bluuebunny/crossref_metadata_2025_split huggingface dataset:
Advances in Alternating Current Electroluminescent Devices
Authors: Wang Lin , Xiao Lian , Gu Haoshuang , Sun Handong 
Published: January 2019

AbstractAlternating current (AC)‐driven electroluminescent (EL) devices have recently attracted attention as potential alternatives to direct current (DC)‐driven organic light‐emitting diodes (OLEDs), as they have the great advantage of easy integration into the AC power system of 110/220 V at 50/60 Hz without complicated back‐end electronics. However, the high driving voltage and low power efficiency inherent to AC‐driven EL devices limit their widespread application. While researchers have made some remarkable progress in this field, the underlying causes during the development process remain to be explored. The strategies for improving the performance of AC‐driven EL devices with different configurations, such as the conventional sandwiched structure and multilayer‐based light‐emitting devices, are summarized in this review. For example, it is crucial to enhance the effective electric field around the emitters for AC‐driven thin film electroluminescent (AC‐TFEL) devices, while the unbalanced generation/injection of charge carriers is the main limiting factor for the performance of AC‐driven light‐emitting devices (AC‐LEDs). The recent advances in AC‐driven EL devices, with some new configurations or new‐type emitting materials, are presented by category. The challenges and opportunities for the further development of AC‐driven EL devices are also discussed.
High‐Efficiency Green InP Quantum Dot‐Based Electroluminescent Device Comprising Thick‐Shell Quantum Dots
Authors: Zhang Han , Hu Ning , Zeng Zaiping , Lin Qingli , Zhang Fengjuan , Tang Aiwei , Jia Yu , Li Lin Song , Shen Huaibin , Teng Feng , Du Zuliang 
Published: January 2019

AbstractIndium phosphide (InP) core/shell quantum dots (QDs) without intrinsic toxicity have shown great potential to replace the widely applied cadmium‐containing QDs in next‐generation commercial display and lighting applications. However, it remains challenging to synthesize InP core/shell QDs with high quantum yields (QYs), uniform particle size, and simultaneously thicker shell thickness to reduce nonradiative Förster resonant energy transfer (FRET). Here, thick InP‐Based QLEDs shell InP/GaP/ZnS//ZnS core/shell QDs with high stability, high QY (≈70%), and large particle size (7.2 ± 1.3 nm) are successfully synthesized through extending the growth time of shell materials along with the timely replenishment of shelling precursor. The existence of GaP interface layer minimizes the lattice mismatch and reduces interfacial defects. While thick ZnS shell, which suppresses the FRET between closely packed QDs, ensures high PL QY and stability. The robustness of such properties is demonstrated by the fabrication of green electroluminescent LEDs based on InP core/shell QDs with the peak external quantum efficiency and current efficiency of 6.3% and 13.7 cd A−1, respectively, which are the most‐efficient InP‐based green quantum dot light‐emitting diodes (QLEDs) till now. This work provides an effective strategy to further improve heavy‐metal‐free QLED performance and moves a significant step toward the commercial application of InP‐based electroluminescent device.
Modeling Gas Adsorption in Flexible Metal–Organic Frameworks via Hybrid Monte Carlo/Molecular Dynamics Schemes
Authors: Rogge Sven M. J. , Goeminne Ruben , Demuynck Ruben , Gutiérrez‐Sevillano Juan José , Vandenbrande Steven , Vanduyfhuys Louis , Waroquier Michel , Verstraelen Toon , Van Speybroeck Veronique 
Published: January 2019

