bluuebunny/crossref_metadata_2025 huggingface dataset:
Graphitized Carbon Fibers as Multifunctional 3D Current Collectors for High Areal Capacity Li Anodes
Authors: Zuo Tong‐Tong , Wu Xiong‐Wei , Yang Chun‐Peng , Yin Ya‐Xia , Ye Huan , Li Nian‐Wu , Guo Yu‐Guo
Published: June 2017

The Li metal anode has long been considered as one of the most ideal anodes due to its high energy density. However, safety concerns, low efficiency, and huge volume change are severe hurdles to the practical application of Li metal anodes, especially in the case of high areal capacity. Here it is shown that that graphitized carbon fibers (GCF) electrode can serve as a multifunctional 3D current collector to enhance the Li storage capacity. The GCF electrode can store a huge amount of Li via intercalation and electrodeposition reactions. The as‐obtained anode can deliver an areal capacity as high as 8 mA h cm−2 and exhibits no obvious dendritic formation. In addition, the enlarged surface area and porous framework of the GCF electrode result in lower local current density and mitigate high volume change during cycling. Thus, the Li composite anode displays low voltage hysteresis, high plating/stripping efficiency, and long lifespan. The multifunctional 3D current collector promisingly provides a new strategy for promoting the cycling lifespan of high areal capacity Li anodes.
Modulation of Metal and Insulator States in 2D Ferromagnetic VS2 by van der Waals Interaction Engineering
Authors: Guo Yuqiao , Deng Haitao , Sun Xu , Li Xiuling , Zhao Jiyin , Wu Junchi , Chu Wangsheng , Zhang Sijia , Pan Haibin , Zheng Xusheng , Wu Xiaojun , Jin Changqing , Wu Changzheng , Xie Yi
Published: June 2017

2D transition‐metal dichalcogenides (TMDCs) are currently the key to the development of nanoelectronics. However, TMDCs are predominantly nonmagnetic, greatly hindering the advancement of their spintronic applications. Here, an experimental realization of intrinsic magnetic ordering in a pristine TMDC lattice is reported, bringing a new class of ferromagnetic semiconductors among TMDCs. Through van der Waals (vdW) interaction engineering of 2D vanadium disulfide (VS2), dual regulation of spin properties and bandgap brings about intrinsic ferromagnetism along with a small bandgap, unravelling the decisive role of vdW gaps in determining the electronic states in 2D VS2. An overall control of the electronic states of VS2 is also demonstrated: bond‐enlarging triggering a metal‐to‐semiconductor electronic transition and bond‐compression inducing metallization in 2D VS2. The pristine VS2 lattice thus provides a new platform for precise manipulation of both charge and spin degrees of freedom in 2D TMDCs availing spintronic applications.
A Game Changer: A Multifunctional Perovskite Exhibiting Giant Ferroelectricity and Narrow Bandgap with Potential Application in a Truly Monolithic Multienergy Harvester or Sensor
Authors: Bai Yang , Tofel Pavel , Palosaari Jaakko , Jantunen Heli , Juuti Jari
Published: June 2017

An ABO3‐type perovskite solid‐solution, (K0.5Na0.5)NbO3 (KNN) doped with 2 mol% Ba(Ni0.5Nb0.5)O3−δ (BNNO) is reported. Such a composition yields a much narrower bandgap (≈1.6 eV) compared to the parental composition—pure KNN—and other widely used piezoelectric and pyroelectric materials (e.g., Pb(Zr,Ti)O3, BaTiO3). Meanwhile, it exhibits the same large piezoelectric coefficient as that of KNN (≈100 pC N−1) and a much larger pyroelectric coefficient (≈130 µC m−2 K−1) compared to the previously reported narrow‐bandgap material (KNbO3)1−x‐BNNOx. The unique combination of these excellent ferroelectric and optical properties opens the door to the development of multisource energy harvesting or multifunctional sensing devices for the simultaneous and efficient conversion of solar, thermal, and kinetic energies into electricity in a single material. Individual and comprehensive characterizations of the optical, ferroelectric, piezoelectric, pyroelectric, and photovoltaic properties are investigated with single and coexisting energy sources. No degrading interaction between ferroelectric and photovoltaic behaviors is observed. This composition may fundamentally change the working principles of state‐of‐the‐art hybrid energy harvesters and sensors, and thus significantly increases the unit‐volume energy conversion efficiency and reliability of energy harvesters in ambient environments.
Synthesis of Ultrathin PdCu Alloy Nanosheets Used as a Highly Efficient Electrocatalyst for Formic Acid Oxidation
Authors: Yang Nailiang , Zhang Zhicheng , Chen Bo , Huang Ying , Chen Junze , Lai Zhuangchai , Chen Ye , Sindoro Melinda , Wang An‐Liang , Cheng Hongfei , Fan Zhanxi , Liu Xiaozhi , Li Bing , Zong Yun , Gu Lin , Zhang Hua
Published: June 2017

Inspired by the unique properties of ultrathin 2D nanomaterials and excellent catalytic activities of noble metal nanostructures for renewable fuel cells, a facile method is reported for the high‐yield synthesis of ultrathin 2D PdCu alloy nanosheets under mild conditions. Impressively, the obtained PdCu alloy nanosheet after being treated with ethylenediamine can be used as a highly efficient electrocatalyst for formic acid oxidation. The study implicates that the rational design and controlled synthesis of an ultrathin 2D noble metal alloy may open up new opportunities for enhancing catalytic activities of noble metal nanostructures.
A Molecular Polycrystalline Ferroelectric with Record‐High Phase Transition Temperature
Authors: Pan Qiang , Liu Zhi‐Bo , Zhang Han‐Yue , Zhang Wan‐Ying , Tang Yuan‐Yuan , You Yu‐Meng , Li Peng‐Fei , Liao Wei‐Qiang , Shi Ping‐Ping , Ma Rong‐Wei , Wei Ru‐Yuan , Xiong Ren‐Gen
Published: June 2017

