortho‐carboxybenzaldehyde group extends the realm of dynamic covalent chemistry of imines to secondary amines and opens new perspectives in this field.
Copper‐Catalyzed γ‐Selective and Stereospecific Allylic Cross‐Coupling with Secondary Alkylboranes
Authors: Yasuda Yuto , Nagao Kazunori , Shido Yoshinori , Mori Seiji , Ohmiya Hirohisa , Sawamura Masaya 
Published: May 2015

AbstractThe scope of the copper‐catalyzed coupling reactions between organoboron compounds and allylic phosphates is expanded significantly by employing triphenylphosphine as a ligand for copper, allowing the use of secondary alkylboron compounds. The reaction proceeds with complete γ‐E‐selectivity and preferential 1,3‐syn stereoselectivity. The reaction of γ‐silicon‐substituted allylic phosphates affords enantioenriched α‐stereogenic allylsilanes.
Novel Xylene‐Linked Maltoside Amphiphiles (XMAs) for Membrane Protein Stabilisation
Authors: Cho Kyung Ho , Du Yang , Scull Nicola J. , Hariharan Parameswaran , Gotfryd Kamil , Loland Claus J. , Guan Lan , Byrne Bernadette , Kobilka Brian K. , Chae Pil Seok 
Published: May 2015

AbstractMembrane proteins are key functional players in biological systems. These biomacromolecules contain both hydrophilic and hydrophobic regions and thus amphipathic molecules are necessary to extract membrane proteins from their native lipid environments and stabilise them in aqueous solutions. Conventional detergents are commonly used for membrane protein manipulation, but membrane proteins surrounded by these agents often undergo denaturation and aggregation. In this study, a novel class of maltoside‐bearing amphiphiles, with a xylene linker in the central region, designated xylene‐linked maltoside amphiphiles (XMAs) was developed. When these novel agents were evaluated with a number of membrane proteins, it was found that XMA‐4 and XMA‐5 have particularly favourable efficacy with respect to membrane protein stabilisation, indicating that these agents hold significant potential for membrane protein structural study.
The Two‐Step Assemblies of Basic‐Amino‐Acid‐Rich Peptide with a Highly Charged Polyoxometalate
Authors: Zhang Teng , Li Hong‐Wei , Wu Yuqing , Wang Yizhan , Wu Lixin 
Published: May 2015

AbstractTwo‐step assembly of a peptide from HPV16 L1 with a highly charged europium‐substituted polyoxometalate (POM) cluster, accompanying a great luminescence enhancement of the inorganic polyanions, is reported. The mechanism is discussed in detail by analyzing the thermodynamic parameters from isothermal titration calorimetry (ITC), time‐resolved fluorescent and NMR spectra. By comparing the actions of the peptide analogues, a binding process and model are proposed accordingly. The driving forces in each binding step are clarified, and the initial POM aggregation, basic‐sequence and hydrophobic C termini of peptide are revealed to contribute essentially to the two‐step assembly. The present study demonstrates both a meaningful preparation for bioinorganic materials and a strategy using POMs to modulate the assembly of peptides and even proteins, which could be extended to other proteins and/or viruses by using peptides and POMs with similar properties.
ChemInform Abstract: Luminescence Matching with the Sensitivity Curve of the Human Eye: Optical Ceramics Mg8‐xMx(BN2)2N4 with M:Al (x:2) and M:Si (x:1).
Authors: Stroebele Markus , Dolabdjian Konstantin , Enseling David , Dutczak Danuta , Mihailova Boriana , Juestel Thomas , Meyer H.‐Juergen 
Published: May 2015

AbstractMg6Al2(BN2)2N4 (I) and Mg7Si(BN2)2N4 (II) are prepared by solid state metathesis reaction (1100 °C) of MgCl2, Li3(BN2), and AlN for (I) and of Mg3N2, BN, and Si3N4 for (II).
ChemInform Abstract: Blue‐Emitting K2Al2B2O7:Eu2+ Phosphor with High Thermal Stability and High Color Purity for Near‐UV‐Pumped White Light‐Emitting Diodes.
Authors: Xiao Wenge , Zhang Xia , Hao Zhendong , Pan Guo‐Hui , Luo Yongshi , Zhang Ligong , Zhang Jiahua 
Published: May 2015

AbstractK2Al2B2O7:Eu2+ phosphor is prepared by reaction of a stoichiometric HNO3 solution of Eu2O3, K2CO3, Al(NO3)3, and H3BO3 followed by drying and sintering in a reducing CO atmosphere (C sticks covered crucible, 1.