AbstractHerein, a hybrid Monte Carlo (MC)/molecular dynamics (MD) simulation protocol that properly accounts for the extraordinary structural flexibility of metal–organic frameworks (MOFs) is developed and validated. This is vital to accurately predict gas adsorption isotherms and guest‐induced flexibility of these materials. First, the performance of three recent models to predict adsorption isotherms and flexibility in MOFs is critically investigated. While these methods succeed in providing qualitative insight in the gas adsorption process in MOFs, their accuracy remains limited as the intrinsic flexibility of these materials is very hard to account for. To overcome this challenge, a hybrid MC/MD simulation protocol that is specifically designed to handle the flexibility of the adsorbent, including the shape flexibility, is introduced, thereby unifying the strengths of the previous models. It is demonstrated that the application of this new protocol to the adsorption of neon, argon, xenon, methane, and carbon dioxide in MIL‐53(Al), a prototypical flexible MOF, substantially decreases the inaccuracy of the obtained adsorption isotherms and predicted guest‐induced flexibility. As a result, this method is ideally suited to rationalize the adsorption performance of flexible nanoporous materials at the molecular level, paving the way for the conscious design of MOFs as industrial adsorbents.
Programmable Collective Behavior in Dynamically Self‐Assembled Mobile Microrobotic Swarms
Authors: Yigit Berk , Alapan Yunus , Sitti Metin 
Published: January 2019

AbstractCollective control of mobile microrobotic swarms is indispensable for their potential high‐impact applications in targeted drug delivery, medical diagnostics, parallel micromanipulation, and environmental sensing and remediation. Without integrated electronics for sensing and actuation, current microrobotic systems should rely on physical interactions among individual microrobots for local communication and cooperation. Here, it is shown that mobile microrobotic swarms with well‐defined collective behavior can be designed by engineering magnetic interactions among individual units. Microrobots, dynamically self‐assembled from magnetic microparticles into linear chains, locomote on surfaces in response to a precessing magnetic field. Control over precessing magnetic field allows engineering attractive and repulsive interactions among microrobots and, thus, collective order with well‐defined spatial organization and stable parallel operation over macroscale distances (≈1 cm) and through confining obstacles. The design approach described here addresses programmable assembly, propulsion, and collective behavior of dense mobile microrobot swarms simultaneously by engineering magnetic interactions and dynamic actuation of microrobots. The presented approach will advance swarm microrobotics by enabling facile and rapid formation of self‐organized and reconfigurable microrobotic swarms with programmable collective order and stability.
Mortality among United States aerospace materials manufacturing workers
Authors: Marsh Gary M. , Buchanich Jeanine M. , Graves Jessica , Zimmerman Sarah , Liu Yimeng 
Published: January 2019

ObjectivesTo evaluate long‐term mortality rates among aerospace material manufacturing workers as follow‐up to an earlier observed excess of nephritis/nephrosis.MethodsSubjects were 2020 workers ever employed in the facility during 1963‐2014. Vital status through 2014 was determined for all subjects and cause of death for 99.2% of 492 deaths. We computed standard mortality ratios (SMR) and internal relative risks.ResultsSMRs for nephritis/nephrosis were unremarkable. We observed statistically significant elevated SMRs for kidney cancer among all workers and for the category “other lymphatic hematopoietic tissue cancer” (4/5 deaths from multiple myeloma) among long‐term workers with potential plant exposure.ConclusionsWe found no evidence of elevated mortality rates for nephritis/nephrosis. Study limitations precluded robust evaluation of whether the elevated rates for kidney cancer and other lymphatic hematopoietic tissue cancer were related to occupational factors at the study site. Our findings for these two cancers warrant continued mortality follow‐up.
Development of the clinical assessment scale in autoimmune encephalitis
Authors: Lim Jung‐Ah , Lee Soon‐Tae , Moon Jangsup , Jun Jin‐Sun , Kim Tae‐Joon , Shin Yong‐Won , Abdullah Suhailah , Byun Jung‐Ick , Sunwoo Jun‐Sang , Kim Keun Tae , Yang Tae‐Won , Lee Woo‐Jin , Moon Hye‐Jin , Kim Dong Wook , Lim Byung Chan , Cho Yong Won , Yang Tae‐Ho , Kim Hee Jin , Kim Young‐Soo , Koo Yong Seo , Park Byeongsu , Jung Keun‐Hwa , Kim Manho , Park Kyung‐Il , Jung Ki‐Young , Chu Kon , Lee Sang Kun 
Published: January 2019

