bluuebunny/crossref_metadata_2025_split huggingface dataset:
Factors associated with fatigue in CNS inflammatory diseases with AQP4 and MOG antibodies
Authors: Yeo Tianrong , dos Passos Giordani Rodrigues , Muhammed Louwai , Everett Rosie , Reeve Sandra , Messina Silvia , Probert Fay , Leite Maria Isabel , Palace Jacqueline 
Published: March 2020

AbstractObjectiveFatigue is a common and disabling symptom amongst people with multiple sclerosis, however it has not been compared across the central nervous system (CNS) inflammatory diseases associated with aquaporin‐4 (AQP4) and myelin oligodendrocyte glycoprotein (MOG) antibodies (Ab). We explored the factors associated with fatigue within and across the two diseases, and compared fatigue levels between them.MethodsWe performed a cross‐sectional study of 90 AQP4‐Ab and 44 MOG‐Ab patients. Fatigue was assessed using the Modified Fatigue Impact Scale (MFIS). Clinical, demographic, and psychometric (anxiety, depression, pain) data were used as independent variables. Multivariable linear regression was used to identify significant independent variables associated with fatigue within and across the two diseases.ResultsWithin AQP4‐Ab patients, age (P = 0.002), disease duration (P = 0.004), number of clinical attacks (P = 0.001), disability (P = 0.007), pain interference (P < 0.001), anxiety (P = 0.026), and depression (P < 0.001) were significant independent variables. Interestingly, disease duration had a negative association with fatigue (P = 0.004). Within MOG‐Ab patients, pain interference score (P < 0.001) and anxiety (P = 0.001) were significant independent variables. Although fatigue was worse in AQP4‐Ab patients compared to MOG‐Ab patients (P = 0.008) in all patients as well as in those who ever had transverse myelitis (P = 0.023), this was driven by the differences in age, disability and pain interference rather than antibody subtype itself.InterpretationMultiple factors, but not the antibody specificity, appear to contribute to fatigue in antibody positive CNS inflammatory diseases. A multifaceted treatment approach is needed to better manage the physical, cognitive, and psychosocial aspects of fatigue in these patients.
Interfacial Band Engineering of MoS2/Gold Interfaces Using Pyrimidine‐Containing Self‐Assembled Monolayers: Toward Contact‐Resistance‐Free Bottom‐Contacts
Authors: Matković Aleksandar , Petritz Andreas , Schider Gerburg , Krammer Markus , Kratzer Markus , Karner‐Petritz Esther , Fian Alexander , Gold Herbert , Gärtner Michael , Terfort Andreas , Teichert Christian , Zojer Egbert , Zojer Karin , Stadlober Barbara 
Published: March 2020

AbstractBottom‐contact architectures with common electrode materials such as gold are crucial for the integration of 2D semiconductors into existing device concepts. The high contact resistance to gold—especially for bottom contacts—is, however, a general problem in 2D semiconductor thin‐film transistors. Pyrimidine‐containing self‐assembled monolayers on gold electrodes are investigated for tuning the electrode work functions in order to minimize that contact resistance. Their frequently ignored asymmetric and bias‐dependent nature is recorded by Kelvin probe force microscopy through a direct mapping of the potential drop across the channel during device operation. A reduction of the contact resistances exceeding two orders of magnitude is achieved via a suitable self‐assembled monolayer, which vastly improves the overall device performance.
Occupational noise exposure and asymmetric hearing loss: Results from the HUNT population study in Norway
Authors: Aarhus Lisa , Engdahl Bo 
Published: March 2020