An outstanding advantage of inorganic ceramic ferroelectrics is their usability in the polycrystalline ceramic or thin film forms, which has dominated applications in the ferroelectric, dielectric, and piezoelectric fields. Although the history of ferroelectrics began with the molecular ferroelectric Rochelle salt in 1921, so far there have been very few molecular ferroelectrics, with lightweight, flexible, low‐cost, and biocompatible superior properties compared to inorganic ceramic ferroelectrics, that can be applied in the polycrystalline form. Here, a multiaxial molecular ferroelectric, guanidinium perchlorate ([C(NH2)3]ClO4), with a record‐high phase transition temperature of 454 K is presented. It is the rectangular polarization–electric field (P–E) hysteresis loops recorded on the powder and thin film samples (with respective large Pr of 5.1 and 8.1 µC cm−2) that confirm the ferroelectricity of [C(NH2)3]ClO4 in the polycrystalline states. Intriguingly, after poling, the piezoelectric coefficient (d33) of the powder sample shows a significant increase from 0 to 10 pC N−1, comparable to that of LiNbO3 single crystal (8 pC N−1). This is the first time that such a phenomenon has been observed in molecular ferroelectrics, indicating the great potential of molecular ferroelectrics being used in the polycrystalline form like inorganic ferroelectrics, as well as being viable alternatives or supplements to conventional ceramic ferroelectrics.
Electric‐Field‐Controlled Dopant Distribution in Organic Semiconductors
Authors: Müller Lars , Rhim Seon‐Young , Sivanesan Vipilan , Wang Dongxiang , Hietzschold Sebastian , Reiser Patrick , Mankel Eric , Beck Sebastian , Barlow Stephen , Marder Seth R. , Pucci Annemarie , Kowalsky Wolfgang , Lovrincic Robert
Published: June 2017

Stable electrical doping of organic semiconductors is fundamental for the functionality of high performance devices. It is known that dopants can be subjected to strong diffusion in certain organic semiconductors. This work studies the impact of operating conditions on thin films of the polymer poly(3‐hexylthiophene) (P3HT) and the small molecule Spiro‐MeOTAD, doped with two differently sized p‐type dopants. The negatively charged dopants can drift upon application of an electric field in thin films of doped P3HT over surprisingly large distances. This drift is not observed in the small molecule Spiro‐MeOTAD. Upon the dopants’ directional movement in P3HT, a dedoped region forms at the negatively biased electrode, increasing the overall resistance of the thin film. In addition to electrical measurements, optical microscopy, spatially resolved infrared spectroscopy, and scanning Kelvin probe microscopy are used to investigate the drift of dopants. Dopant mobilities of 10−9 to 10−8 cm2 V−1 s−1 are estimated. This drift over several micrometers is reversible and can be controlled. Furthermore, this study presents a novel memory device to illustrate the applicability of this effect. The results emphasize the importance of dynamic processes under operating conditions that must be considered even for single doped layers.
A Supramolecular Artificial Light‐Harvesting System with an Ultrahigh Antenna Effect
Authors: Li Jing‐Jing , Chen Yong , Yu Jie , Cheng Ni , Liu Yu
Published: June 2017

An efficient artificial light‐harvesting system is fabricated from a cyclic polysaccharide, sulfato‐β‐cyclodextrin (SCD); an aggregation‐induced emission molecule, an oligo(phenylenevinylene) derivative (OPV‐I); and a fluorescent dye, nile red (NiR), via noncovalent interactions in an aqueous solution. In this system, the OPV‐I/SCD supramolecular assembly acts as a donor, and NiR that is loaded into the OPV‐I/SCD assembly acts as an acceptor. Significantly, an efficient energy‐transfer process occurs between the OPV‐I/SCD assembly and the loaded NiR, leading to an extremely high antenna effect.
All‐Dielectric Heterogeneous Metasurface as an Efficient Ultra‐Broadband Reflector
Authors: Yao Yuhan , Wu Wei
Published: June 2017

Conventional all‐dielectric metasurfaces made from high‐index and low‐loss materials (such as Si or GaAs) can achieve high optical efficiencies as well as broadband characteristics, mostly for the infrared (IR) light. However, maintaining the bandwidth and efficiency for conventional all‐dielectric metasurfaces for visible or near‐IR light becomes challenging, due to the limitations from material selection as well as fabrication techniques. In this paper, the idea of heterogeneous all‐dielectric metasurfaces is proposed for a better metasurface design in shorter‐wavelength ranges. An ultra‐broadband reflector, as a proof‐of‐principle demonstration, is presented in this paper, both numerically and experimentally. The broadband reflector demonstrates a good optical efficiency, a broadband reflectance, as well as a great manufacturability. Nanoimprint lithography patterning process and advanced etching recipes are developed for the large‐area and low‐cost heterogeneous metasurface fabrication.
Broadband Nonlinear Optical Response in Few‐Layer Antimonene and Antimonene Quantum Dots: A Promising Optical Kerr Media with Enhanced Stability
Authors: Lu Lu , Tang Xian , Cao Rui , Wu Leiming , Li Zhongjun , Jing Guanghui , Dong Biqin , Lu Shunbin , Li Ying , Xiang Yuanjiang , Li Jianqing , Fan Dianyuan , Zhang Han
Published: June 2017