ObjectiveThere is no scale for rating the severity of autoimmune encephalitis (AE). In this study, we aimed to develop a novel scale for rating severity in patients with diverse AE syndromes and to verify the reliability and validity of the developed scale.MethodsThe key items were generated by a panel of experts and selected according to content validity ratios. The developed scale was initially applied to 50 patients with AE (development cohort) to evaluate its acceptability, reproducibility, internal consistency, and construct validity. Then, the scale was applied to another independent cohort (validation cohort, n = 38).ResultsA new scale consisting of 9 items (seizure, memory dysfunction, psychiatric symptoms, consciousness, language problems, dyskinesia/dystonia, gait instability and ataxia, brainstem dysfunction, and weakness) was developed. Each item was assigned a value of up to 3 points. The total score could therefore range from 0 to 27. We named the scale the Clinical Assessment Scale in Autoimmune Encephalitis (CASE). The new scale showed excellent interobserver (intraclass correlation coefficient [ICC] = 0.97) and intraobserver (ICC = 0.96) reliability for total scores, was highly correlated with modified Rankin scale (r = 0.86, p < 0.001), and had acceptable internal consistency (Cronbach α = 0.88). Additionally, in the validation cohort, the scale showed high interobserver reliability (ICC = 0.99) and internal consistency (Cronbach α = 0.92).InterpretationCASE is a novel clinical scale for AE with a high level of clinimetric properties. It would be suitable for application in clinical practice and might help overcome the limitations of current outcome scales for AE. ANN NEUROL 2019;85:352–358.
Quantitative Mapping of Endosomal DNA Processing by Single Molecule Counting
Authors: Prakash Ved , Tsekouras Konstantinos , Venkatachalapathy Muthukumaran , Heinicke Laurie , Pressé Steve , Walter Nils G. , Krishnan Yamuna 
Published: January 2019

AbstractExtracellular DNA is engulfed by innate immune cells and digested by endosomal DNase II to generate an immune response. Quantitative information on endosomal stage‐specific cargo processing is a critical parameter to predict and model the innate immune response. Biochemical assays quantify endosomal processing but lack organelle‐specific information, while fluorescence microscopy has provided the latter without the former. Herein, we report a single molecule counting method based on fluorescence imaging that quantitatively maps endosomal processing of cargo DNA in innate immune cells with organelle‐specific resolution. Our studies reveal that endosomal DNA degradation occurs mainly in lysosomes and is negligible in late endosomes. This method can be used to study cargo processing in diverse endocytic pathways and measure stage‐specific activity of processing factors in endosomes.
An N‐Heterocyclic Boryloxy Ligand Isoelectronic with N‐Heterocyclic Imines: Access to an Acyclic Dioxysilylene and its Heavier Congeners
Authors: Loh Ying Kai , Ying Lu , Ángeles Fuentes M. , Do Dinh Cao Huan , Aldridge Simon 
Published: January 2019

AbstractIntroduced here is a new type of strongly donating N‐heterocyclic boryloxy (NHBO) ligand, [(HCDippN)2BO]− (Dipp=2,6‐diisopropylphenyl), which is isoelectronic with the well‐known N‐heterocyclic iminato (NHI) donor class. This 1,3,2‐diazaborole functionalized oxy ligand has been used to stabilize the first acyclic two‐coordinate dioxysilylene and its Ge, Sn, and Pb congeners, thereby presenting the first complete series of heavier group 14 dioxycarbene analogues. All four compounds have been characterized by X‐ray crystallography and density‐functional theory, enabling analysis of periodic trends: the potential for the [(HCDippN)2BO]− ligand to subtly vary its electronic‐donor capabilities is revealed by snapshots showing the gradual evolution of arene π coordination on going from Si to Pb.
2,2′‐Diamino‐6,6′‐diboryl‐1,1′‐binaphthyl: A Versatile Building Block for Temperature‐Dependent Dual Fluorescence and Switchable Circularly Polarized Luminescence
Authors: Sun Zuo‐Bang , Liu Jun‐Kai , Yuan Da‐Fei , Zhao Zheng‐Hua , Zhu Xiao‐Zhang , Liu Di‐Hong , Peng Qian , Zhao Cui‐Hua 
Published: January 2019

