bluuebunny/crossref_metadata_2025 huggingface dataset:
Modellierung, Simulation und Implementierung von Zellen für die solargetriebene Wasserspaltung
Authors: Xiang Chengxiang , Weber Adam Z. , Ardo Shane , Berger Alan , Chen YiKai , Coridan Robert , Fountaine Katherine T. , Haussener Sophia , Hu Shu , Liu Rui , Lewis Nathan S. , Modestino Miguel A. , Shaner Matthew M. , Singh Meenesh R. , Stevens John C. , Sun Ke , Walczak Karl
Published: July 2016

Eine integrierte Zelle für die solargetriebene Wasserspaltung besteht aus mehreren funktionellen Komponenten und kombiniert verschiedene photoelektrochemische (PEC‐)Prozesse auf unterschiedlichen Längen‐ und Zeitskalen. Der Gesamtwirkungsgrad eines derartigen Systems für die Umwandlung von Solarenergie in Wasserstoff (solar‐to‐hydrogen; STH) wird von der Leistung und den Materialeigenschaften seiner Einzelkomponenten sowie ihrer Integration, von seiner Gesamtarchitektur und den Betriebsbedingungen bestimmt. Dieser Aufsatz beschäftigt sich mit der Implementierung von solargetriebenen Prototypen für die Wasserspaltung auf der Basis von Modellierungen und Simulationen, welche die Wechselwirkungen zwischen den Einzelbauteilen in ihrer Gesamtheit berücksichtigen. Physik und Wechselwirkungen innerhalb der Zelle werden diskutiert, und die Anwendung des Zellmodells für die Bestimmung der benötigten Materialeigenschaften sowie beim Design von herkömmlichen und ungewöhnlichen Architekturen wird erörtert.
Design of Highly Stable Echogenic Microbubbles through Controlled Assembly of Their Hydrophobin Shell
Authors: Gazzera Lara , Milani Roberto , Pirrie Lisa , Schmutz Marc , Blanck Christian , Resnati Giuseppe , Metrangolo Pierangelo , Krafft Marie Pierre
Published: July 2016

Dispersing hydrophobin HFBII under air saturated with perfluorohexane gas limits HFBII aggregation to nanometer‐sizes. Critical basic findings include an unusual co‐adsorption effect caused by the fluorocarbon gas, a strong acceleration of HFBII adsorption at the air/water interface, the incorporation of perfluorohexane into the interfacial film, the suppression of the fluid‐to‐solid 2D phase transition exhibited by HFBII monolayers under air, and a drastic change in film elasticity of both Gibbs and Langmuir films. As a result, perfluorohexane allows the formation of homogenous populations of spherical, narrowly dispersed, exceptionally stable, and echogenic microbubbles.
Diverse N‐Heterocyclic Ring Systems via Aza‐Heck Cyclizations of N‐(Pentafluorobenzoyloxy)sulfonamides
Authors: Hazelden Ian R. , Ma Xiaofeng , Langer Thomas , Bower John F.
Published: July 2016

Aza‐Heck cyclizations initiated by oxidative addition of Pd0‐catalysts into the N−O bond of N‐(pentafluoro‐benzoyloxy)sulfonamides are described. These studies, which encompass only the second class of aza‐Heck reaction developed to date, provide direct access to diverse N‐heterocyclic ring systems.
Carbon‐Based Metal‐Free Catalysts for Electrocatalysis beyond the ORR
Authors: Hu Chuangang , Dai Liming
Published: July 2016

Besides their use in fuel cells for energy conversion through the oxygen reduction reaction (ORR), carbon‐based metal‐free catalysts have also been demonstrated to be promising alternatives to noble‐metal/metal oxide catalysts for the oxygen evolution reaction (OER) in metal–air batteries for energy storage and for the splitting of water to produce hydrogen fuels through the hydrogen evolution reaction (HER). This Review focuses on recent progress in the development of carbon‐based metal‐free catalysts for the OER and HER, along with challenges and perspectives in the emerging field of metal‐free electrocatalysis.
Modeling, Simulation, and Implementation of Solar‐Driven Water‐Splitting Devices
Authors: Xiang Chengxiang , Weber Adam Z. , Ardo Shane , Berger Alan , Chen YiKai , Coridan Robert , Fountaine Katherine T. , Haussener Sophia , Hu Shu , Liu Rui , Lewis Nathan S. , Modestino Miguel A. , Shaner Matthew M. , Singh Meenesh R. , Stevens John C. , Sun Ke , Walczak Karl
Published: July 2016

An integrated cell for the solar‐driven splitting of water consists of multiple functional components and couples various photoelectrochemical (PEC) processes at different length and time scales. The overall solar‐to‐hydrogen (STH) conversion efficiency of such a system depends on the performance and materials properties of the individual components as well as on the component integration, overall device architecture, and system operating conditions. This Review focuses on the modeling‐ and simulation‐guided development and implementation of solar‐driven water‐splitting prototypes from a holistic viewpoint that explores the various interplays between the components. The underlying physics and interactions at the cell level is are reviewed and discussed, followed by an overview of the use of the cell model to provide target properties of materials and guide the design of a range of traditional and unique device architectures.
A Dual‐Phase Ceramic Membrane with Extremely High H2 Permeation Flux Prepared by Autoseparation of a Ceramic Precursor
Authors: Cheng Shunfan , Wang Yanjie , Zhuang Libin , Xue Jian , Wei Yanying , Feldhoff Armin , Caro Jürgen , Wang Haihui
Published: July 2016