Antimonene, a new type of 2D group‐VA material beyond phosphorene, is theoretically predicted to exhibit remarkable electronics and optical properties with enhanced stability. However, its more general and practical applications seriously lag behind due to a shortage of effective synthesis techniques in delivering high‐quality few‐layer antimonene (FLA) and antimonene quantum dots (AQDs), and deep understanding of the mechanism in light‐antimonene interaction. Herein, based on electrochemical exfoliation and sonochemical approaches, FLA is synthesized with an average thickness down to 31.6 nm and AQDs with an average lateral size of 3.4 nm, and the corresponding nonlinear optical response is further investigated at the visible wavelength for the first time. It is shown that antimonene possesses a giant nonlinear refractive index of ≈10−5 cm2 W−1 and a high stability in ambient condition for months. The experimental findings may be considered as an important step toward antimonene‐based nonlinear photonics devices (Optical Switcher, Kerr shutter, beam shaper, etc.), in which their unstable counterpart phosphorene may not compete with.
Effect of strain‐induced crystallization on the tear strength of natural rubber/styrene butadiene rubber blend
Authors: Noguchi Fumitoshi , Zhou Yuanbing , Kosugi Kenichiro , Yamamoto Yoshimasa , Nghia Phan Trung , Fukuda Masao , Kawahara Seiichi
Published: June 2017

Strain‐induced crystallization of natural rubber (NR) can greatly influence the mechanical properties of NR blends. In this study, we investigated the effect of strain‐induced crystallization on the tear energy (G) of NR/styrene butadiene rubber (SBR) blends with different compositions and cross‐link densities. Using a shift factor, we could superimpose G of an SBR blend and an NR/SBR (1/9) blend onto a single master curve. In contrast, G of NR was split into two master curves. Although the master curve of G for the NR/SBR (3:7) blend was split, increasing the cross‐link density threefold made it possible to superimpose it onto a single master curve. Strain‐induced crystallization of NR in the NR/SBR blend did not occur as a result of decreasing the NR content, increasing the cross‐link density, or removing fatty acids. Together, these findings indicate that strain‐induced crystallization of NR plays an important role in the mechanical properties of the blend.
Supramolecular Approaches to Improve the Performance of Ruthenium‐Based Water Oxidation Catalysts
Authors: Kunz Valentin , Schmidt David , Röhr Merle I. S. , Mitrić Roland , Würthner Frank
Published: June 2017

Supramolecular principles have been widely applied to enhance the activity of homogeneous ruthenium‐based water oxidation catalysts. For catalytic systems in which the OO bond is formed via radical coupling of two metal oxyl subunits, self‐assembly of mononuclear catalysts into vesicles or fibrous aggregates can be used to improve the interaction of two catalytic centers. Similarly, the catalytic subunits can be brought into spatial proximity by coordination chemistry, which allows the construction of highly efficient metallosupramolecular multinuclear structures. However, if the OO bond is formed by the nucleophilic attack of water at a metal oxide species, the interaction of the catalytic center with substrate water molecules has to be improved. Here, by introducing tailored ligand systems, the second coordination sphere can be adjusted specifically to preorganize water for OO bond formation whereas the implementation of proton accepting residues can be used to lower the activation barrier of crucial proton‐coupled reaction steps. In a particularly outstanding example, both principles were combined in a multinuclear metallosupramolecular macrocycle.
A heterozygous microdeletion of 20p12.2–3 encompassing PROKR2 and BMP2 in a patient with congenital hypopituitarism and growth hormone deficiency
Authors: Parsons Samuel J. H. , Wright Neville B. , Burkitt‐Wright Emma , Skae Mars S. , Murray Phillip G.
Published: June 2017

Congenital growth hormone deficiency is a rare disorder with an incidence of approximately 1 in 4,000 live births. Pituitary development is under the control of a multitude of spatiotemporally regulated signaling molecules and transcription factors. Mutations in the genes encoding these molecules can result in hypopituitarism but for the majority of children with congenital hypopituitarism, the aetiology of their disease remains unknown. The proband is a 5‐year‐old girl who presented with neonatal hypoglycaemia and prolonged jaundice. No definitive endocrine cause of hypoglycaemia was identified in the neonatal period. She was born of normal size at 42 weeks but demonstrated growth failure with a progressive reduction in height to −3.2 SD by age 4.5 years and failed a growth hormone stimulation test with a peak growth hormone of 4.2 mcg/L. MRI of the pituitary gland demonstrated a hypoplastic anterior lobe and ectopic posterior lobe. Array CGH demonstrated an inherited 0.2 Mb gain at 1q21.1 and a de novo 4.8 Mb heterozygous deletion at 20p12.2–3. The deletion contained 17 protein coding genes including PROKR2 and BMP2, both of which are expressed during embryological development of the pituitary gland. PROKR2 mutations have been associated with hypopituitarism but a heterozygous deletion of this gene with hypopituitarism is a novel observation. In conclusion, congenital hypopituitarism can be present in individuals with a 20p12.3 deletion, observed with incomplete penetrance. Array CGH may be a useful investigation in select cases of early onset growth hormone deficiency, and patients with deletions within this region should be evaluated for pituitary hormone deficiencies.
Co‐occurrence of Jalili syndrome and muscular overgrowth
Authors: Wawrocka Anna , Walczak‐Sztulpa Joanna , Badura‐Stronka Magdalena , Owecki Michal , Kopczynski Przemysław , Mrukwa‐Kominek Ewa , Skorczyk‐Werner Anna , Gasperowicz Piotr , Ploski Rafal , Krawczynski Maciej R.
Published: June 2017

