bluuebunny/crossref_metadata_2025_split huggingface dataset:
Tailoring Sodium Anodes for Stable Sodium–Oxygen Batteries
Authors: Wu Shichao , Qiao Yu , Jiang Kezhu , He Yibo , Guo Shaohua , Zhou Haoshen 
Published: January 2018

AbstractSodium–oxygen batteries based on abundant sodium resource have caused increasing interest due to their high energy density and low cost. However, the reactive sodium anode always induces unpredictable side reactions especially in oxygen atmosphere and battery short circuit due to the uncontrolled formation of dendrites. Here, an accessible method to grow a durable protective passivation film on the surface of sodium anodes is reported. The sodium fluoride‐rich film efficiently suppresses O2 crossover and electrolyte decay related side reactions on sodium anodes. Significantly, no dendrites form during long‐term stripping/plating cycles. Benefiting from these superiorities, sodium–oxygen batteries achieve impressive improvement of discharge–charge ability and reliable safety. These results enrich the approaches for stabilizing sodium anodes and allow researchers to focus on the investigations on the air cathode and the overall chemistry of sodium–oxygen batteries.
NixSy Nanowalls/Nitrogen‐Doped Graphene Foam Is an Efficient Trifunctional Catalyst for Unassisted Artificial Photosynthesis
Authors: Zou Haiyuan , He Bowen , Kuang Panyong , Yu Jiaguo , Fan Ke 
Published: January 2018

AbstractSolar‐to‐hydrogen (STH) conversion through unassisted artificial photosynthesis (APS) devices is one of the promising and environmentally friendly strategies for sustainable development. However, the practical large‐scale application of the unassisted APS devices is impeded by the need for expensive noble metal‐based catalysts in photovoltaics and/or electrolyzers. Herein, well‐aligned 2D NixSy nanowalls (2D NixSy NWs) on a 3D nitrogen‐doped graphene foam (3D NGF) are synthesized and further employed it in unassisted APS. Due to the positive synergistic effect between the highly electrocatalytic activity of NixSy NW and excellent conductivity of NGF, this low cost material of (2D/3D) NixSy NW/NGF is highly efficient as a multifunctional catalyst in various applications: a counterelectrode for dye‐sensitized solar cell (DSSC) and a “bifunctional” electrocatalyst for oxygen and hydrogen evolution for electrocatalytic overall water splitting. Furthermore, three NixSy NW/NGF‐based DSSCs as a tandem cell for unassisted solar‐driven overall water splitting is connected, using NixSy NW/NGF itself on nickel foams as the anode and cathode. Impressively, such integrated photovoltaic‐electrolyzer APS device can achieve an STH efficiency of 3.2% with an excellent stability and low cost. This work opens an avenue to advanced multifunctional materials for the low‐cost and unassisted solar‐driven overall water splitting.
New Bichromophoric Triplet Photosensitizer Designs and Their Application in Triplet–Triplet Annihilation Upconversion
Authors: Guo Xinyan , Liu Yiming , Chen Qi , Zhao Dahui , Ma Yuguo 
Published: January 2018

AbstractAs indispensable molecular components, photosensitizers play a crucial role in determining the quantum efficiency of triplet–triplet annihilation upconversion (TTA UC). This emergent technology has attracted great attention in recent years for realizing large anti‐Stokes shifts with noncoherent excitation sources. In a typical TTA UC, low‐energy photons are first harvested by the photosensitizers, which upon intersystem crossing (ISC) undergo triplet–triplet energy transfer (TTET) to emitters (i.e., annihilators). Following the bimolecular TTA among the emitters, high‐energy photons are given off by the singlet excited state of the emitters. Apparently, the efficiencies of photon absorption, ISC, and TTET are all dependent on the sensitizers. With a Dexter‐type ET mechanism requiring collisional interactions, a long triplet lifetime of the energy donor (photosensitizer) is evidently favorable for enhancing the efficiency of TTET. This progress report summarizes the recent developments of photosensitizers used for TTA UC, many of which feature a bichromophoric molecular scaffold. Among the various consequences and functions entailed by such bichromophoric designs, the extended triplet lifetime is a particularly advantageous property for TTA UC. Additionally, these new potent photosensitizers with long triplet lifetimes are also useful for other applications such as singlet oxygen sensitization and oxygen sensing.
Fully Digitally Printed Image Sensor Based on Organic Photodiodes
Authors: Eckstein Ralph , Strobel Noah , Rödlmeier Tobias , Glaser Konstantin , Lemmer Uli , Hernandez‐Sosa Gerardo 
Published: January 2018