AbstractTemperature‐dependent dual fluorescence and switchable circularly polarized luminescence (CPL) are two highly pursued but challenging properties for small organic molecules (SOMs). We herein disclose a triarylborane π‐system based on a 2,2′‐diamino‐6,6′‐diboryl‐1,1′‐binaphthyl scaffold that can serve as a versatile building block for achieving these two properties by simply choosing different amino groups. BNMe2‐BNaph with less bulky dimethylamino groups displays temperature‐dependent dual fluorescence, and can thus be used as a highly sensitive ratiometric fluorescence thermometer. On the other hand, BNPh2‐BNaph with bulky diphenylamino groups exhibits intense fluorescence in both solution and in the solid state. A change of solvent from nonpolar cyclohexane to highly polar MeCN not only shifts the CPL position to much longer wavelength but also inverts the CPL sign. In addition, the complexation of BNPh2‐BNaph with fluoride greatly enhances the CPL intensity.
Selective Ion Exchange in Supramolecular Channels in the Crystalline State
Authors: Ichihashi Katsuya , Konno Daisuke , Maryunina Kseniya Yu. , Inoue Katsuya , Toyoda Kazuhiro , Kawaguchi Shogo , Kubota Yoshiki , Tatewaki Yoko , Akutagawa Tomoyuki , Nakamura Takayoshi , Nishihara Sadafumi 
Published: January 2019

AbstractArtificial ion channels are of increasing interest because of potential applications in biomimetics, for example, for realizing selective ion permeability through the transport and/or exchange of selected ions. However, selective ion transport and/or exchange in the crystalline state is rare, and to the best of our knowledge, such a process has not been successfully combined with changes in the physical properties of a material. Herein, by soaking single crystals of Li2([18]crown‐6)3[Ni(dmit)2]2(H2O)4 (1) in an aqueous solution containing K+, we succeeded in complete ion exchange of the Li+ ions in 1 with K+ ions in the solution, while maintaining the crystalline state of the material. This ion exchange with K+ was selectively conducted even in mixed solutions containing K+ as well as Na+/Li+. Furthermore, remarkable changes in the physical properties of 1 resulted from the ion exchange. Our finding enables not only the realization of selective ion permeability but also the development of highly sensitive biosensors and futuristic ion exchange agents, for example.
Super‐Bulky Penta‐arylcyclopentadienyl Ligands: Isolation of the Full Range of Half‐Sandwich Heavy Alkaline‐Earth Metal Hydrides
Authors: Shi Xianghui , Qin Guorui , Wang Yang , Zhao Lanxiao , Liu Zhizhou , Cheng Jianhua 
Published: January 2019

AbstractHydrogenolysis of the half‐sandwich penta‐arylcyclopentadienyl‐supported heavy alkaline‐earth‐metal alkyl complexes (CpAr)Ae[CH(SiMe3)2](S) (CpAr=C5Ar5, Ar=3,5‐iPr2‐C6H3; S=THF or DABCO) in hexane afforded the calcium, strontium, and barium metal–hydride complexes as the same dimers [(CpAr)Ae(μ‐H)(S)]2 (Ae=Ca, S=THF, 2‐Ca; Ae=Sr, Ba, S=DABCO, 4‐Ae), which were characterized by NMR spectroscopy and single‐crystal X‐ray analysis. 2‐Ca, 4‐Sr, and 4‐Ba catalyzed alkene hydrogenation under mild conditions (30 °C, 6 atm, 5 mol % cat.), with the activity increasing with the metal size. A variety of activated alkenes including tri‐ and tetra‐substituted olefins, semi‐activated alkene (Me3SiCH=CH2), and unactivated terminal alkene (1‐hexene) were evaluated.
Copper‐Catalyzed C(sp3)−H Amidation: Sterically Driven Primary and Secondary C−H Site‐Selectivity
Authors: Bakhoda Abolghasem (Gus) , Jiang Quan , Badiei Yosra M. , Bertke Jeffery A. , Cundari Thomas R. , Warren Timothy H. 
Published: January 2019