Jalili syndrome is a rare disorder inherited in an autosomal recessive pattern manifesting as a combination of cone‐rod dystrophy including progressive loss of visual acuity, color blindness, photophobia, and amelogenesis imperfecta with hypoplastic, immature, or hypocalcified dental enamel. It is caused by mutations in CNNM4, which encodes the ancient conserved domain protein 4. Here we report three brothers with Jalili syndrome and muscle overgrowth of the legs. Myopathic changes were found in needle electromyography. Mutational analysis showed in all three brothers a novel likely pathogenic homozygous missense substitution in exon 1 (c.1076T>C, p.(Leu359Pro)) of CNNM4. Both parents were carriers for the variant. In order to exclude other causative variants that could modify the patients’ phenotype we performed exome sequencing and MLPA analysis of the DMD gene in Patient 1. These analyses did not identify any additional variants. Our results expand the mutational spectrum associated with Jalili syndrome and suggest that mild myopathy with muscle overgrowth of the legs could be a newly identified manifestation of the disorder.
Electrically Activated Conductivity and White Light Emission of a Hydrocarbon Nanoring–Iodine Assembly
Authors: Ozaki Noriaki , Sakamoto Hirotoshi , Nishihara Taishi , Fujimori Toshihiko , Hijikata Yuh , Kimura Ryuto , Irle Stephan , Itami Kenichiro
Published: June 2017

Numerous otherwise difficult applications have been realized with materials, the chemical/physical properties of which can be controlled by external stimuli such as heat, pressure, photo‐irradiation, and voltage bias. However, the complexity of design and the lack of easy‐to‐conduct synthetic methods make the creation of on‐demand stimuli responsive materials a formidable task. Here we report an electric‐stimuli‐responsive multifunctional material, [10]CPP‐I: crystalline assembly of a hydrocarbon nanoring ([10]cycloparaphenylene: [10]CPP) as an “electro‐responsive porous host” and iodine as a “potentially functional molecule”. Through applying electric stimulus, [10]CPP‐I turned to exhibit two attractive properties: electronic conductivity and white light emission. We revealed that electric stimuli trigger the cascade formation of polyiodide chains inside the [10]CPP assembly through charge transfer, leading to the emergence of these properties. This “responsive porous host” approach is expected to be applicable for different stimuli, and opens the path for devising a generic strategy to the development of stimuli‐responsive materials.
Automated Quantum Mechanical Predictions of Enantioselectivity in a Rhodium‐Catalyzed Asymmetric Hydrogenation
Authors: Guan Yanfei , Wheeler Steven E.
Published: June 2017

A computational toolkit (AARON: An automated reaction optimizer for new catalysts) is described that automates the density functional theory (DFT) based screening of chiral ligands for transition‐metal‐catalyzed reactions with well‐defined reaction mechanisms but multiple stereocontrolling transition states. This is demonstrated for the Rh‐catalyzed asymmetric hydrogenation of (E)‐β‐aryl‐N‐acetyl enamides, for which a new C2‐symmetric phosphorus ligand is designed.
Capturing Elusive Cobaltacycle Intermediates: A Real‐Time Snapshot of the Cp*CoIII‐Catalyzed Oxidative Alkyne Annulation
Authors: Sanjosé‐Orduna Jesús , Gallego Daniel , Garcia‐Roca Alèria , Martin Eddy , Benet‐Buchholz Jordi , Pérez‐Temprano Mónica H.
Published: June 2017

Despite Cp*CoIII catalysts having emerged as a very attractive alternative to noble transition metals for the construction of heterocyclic scaffolds through C−H activation, the structure of the reactive species remains uncertain. Herein, we report the identification and unambiguous characterization of two long‐sought cyclometalated Cp*CoIII complexes that have been proposed as key intermediates in C−H functionalization reactions. The addition of MeCN as a stabilizing ligand plays a crucial role, allowing the access to otherwise highly reactive species. Mechanistic investigations demonstrate the intermediacy of these species in oxidative annulations with alkynes, including the direct observation, under catalytic conditions, of a previously elusive post‐migratory insertion seven‐membered cobaltacycle.
Preparation of Solid Polyfunctional Alkynylzinc Pivalates with Enhanced Air and Moisture Stability for Organic Synthesis
Authors: Chen Yi‐Hung , Tüllmann Carl Phillip , Ellwart Mario , Knochel Paul
Published: June 2017

We report the preparation of solid and air‐stable polyfunctionalized alkynylzinc pivalates from the corresponding alkynes using TMPZnOPiv (TMP=2,2,6,6‐tetramethylpiperidyl) as base. These organozinc pivalates are obtained as powders under mild conditions in excellent yields and can be manipulated in air for several hours without significant decomposition. These zinc reagents show an excellent reactivity in various carbon–carbon bond‐ forming reactions and 1,3‐dipolar cycloadditions. An alkynylzinc pivalate has been used to prepare a carboxyamidotriazole with potential antineoplastic activity in eight steps and 38 % overall yield.
Fe3O4–cysteamine hydrochloride magnetic nanoparticles: New, efficient and recoverable nanocatalyst for Knoevenagel condensation reaction
Authors: Maleki Razieh , Kolvari Eskandar , Salehi Mehdi , Koukabi Nadiya
Published: June 2017

Fe3O4 magnetic nanoparticles (MNPs) were obtained using a reduction–precipitation method. These MNPs were modified with cysteamine hydrochloride. This catalyst was characterized using a number of physicochemical measurements. The Fe3O4–cysteamine MNPs, as an efficient and heterogeneous catalyst, were successfully used for Knoevenagel condensation under mild conditions. The activity of this nanomagnetic catalyst in the Knoevenagel condensation of aromatic aldehydes and malononitrile is described. Easy preparation of the catalyst, easy work‐up procedure, excellent yields and short reaction times are some of the advantages.
Improvement of thermal ageing and transparency of methacrylate based poly(siloxane–silsesquioxane) for optoelectronic application
Authors: Loh T. C. , Ng C. M. , Kumar R. N. , Ismail H. , Ahmad Z.
Published: June 2017