A novel concept for the preparation of multiphase composite ceramics based on demixing of a single ceramic precursor has been developed and used for the synthesis of a dual‐phase H2‐permeable ceramic membrane. The precursor BaCe0.5Fe0.5O3−δ decomposes on calcination at 1370 °C for 10 h into two thermodynamically stable oxides with perovskite structures: the cerium‐rich oxide BaCe0.85Fe0.15O3−δ (BCF8515) and the iron‐rich oxide BaCe0.15Fe0.85O3−δ (BCF1585), 50 mol % each. In the resulting dual‐phase material, the orthorhombic perovskite BCF8515 acts as the main proton conductor and the cubic perovskite BCF1585 as the main electron conductor. The dual‐phase membrane shows an extremely high H2 permeation flux of 0.76 mL min−1 cm−2 at 950 °C with 1.0 mm thickness. This auto‐demixing concept should be applicable to the synthesis of other ionic‐electronic conducting ceramics.
The Molecular Mechanism of P2Y1 Receptor Activation
Authors: Yuan Shuguang , Chan H. C. Stephen , Vogel Horst , Filipek Slawomir , Stevens Raymond C. , Palczewski Krzysztof
Published: July 2016

Human purinergic G protein‐coupled receptor P2Y1 (P2Y1R) is activated by adenosine 5′‐diphosphate (ADP) to induce platelet activation and thereby serves as an important antithrombotic drug target. Crystal structures of P2Y1R revealed that one ligand (MRS2500) binds to the extracellular vestibule of this GPCR, whereas another (BPTU) occupies the surface between transmembrane (TM) helices TM2 and TM3. We introduced a total of 20 μs all‐atom long‐timescale molecular dynamic (MD) simulations to inquire why two molecules in completely different locations both serve as antagonists while ADP activates the receptor. Our results indicate that BPTU acts as an antagonist by stabilizing extracellular helix bundles leading to an increase of the lipid order, whereas MRS2500 blocks signaling by occupying the ligand binding site. Both antagonists stabilize an ionic lock within the receptor. However, binding of ADP breaks this ionic lock, forming a continuous water channel that leads to P2Y1R activation.
Biomimetic Total Synthesis of Hyperjapones A–E and Hyperjaponols A and C
Authors: Lam Hiu C. , Spence Justin T. J. , George Jonathan H.
Published: July 2016

Hyperjapones A–E and hyperjaponols A–C are complex natural products of mixed aromatic polyketide and terpene biosynthetic origin that have recently been isolated from Hypericum japonicum. We have synthesized hyperjapones A–E using a biomimetic, oxidative hetero‐Diels–Alder reaction to couple together dearomatized acylphloroglucinol and cyclic terpene natural products. Hyperjapone A is proposed to be the biosynthetic precursor of hyperjaponol C through a sequence of: 1) epoxidation; 2) acid‐catalyzed epoxide ring‐opening; and 3) a concerted, asynchronous alkene cyclization and 1,2‐alkyl shift of a tertiary carbocation. Chemical mimicry of this proposed biosynthetic sequence allowed a concise total synthesis of hyperjaponol C to be completed in which six carbon–carbon bonds, six stereocenters, and three rings were constructed in just four steps.
Cellular perception and misperception: Internal models for decision‐making shaped by evolutionary experience
Authors: Mitchell Amir , Lim Wendell
Published: July 2016

Cells live in dynamic environments that necessitate perpetual adaptation. Since cells have limited resources to monitor external inputs, they are required to maximize the information content of perceived signals. This challenge is not unique to microscopic life: Animals use senses to perceive inputs and adequately respond. Research showed that sensory‐perception is actively shaped by learning and expectation allowing internal cognitive models to “fill in the blanks” in face of limited information. We propose that cells employ analogous strategies and use internal models shaped through the long process of evolutionary adaptation. Given this perspective, we postulate that cells are prone to “misperceptions,” analogous to visual illusions, leading them to incorrectly decode patterns of inputs that lie outside of their evolutionary experience. Mapping cellular misperception can serve as a fundamental approach for dissecting regulatory networks and could be harnessed to modulate cell behavior, a potentially new avenue for therapy.
Pure red cell aplasia caused by parvovirus B19 in a heart transplant recipient
Authors: Invernizzi Rosangela , Bastia Raffaella , Quaglia Federica
Published: July 2016

Key Clinical Message

A case of parvovirus B19‐induced pure red cell aplasia occurring in a heart transplant recipient is reported. The diagnosis of this rare but clinically important complication can be suspected on the basis of the pathognomonic morphological features of the bone marrow.
Press‐Printed Conductive Carbon Black Nanoparticle Films for Molecular Detection at the Microscale
Authors: Della Pelle Flavio , Vázquez Luis , Del Carlo Michele , Sergi Manuel , Compagnone Dario , Escarpa Alberto
Published: July 2016

Carbon black nanoparticle (CBNP) press‐transferred film‐based transducers for the molecular detection at the microscale level were proposed for the first time. Current‐sensing atomic force microscopy (CS‐AFM) revealed that the CBNP films were effectively press‐transferred, retaining their good conductivity. A significant correlation between the morphology and the resistance was observed. The highest resistance was localized at the top of the press‐transferred film protrusions, whereas low values are usually obtained at the deep crevices or grooves. The amount of press‐transferred CBNPs is the key parameter to obtain films with improved conductivity, which is in good agreement with the electrochemical response. In addition, the conductivity of such optimum films was not only Ohmic; in fact, tunneling/hopping contributions were observed, as assessed by CS‐AFM. The CBNP films acted as exclusive electrochemical transducers as evidenced by using two classes of molecules, that is, neurotransmitters and environmental organic contaminants. These results revealed the potential of these CBNP press‐transferred films for providing new options in microfluidics and other related micro‐ and nanochemistry applications.
Base‐Promoted Tandem Reaction Involving Insertion into Carbon–Carbon σ‐Bonds: Synthesis of Xanthone and Chromone Derivatives
Authors: Cheng Xingcan , Zhou Yuanyuan , Zhang Fangfang , Zhu Kai , Liu Yuanyuan , Li Yanzhong
Published: July 2016

Tandem reactions using base‐promoted processes have been developed for the synthesis of xanthone and chromone derivatives. The first examples of base‐promoted insertion reactions of isolated carbon–carbon triple bonds into carbon–carbon σ‐bonds have been reported. Using these approaches, polycyclic structures can be prepared. This reaction has the potential to become a general synthetic protocol for the preparation of multi‐substituted xanthones and chromones due to the abundance of easily accessible starting materials possessing diverse substituent groups.
High Performance Fe Porphyrin/Ionic Liquid Co‐catalyst for Electrochemical CO2 Reduction
Authors: Choi Jaecheol , Benedetti Tania M. , Jalili Rouhollah , Walker Ashley , Wallace Gordon G. , Officer David L.
Published: July 2016