AbstractBackgroundA large population study with adequate data on confounders is required to determine whether asymmetric hearing loss (AHL) is associated with occupational noise exposure.MethodsWe performed a cross‐sectional population study in Norway (the Health Investigation in Nord‐Trøndelag: HUNT) with 24 183 participants, using pure‐tone audiometry and questionnaires. AHL was defined as a difference in hearing threshold between the right and left ears of greater than or equal to 15 dB for the pure‐tone average of 0.5 to 2 or 3 to 6 kHz.ResultsThe mean age of the participants was 53 years (range, 19‐99); 53% were women. The prevalence of AHL in this general Norwegian population was 6% for the 0.5 to 2 kHz range and 15% for 3 to 6 kHz. In unadjusted regression models, subjects reporting prolonged occupational noise exposure to high‐level noise sources (N = 1652) had a higher risk of AHL at 3 to 6 kHz than those reporting no prior exposure (odds ratio [OR], 1.98; 95% confidence interval [CI], 1.75‐2.25). After adjustment for age and sex, OR was 1.08; (95% CI, 0.95‐1.24). After additional adjustment for head trauma, ear infections, blasting or shooting (all associated with AHL), smoking, and diabetes, OR was 1.00 (95% CI, 0.87‐1.16). No association between occupational noise and right‐ear hearing threshold advantage (left‐right ear difference) was observed after adjustment for confounders.ConclusionOur study suggests that AHL is relatively common in the general population, especially at the high‐frequency range in men and elderly subjects. Our study showed no relation between occupational noise exposure and AHL after confounder adjustment.
Grouping behavior of Sumatran orangutans (Pongo abelii) and Tapanuli orangutans (Pongo tapanuliensis) living in forest with low fruit abundance
Authors: Roth Tom S. , Rianti Puji , Fredriksson Gabriella M. , Wich Serge A. , Nowak Matthew G. 
Published: March 2020

AbstractIn contrast to the African great apes, orangutans (Pongo spp.) are semisolitary: Individuals are often on their own, but form aggregations more often than expected by chance. These temporary aggregations provide social benefits such as mating opportunities. When fruit availability is high, costs of aggregating should be lower, because competition is less pronounced. Therefore, average party size is expected to be higher when fruit availability is high. This hypothesis would also explain why orangutans in highly fruit‐productive habitats on Sumatra are more gregarious than in the usually less productive habitats of Borneo. Here, we describe the aggregation behavior of orangutans in less productive Sumatran habitats (Sikundur and Batang Toru), and compare results with those of previously surveyed field sites. Orangutans in Sikundur were more likely to form parties when fruit availability was higher, but the size of daily parties was not significantly affected by fruit availability. With regard to between‐site comparisons, average party sizes of females and alone time of parous females in Sikundur and Batang Toru were substantially lower than those for two previously surveyed Sumatran sites, and both fall in the range of values for Bornean sites. Our results indicate that the assessment of orangutans on Sumatra as being more social than those on Borneo needs revision. Instead, between‐site differences in sociality seem to reflect differences in average fruit availability.
Direct Visualization of a Mechanochemically Induced Molecular Rearrangement
Authors: Ardila‐Fierro Karen J. , Lukin Stipe , Etter Martin , Užarević Krunoslav , Halasz Ivan , Bolm Carsten , Hernández José G. 
Published: March 2020

AbstractRecent progress in the field of mechanochemistry has expanded the discovery of mechanically induced chemical transformations to several areas of science. However, a general fundamental understanding of how mechanochemical reactions by ball milling occur has remained unreached. For this, we have now implemented in situ monitoring of a mechanochemically induced molecular rearrangement by synchrotron X‐ray powder diffraction, Raman spectroscopy, and real‐time temperature sensing. The results of this study demonstrate that molecular rearrangements can be accomplished in the solid state by ball milling and how in situ monitoring techniques enable the visualization of changes occurring at the exact instant of a molecular migration. The mechanochemical benzil–benzilic acid rearrangement is the focal point of the study.
Formation of a Single‐Crystal Aluminum‐Based MOF Nanowire with Graphene Oxide Nanoscrolls as Structure‐Directing Agents
Authors: Muschi Mégane , Lalitha Anusha , Sene Saad , Aureau Damien , Fregnaux Mathieu , Esteve Imène , Rivier Lucie , Ramsahye Naseem , Devautour‐Vinot Sabine , Sicard Clémence , Menguy Nicolas , Serre Christian , Maurin Guillaume , Steunou Nathalie 
Published: March 2020