Trisilanolphenyl–polyhedral oligosilsesquioxane (trisilanolphenyl–POSS) structure is introduced into a polysiloxane network in an attempt to produce thermally stable material with improved transparency. A series of organic–inorganic resins comprised of diphenylsilanediol, 3‐methacryloxypropyl trimethoxysilane, and varying content of trisilanolphenyl–POSS were copolymerized through condensation followed by curing using phenyltris(hydrogendimethylsiloxy)silane as curing agent. Fourier transform infrared spectroscopy (FTIR), proton‐nuclear magnetic resonance spectroscopy (1H‐NMR), and silicon‐nuclear magnetic resonance spectroscopy (29Si‐NMR) were used to confirm the synthesized product. Excellent thermal stability, improved glass transition temperature (Tg), and lower coefficient of thermal expansion with the increasing POSS content were observed from thermomechanical analysis. Its extreme thermal degradation stability was attributable to the crosslinked network as well as the heavily substituted aromatic ring present in the system. Steric hindrance effect is noticeable beyond 5.66 mol % trisilanolphenyl–POSS content. Incorporation of POSS substituent in methacrylate‐based polysiloxane give excellent transparency and improved thermal discoloration resistance as deduced from UV/vis Spectrophotometer, making it a potential material to be used in optoelectronics. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 45285.
Poly(ɛ‐caprolactone) nanocomposites with layered double hydroxides modified by in situ grafting polymerization: Structure characterization and barrier properties
Authors: Mao Long , Liu Yue‐Jun , Bai Yong‐Kang , Wu Hui‐Qing , Liu Xiao‐Chao
Published: June 2017

The synthesis of multimetallic layered double hydroxides‐g‐poly(ɛ‐caprolactone) (LDHs‐g‐PCL) was explored by in situ ring‐opening polymerization, considering layered clay's improvement on barrier properties in polymer films. LDHs/PCL nanocomposites were prepared by blending LDHs‐g‐PCL and pure PCL via solution casting method. With incorporation of as low as 0.2 wt % of LDHs, LDHs/PCL nanocomposites exhibited excellent mechanical performance with tensile strength and elongation at break over 45 MPa and 837%, respectively. Compared with pure PCL, the O2 permeability of LDHs/PCL nanocomposites decreased by nearly 78% as LDHs content increased up to 1 wt %. It was revealed that the key parameter to improve the barrier properties is not only the high aspect ratio of layered clays but also the specific interactions that they develop in the polymers matrix. Due to the merits of its biodegradation and physical properties, LDHs/PCL nanocomposites could be potential materials applied in packaging industry widely. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 45320.
Characteristics of poly(vinyl alcohol) films crosslinked by cinnamaldehyde with improved transparency and water resistance
Authors: Gao Hongfang , Yang Hui
Published: June 2017

Poly(vinyl alcohol) (PVA) films crosslinked by cinnamaldehyde (CIN) at various concentrations were prepared. Their physicochemical and antibacterial properties were compared with those of uncrosslinked films. The results suggest that the crosslinked films exhibited higher transparency, tensile strength, and elongation at break in a certain CIN concentration range. They also displayed decreased water vapor permeability and water solubility. Although the antibacterial activity of the crosslinked film‐forming solution was less slightly than that of the uncrosslinked film‐forming solution, the crosslinked film‐forming solution still demonstrated strong antibacterial activity when the concentration of CIN was 2% v/v. The aldol condensation reaction between the aldehyde group of CIN and the alcoholic hydroxyl group of PVA was determined by Fourier transform infrared spectroscopy. By the crosslinking reaction, the heat stability of the crosslinked film was enhanced compared with that of the uncrosslinked film. Meanwhile, a compact, smooth, and continuous cross‐sectional microstructure present in the crosslinked film was observed by scanning electron microscopy. The higher water resistance and transparency gave the crosslinked films priority for use in food packaging. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 45324.
Delivery of dsRNA through topical feeding for RNA interference in the citrus sap piercing‐sucking hemipteran, Diaphorina citri
Authors: Killiny Nabil , Kishk Abdelaziz
Published: June 2017

RNA interference (RNAi) is a powerful means to study functional genomics in insects. The delivery of dsRNA is a challenging step in the development of RNAi assay. Here, we describe a new delivery method to increase the effectiveness of RNAi in the Asian citrus psyllid Diaphorina citri. Bromophenol blue droplets were topically applied to fifth instar nymphs and adults on the ventral side of the thorax between the three pairs of legs. In addition to video recordings that showed sucking of the bromophenol blue by the stylets, dissected guts turned blue indicating that the uptake was through feeding. Thus, we called the method topical feeding. We targeted the abnormal wing disc gene (awd), also called nucleoside diphosphate kinase (NDPK), as a reporter gene to prove the uptake of dsRNA via this method of delivery. Our results showed that dsRNA‐awd caused reduction of awd expression and nymph mortality. Survival and lifespan of adults emerged from treated nymphs and treated adults were affected. Silencing awd caused wing malformation in the adults emerged from treated nymphs. Topical feeding as a delivery of dsRNA is highly efficient for both nymphs and adults. The described method could be used to increase the efficiency of RNAi in D. citri and other sap piercing‐sucking hemipterans.
2017 American College of Rheumatology Guideline for the Prevention and Treatment of Glucocorticoid‐Induced Osteoporosis
Authors: Buckley Lenore , Guyatt Gordon , Fink Howard A. , Cannon Michael , Grossman Jennifer , Hansen Karen E. , Humphrey Mary Beth , Lane Nancy E. , Magrey Marina , Miller Marc , Morrison Lake , Rao Madhumathi , Robinson Angela Byun , Saha Sumona , Wolver Susan , Bannuru Raveendhara R. , Vaysbrot Elizaveta , Osani Mikala , Turgunbaev Marat , Miller Amy S. , McAlindon Timothy
Published: June 2017

Objective

To develop recommendations for prevention and treatment of glucocorticoid‐induced osteoporosis (GIOP).