The efficient and selective catalytic reduction of CO2 is a highly promising process for both of the storage of renewable energy as well as the production of valuable chemical feedstocks. In this work, we show that the addition of an ionic liquid, 1‐butyl‐3‐methylimidazolium tetrafluoroborate, in an aprotic electrolyte containing a proton source and FeTPP, promotes the in situ formation of the [Fe0TPP]2− homogeneous catalyst at a less negative potential, resulting in lower overpotentials for the CO2 reduction (670 mV) and increased kinetics of electron transfer. This co‐catalysis exhibits high Faradaic efficiency for CO production (93 %) and turnover number (2 740 000 after 4 hour electrolysis), with a four‐fold increase in turnover frequency (TOF) when compared with the standard system without the ionic liquid.
ChemInform Abstract: The Crystal Structure of Cs2S2O3·H2O.
Authors: Winkler Verena , Schlosser Marc , Pfitzner Arno
Published: July 2016

Cs2S2O3·H2O, being first obtained as a byproduct in the preparation of Cs4In2S5, is prepared from an aqueous solution of Cs2CO3 to which an excess of BaS2O3 is given (90 °C, 1 d).
ChemInform Abstract: A Highly Efficient Metal‐Free Oxygen Reduction Electrocatalyst Assembled from Carbon Nanotubes and Graphene.
Authors: Yang Jia , Sun Haiyan , Liang Haiyi , Ji Hengxing , Song Li , Gao Chao , Xu Hangxun
Published: July 2016

Carbon nanotubes and graphene are assembled into hybrid nanospheres by a one‐step aerosol route from aqueous solutions containing oxidized carbon nanotubes and graphene oxides, which are nebulized to generate aerosol droplets flowing through a tube furnace preheated at 350 °C.
ChemInform Abstract: Synthesis and Complex Study of the Crystal Hydrate Zn2ZrF8·12H2O.
Authors: Voit Elena , Didenko Nina , Gayvoronskaya Kseniya , Slobodyuk Arseniy , Gerasimenko Andrey
Published: July 2016

The title compound is prepared in two steps.
ChemInform Abstract: Metal—Organic Frameworks Stabilize Solution‐Inaccessible Cobalt Catalysts for Highly Efficient Broad‐Scope Organic Transformations.
Authors: Zhang Teng , Manna Kuntal , Lin Wenbin
Published: July 2016

Mixed ligand metal‐organic frameworks (MOF) and UiO‐type MOFs are prepared and their Co‐complexes are used as highly robust and recyclable catalysts in hydrogenation and boration reactions as shown for the UiO‐type CoCl2(bipyv‐MOF) complex.
ChemInform Abstract: Synthesis of Imidates: TFA‐Mediated Regioselective Amide Alkylation Using Meerwein′s Reagent.
Authors: Popov Kirill , Somfai Peter
Published: July 2016

A simple protocol for the synthesis of imidates from a variety of lactams is described using triethyloxonium tetrafluoroborate in the presence of catalytic TFA.
ChemInform Abstract: Zinc‐Catalyzed Stereo‐ and Regioselective 1,4‐Hydrative Fluorination of 3‐En‐1‐ynamides with Selectfluor.
Authors: Jadhav Appaso Mahadev , Huple Deepak B. , Singh Rahulkumar Rajmani , Liu Rai Shung
Published: July 2016

The efficient procedure provides diverse 4‐fluoro‐2‐en‐1‐amides with high (E)‐stereoselectivity.
ChemInform Abstract: Efficient Syntheses of Climate Relevant Isoprene Nitrates and (1R,5S)‐(‐)‐Myrtenol Nitrate.
Authors: Bew Sean P. , Hiatt‐Gipson Glyn D. , Mills Graham P. , Reeves Claire E.
Published: July 2016

A chemoselective synthesis of isoprene nitrates via substitution of allylic halides using silver nitrate is developed.
ChemInform Abstract: Synthesis of β‐Arylated Alkylamides via Pd‐Catalyzed One‐Pot Installation of a Directing Group and C(sp3)—H Arylation.
Authors: Liu Yunyun , Zhang Yi , Cao Xiaoji , Wan Jie‐Ping
Published: July 2016

The title alkylamides are prepared by one‐pot three‐component condensation of various acyl chlorides, aryl iodides, and aminoquinoline.
ChemInform Abstract: Microwave‐Assisted Transamidation of Ureas.
Authors: Wang Tammy C. , Qiao Jennifer X.
Published: July 2016

A novel one‐step synthesis of ureas via the transamidation of the cyclopentyl or isopropyl ureas with excess amines under microwave irradiation is reported.
ChemInform Abstract: Sustainable Diels—Alder Syntheses in Imidazolium Ionic Liquids.
Authors: Kumar Ganesan Vinoth , Rajendran Annamalai
Published: July 2016

Diels—Alder adducts are synthesized in excellent yields within a few minutes under microwave irradiation and using the ionic liquid 3‐methyl‐1‐octyl‐imidazolium tetrachloroaluminate both as catalyst and solvent.
ChemInform Abstract: Reductive Hydrazination with Trichlorosilane: A Method for the Preparation of 1,1‐Disubstituted Hydrazines.
Authors: Wang Tao , Di Xiao , Wang Chao , Zhou Li , Sun Jian
Published: July 2016

Trichlorosilane is shown to be a powerful reducing agent allowing for direct reductive hydrazination of various aldehydes and ketones with phenylhydrazines in the presence of Lewis bases.
ChemInform Abstract: Exploiting Aryl Mesylates and Tosylates in Catalytic Mono‐α‐arylation of Aryl‐ and Heteroarylketones.
Authors: Fu Wai Chung , So Chau Ming , Yuen On Ying , Lee Irene Toi Chuk , Kwong Fuk Yee
Published: July 2016