AbstractHere, an entirely printed passive matrix image detector composed of 256 individual pixels with an individual active area of ≈250 µm × 300 µm is fabricated. The fabrication of the organic photodetector (OPD) array is enabled by exploiting a self‐alignment process of the functional layers induced by digitally printed dewetting patterns resulting in high‐performance reproducibility and fabrication yields of 100%. The single OPD pixels fabricated under ambient conditions exhibit state‐of‐the art performances with spectral responsivities of up to 0.3 A W−1, a linear dynamic range of 114 dB, and calculated specific detectivities (D*) > 1012 Jones, thereby, competing with performances of current inorganic devices.
Visible Light Activated Radical Denitrative Benzoylation of β‐Nitrostyrenes: A Photocatalytic Approach to Chalcones
Authors: Tripathi Shubhangi , Kapoor Ritu , Yadav Lal Dhar S. 
Published: January 2018

AbstractA metal‐free, convenient photocatalytic approach to chalcones from β‐nitrostyrenes and benzaldehydes via a radical denitrative benzoylation pathway is reported. The salient features of the protocol include the utilization of visible light as an inexpensive and ecosustainable energy source, N‐hydroxyphthalimide (NHPI) as a reusable organophotocatalyst and acetonitrile as an acceptable green solvent to afford chalcones in excellent yields at room temperature in a one‐pot procedure. Notably, this is the first application of β‐nitrostyrenes as readily available substrates for chalcone synthesis and the first example of photocatalysis in this field.magnified image
Materials for Transparent Electrodes: From Metal Oxides to Organic Alternatives
Authors: Hofmann Anna Isabel , Cloutet Eric , Hadziioannou Georges 
Published: January 2018

AbstractOptoelectronic devices, such as displays, are now omnipresent in our daily life. A crucial component of these devices is a transparent electrode, which allows the in‐ and outcoupling of light. With the goal of optimizing the electrode characteristics and improving device efficiencies, many approaches for the fabrication of thin, transparent, conducting films have been studied. This review gives an overview of the different material classes which are used as transparent electrodes, ranging from metal oxides, such as indium tin oxide, metal, and carbonaceous nanostructures, to conducting polymers and composites. For every material class, a brief description of the fundamental principles, processing routes, and the latest achievements is given. Furthermore, the optoelectronic performance, flexibility, and surface roughness of the different electrodes are compared. Ultimately, advantages and drawbacks of the respective electrodes are discussed. This critical comparison of fundamentally different transparent conducting materials allows, on one hand, to make a sensible choice of electrode for specific applications, and, on the other hand, to point out scientific challenges that must still be addressed.
Silica‐Protected Ultrathin Ni3FeN Nanocatalyst for the Efficient Hydrolytic Dehydrogenation of NH3BH3
Authors: Zhang Xin , Zhao Yufei , Jia Xiaodan , Zhao Yunxuan , Shang Lu , Wang Qing , Waterhouse Geoffrey I. N. , Wu Li‐Zhu , Tung Chen‐Ho , Zhang Tierui 
Published: January 2018