AbstractAn innovative strategy is proposed to synthesize single‐crystal nanowires (NWs) of the Al3+ dicarboxylate MIL‐69(Al) MOF by using graphene oxide nanoscrolls as structure‐directing agents. MIL‐69(Al) NWs with an average diameter of 70±20 nm and lengths up to 2 μm were found to preferentially grow along the [001] crystallographic direction. Advanced characterization methods (electron diffraction, TEM, STEM‐HAADF, SEM, XPS) and molecular modeling revealed the mechanism of formation of MIL‐69(Al) NWs involving size‐confinement and templating effects. The formation of MIL‐69(Al) seeds and the self‐scroll of GO sheets followed by the anisotropic growth of MIL‐69(Al) crystals are mediated by specific GO sheets/MOF interactions. This study delivers an unprecedented approach to control the design of 1D MOF nanostructures and superstructures.
A Pressure‐Induced Inverse Order–Disorder Transition in Double Perovskites
Authors: Deng Zheng , Kang Chang‐Jong , Croft Mark , Li Wenmin , Shen Xi , Zhao Jianfa , Yu Richeng , Jin Changqing , Kotliar Gabriel , Liu Sizhan , Tyson Trevor A. , Tappero Ryan , Greenblatt Martha 
Published: March 2020

AbstractGiven the consensus that pressure improves cation ordering in most of known materials, a discovery of pressure‐induced disordering could require recognition of an order–disorder transition in solid‐state physics/chemistry and geophysics. Double perovskites Y2CoIrO6 and Y2CoRuO6 polymorphs synthesized at 0, 6, and 15 GPa show B‐site ordering, partial ordering, and disordering, respectively, accompanied by lattice compression and crystal structure alteration from monoclinic to orthorhombic symmetry. Correspondingly, the long‐range ferrimagnetic ordering in the B‐site ordered samples are gradually overwhelmed by B‐site disorder. Theoretical calculations suggest that unusual unit‐cell compressions under external pressures unexpectedly stabilize the disordered phases of Y2CoIrO6 and Y2CoRuO6.
Iridium‐Catalyzed Selective Cross‐Coupling of Ethylene Glycol and Methanol to Lactic Acid
Authors: Wu Jiajie , Shen Lingyun , Chen Zhe‐Ning , Zheng Qingshu , Xu Xin , Tu Tao 
Published: March 2020

AbstractAn atom‐economic approach that has an unprecedented high selectivity for the synthesis of lactic acid (LA) based on a catalytic dehydrogenative cross‐coupling by using inexpensive bulk ethylene glycol and methanol is described. This method relies on the synthesis and utilization of a novel iridium catalyst bearing three N‐heterocyclic carbenes derived from 1,3‐dimethylbenzimidazolium salts, and exhibits outstanding activity in the production of LA [turnover frequency (TOF) up to 3660 h−1] owing to an elegant metal–ligand cooperation.
Constant Electricity Generation in Nanostructured Silicon by Evaporation‐Driven Water Flow
Authors: Qin Yuanshuai , Wang Yusheng , Sun Xiaoyue , Li Yajuan , Xu Hao , Tan Yeshu , Li Ya , Song Tao , Sun Baoquan 
Published: March 2020

AbstractRecently, hydrovoltaic technology emerged as a novel renewable energy harvesting method, which dramatically extends the capability to harvest water energy. However, the urgent issue restricting its device performance is poor carrier transport properties of the solid surface if large charged interface is considered simultaneously. Herein, a hydrovoltaic device based on silicon nanowire arrays (SiNWs), which provide large charged surface/volume ratio and excellent carrier transport properties, yields sustained electricity by a carrier concentration gradient induced by evaporation‐induced water flow inside nanochannels. The device can yield direct current with a short‐circuit current density of over 55 μA cm−2, which is three orders larger than a previously reported analogous device (approximately 40 nA cm−2). Moreover, it exhibits a constant output power density of over 6 μW cm−2 and an open‐circuit voltage of up to 400 mV. Our finding may pave a way for developing energy‐harvesting devices from ubiquitous evaporation‐driven internal water flow in nature with semiconductor material of silicon.
Synthesis and Application of a Perfluorinated Ammoniumyl Radical Cation as a Very Strong Deelectronator
Authors: Schorpp Marcel , Heizmann Tim , Schmucker Maximillian , Rein Stephan , Weber Stefan , Krossing Ingo 
Published: March 2020

