bluuebunny/crossref_metadata_2025_split huggingface dataset:
Antinuclear Antibody–Negative Systemic Lupus Erythematosus in an International Inception Cohort
Authors: Choi May Y. , Clarke Ann E. , St. Pierre Yvan , Hanly John G. , Urowitz Murray B. , Romero‐Diaz Juanita , Gordon Caroline , Bae Sang‐Cheol , Bernatsky Sasha , Wallace Daniel J. , Merrill Joan T. , Isenberg David A. , Rahman Anisur , Ginzler Ellen M. , Petri Michelle , Bruce Ian N. , Dooley Mary A. , Fortin Paul R. , Gladman Dafna D. , Sanchez‐Guerrero Jorge , Steinsson Kristjan , Ramsey‐Goldman Rosalind , Khamashta Munther A. , Aranow Cynthia , Alarcón Graciela S. , Manzi Susan , Nived Ola , Zoma Asad A. , van Vollenhoven Ronald F. , Ramos‐Casals Manuel , Ruiz‐Irastorza Guillermo , Lim S. Sam , Kalunian Kenneth C. , Inanc Murat , Kamen Diane L. , Peschken Christine A. , Jacobsen Soren , Askanase Anca , Stoll Thomas , Buyon Jill , Mahler Michael , Fritzler Marvin J. 
Published: July 2018

ObjectiveThe spectrum of antinuclear antibodies (ANAs) is changing to include both nuclear staining as well as cytoplasmic and mitotic cell patterns (CMPs) and accordingly a change is occurring in terminology to anticellular antibodies. This study examined the prevalence of indirect immunofluorescence (IIF) anticellular antibody staining using the Systemic Lupus International Collaborating Clinics inception cohort.MethodsAnticellular antibodies were detected by IIF on HEp‐2000 substrate using the baseline serum. Three serologic subsets were examined: ANA positive (presence of either nuclear or mixed nuclear/CMP staining), anticellular antibody negative (absence of any intracellular staining), and isolated CMP staining. The odds of being anticellular antibody negative versus ANA or isolated CMP positive was assessed by multivariable analysis.ResultsA total of 1,137 patients were included; 1,049 (92.3%) were ANA positive, 71 (6.2%) were anticellular antibody negative, and 17 (1.5%) had an isolated CMP. The isolated CMP–positive group did not differ from the ANA‐positive or anticellular antibody–negative groups in clinical, demographic, or serologic features. Patients who were older (odds ratio [OR] 1.02 [95% confidence interval (95% CI) 1.00, 1.04]), of white race/ethnicity (OR 3.53 [95% CI 1.77, 7.03]), or receiving high‐dose glucocorticoids at or prior to enrollment (OR 2.39 [95% CI 1.39, 4.12]) were more likely to be anticellular antibody negative. Patients on immunosuppressants (OR 0.35 [95% CI 0.19, 0.64]) or with anti‐SSA/Ro 60 (OR 0.41 [95% CI 0.23, 0.74]) or anti–U1 RNP (OR 0.43 [95% CI 0.20, 0.93]) were less likely to be anticellular antibody negative.ConclusionIn newly diagnosed systemic lupus erythematosus, 6.2% of patients were anticellular antibody negative, and 1.5% had an isolated CMP. The prevalence of anticellular antibody–negative systemic lupus erythematosus will likely decrease as emerging nomenclature guidelines recommend that non‐nuclear patterns should also be reported as a positive ANA.
Chitosan‐Based Heparan Sulfate Mimetics Promote Epidermal Formation in a Human Organotypic Skin Model
Authors: Farrugia Brooke L. , Mi Yaolei , Kim Ha Na , Whitelock John M. , Baker Shenda M. , Wiesmann William P. , Li Zhe , Maitz Peter , Lord Megan S. 
Published: July 2018

AbstractBiomimetic materials that replicate biological functions have great promise for use as therapeutics in regenerative medicine applications. Heparan sulfate (HS) is the natural binding partner for growth factors enabling longer half‐lives and potentiation of their signaling. In this study a water soluble chitosan‐arginine is modified with sulfate moieties in order to mimic the structure of HS. Sulfated chitosan‐arginine with a degree of sulfation of 58% binds fibroblast growth factor 2 with higher affinity than HS. The sulfated chitosan‐arginine also promotes epithelial cell migration and supports the formation of an expanded epidermis in an organotypic skin model. Furthermore, sulfated chitosan‐arginine promotes the expression of the HS proteoglycan, perlecan, by both epithelial and fibroblast cells. Perlecan itself modulates the activity of mitogens and is essential for the formation of the epidermis. The synthesized sulfated Ch‐Arg derivatives mimic HS, support formation of the epidermis, and thus have the potential to assist in wound healing.
High Efficiency Deep‐Blue Phosphorescent Organic Light‐Emitting Diodes with CIE x, y (≤ 0.15) and Low Efficiency Roll‐Off by Employing a High Triplet Energy Bipolar Host Material
Authors: Maheshwaran Athithan , Sree Vijaya Gopalan , Park Ho‐Yeol , Kim Hyein , Han Si Hyun , Lee Jun Yeob , Jin Sung‐Ho 
Published: July 2018