AbstractTransition metal nitrides (TMNs) inevitably aggregate in the high‐temperature thermal ammonolysis process, resulting in blocking of the active catalytic sites and serious decreases in their corresponding catalytic performance. Therefore, how to synthesize ultrasmall TMNs with higher exposed unsaturated coordination sites is still a challenge. Herein, ultrathin Ni3FeN (Ni3FeN@SiO2) with the size of ≈20 nm and thickness of ≈3.0 nm is fabricated by SiO2 protection strategy. The obtained Ni3FeN@SiO2 displays outstanding performance in NH3BH3 hydrolytic dehydrogenation due to the high specific surface area, intrinsic metal‐vacancies, and hydrophilic SiO2 layer.
KVP2O7 as a Robust High‐Energy Cathode for Potassium‐Ion Batteries: Pinpointed by a Full Screening of the Inorganic Registry under Specific Search Conditions
Authors: Park Woon Bae , Han Su Cheol , Park Chunguk , Hong Sung Un , Han Ugyu , Singh Satendra Pal , Jung Young Hwa , Ahn Docheon , Sohn Kee‐Sun , Pyo Myoungho 
Published: January 2018

AbstractCandidates for high‐energy cathodes in potassium‐ion batteries (KIBs) are selected by fully screening the inorganic compound structure database. The compounds that satisfy the specific conditions for plausible KIB cathodes are further subjected to theoretical and electrochemical verification, and KVP2O7 is finally pinpointed. KVP2O7 can reversibly desert/insert ≈60% of K+ (60 mA h g−1) during either chemical or electrochemical oxidation/reduction. KVP2O7 shows an average discharge potential of ≈4.2 V versus K/K+, which corresponds to an energy density of 253 W h kg−1 at 0.25 C. This high energy density characteristic of KVP2O7 is maintained both during fast charge/discharge (C/D) and prolonged redox cycles. The C/D of KVP2O7 is also accompanied by a phase transition between a monoclinic KVP2O7 (P21/c) and a triclinic K1−xVP2O7. The structure interpretation of a new K1−xVP2O7 phase indicates that K+‐extraction induces a conformational change of two tetrahedral PO4 units in pyrophosphates. The phase of K1−xVP2O7 (x ≈0.6) remains stable during the C/D process, although it returns to the inborn P21/c phase after thermal treatment. It is believed that the data‐mining protocol designed for this study will provide a new strategy for materials discovery and that the pinpointed KVP2O7 can be utilized as a reliable KIB cathode.
Randomized trial of transcranial direct current stimulation for poststroke dysphagia
Authors: Suntrup‐Krueger Sonja , Ringmaier Corinna , Muhle Paul , Wollbrink Andreas , Kemmling Andre , Hanning Uta , Claus Inga , Warnecke Tobias , Teismann Inga , Pantev Christo , Dziewas Rainer 
Published: January 2018

ObjectiveWe evaluated whether transcranial direct current stimulation (tDCS) is able to enhance dysphagia rehabilitation following stroke. Besides relating clinical effects with neuroplastic changes in cortical swallowing processing, we aimed to identify factors influencing treatment success.MethodsIn this double‐blind, randomized study, 60 acute dysphagic stroke patients received contralesional anodal (1mA, 20 minutes) or sham tDCS on 4 consecutive days. Swallowing function was thoroughly assessed before and after the intervention using the validated Fiberoptic Endoscopic Dysphagia Severity Scale (FEDSS) and clinical assessment. In 10 patients, swallowing‐related brain activation was recorded applying magnetoencephalography before and after the intervention. Voxel‐based statistical lesion pattern analysis was also performed.ResultsStudy groups did not differ according to demographic data, stroke characteristics, or baseline dysphagia severity. Patients treated with tDCS showed greater improvement in FEDSS than the sham group (1.3 vs 0.4 points, mean difference = 0.9, 95% confidence interval [CI] = 0.4–1.4, p < 0.0005). Functional recovery was accompanied by a significant increase of activation (p < 0.05) in the contralesional swallowing network after real but not sham tDCS. Regarding predictors of treatment success, for every hour earlier that treatment was initiated, there was greater improvement on the FEDSS (adjusted odds ratio = 0.99, 95% CI = 0.98–1.00, p < 0.05) in multivariate analysis. Stroke location in the right insula and operculum was indicative of worse response to tDCS (p < 0.05).InterpretationApplication of tDCS over the contralesional swallowing motor cortex supports swallowing network reorganization, thereby leading to faster rehabilitation of acute poststroke dysphagia. Early treatment initiation seems beneficial. tDCS may be less effective in right‐hemispheric insulo‐opercular stroke. Ann Neurol 2018;83:328–340
Synthesis, properties and mechanism of photodegradation of core–shell structured upconversion luminescent NaYF4:Yb3+,Er3+@BiOCl
Authors: Zhou Shiyu , Zhang Qiyan , Zhao Deqiang , Zong Wenjuan , Fan Zihong , Sun Yaofang , Xu Xuan 
Published: January 2018