Key to this general protocol for mono‐α‐arylation is the indolyl‐derived phosphine ligand which enhances the steric congestion of the catalyst.
ChemInform Abstract: BF3·OEt2‐AgSCF3 Mediated Trifluoromethylthiolation/Cascade Cyclization of Propynols: Synthesis of 4‐((Trifluoromethyl)thio)‐2H‐chromene and 4‐((Trifluoromethyl)thio)‐1,2‐dihydroquinoline Derivatives.
Authors: Liang Yong‐Min , et al.
Published: July 2016

The reaction can be scaled up.
ChemInform Abstract: Organocatalytic Kinetic Resolution of Sulfoximines.
Authors: Dong Shunxi , Frings Marcus , Cheng Hanchao , Wen Jian , Zhang Duo , Raabe Gerhard , Bolm Carsten
Published: July 2016

An efficient kinetic resolution of sulfoximines with enals using chiral N‐heterocyclic carbene catalysts is investigated.
ChemInform Abstract: Three‐ and Four‐Component Syntheses of 3‐Arylmethylindoles by Microwave‐Assisted One‐Pot Heck Isomerization—Fischer Indolization (Alkylation) (HIFI and HIFIA) Sequences
Authors: Panther Jesco , Mueller Thomas J. J.
Published: July 2016

starting from simple materials such as (hetero)aryl bromides, allyl alcohols, hydrazines, and alkyl bromides
ChemInform Abstract: Z‐Shaped Pyrrolo[3,2‐b]pyrroles and Their Transformation into π‐Expanded Indolo[3,2‐b]indoles.
Authors: Stezycki Rafal , Grzybowski Marek , Clermont Guillaume , Blanchard‐Desce Mireille , Gryko Daniel T.
Published: July 2016

The unique Z‐shaped pyrrolopyrrole dyes show relatively strong fluorescence in solution.
ChemInform Abstract: Organocatalytic Asymmetric Conjugate Addition of Diaryloxazolidin‐2,4‐diones to Nitroolefins: An Efficient Approach to Chiral α‐Aryl‐α‐hydroxy Carboxylic Acids.
Authors: Jiao Lihui , Zhao Xiaowei , Liu Huixin , Ye Xinyi , Li Yun , Jiang Zhiyong
Published: July 2016

A series of chiral oxazolidin‐2,4‐diones is prepared by an asymmetric conjugate addition of diones (I) to nitroalkenes (II) in the presence of the urea catalyst PUFP.
ChemInform Abstract: 1,3‐Dipolar Cycloaddition of Azinium Ylides to Alkynyl Hetarenes: A Synthetic Route to Indolizine and Pyrrolo[2,1‐a]isoquinoline Based Heterobiaryls.
Authors: Nelina‐Nemtseva Julia I. , Gulevskaya Anna V. , Pozharskii Alexander F. , Nguyen Huong T. L. , Filatova Ekaterina A.
Published: July 2016

For the first time, π‐deficient alkynyl hetarenes are used as dipolarophiles in a 1,3‐dipolar cycloaddition with in situ generated azinium ylides.
ChemInform Abstract: Synthesis of 1,8‐Naphthyridines from 2‐Aminonicotinaldehydes and Terminal Alkynes.
Authors: Li Binbin , Nguyen Steven , Huang Jianjun , Wang Gaigai , Wei Huiping , Pereshivko Olga P. , Peshkov Vsevolod A.
Published: July 2016

A novel copper(II) triflate‐catalyzed reaction of 2‐aminonicotinaldehydes with terminal alkynes providing access to 1,8‐naphthyridine core is described.
ChemInform Abstract: Gold(I)‐Catalyzed Hydroaminaloxylation and Petasis—Ferrier Rearrangement Cascade of Aminaloalkynes.
Authors: Gade Amol B. , Patil Nitin T.
Published: July 2016

An efficient approach towards various indolizidines and quinolizidines is developed.
ChemInform Abstract: Synthesis of 1,1‐Diboronate Esters by Cobalt‐Catalyzed Sequential Hydroboration of Terminal Alkynes.
Authors: Zuo Ziqing , Huang Zheng
Published: July 2016

An efficient procedure for the Co‐catalyzed conversion of terminal alkyl and aryl alkynes with pinacolborane affording 1,1‐diboronate esters is developed.
ChemInform Abstract: Approach to Merosesquiterpenes via Lewis Acid Catalyzed Nazarov‐Type Cyclization: Total Synthesis of Akaol A.
Authors: Kakde Badrinath N. , Kumar Nivesh , Mondal Pradip Kumar , Bisai Alakesh
Published: July 2016

The new and efficient Lewis acid catalyzed Nazarov‐type cyclization employs only 2 mol% of Sn(OTf)2 and Bi(OTf)3 under mild conditions whereby, with Sn(OTf)2 products are obtained in somewhat lower yields.
ChemInform Abstract: Hyperjapones A—E, Terpenoid Polymethylated Acylphloroglucinols from Hypericum japonicum.
Authors: Yang Xing‐Wei , Li Yan‐Ping , Su Jia , Ma Wei‐Guang , Xu Gang
Published: July 2016

Novel terpenoid polymethylated acylphloroglucinols hyperjapone A (I), hyperjapone B (II), and hyperjapones C—E are isolated from Hypericum japonicum.
ChemInform Abstract: Seven New Acyl Glycosides from Erycibe obtusifolia.
Authors: Feng Zi‐Ming , Liu Zhao‐Zhen , Xu Kuo , Yang Ya‐Nan , Jiang Jian‐Shuang , Zhang Pei‐Cheng
Published: July 2016

Seven new acyl glycosides (Ia—c), (II), (III), (IV), and (V) are isolated from the dried stems of the Chinese folk herb Erycibe obtusifolia.
ChemInform Abstract: Myrothecoside, a Novel Glycosylated Polyketide from the Terrestrial Fungus Myrothecium sp. GS‐17.
Authors: Zhang Songya , Zhu Jing , Liu Tao , Samra Suzan , Pan Huaqi , Bai Jiao , Hua Huiming , Bechthold Andreas
Published: July 2016