Methods

We conducted a systematic review to synthesize the evidence for the benefits and harms of GIOP prevention and treatment options. The Grading of Recommendations Assessment, Development and Evaluation methodology was used to rate the quality of evidence. We used a group consensus process to determine the final recommendations and grade their strength. The guideline addresses initial assessment and reassessment in patients beginning or continuing long‐term (≥3 months) glucocorticoid (GC) treatment, as well as the relative benefits and harms of lifestyle modification and of calcium, vitamin D, bisphosphonate, raloxifene, teriparatide, and denosumab treatment in the general adult population receiving long‐term GC treatment, as well as in special populations of long‐term GC users.

Results

Because of limited evidence regarding the benefits and harms of interventions in GC users, most recommendations in this guideline are conditional (uncertain balance between benefits and harms). Recommendations include treating only with calcium and vitamin D in adults at low fracture risk, treating with calcium and vitamin D plus an additional osteoporosis medication (oral bisphosphonate preferred) in adults at moderate‐to‐high fracture risk, continuing calcium plus vitamin D but switching from an oral bisphosphonate to another antifracture medication in adults in whom oral bisphosphonate treatment is not appropriate, and continuing oral bisphosphonate treatment or switching to another antifracture medication in adults who complete a planned oral bisphosphonate regimen but continue to receive GC treatment. Recommendations for special populations, including children, people with organ transplants, women of childbearing potential, and people receiving very high‐dose GC treatment, are also made.

Conclusion

This guideline provides direction for clinicians and patients making treatment decisions. Clinicians and patients should use a shared decision‐making process that accounts for patients’ values, preferences, and comorbidities. These recommendations should not be used to limit or deny access to therapies.
Does it matter how you play? The effects of collaboration and competition among players of human computation games
Authors: Pe‐Than Ei Pa Pa , Goh Dion Hoe‐Lian , Lee Chei Sian
Published: June 2017

Human computation games (HCGs) harness human intelligence through enjoyable gameplay to address computational problems that are beyond the power of computer programs but trivial for humans. With the popularity of crowdsourcing, different types of HCGs have been developed using various gameplay mechanics to attract online users to contribute outputs. Two commonly used mechanics are collaboration and competition. Yet there is little research examining whether HCGs perform better than nongame applications in terms of motivations and perceptions. Thus, this study investigates the effects of collaborative and competitive mechanics on intrinsic motivation and perceived output quality in mobile content sharing HCGs. Using a within‐subjects experiment, 160 participants were recruited from 2 local universities. The findings suggest that the nongame application was perceived to yield better quality output than both HCGs, but the latter offered a greater satisfaction of motivational needs, which may motivate individuals to continue playing them. Taken together, the present findings inform researchers and designers of HCGs that games could serve as a motivator to encourage participation. However, the usefulness of HCGs may be dependent on how one can effectively manage the entertainment–output generation duality of such games. This article concludes by presenting implications, limitations, and future research directions.
Strongly Luminescent Cyclometalated Gold(III) Complexes Supported by Bidentate Ligands Displaying Intermolecular Interactions and Tunable Emission Energy
Authors: Chan Kaai Tung , Tong Glenna So Ming , Wan Qingyun , Cheng Gang , Yang Chen , Che Chi‐Ming
Published: June 2017

A series of charge‐neutral AuIII complexes, which comprise a dicarbanionic C‐deprotonated biphenyl ligand and bidentate ancillary ligands ([Au(C^C)(L^X)]; L^X=β‐diketonate and relatives (O^O), quinolinolate and relatives (N^O), and diphosphino (P^P) ligands), were prepared. All the complexes are emissive in degassed CH2Cl2 solutions and in thin‐film samples with Φem up to 18 and 35 %, respectively, except for 5 and 6, which bear (N^O)‐type ancillary ligands. Variation of the electronic characteristics of the β‐diketonate ancillary ligand was demonstrated to be a viable route for tuning the emission color from blue‐green (peak λem at ca. 466 nm for 1 and 2; 501 nm for 4 a and 4 b) to orange (peak λem at 585 nm for 3), in contrast to the common observations that the ancillary ligand has a negligible effect on the excited‐state energy of the AuIII complexes reported in the literature. DFT/time‐dependent (TD) DFT calculations revealed that the energies of the 3ππ*(C^C) and the 3ILCT(O^O) excited states (ILCT=intraligand charge transfer) switch in order on going from O^O=acetylacetonate (acac) to aryl‐substituted β‐diketonate ligands. Solution‐processed and vacuum‐deposited organic light‐emitting diode (OLED) devices of selected complexes were prepared. The vacuum‐deposited OLED fabricated with 2 displays a sky‐blue emission with a maximum external quantum efficiency (EQE) of 6.71 % and CIE coordinates of (0.22, 0.40). The crystal structures of 7 and 9 reveal short intermolecular AuIII⋅⋅⋅AuIII contacts, with intermetal distances of 3.408 and 3.453 Å, respectively. DFT/TDDFT calculations were performed on 7 and 9 to account for the noncovalent interactions. Solid samples of 1, 3, and 9 exhibit excimeric emission at room temperature, which is rarely reported in AuIII complexes.
A DNA‐Based Label‐Free Artificial Tongue for Pattern Recognition of Metal Ions
Authors: Qiu Hao , Pu Fang , Ran Xiang , Ren Jinsong , Qu Xiaogang
Published: June 2017