AbstractThe perfluorinated dihydrophenazine derivative (perfluoro‐5,10‐bis(perfluorophenyl)‐5,10‐dihydrophenazine) (“phenazineF”) can be easily transformed to a stable and weighable radical cation salt by deelectronation (i.e. oxidation) with Ag[Al(ORF)4]/ Br2 mixtures (RF=C(CF3)3). As an innocent deelectronator it has a strong and fully reversible half‐wave potential versus Fc+/Fc in the coordinating solvent MeCN (E°′=1.21 V), but also in almost non‐coordinating oDFB (=1,2‐F2C6H4; E°′=1.29 V). It allows for the deelectronation of [FeIIICp*2]+ to [FeIV(CO)Cp*2]2+ and [FeIV(CN‐tBu)Cp*2]2+ in common laboratory solvents and is compatible with good σ‐donor ligands, such as L=trispyrazolylmethane, to generate novel [M(L)x]n+ complex salts from the respective elemental metals.
Regioselektive Insertion von Aluminium(I) in den cyclo‐P5‐Ring von Pentaphosphaferrocen
Authors: Yadav Ravi , Simler Thomas , Goswami Bhupendra , Schoo Christoph , Köppe Ralf , Dey Subhayan , Roesky Peter W. 
Published: March 2020

AbstractDurch Untersuchung der Reaktivität von Pentaphosphaferrocen [Cp*Fe(η5‐P5)] (Cp*=C5Me5) mit zwei verschiedenen niedervalenten Aluminiumverbindungen wurde ein direkter Zugang zu gemischten Al‐Fe‐Polyphosphidkomplexen entwickelt. Die sterische und elektronische Umgebung um das [AlI]‐Zentrum erwies sich für die Bildung der resultierenden Al‐Fe‐Polyphosphide als entscheidend. So führte die Reaktion mit dem sterisch anspruchsvollen Reagenz [Dipp‐BDIAlI] (Dipp‐BDI={[2,6‐iPr2C6H3NCMe]2CH}−) zum ersten neutralen Al‐basierten Tripeldecker‐Polyphosphidkomplex. Im Fall von [(Cp*AlI)4] wurde eine bisher nicht beschriebene regioselektive Insertion von drei [Cp*AlIII]2+‐Einheiten in zwei benachbarte P‐P‐Bindungen des cyclo‐P5‐Rings von [Cp*Fe(η5‐P5)] beobachtet. Die Regioselektivität der Insertionsreaktion kann durch die Isolierung eines σ‐donorcarbenstabilisierten Analogons des Reaktionszwischenprodukts erklärt werden.
An Exceptional Peroxide Birefringent Material Resulting from d–π Interactions
Authors: Liu Shuai , Liu Xiaomeng , Zhao Sangen , Liu Youchao , Li Lina , Ding Qingran , Li Yanqiang , Lin Zheshuai , Luo Junhua , Hong Maochun 
Published: March 2020

AbstractBirefringent materials, which can modulate the polarization of light, are almost exclusively limited to oxides. Peroxides have long been overlooked as birefringent materials, because they are usually not stable in air. Now, the first peroxide birefringent material Rb2VO(O2)2F is reported, the single crystals of which keep transparency after being exposed in the air for two weeks. Interestingly, Rb2VO(O2)2F does not feature an optimal anisotropic structure, but its birefringence (Δn=0.189 at 546 nm) exceeds those of the majority of oxides. According to the first‐principles calculations, this exceptional birefringence should be attributed to the strong electronic interactions between localized π orbital of O22− anions and V5+ 3d orbitals, which may be also favorable to the stability in the air for Rb2VO(O2)2F. These findings distinguish peroxides as a brand‐new class of birefringent materials that may possess birefringence superior to the traditional oxides.
Evolvierte, selektive Eraser für spezifische Lysinacylierungen
Authors: Spinck Martin , Neumann‐Staubitz Petra , Ecke Maria , Gasper Raphael , Neumann Heinz 
Published: March 2020