Microspherical bismuth oxychloride (BiOCl) can only utilize ultraviolet (UV) light to promote photocatalytic reactions. To overcome this limitation, a uniform and thin BiOCl nanosheet was synthesized with a particle size of about 200 nm. As results of UV–visible diffuse reflectance spectroscopy showed, the band gap of this nanostructure was reduced to 2.78 eV, indicating that the BiOCl nanosheet could absorb and utilize visible light. Furthermore, the upconversion material NaYF4 doped with rare earth ions Yb3+ and Er3+ emitted visible light at 410 nm following excitation with near‐infrared (NIR) light (980 nm), which could be utilized by BiOCl to produce a photocatalytic reaction. To produce a high‐efficiency photocatalyst (NaYF4:Yb3+,Er3+@BiOCl), BiOCl‐loaded NaYF4:Yb3+,Er3+ was successfully synthesized via a simple two‐step hydrothermal method. The as‐synthesized material was confirmed using X‐ray diffraction, scanning electron microscopy, X‐ray photoelectron spectroscopy as well as other characterizations. The removal ratio of methylene blue by NaYF4:Yb3+,Er3+@BiOCl was much higher than that of BiOCl alone. Recycling experiments verified the stability of NaYF4:Yb3+,Er3+@BiOCl, which demonstrated excellent adsorption, strong visible‐light absorption and high electron–hole separation efficiency. Such properties are expected to be useful in practical applications, and a further understanding of the NIR‐light‐responsive photocatalytic mechanism of this new catalytic material would be conducive to improving its structural design and function.
Selective hydrogenation of aromatic compounds using modified iridium nanoparticles
Authors: Jiang He‐yan , Xu Jie , Sun Bin 
Published: January 2018

Till now, Ionic liquid‐stabilized metal nanoparticles were investigated as catalytic materials, mostly in the hydrogenation of simple substrates like olefins or arenes. The adjustable hydrogenation products of aromatic compounds, including quinoline and relevant compounds, aromatic nitro compounds, aromatic ketones as well as aromatic aldehydes, are always of special interest, since they provide more choices for additional derivatization. Iridium nanoparticles (Ir NPs) were synthesized by the H2 reduction in imidazolium ionic liquid. TEM indicated that the Ir NPs is worm‐like shape with the diameter around 12.2 nm and IR confirmed the modification of phosphine‐functionalized ionic liquids (PFILs) to the Ir NPs. With the variation of the modifier, solvent and reaction temperature, substrate like quinoline and relevant compounds, aromatic nitro compounds, aromatic ketones as well as aromatic aldehydes could be hydrogenated by Ir NPs with interesting adjustable catalytic activity and chemoselectivity. Ir NPs modified by PFILs are simple and efficient catalysts in challenging chemoselective hydrogenation of quinoline and relevant compounds, aromatic nitro compounds, aromatic ketones as well as aromatic aldehydes. The activity and chemoselectivity of the Ir NPs could be obviously impacted or adjusted by altering the modifier, solvent and reaction temperature.
Validated UPLC‐MS/MS method for quantification of seven compounds in rat plasma and tissues: Application to pharmacokinetic and tissue distribution studies in rats after oral administration of extract of Eclipta prostrata L.
Authors: Du Guangyan , Fu Lingling , Jia Jun , Pang Xu , Yu Haiyang , Zhang Youcai , Fan Guanwei , Gao Xiumei , Han Lifeng 
Published: January 2018