An array‐based sensing method offers several advantages for detecting various analytes. DNA molecules as sensor elements have attracted considerable interest owing to their unique properties. Here, a label‐free sensor array using DNA and commercially available dyes to differentiate metal ions is reported. Based on the different interactions between dye‐bound DNA and metal ions, the fluorescence intensities of the sensor elements are changed to different degrees. In this way, fourteen metal ions can be efficiently distinguished by principal component analysis (PCA) and hierarchical cluster analysis (HCA). A highly sensitive discrimination of metal ions with 92.8 % identification accuracy can be achieved. The present work provides a simple and convenient method for the construction of a DNA‐based sensor array.
Process control performance evaluation in the case of variable set‐point with experimental applications
Authors: Bacci di Capaci Riccardo , Scali Claudio
Published: June 2017

The purpose of this paper is to contribute with some refinements to recent methods of analysis of control loop performance, based on the well‐established principle of Internal Model Control (IMC). Lower limits for the absolute value of the integral of control error (IAE) and the total variation of control action (TV) are assumed as reference values for a control considered good or at least acceptable. The overall performance index assumes as a benchmark a controller tuned according to rules of S(implified)IMC technique and is appropriately defined with respect to the lower limits of the two metrics IAE and TV. This allows the assessment of control loop performance, that is, the validity of tuning for PID‐type controllers in response to different types of reference change. In fact, one can assess performance in the case of set‐point changes as steps, ramps, or generic varying trends over time. In order to demonstrate the validity of the refined technique, several examples of simulation, case studies on a pilot plant, and real industrial data are presented.
Obstructive sleep apnea is associated with increased readmission in heart failure patients
Authors: Sommerfeld Alex , Althouse Andrew D. , Prince Jennifer , Atwood Charles W. , Mulukutla Suresh R. , Hickey Gavin W.
Published: June 2017

Background

Heart failure (HF) readmission rates have become an increasingly important quality metric since the advent of the Hospital Readmissions Reduction Program. Despite many well‐intentioned efforts to reduce readmissions, clinicians continue to struggle with the problem of high HF readmission rates.

Hypothesis

HF patients with obstructive sleep apnea (OSA) will have higher burden of rehospitalization and mortality than HF patients without OSA.

Methods

Our study included 344 patient encounters (among 271 unique patients) with a diagnosis of HF from September 2014 through September 2015. Our primary endpoints were all‐cause readmission within 30 and 90 days. Multivariate logistic regression was used to assess the relationship between OSA and readmission when accounting for potential confounders.

Results

The patients’ were 72 ± 10 years old, and predominantly white (76.2%) and male (99.4%). Among the 344 patient encounters, 247 (71.8%) had diagnosed coronary artery disease, 159 (46.2%) had atrial fibrillation, and 99 (28%) had obstructive sleep apnea (OSA). Notably, patients with OSA had an elevated rate of readmission within 30 days (OSA: 30.3% vs no OSA: 19.6%, P = 0.037) and within 90 days (OSA: 57.6% vs no OSA: 36.3P < 0.01). Patients with OSA had increased risk of readmission within 90 days (odds ratio: 2.38, 95% confidence interval: 1.47‐3.83, P < 0.01) even after adjustment for potential confounders of age, race, obesity, diabetes, and chronic obstructive pulmonary disease.

Conclusions

HF patients with OSA have an elevated rate of readmission compared to the general HF population, particularly within the first 90 days after discharge.
2,6‐Difluorobenzamide Inhibitors of Bacterial Cell Division Protein FtsZ: Design, Synthesis, and Structure–Activity Relationships
Authors: Straniero Valentina , Zanotto Carlo , Straniero Letizia , Casiraghi Andrea , Duga Stefano , Radaelli Antonia , De Giuli Morghen Carlo , Valoti Ermanno
Published: June 2017

A wide variety of drug‐resistant microorganisms are continuously emerging, restricting the therapeutic options for common bacterial infections. Antimicrobial agents that were originally potent are now no longer helpful, due to their weak or null activity toward these antibiotic‐resistant bacteria. In addition, none of the recently approved antibiotics affect innovative targets, resulting in a need for novel drugs with innovative antibacterial mechanisms of action. The essential cell division protein filamentous temperature‐sensitive Z (FtsZ) has emerged as a possible target, thanks to its ubiquitous expression and its homology to eukaryotic β‐tubulin. In the latest years, several compounds were shown to interact with this prokaryotic protein and selectively inhibit bacterial cell division. Recently, our research group developed interesting derivatives displaying good antibacterial activities against methicillin‐resistant Staphylococcus aureus, as well as vancomycin‐resistant Enterococcus faecalis and Mycobacterium tuberculosis. The aim of the present study was to summarize the structure–activity relationships of differently substituted heterocycles, linked by a methylenoxy bridge to the 2,6‐difluorobenzamide, and to validate FtsZ as the real target of this class of antimicrobials.
1H NMR application in characterizing the refinery products of gasoline
Authors: Sun Cheng , Wang Zhixiao
Published: June 2017

We report on an application of 1H NMR spectroscopy in characterizing the gasoline properties of its refinery products. In this work, a variety of gasoline samples obtained from different refinery stages are studied, and the aromatic, olefin, and paraffin contents as well as the octane number (ON) of the gasoline samples are characterized by 1H NMR. The properties of two product gasoline samples are also studied by 1H NMR spectroscopy; the NMR‐determined values for the ONs are compared with the research octane number values measured in a standard test engine, and a good agreement is achieved. This work indicates that the characteristics of gasoline can be revealed by 1H NMR, and the values derived from the NMR spectroscopy can be used to assess the gasoline quality during its refinery processes. Based on this work, we demonstrate that the 1H NMR spectroscopy is a convenient tool in the continuous monitoring of the refinery processes of gasoline.
A task‐based approach for finding SCCs in real‐world graphs on external memory
Authors: Lv Huiming , Shao Zhiyuan , Li Lang , Shi Xuanhua , Jin Hai
Published: June 2017

Finding strongly connected components (SCCs) in graphs is one of the important research topics of graph data mining. Traditional SCC‐finding methods need to load the whole graph into main memory before actual processing, which makes them inappropriate to process today's large graphs. Although it is cost‐effective to conductive SCC‐finding in the external memory (EM) graph processing systems, existing EM systems are still inefficient on such workload for 2 reasons: data‐parallel processing model and inefficient graph mutation mechanism.