Myrothecoside (I), a novel glycosylated polyketide, is isolated from the terrestrial halotolerant fungus Myrothecium sp.
ChemInform Abstract: Ligand‐Controlled Monoselective C‐Aryl Glycoside Synthesis via Palladium‐Catalyzed C—H Functionalization of N‐Quinolyl Benzamides with 1‐Iodoglycals.
Authors: Liu Minglong , Niu Youhong , Wu Yan‐Fen , Ye Xin‐Shan
Published: July 2016

An atom economic and environmentally friendly protocol for C‐glycosylation of iodoglycals is presented.
ChemInform Abstract: Synthesis and Absolute Configuration of Formosusin A, a Specific Inhibitor of Mammalian DNA Polymerase β.
Authors: Yajima Arata , Iizuka Yuu , Katsuta Ryo , Nukada Tomoo
Published: July 2016

The first synthesis of formosusin A (I), with Sharpless asymmetric dihydroxylation of a vinyliodide being the key step, is described.
ChemInform Abstract: Flexible, High Temperature, Planar Lighting with Large Scale Printable Nanocarbon Paper.
Authors: Dames Chris , et al.
Published: July 2016

An ultrapure, highly conductive nanocarbon paper composed of monolayer graphene oxide nanosheets interpenetrated with 10 wt.% single walled carbon nanotubes is fabricated by solution‐printing followed by a self‐stabilizing annealing process under an electrical bias, causing reduction of graphene oxide at high temperatures by Joule heating.
ChemInform Abstract: The Role of Naked Fluoride Ion as Base or Catalyst in Organic Synthesis
Authors: Hameed Abdul , Alharthy Rima D. , Iqbal Jamshed , Langer Peter
Published: July 2016

Review: 163 refs.
ChemInform Abstract: N‐Alkyl‐2‐halo‐ and 2,2‐Dihaloaldimines in the Pudovik Reaction
Authors: Gazizov M. B. , Khairullin R. A. , Perina A. I. , Minnikhanova A. A. , Aksenov N. G. , Gnezdilov O. I. , Il'yasov A. V. , Khayarov Kh. R.
Published: July 2016

Review: 35 refs.
ChemInform Abstract: Reactions of C‐Phosphorylated Acetimidates and Acetamidines, Involving the CH‐Acid Methylene Group
Authors: Shishkin V. E. , Mednikov E. V. , Popov Yu. V. , Shevchenko M. A. , Anishchenko O. V.
Published: July 2016

Review: 47 refs.
ChemInform Abstract: Synthetic Routes to Imidazothiazines
Authors: Radini Ibrahim Ali M. , Abdel‐Wahab Bakr F. , Khidre Rizk E.
Published: July 2016

Review: 57 refs.
Limits in Proton Nuclear Singlet‐State Lifetimes Measured with para‐Hydrogen‐Induced Polarization
Authors: Zhang Yuning , Duan Xueyou , Soon Pei Che , Sychrovský Vladimír , Canary James W. , Jerschow Alexej
Published: July 2016

The synthesis of a hyperpolarized molecule was developed, where the polarization and the singlet state were preserved over two controlled chemical steps. Nuclear singlet‐state lifetimes close to 6 min for protons are reported in dimethyl fumarate. Owing to the high symmetry (AA′X3X3′ and A2 systems), the singlet‐state readout requires either a chemical desymmetrization or a long and repeated spin lock. Using DFT calculations and relaxation models, we further determine nuclear spin singlet lifetime limiting factors, which include the intramolecular dipolar coupling mechanism (proton–proton and proton–deuterium), the chemical shift anisotropy mechanism (symmetric and antisymmetric), and the intermolecular dipolar coupling mechanism (to oxygen and deuterium). If the limit of paramagnetic relaxation caused by residual oxygen could be lifted, the intramolecular dipolar coupling to deuterium would become the limiting relaxation mechanism and proton lifetimes upwards of 26 min could become available in the molecules considered here (dimethyl maleate and dimethyl fumarate).
Coating Pt–Ni Octahedra with Ultrathin Pt Shells to Enhance the Durability without Compromising the Activity toward Oxygen Reduction
Authors: Park Jinho , Liu Jingyue , Peng Hsin‐Chieh , Figueroa‐Cosme Legna , Miao Shu , Choi Sang‐Il , Bao Shixiong , Yang Xuan , Xia Younan
Published: July 2016

We describe a new strategy to enhance the catalytic durability of Pt–Ni octahedral nanocrystals in the oxygen reduction reaction (ORR) by conformally depositing an ultrathin Pt shell on the surface. The Pt–Ni octahedra were synthesized according to a protocol reported previously and then employed directly as seeds for the conformal deposition of ultrathin Pt shells by introducing a Pt precursor dropwise at 200 °C. The amount of Pt precursor was adjusted relative to the number of Pt–Ni octahedra involved to obtain Pt–Ni@Pt1.5L octahedra of 12 nm in edge length for the systematic evaluation of their chemical stability and catalytic durability compared to Pt–Ni octahedra. Specifically, we compared the elemental compositions of the octahedra before and after treatment with acetic and sulfuric acids. We also examined their electrocatalytic stability toward the ORR through an accelerated durability test by using a rotating disk electrode method. Even after treatment with sulfuric acid for 24 h, the Pt–Ni@Pt1.5L octahedra maintained their original Ni content, whereas 11 % of the Ni was lost from the Pt–Ni octahedra. After 10 000 cycles of ORR, the mass activity of the Pt–Ni octahedra decreased by 75 %, whereas the Pt–Ni@Pt1.5L octahedra only showed a 25 % reduction.
Enrichment of Pyrrolic Nitrogen by Hole Defects in Nitrogen and Sulfur Co‐Doped Graphene Hydrogel for Flexible Supercapacitors
Authors: Tran Ngoc Quang , Kang Bong Kyun , Woo Moo Hyun , Yoon Dae Ho
Published: July 2016