AbstractUndirected C(sp3)−H functionalization reactions often follow site‐selectivity patterns that mirror the corresponding C−H bond dissociation energies (BDEs). This often results in the functionalization of weaker tertiary C−H bonds in the presence of stronger secondary and primary bonds. An important, contemporary challenge is the development of catalyst systems capable of selectively functionalizing stronger primary and secondary C−H bonds over tertiary and benzylic C−H sites. Herein, we report a Cu catalyst that exhibits a high degree of primary and secondary over tertiary C−H bond selectivity in the amidation of linear and cyclic hydrocarbons with aroyl azides ArC(O)N3. Mechanistic and DFT studies indicate that C−H amidation involves H‐atom abstraction from R‐H substrates by nitrene intermediates [Cu](κ2‐N,O‐NC(O)Ar) to provide carbon‐based radicals R. and copper(II)amide intermediates [CuII]‐NHC(O)Ar that subsequently capture radicals R. to form products R‐NHC(O)Ar. These studies reveal important catalyst features required to achieve primary and secondary C−H amidation selectivity in the absence of directing groups.
NMR Crystallography: Evaluation of Hydrogen Positions in Hydromagnesite by 13C{1H} REDOR Solid‐State NMR and Density Functional Theory Calculation of Chemical Shielding Tensors
Authors: Cui Jinlei , Olmsted David L. , Mehta Anil K. , Asta Mark , Hayes Sophia E. 
Published: January 2019

AbstractSolid‐state NMR measurements coupled with density functional theory (DFT) calculations demonstrate how hydrogen positions can be refined in a crystalline system. The precision afforded by rotational‐echo double‐resonance (REDOR) NMR to interrogate 13C–1H distances is exploited along with DFT determinations of the 13C tensor of carbonates (CO32−). Nearby 1H nuclei perturb the axial symmetry of the carbonate sites in the hydrated carbonate mineral, hydromagnesite [4 MgCO3⋅Mg(OH)2⋅4 H2O]. A match between the calculated structure and solid‐state NMR was found by testing multiple semi‐local and dispersion‐corrected DFT functionals and applying them to optimize atom positions, starting from X‐ray diffraction (XRD)‐determined atomic coordinates. This was validated by comparing calculated to experimental 13C{1H} REDOR and 13C chemical shift anisotropy (CSA) tensor values. The results show that the combination of solid‐state NMR, XRD, and DFT can improve structure refinement for hydrated materials.
A Dissolution/Precipitation Equilibrium on the Surface of Iridium‐Based Perovskites Controls Their Activity as Oxygen Evolution Reaction Catalysts in Acidic Media
Authors: Zhang Ronghuan , Dubouis Nicolas , Ben Osman Manel , Yin Wei , Sougrati Moulay T. , Corte Daniel A. D. , Giaume Domitille , Grimaud Alexis 
Published: January 2019