In this paper, we propose a task‐based approach, named as TAS, for finding SCCs in large real‐world graphs. TAS encapsulates individual graph dataset and the SCC‐finding algorithms conducted on it as an independent task. By this strategy, different algorithms can be assigned to different datasets according to the stage of processing or the size of the dataset. By gradually removing unneeded data, ie, the known SCCs, with an efficient graph mutation method, TAS continuously reduces the scale of the problem to accelerate processing. Performance evaluation on large real‐world graphs show that TAS greatly outperforms existing EM solutions on finding SCCs (eg, 55.2x faster than GraphChi and 40.3x faster than X‐Stream).
A framework for dense triangular matrix kernels on various manycore architectures
Authors: Charara Ali , Keyes David , Ltaief Hatem
Published: June 2017

We present a new high‐performance framework for dense triangular Basic Linear Algebra Subroutines (BLAS) kernels, ie, triangular matrix‐matrix multiplication (TRMM) and triangular solve (TRSM), on various manycore architectures. This is an extension of a previous work on a single GPU by the same authors, presented at the EuroPar'16 conference, in which we demonstrated the effectiveness of recursive formulations in enhancing the performance of these kernels. In this paper, the performance of triangular BLAS kernels on a single GPU is further enhanced by implementing customized in‐place CUDA kernels for TRMM and TRSM, which are called at the bottom of the recursion. In addition, a multi‐GPU implementation of TRMM and TRSM is proposed and we show an almost linear performance scaling, as the number of GPUs increases. Finally, the algorithmic recursive formulation of these triangular BLAS kernels is in fact oblivious to the targeted hardware architecture. We, therefore, port these recursive kernels to homogeneous x86 hardware architectures by relying on the vendor optimized BLAS implementations. Results reported on various hardware architectures highlight a significant performance improvement against state‐of‐the‐art implementations. These new kernels are freely available in the KAUST BLAS (KBLAS) open‐source library at https://github.com/ecrc/kblas.
Effect of addition of different antisolvents on the crystallization of aqueous ammonium dihydrogen phosphate solutions
Authors: Sangwal Keshra , Mielniczek‐Brzóska Ewa
Published: June 2017

The effect of addition of three different antisolvents (namely: methanol, ethanol and acetone) on the metastable zone width (MSZW) for the crystallization of ammonium dihydrogen phosphate (ADP) from their aqueous solutions saturated at 30°C is studied by in situ measurements of solution temperature T as a function of feeding time t of the antisolvents at preselected rate RA. It is found that the value of MSZW, as determined by the value of the maximum antisolvent content Δxmax, for a given RA decreases with decreasing dielectric constant εa of the antisolvent. The experimental Δxmax(RA) data for different antisolvents are analyzed by using two dependences: lnΔxmax) = Φ + (1/m)lnRA) and (Δxmax)−2 = F(1−ZlnRA), with constants Φ, m, Z and F, predicted by self‐consistent Nývlt‐like approach and an approach based on the classical three‐dimensional nucleation theory, respectively. Analysis of the Δxmax(RA) data revealed that: (1) the empirical constants Φ and m increase linearly with εa−1 of the antisolvents, and (2) Φ = −lnF/2 and m = −2/Z. The observations are discussed from consideration of solute−solvent and solute−antisolvent interactions. The results show that the parameter FZ for different antisolvents provides information of solute−solvent interfacial energy γ and diffusion processes.
Intensified Biobutanol Recovery by using Zeolites with Complementary Selectivity
Authors: Van der Perre Stijn , Gelin Pierre , Claessens Benjamin , Martin‐Calvo Ana , Cousin Saint Remi Julien , Duerinck Tim , Baron Gino V. , Palomino Miguel , Sánchez Ledys Y. , Valencia Susana , Shang Jin , Singh Ranjeet , Webley Paul A. , Rey Fernando , Denayer Joeri F. M.
Published: June 2017

A vapor‐phase adsorptive recovery process is proposed as an alternative way to isolate biobutanol from acetone–butanol–ethanol (ABE) fermentation media, offering several advantages compared to liquid phase separation. The effect of water, which is still present in large quantities in the vapor phase, on the adsorption of the organics could be minimized by using hydrophobic zeolites. Shape‐selective all‐silica zeolites CHA and LTA were prepared and evaluated with single‐component isotherms and breakthrough experiments. These zeolites show opposite selectivities; adsorption of ethanol is favorable on all‐silica CHA, whereas the LTA topology has a clear preference for butanol. The molecular sieving properties of both zeolites allow easy elimination of acetone from the mixture. The molecular interaction mechanisms are studied by density functional theory (DFT) simulations. The effects of mixture composition, humidity and total pressure of the vapor stream on the selectivity and separation behavior are investigated. Desorption profiles are studied to maximize butanol purity and recovery. The combination of LTA with CHA‐type zeolites (Si‐CHA or SAPO‐34) in sequential adsorption columns with alternating adsorption and desorption steps allows butanol to be recovered in unpreceded purity and yield. A butanol purity of 99.7 mol % could be obtained at nearly complete butanol recovery, demonstrating the effectiveness of this technique for biobutanol separation processes.