AbstractA rapid, sensitive and specific ultra‐high‐performance liquid chromatography coupled with tandem mass spectrometry (UPLC‐MS/MS) method was developed to investigate the pharmacokinetics and tissue distribution of Eclipta prostrata extract. Rats were orally administrated the 70% ethanol extract of E. prostrata, and their plasma as well as various organs were collected. The concentrations of seven main compounds, ecliptasaponin IV, ecliptasaponin A, apigenin, 3′‐hydroxybiochanin A, luteolin, luteolin‐7‐O‐glucoside and wedelolactone, were quantified by UPLC‐MS/MS through multiple reactions monitoring method. The precisions (RSD) of the analytes were all <15.00%. The extraction recoveries ranged from 74.65 to 107.45% with RSD ≤ 15.36%. The matrix effects ranged from 78.00 to 118.06% with RSD ≤ 15.04%. To conclude, the present pharmacokinetic and tissue distribution studies provided useful information for the clinical usage of Eclipta prostrata L.
Quantification of acyclovir in dermal interstitial fluid and human serum by ultra‐high‐performance liquid–high‐resolution tandem mass spectrometry for topical bioequivalence evaluation
Authors: Schimek Denise , Raml Reingard , Francesconi Kevin A. , Bodenlenz Manfred , Sinner Frank 
Published: January 2018

AbstractTime–concentration curves for the topical anti‐viral drug acyclovir can provide valuable information for drug development. Open flow microperfusion is used for continuous sampling of dermal interstitial fluid but it requires validated methods for subsequent sample analysis. Therefore, we developed a sensitive, selective and high‐throughput ultra‐high‐performance liquid chromatography–high‐resolution tandem mass spectrometry method to determine acyclovir in human dermal interstitial fluid and serum. We validated the method over a concentration range of 0.1–25 ng/mL for a sample volume of just 20 μL and employed cation‐exchange solid‐phase extraction in a fully automated sample treatment procedure. Short‐ and long‐term sample stability data and the analysis of 5000 samples from a clinical trial demonstrate the successful application of our method.
Identification of the absorbed components and metabolites of modified Huo Luo Xiao Ling Dan in rat plasma by UHPLC‐Q‐TOF/MS/MS
Authors: Wang Nannan , Zhao Xiaoning , Li Yiran , Cheng Congcong , Huai Jiaxin , Bi Kaishun , Dai Ronghua 
Published: January 2018

AbstractTo reveal the material basis of Huo Luo Xiao Ling Dan (HLXLD), a sensitive and selective ultra‐high performance liquid chromatography coupled with quadrupole‐time‐of‐flight mass spectrometry (UHPLC‐Q‐TOF/MS) method was developed to identify the absorbed components and metabolites in rat plasma after oral administration of HLXLD. The plasma samples were pretreated by liquid–liquid extraction and separated on a Shim‐pack XR‐ODS C18 column (75 × 3.0 mm, 2.2 μm) using a gradient elution program. With the optimized conditions and single sample injection of each positive or negative ion mode, a total of 109 compounds, including 78 prototype compounds and 31 metabolites, were identified or tentatively characterized. The fragmentation patterns of representative compounds were illustrated as well. The results indicated that aromatization and hydration were the main metabolic pathways of lactones and tanshinone‐related metabolites; demethylation and oxidation were the major metabolic pathways of alkaloid‐related compounds; methylation and sulfation were the main metabolic pathways of phenolic acid‐related metabolites. It is concluded the developed UHPLC‐Q‐TOF/MS method with high sensitivity and resolution is suitable for identifying and characterizing the absorbed components and metabolites of HLXLD, and the results will provide essential data for further studying the relationship between the chemical components and pharmacological activity of HLXLD.
Two‐Stage Dry Anaerobic Digestion Process Control of Biowaste for Hydrolysis and Biogas Optimization
Authors: Micolucci Federico , Uellendhal Hinrich 
Published: January 2018