The effect of the doping configuration and concentration of nitrogen (N) and sulfur (S) on the electrochemical performance of 3 D N and S co‐doped hole defect graphene hydrogel (NS‐HGH) electrodes is investigated. Surprisingly, by introducing a hole defect on the graphene surface, the difference in the doping concentrations of N and S can be used to effectively modulate the electrochemical behavior of the NS‐HGH. The hole defects provide a rapid ion diffusion path. Finally, we showed that the intriguing specific capacitance (536 F g−1) of the NS‐HGH could enhance the overall performance of the pseudocapacitance and electric double layer capacitance. The rational design of the NS‐HGH‐based flexible solid state supercapacitor results in not only outstanding electrochemical performance with a maximum energy density of 14.8 Wh kg−1 and power density of 5.2 KW kg−1 but also in extraordinary mechanical flexibility and excellent cycle stability.
Saltmarsh plant responses to eutrophication
Authors: Johnson David Samuel , Warren R. Scott , Deegan Linda A. , Mozdzer Thomas J.
Published: July 2016

In saltmarsh plant communities, bottom‐up pressure from nutrient enrichment is predicted to increase productivity, alter community structure, decrease biodiversity, and alter ecosystem functioning. Previous work supporting these predictions has been based largely on short‐term, plot‐level (e.g., 1–300 m2) studies, which may miss landscape‐level phenomena that drive ecosystem‐level responses. We implemented an ecosystem‐scale, nine‐year nutrient experiment to examine how saltmarsh plants respond to simulated conditions of coastal eutrophication. Our study differed from previous saltmarsh enrichment studies in that we applied realistic concentrations of nitrate (70–100 μM NO3−), the most common form of coastal nutrient enrichment, via tidal water at the ecosystem scale (~60,000 m2 creeksheds). Our enrichments added a total of 1,700 kg N·creek−1·yr−1, which increased N loading 10‐fold vs. reference creeks (low‐marsh, 171 g N·m−2·yr−1; high‐marsh, 19 g N·m−2·yr−1). Nutrients increased the shoot mass and height of low marsh, tall Spartina alterniflora; however, declines in stem density resulted in no consistent increase in aboveground biomass. High‐marsh plants S. patens and stunted S. alterniflora did not respond consistently to enrichment. Nutrient enrichment did not shift community structure, contrary to the prediction of nutrient‐driven dominance of S. alterniflora and Distichlis spicata over S. patens. Our mild responses may differ from the results of previous studies for a number of reasons. First, the limited response of the high marsh may be explained by loading rates orders of magnitude lower than previous work. Low loading rates in the high marsh reflect infrequent inundation, arguing that inundation patterns must be considered when predicting responses to estuarine eutrophication. Additionally, we applied nitrate instead of the typically used ammonium, which is energetically favored over nitrate for plant uptake. Thus, the form of nitrogen enrichment used, not just N‐load, may be important in predicting plant responses. Overall, our results suggest that when coastal eutrophication is dominated by nitrate and delivered via flooding tidal water, aboveground saltmarsh plant responses may be limited despite moderate‐to‐high water‐column N concentrations. Furthermore, we argue that the methodological limitations of nutrient studies must be considered when using results to inform management decisions about wetlands.
The predictability of mosquito abundance from daily to monthly timescales
Authors: Jian Yun , Silvestri Sonia , Brown Jeff , Hickman Rick , Marani Marco
Published: July 2016

The prediction of mosquito abundance is of central interest in addressing mosquito population dynamics and in forecasting the associated emerging and re‐emerging diseases. However, little work has focused on the systematic evaluation of how well adult mosquito abundance can be predicted as a function of observational resolutions, aggregation scales, and prediction lead time. We use a state space reconstruction (SSR) approach to compare the predictability of mosquito population dynamics at weekly, biweekly, and monthly scales. We focus on the analysis of Aedes vexans and Culiseta melanura populations monitored in Brunswick County (North Carolina, USA) and find that prediction over a 7‐d lead time is improved when daily observations are used, compared to the commonly used once‐per‐week sample. Our results demonstrate that daily observations of mosquito abundance contribute to improving mosquito predictability in two ways: (1) daily observations better capture fluctuations over short timescales, which are missed when sampling at coarser resolutions, and (2) the aggregation of daily abundance observations reduces the impact of noise, thereby increasing the predictability of mosquito population dynamics as the aggregation scale is increased. We show that the evaluation of population dynamical models based on observed and predicted abundance can lead to a spuriously high apparent performance, due to the high autocorrelation in the observations used to update the model state at each successive time step. We show that the comparison of predicted and observed population change, expressed through per capita growth rates, leads to a more informative performance measure.
Predictors for future clinically significant pain in patients with temporomandibular disorder: A prospective cohort study
Authors: Forssell H. , Kauko T. , Kotiranta U. , Suvinen T.
Published: July 2016

Background

Up to 30% of patients with temporomandibular disorder (TMD) run the risk of progressing to chronic pain with significant disability. This prospective cohort study assessed the effects of baseline pain and general health and psychosocial factors on the presence of clinically significant pain in patients with TMD pain at 1 year after initial consultation.

Methods

263 primary care patients with TMD pain were included. At the baseline, patients completed a pain questionnaire including a wide range of putative prognostic factors, which were assessed using validated self‐report scales. The outcome, clinically significant pain at 1 year was defined as grades IV and III and grades II and I with any disability points on the Graded Chronic Pain Scale (GCPS). Multivariable logistic regression was used to study the association between the outcome and each predictor variable.

Results

At 1 year, 26.9% of the patients reported clinically significant pain. The number of previous healthcare visits (OR 1.19, 95% CI 1.02–1.39), pain intensity/dysfunction of other pain conditions (OR 1.35, 95% CI 1.07–1.69), the number of other pain conditions (OR 1.31, 95% CI 0.98–1.74), the number of disability days (OR 1.05, 95% CI 1.00–1.12), and perceived ability to control pain (OR 0.79, 95% CI 0.61–1.01) were associated with the outcome. The area under the curve (AUC) for the whole model indicated acceptable discriminative ability (0.74, 95% CI 0.66–0.82).