AbstractLysinacylierungen treten in vielen wichtigen physiologischen Prozessen auf. Nur eine kleine Anzahl Substrat‐promisker Lysin‐Acetyltransferasen und ‐Deacetylasen (KDACs) installiert und entfernt diese zahlreichen Modifikationen. Mit evolvierten KDACs, die nur bestimmte Acylierungen entfernen können, könnte die physiologische Bedeutung verschiedener Acylierungen für die Zelle analysiert werden. Wir haben ein bakterielles Selektionssystem für die gerichtete Evolution von KDACs entwickelt, mit dessen Hilfe wir Varianten identifizieren konnten, die Butyrylgruppen bis zu 400‐mal effizienter von Lysin entfernen als Crotonylreste. Strukturanalysen ergaben, dass das Enzym, abhängig von der Acylierung des Substrats, einen aktive oder inaktive Konformation annimmt. Mithilfe einer Butyryl‐selektiven KDAC‐Variante war es möglich, das zelluläre Acylierungsspektrum in Richtung erhöhter Lysincrotonylierung zu verschieben. Unser Selektionssystem ermöglicht es, KDAC‐Enzyme zu evolvieren, um die physiologische Signifikanz einzelner Acyllysinmodifikationen auf die Zelle zu untersuchen.
Electrochemical Oxidation of Nitrogen towards Direct Nitrate Production on Spinel Oxides
Authors: Dai Chencheng , Sun Yuanmiao , Chen Gao , Fisher Adrian C. , Xu Zhichuan J. 
Published: March 2020

AbstractNitrates are widely used as fertilizer and oxidizing agents. Commercial nitrate production from nitrogen involves high‐temperature‐high‐pressure multi‐step processes. Therefore, an alternative nitrate production method under ambient environment is of importance. Herein, an electrochemical nitrogen oxidation reaction (NOR) approach is developed to produce nitrate catalyzed by ZnFexCo2−xO4spinel oxides. Theoretical and experimental results show Fe aids the formation of the first N−O bond on the *N site, while high oxidation state Co assists in stabilizing the absorbed OH−for the generation of the second and third N−O bonds. Owing to the concerted catalysis, the ZnFe0.4Co1.6O4oxide demonstrates the highest nitrate production rate of 130±12 μmol h−1 gMO−1at an applied potential of 1.6 V versus the reversible hydrogen electrode (RHE).
Freeze–Thaw‐Promoted Fabrication of Clean and Hierarchically Structured Noble‐Metal Aerogels for Electrocatalysis and Photoelectrocatalysis
Authors: Du Ran , Joswig Jan‐Ole , Hübner René , Zhou Lin , Wei Wei , Hu Yue , Eychmüller Alexander 
Published: March 2020

AbstractNoble‐metal aerogels (NMAs) have drawn increasing attention because of their self‐supported conductive networks, high surface areas, and numerous optically/catalytically active sites, enabling their impressive performance in diverse fields. However, the fabrication methods suffer from tedious procedures, long preparation times, unavoidable impurities, and uncontrolled multiscale structures, discouraging their developments. By utilizing the self‐healing properties of noble‐metal aggregates, the freezing‐promoted salting‐out behavior, and the ice‐templating effect, a freeze–thaw method is crafted that is capable of preparing various hierarchically structured noble‐metal gels within one day without extra additives. In light of their cleanliness, the multi‐scale structures, and combined catalytic/optical properties, the electrocatalytic and photoelectrocatalytic performance of NMAs are demonstrated, which surpasses that of commercial noble‐metal catalysts.
Haruspex: A Neural Network for the Automatic Identification of Oligonucleotides and Protein Secondary Structure in Cryo‐Electron Microscopy Maps
Authors: Mostosi Philipp , Schindelin Hermann , Kollmannsberger Philip , Thorn Andrea 
Published: March 2020