AbstractRecently, bipolar host materials are the most promising candidates for achieving high performance phosphorescent organic light‐emitting diodes (PHOLEDs) in order to maximize recombination efficiency. However, the development of host material with high triplet energy (E
T) is still a great challenge to date to overcome the limitations associated with the present PHOLEDs. Herein, a highly efficient donor‐π‐acceptor (D‐π‐A) type bipolar host (4′‐(9H‐carbazol‐9‐yl)‐2,2′‐dimethyl‐[1,1′‐biphenyl]‐4‐yl)diphenylphosphine oxide (m‐CBPPO) comprising of carbazole, 2,2′‐dimethylbiphenyl and diphenylphosphoryl as D‐π‐A unit, respectively, is developed. Interestingly, a high E
T of 3.02 eV is observed for m‐CBPPO due to highly twisted conformation. Furthermore, the new host material is incorporated in PHOLEDs as emissive layer with a new carbene type Ir(cb)3 material as a deep‐blue emitter. The optimized devices show an excellent external quantum efficiency (EQE) of 24.8% with a notable Commission internationale de l'éclairage (x, y) ≤ 0.15, (0.136, 0.138) and high electroluminescence performance with extremely low efficiency roll‐off. Overall, the above EQE is the highest reported for deep‐blue PHOLEDs with very low efficiency roll‐off and also indicate the importance of appropriate host for the development of high performance deep‐blue PHOLEDs.
3D‐Plotted Beta‐Tricalcium Phosphate Scaffolds with Smaller Pore Sizes Improve In Vivo Bone Regeneration and Biomechanical Properties in a Critical‐Sized Calvarial Defect Rat Model
Authors: Diao Jingjing , OuYang Jun , Deng Ting , Liu Xiao , Feng Yanting , Zhao Naru , Mao Chuanbin , Wang Yingjun 
Published: July 2018

AbstractDue to the difficulty in fabricating bioceramic scaffolds with smaller pore sizes by the current 3D printing technique, the effect of smaller pore sizes (below 400 µm) of 3D printed bioceramic scaffolds on the bone regeneration and biomechanical behavior is never studied. Herein beta‐tricalcium phosphate (β‐TCP) scaffolds with interconnected smaller pores of three different sizes (100, 250, and 400 µm) are fabricated by 3D plotting. The resultant scaffolds are then implanted into rat critical‐sized calvarial defects without any seeded cells. A custom‐designed device is developed to investigate the biomechanical properties of the scaffolds after surgical implantation for 4, 8, and 12 weeks. The scaffolds with the 100 µm pore size are found to present the highest maximum load and stiffness, comparable to those of the autogenous bone, after being implanted for 12 weeks. Micro‐computed tomography (micro‐CT) and histological analysis further indicate that the scaffolds with the 100 µm pore size achieve the highest percentage of new bone ingrowth, which correlates to their best in vivo biomechanical properties. This study demonstrates that tailoring the pore size of β‐TCP scaffolds to a smaller range by 3D‐plotting can be a facile and efficient approach to enhanced bone regeneration and biomechanical behaviors in bone repair.
Carbon‐Rich Nanomaterials: Fascinating Hydrogen and Oxygen Electrocatalysts
Authors: Zhang Jian , Chen Guangbo , Müllen Klaus , Feng Xinliang 
Published: July 2018

AbstractHydrogen energy is commonly considered as a clean and sustainable alternative to the traditional fossil fuels. Toward universal utilization of hydrogen energy, developing high‐efficiency, low‐cost, and sustainable energy conversion technologies, especially water‐splitting electrolyzers and fuel cells, is of paramount significance. In order to enhance the energy conversion efficiency of the water‐splitting electrolyzers and fuel cells, earth‐abundant and stable electrocatalysts are essential for accelerating the sluggish kinetics of hydrogen and oxygen reactions. In the past decade, carbon‐rich nanomaterials have emerged as a promising class of hydrogen and oxygen electrocatalysts. Here, the development and electrocatalytic activity of various carbon‐rich materials, including metal‐free carbon, conjugated porous polymers, graphdiyne, covalent organic frameworks (COFs), atomic‐metal‐doped carbon, as well as metal–organic frameworks (MOFs), are demonstrated. In particular, the correlations between their porous nanostructures/electronic structures of active centers and electrocatalytic performances are emphatically discussed. Therefore, this review article guides the rational design and synthesis of high‐performance, metal‐free, and noble‐metal‐free carbon‐rich electrocatalysts and eventually advances the rapid development of water‐splitting electrolyzers and fuel cells toward practical applications.
High‐Efficiency and Wide‐Angle Beam Steering Based on Catenary Optical Fields in Ultrathin Metalens
Authors: Guo Yinghui , Ma Xiaoliang , Pu Mingbo , Li Xiong , Zhao Zeyu , Luo Xiangang 
Published: July 2018