Conclusions

Reporting several previous healthcare visits and comorbid pains with high pain intensity and disability signal increased risk for poor prognosis of TMD pain.

Significance

About 27% of primary care TMD pain patients reported clinically significant pain at 1 year after initial consultation. Reporting several previous healthcare visits and comorbid pains with high pain intensity and disability were associated with poor prognosis of TMD pain.
Not all that glitters is gold: A guide to surgical trials in epilepsy
Authors: Jehi Lara , Jetté Nathalie
Published: July 2016

Epilepsy surgery is often the only effective treatment in appropriately selected patients with drug‐resistant epilepsy, a disease affecting about 30% of those with epilepsy. We review the evidence supporting the use of epilepsy surgery, with a focus on randomized controlled trials (RCTs). Second, we identify gaps in knowledge about the benefits of epilepsy surgery for certain populations, the challenges of individualizing the choice of surgery, and our lack of understanding of the mechanisms of surgical outcomes. We conducted a search (MEDLINE, Embase, Cochrane, Clinicaltrials.gov) on March 2, 2016, to identify epilepsy surgery RCTs, systematic reviews, or health technology assessments (HTAs). Abstracts were screened to identify resective, palliative (e.g., corpus callosotomy, multiple subpial transection [MST]), ablative (e.g., Laser interstitial thermal therapy [LITT], gamma knife radiosurgery [RS]), and neuromodulation (e.g., cerebellar stimulation [CS], hippocampal stimulation [HS], repetitive transcranial magnetic stimulation [rTMS], responsive neurostimulation [RNS], thalamic stimulation [TS], trigeminal nerve stimulation [TNS], and vagal nerve stimulation [VNS]) RCTs. Study characteristics and outcomes were extracted. Knowledge gaps were identified. Of 1,205 abstracts, 20 RCTs were identified (resective surgery including corpus callosotomy [n = 7], MST [n = 0], RS [n = 1, 3 papers], LITT [n = 0], CS [n = 1], HS [n = 2], RNS [n = 1], rTMS [n = 1], TNS [n = 1], TS [n = 1], and VNS [n = 5]). Most studies targeted patients with temporal lobe epilepsy (TLE) and none examined the effectiveness of resective surgical therapies in patients with extra‐TLE (ETLE) or with specific lesions aside from mesial temporal lobe sclerosis. No pediatric surgical RCTs were identified except for VNS. Few RCTs address the effectiveness of surgery in epilepsy and most are of limited generalizability. Future studies are needed to compare the effectiveness of different surgical strategies, better understand the mechanisms of surgical outcomes, and define the ideal surgical approaches, particularly for patients with high or very low cognitive function, normal imaging, or ETLE.
Correlation and Lead–Lag Relationships in a Hawkes Microstructure Model
Authors: Da Fonseca José , Zaatour Riadh
Published: July 2016

The aim of this paper is to develop a multi‐asset model based on the Hawkes process describing the evolution of assets at high frequency and to study the lead–lag relationship as well as the correlation between the assets within this framework. We compute several statistical quantities and the covariance matrix associated with the diffusive limit of the model so that the relation between the parameters driving the assets at high and low frequencies is explicit. We illustrate the results using several financial assets quoted in the Eurex market and show how the model captures the lead–lag relationship between them. © 2016 Wiley Periodicals, Inc. Jrl Fut Mark 37:260–285, 2017
Flexing the PECs: Predicting environmental concentrations of veterinary drugs in Canadian agricultural soils
Authors: Kullik Sigrun A , Belknap Andrew M
Published: July 2016

Veterinary drugs administered to food animals primarily enter ecosystems through the application of livestock waste to agricultural land. Although veterinary drugs are essential for protecting animal health, their entry into the environment may pose a risk for nontarget organisms. A means to predict environmental concentrations of new veterinary drug ingredients in soil is required to assess their environmental fate, distribution, and potential effects. The Canadian predicted environmental concentrations in soil (PECsoil) for new veterinary drug ingredients for use in intensively reared animals is based on the approach currently used by the European Medicines Agency for VICH Phase I environmental assessments. The calculation for the European Medicines Agency PECsoil can be adapted to account for regional animal husbandry and land use practices. Canadian agricultural practices for intensively reared cattle, pigs, and poultry differ substantially from those in the European Union. The development of PECsoil default values and livestock categories representative of typical Canadian animal production methods and nutrient management practices culminates several years of research and an extensive survey and analysis of the scientific literature, Canadian agricultural statistics, national and provincial management recommendations, veterinary product databases, and producers. A PECsoil can be used to rapidly identify new veterinary drugs intended for intensive livestock production that should undergo targeted ecotoxicity and fate testing. The Canadian PECsoil model is readily available, transparent, and requires minimal inputs to generate a screening level environmental assessment for veterinary drugs that can be refined if additional data are available. PECsoil values for a hypothetical veterinary drug dosage regimen are presented and discussed in an international context. Integr Environ Assess Manag 2017;13:331–341. © 2016 Her Majesty the Queen in Right of Canada. Integrated Environmental Assessment and Management published by Wiley Periodicals, Inc. on behalf of SETAC. Reproduced with the permission of the Minister of Health.