AbstractIn recent years, three‐dimensional density maps reconstructed from single particle images obtained by electron cryo‐microscopy (cryo‐EM) have reached unprecedented resolution. However, map interpretation can be challenging, in particular if the constituting structures require de‐novo model building or are very mobile. Herein, we demonstrate the potential of convolutional neural networks for the annotation of cryo‐EM maps: our network Haruspex has been trained on a carefully curated set of 293 experimentally derived reconstruction maps to automatically annotate RNA/DNA as well as protein secondary structure elements. It can be straightforwardly applied to newly reconstructed maps in order to support domain placement or as a starting point for main‐chain placement. Due to its high recall and precision rates of 95.1 % and 80.3 %, respectively, on an independent test set of 122 maps, it can also be used for validation during model building. The trained network will be available as part of the CCP‐EM suite.
An Unexpected Chromophore–Solvent Reaction Leads to Bicomponent Aggregation‐Induced Phosphorescence
Authors: Chen Biao , Huang Wenhuan , Su Hao , Miao Hui , Zhang Xuepeng , Zhang Guoqing 
Published: March 2020

AbstractOrganic luminogens with persistent room‐temperature phosphorescence (RTP) have found a wide range of applications. However, many RTP luminogens are prone to severe quenching in the crystalline state. Herein, we report a strategy to construct a donor‐sp3‐acceptor type luminogen that exhibits aggregation‐induced emission (AIE) while the donor‐sp2‐acceptor counterpart structure exhibits a non‐emissive solid state. Unexpectedly, it was discovered that a trace amount (0.01 %) of the structurally similar derivative, produced by a side reaction with the DMF solvent, could induce strong RTP with an absolute RTP yield up to 25.4 % and a lifetime of 48 ms, although the substance does not show RTP by itself. Single‐crystal XRD‐based calculations suggest that n–σ* orbital interactions as a result of structural similarity may be responsible for the strong RTP in the bicomponent system. This study provides a new insight into the design of multi‐component, solid‐state RTP materials from organic molecular systems.
A Stable Silanol Triad in the Zeolite Catalyst SSZ‐70
Authors: Schroeder Christian , Mück‐Lichtenfeld Christian , Xu Le , Grosso‐Giordano Nicolás A. , Okrut Alexander , Chen Cong‐Yan , Zones Stacey I. , Katz Alexander , Hansen Michael Ryan , Koller Hubert 
Published: March 2020

AbstractNests of three silanol groups are located on the internal pore surface of calcined zeolite SSZ‐70. 2D 1H double/triple‐quantum single‐quantum correlation NMR experiments enable a rigorous identification of these silanol triad nests. They reveal a close proximity to the structure directing agent (SDA), that is, N,N′‐diisobutyl imidazolium cations, in the as‐synthesized material, in which the defects are negatively charged (silanol dyad plus one charged SiO− siloxy group) for charge balance. It is inferred that ring strain prevents the condensation of silanol groups upon calcination and removal of the SDA to avoid energetically unfavorable three‐rings. In contrast, tetrad nests, created by boron extraction from B‐SSZ‐70 at various other locations, are not stable and silanol condensation occurs. Infrared spectroscopic investigations of adsorbed pyridine indicate an enhanced acidity of the silanol triads, suggesting important implications in catalysis.
Chromium‐Catalyzed Alkylation of Amines by Alcohols
Authors: Kallmeier Fabian , Fertig Robin , Irrgang Torsten , Kempe Rhett 
Published: March 2020

AbstractThe alkylation of amines by alcohols is a broadly applicable, sustainable, and selective method for the synthesis of alkyl amines, which are important bulk and fine chemicals, pharmaceuticals, and agrochemicals. We show that Cr complexes can catalyze this C−N bond formation reaction. We synthesized and isolated 35 examples of alkylated amines, including 13 previously undisclosed products, and the use of amino alcohols as alkylating agents was demonstrated. The catalyst tolerates numerous functional groups, including hydrogenation‐sensitive examples. Compared to many other alcohol‐based amine alkylation methods, where a stoichiometric amount of base is required, our Cr‐based catalyst system gives yields higher than 90 % for various alkyl amines with a catalytic amount of base. Our study indicates that Cr complexes can catalyze borrowing hydrogen or hydrogen autotransfer reactions and could thus be an alternative to Fe, Co, and Mn, or noble metals in (de)hydrogenation catalysis.