AbstractAn advanced management system is offered which adapts to most of the two‐stage anaerobic dry treatment plants that do not benefit from a local expert in biowaste treatment. This approach takes advantage of pH sensors to control the process within the optimal range to enhance the hydrolysis and to stabilize and increase the biogas production. By applying automatic pH control in the operational regime by a shift between direct recirculation in the first stage or using digestate of the second stage for percolation, the pH in the first stage could be kept low at pH 5.2 ± 0.2 over the whole operation period. The results demonstrate that the energy efficiency of the two‐stage dry anaerobic digestion process can be significantly increased by controlling the pH in the first stage.
Synthesis and Structure of a Longitudinally Twisted Hexacene
Authors: Clevenger Robert G. , Kumar Bharat , Menuey Elizabeth M. , Kilway Kathleen V. 
Published: January 2018

AbstractThe addition of phenyllithium to a polycyclic quinone, 9,11,12,21,22,24‐hexaphenyltetrabenzo[a,c,n,p]hexacene‐10,23‐dione (10), followed by SnCl2‐mediated reduction of the diol intermediate, yielded 9,10,11,12,21,22,23,24‐octaphenyltetrabenzo‐[a,c,n,p]hexacene (4). Crystallographic analysis of hexacene 4 showed it to possess a longitudinal twist of 184°, which was in good agreement with AM1 calculations. In addition to being the most twisted acene synthesized to this point, compound 4 contains within its substructure the most twisted naphthalene, anthracene, tetracene, and pentacene moieties described.
Synthesis of Single and Double Dibenzohelicenes by Rhodium‐Catalyzed Intramolecular [2+2+2] and [2+1+2+1] Cycloaddition
Authors: Yamano Ryota , Shibata Yu , Tanaka Ken 
Published: January 2018

AbstractDibenzo[7]helicenes were synthesized with up to 99 % ee by rhodium(I)/binap‐catalyzed enantioselective intramolecular [2+2+2] cycloaddition of 2‐phenylnaphthalene‐linked triynes. Additionally, [2+1+2+1] cycloaddition products, that is, twisted anthracenes, were also synthesized by using difluorphos as ligand. Although these compounds are not configurationally stable at elevated temperature, their Scholl reactions afforded configurationally stable double dibenzo[6]helicenes. The thus‐obtained dibenzo[7]helicene exhibited good circularly polarized luminescence property and the double dibenzo[6]helicene showed high fluorescence quantum yield.
Helenalin Analogues Targeting NF‐κB p65: Thiol Reactivity and Cellular Potency Studies of Varied Electrophiles
Authors: Widen John C. , Kempema Aaron M. , Baur Jordan W. , Skopec Hannah M. , Edwards Jacob T. , Brown Tenley J. , Brown Dennis A. , Meece Frederick A. , Harki Daniel A. 
Published: January 2018

AbstractHelenalin is a pseudoguaianolide natural product that targets Cys38 within the DNA binding domain of NF‐κB transcription factor p65 (RelA). Helenalin contains two Michael acceptors that covalently modify cysteines: a α‐methylene‐γ‐butyrolactone and a cyclopentenone. We recently reported two simplified helenalin analogues that mimic the biological activity of helenalin and contain both electrophilic moieties. To determine the individual contributions of the Michael acceptors toward NF‐κB inhibition, we synthesized a small library of helenalin‐based analogues containing various combinations of α‐methylene‐γ‐butyrolactones and cyclopentenones. The kinetics of thiol addition to a subset of the analogues was measured to determine the relative thiol reactivities of the embedded electrophiles. Additionally, the cellular NF‐κB inhibitory activities of the analogues were determined to elucidate the contributions of each Michael acceptor to biological potency. Our studies suggest the α‐methylene‐γ‐butyrolactone contributes most significantly to the NF‐κB inhibition of our simplified helenalin analogues.