Key Points

Defaults and production classes that correspond to predominant Canadian agricultural practices have been developed for the PECsoil calculation for intensively reared livestock used in the European Union during VICH Phase I. The Canadian PECsoil model is readily available, transparent, and requires minimal inputs to generate a screening level environmental assessment for veterinary drugs that can be refined if additional data are available. PECsoil values for a hypothetical veterinary drug dosage regimen for cattle, pork, and poultry are presented and discussed in an international context. The Canadian PECsoil can serve as a template for adaptation of the EMA PECsoil model for VICH Phase I environmental assessment of new veterinary drugs in other regions.
Aging Selectively Modulates Vitamin C Transporter Expression Patterns in the Kidney
Authors: Forman Katherine , Martínez Fernando , Cifuentes Manuel , Bertinat Romina , Salazar Katterine , Nualart Francisco
Published: July 2016

In the kidney, vitamin C is reabsorbed from the glomerular ultrafiltrate by sodium‐vitamin C cotransporter isoform 1 (SVCT1) located in the brush border membrane of the proximal tubules. Although we know that vitamin C levels decrease with age, the adaptive physiological mechanisms used by the kidney for vitamin C reabsorption during aging remain unknown. In this study, we used an animal model of accelerated senescence (SAMP8 mice) to define the morphological alterations and aging‐induced changes in the expression of vitamin C transporters in renal tissue. Aging induced significant morphological changes, such as periglomerular lymphocytic infiltrate and glomerular congestion, in the kidneys of SAMP8 mice, although no increase in collagen deposits was observed using 2‐photon microscopy analysis and second harmonic generation. The most characteristic histological alteration was the dilation of intracellular spaces in the basolateral region of proximal tubule epithelial cells. Furthermore, a combination of laser microdissection, qRT‐PCR, and immunohistochemical analyses allowed us to determine that SVCT1 expression specifically increased in the proximal tubules from the outer strip of the outer medulla (segment S3) and cortex (segment S2) during aging and that these tubules also express GLUT1. We conclude that aging modulates vitamin C transporter expression and that renal over‐expression of SVCT1 enhances vitamin C reabsorption in aged animals that may synthesize less vitamin C. J. Cell. Physiol. 232: 2418–2426, 2017. © 2016 Wiley Periodicals, Inc.
Global solutions for the incompressible rotating stably stratified fluids
Authors: Iwabuchi Tsukasa , Mahalov Alex , Takada Ryo
Published: July 2016

We consider the initial value problem of the 3D incompressible Boussinesq equations for rotating stratified fluids. We establish the dispersive and the Strichartz estimates for the linear propagator associated with both the rotation and the stable stratification. As an application, we give a simple proof of a unique existence of global in time solutions to our system using just a contraction mapping principle.
Levodopa modulates small‐world architecture of functional brain networks in Parkinson's disease
Authors: Berman Brian D. , Smucny Jason , Wylie Korey P. , Shelton Erika , Kronberg Eugene , Leehey Maureen , Tregellas Jason R.
Published: July 2016

Background

PD is associated with disrupted connectivity to a large number of distributed brain regions. How the disease alters the functional topological organization of the brain, however, remains poorly understood. Furthermore, how levodopa modulates network topology in PD is largely unknown. The objective of this study was to use resting‐state functional MRI and graph theory to determine how small‐world architecture is altered in PD and affected by levodopa administration.

Methods

Twenty‐one PD patients and 20 controls underwent functional MRI scanning. PD patients were scanned off medication and 1 hour after 200 mg levodopa. Imaging data were analyzed using 226 nodes comprising 10 intrinsic brain networks. Correlation matrices were generated for each subject and converted into cost‐thresholded, binarized adjacency matrices. Cost‐integrated whole‐brain global and local efficiencies were compared across groups and tested for relationships with disease duration and severity.

Results

Data from 2 patients and 4 controls were excluded because of excess motion. Patients off medication showed no significant changes in global efficiency and overall local efficiency, but in a subnetwork analysis did show increased local efficiency in executive (P = 0.006) and salience (P = 0.018) networks. Levodopa significantly decreased local efficiency (P = 0.039) in patients except within the subcortical network, in which it significantly increased local efficiency (P = 0.007).

Conclusions

Levodopa modulates global and local efficiency measures of small‐world topology in PD, suggesting that degeneration of nigrostriatal neurons in PD may be associated with a large‐scale network reorganization and that levodopa tends to normalize the disrupted network topology in PD. © 2016 International Parkinson and Movement Disorder Society
Ultra‐wideband and high‐efficiency cross polarization converter based on anisotropic metasurface
Authors: Lin Bao‐Qin , Da Xin‐Yu , Wu Jia‐Liang , Li Wei , Fang Yin‐Wu , Zhu Zi‐Hang
Published: July 2016

In this letter, an ultra‐wideband and high‐efficiency reflective cross‐polarization converter based on an anisotropic metasurface for linearly polarized EM waves is proposed. Its unit cell is composed of a two‐corner‐cut square patch mounted on grounded dielectric substrate, which is an anisotropic structure with a pair of mutually perpendicular symmetric axes u and v along
directions with respect to y‐axis direction. Numerical simulations indicate that the polarization converter can convert x‐ or y‐polarized incident wave to its cross‐polarized wave in the frequency range from 10.0 to 18.4 GHz with a relative bandwidth of 59.2% and a conversion efficiency higher than 99%. We present a detailed analysis for its polarization conversion, and derive one equation which can calculate the co‐ and cross‐polarized reflected magnitudes at y‐polarized incidence according to the phase differences between the two reflected coefficients at u‐polarized and v‐polarized incidences. The simulated, calculated, and measured results are all in agreement. © 2016 Wiley Periodicals, Inc. Microwave Opt Technol Lett 58:2402–2405, 2016
Design of compact multiband MIMO antenna for the mobile handsets
Authors: Fu Yu , Yang Guo‐Min
Published: July 2016

A compact multiband MIMO antenna with four cubic elements covering DCS1800, PCS1900, UMTS2100, LTE2300, WLAN 2.4 GHz and WiMAX 3.5 GHz bands for the mobile handhelds is presented. For each cubic element, a novel structure with slots around the feeding point is designed for the impedance matching and a parasitic element under the radiating cubic element is designed for the bandwidth enhancement. To improve the performance of the signal correlation in the MIMO system, four interdigital structures are etched in the ground plane to achieve great isolation within a wide frequency band. The obtained isolation between each two ports is less than −20 dB in the wide operational bandwidth and the envelope correlation coefficient is reduced below 0.08. © 2016 Wiley Periodicals, Inc. Microwave Opt Technol Lett 58:2411–2415, 2016