AbstractRecently, IrV‐based perovskite‐like materials were proposed as oxygen evolution reaction (OER) catalysts in acidic media with promising performance. However, iridium dissolution and surface reconstruction were observed, questioning the real active sites on the surface of these catalysts. In this work, Sr2MIr(V)O6(M=Fe, Co) and Sr2Fe0.5Ir0.5(V)O4were explored as OER catalysts in acidic media. Their activities were observed to be roughly equal to those previously reported for La2LiIrO6or Ba2PrIrO6. Coupling electrochemical measurements with iridium dissolution studies under chemical or electrochemical conditions, we show that the deposition of an IrOxlayer on the surface of these perovskites is responsible for their OER activity. Furthermore, we experimentally reconstruct the iridium Pourbaix diagram, which will help guide future research in controlling the dissolution/precipitation equilibrium of iridium species for the design of better Ir‐based OER catalysts.
Spatially Controlled Occlusion of Polymer‐Stabilized Gold Nanoparticles within ZnO
Authors: Ning Yin , Fielding Lee A. , Nutter John , Kulak Alexander N. , Meldrum Fiona C. , Armes Steven P. 
Published: January 2019

AbstractIn principle, incorporating nanoparticles into growing crystals offers an attractive and highly convenient route for the production of a wide range of novel nanocomposites. Herein we describe an efficient aqueous route that enables the spatially controlled occlusion of gold nanoparticles (AuNPs) within ZnO crystals at up to 20 % by mass. Depending on the precise synthesis protocol, these AuNPs can be (i) solely located within a central region, (ii) uniformly distributed throughout the ZnO host crystal or (iii) confined to a surface layer. Remarkably, such efficient occlusion is mediated by a non‐ionic water‐soluble polymer, poly(glycerol monomethacrylate)70(G70), which is chemically grafted to the AuNPs; pendentcis‐diol side groups on this steric stabilizer bind Zn2+cations, which promotes nanoparticle interaction with the growing ZnO crystals. Finally, uniform occlusion of G70‐AuNPs within this inorganic host leads to faster UV‐induced photodegradation of a model dye.
Chiral Heterobimetallic Bismuth–Rhodium Paddlewheel Catalysts: A Conceptually New Approach to Asymmetric Cyclopropanation
Authors: Collins Lee R. , Auris Sebastian , Goddard Richard , Fürstner Alois 
Published: January 2019

AbstractCyclopropanation reactions of styrene derivatives with donor–acceptor carbenes formed in situ are significantly more enantioselective when catalyzed by the heterobimetallic bismuth–rhodium complex 5 a endowed with N‐phthalimido tert‐leucine paddlewheel ligands rather than by its homobimetallic dirhodium analogue 1 a. This virtue is likely the result of two synergizing factors: the conical shape of 5 a translates into a narrower calyx‐like chiral binding site about the catalytically active Rh center; the Bi atom, although fully solvent exposed, does not decompose aryl diazoacetates and is hence incapable of promoting a racemic background reaction. Moreover, ligand variation proved that successful catalyst design mandates that the anisotropy of the conical heterobimetallic core be matched by proper directionality of the ligand sphere.
Structure Switching and Modulation of the Magnetic Properties in Diarylethene‐Bridged Metallosupramolecular Compounds by Controlled Coordination‐Driven Self‐Assembly
Authors: Li Zhao‐Yang , Dai Jing‐Wei , Damjanović Marko , Shiga Takuya , Wang Jin‐Hua , Zhao Jia , Oshio Hiroki , Yamashita Masahiro , Bu Xian‐He 
Published: January 2019

AbstractWe report three self‐assembled iron complexes that comprised an anti‐parallel open form (o‐Lanti), a parallel open form (o‐Lsyn), and a closed form (c‐L) of diarylethene conformers. Under kinetic control, FeII2(o‐Lanti)3 was isolated, which exhibited a dinuclear structure with diamagnetic properties. Under light‐irradiation control, FeII2(c‐L)3 was prepared and exhibited paramagnetism and spin‐crossover behaviour. Under thermodynamic control and in the presence of indispensable [FeIII(Tp*)(CN)3]−, FeII2(o‐Lanti)3 and FeII2(c‐L)3 transformed into tetranuclear FeIII2FeII2(o‐Lsyn)2, which exhibited complete spin‐crossover behaviour at T1/2=353 K.