AbstractRecent advances in artificial subwavelength structures promise the realization of ultrathin, lightweight, and flat metalens, providing a potential candidate for traditional bulky and curved lens. Nevertheless, most metalenses are generally suffering from serious off‐axis aberration, resulting in a limited field‐of‐view (FOV). Here, a methodology to extend the FOV of metalens is presented by exploring the local catenary optical fields and symmetry transformation from rotational symmetry to transversal symmetry. As a proof of the concept, a high efficiency (>80% even when the incidence angle is titled by 60°) and ultrathin (≈0.127 λ) metalens consisting of bilayer geometric metasurface is designed, fabricated, and characterized. The wide FOV of metalens benefiting from local catenary fields and symmetry transformation is numerically demonstrated by full‐wave simulation and ray tracing method. Moreover, the wide‐angle beam steering ability beyond ± 60° is experimentally demonstrated, which exhibits obvious advantages compared with previous beam steering transmitarrays. The novelty of the proposed methodology lies at the fact that both transversal and longitudinal local catenary fields are excited in a single component: the transversal catenary field is utilized for high efficiency spin–orbit interaction and phase modulation, while the longitudinal catenary field and symmetry transformation ensure wide‐angle operation.
Rh(III)‐Catalyzed C‐H Amination of Azobenzenes with Anthranils
Authors: Fu Ting , Yang Jun , Sun Huihui , Zhang Chichen , Xiang Haifeng , Zhou Xiangge 
Published: July 2018

AbstractAn efficient Rh(III)‐catalyzed C−H amination of azobenzenes with anthranils was developed. A range of azobenzenes were aminated under mild conditions in high yields (up to 92%) with good regioselectivity and atomic economy. The formed ortho‐aminocarbonyl skeleton could be converted to a series of biologically interesting heterocyclic compounds including a dibenzodiazepine, an acridine and an N‐aryl indole.
Concurrent Radical Addition and [3+2] Cycloaddition between Nitrones and Maleimide‐Based Acyclic Enediynes
Authors: Li Jing , Zhang Mengsi , Huang Shuai , Ding Yun , Hu Aiguo 
Published: July 2018

AbstractEnediyne compounds undergo Bergman cyclization while being activated with thermal or UV‐light triggers, and generate benzyne diradical intermediates, endowing their great potential as antitumor agents. The radical nature of the Bergman cyclization is generally confirmed through radical trapping experiments. While using phenyl tert‐butyl nitrone (PBN) as a radical trapping agent to study the Bergman cyclization of maleimide‐based enediyne compounds, we uncovered concurrent radical addition and [3+2] cycloaddition reactions between nitrones and enediyne compounds. The radical addition between the diradical intermediates and PBN was revealed through EPR analysis, while the [3+2] cycloaddition products were separated out and their structures were confirmed by NMR, HRMS and single crystal XRD analysis. Computational investigations showed that the energy barrier of the [3+2] cycloaddition was much lower than that of the Bergman reaction, corroborating the dominance of [3+2] cycloaddition between nitrone and enediyne compounds.
Förster‐Resonanzenergietransfer‐basierter Nachweis intrazellulärer Ketal‐Hydrolyse in synthetisch vernetzten Nanopartikeln
Authors: Nuhn Lutz , Van Herck Simon , Best Andreas , Deswarte Kim , Kokkinopoulou Maria , Lieberwirth Ingo , Koynov Kaloian , Lambrecht Bart N. , De Geest Bruno G. 
Published: July 2018

AbstractDer Einbau abbaubarer Vernetzungen gilt als vielversprechende Strategie, synthetische Nanopartikel, die durch Verdünnungs‐ und Verdrängungseffekte zerfallen könnten, in komplexen physiologischen Umgebung besser zu stabilisieren. Hierbei haben sich in vielen biomedizinischen Anwendungen Ketale als äußerst nützlich erwiesen, da sie unter physiologischen Bedingungen recht stabil sind, aber gegenüber krankheitsbedingt oder intrazellulär niedrigen pH‐Werten eine hohe Hydrolyseempfindlichkeit aufweisen. Trotz der Vielzahl an spektroskopisch oder chromatographisch zugänglichen Nachweismethoden, mit denen der chemische Abbau in Lösung recht einfach gezeigt werden kann, gestaltet sich der Nachweis einer Ketalhydrolyse innerhalb synthetischer Nanomaterialien durch lebende Organismen als schwierig. In dieser Arbeit stellen wir eine Förster‐Resonanzenergietransfer(FRET)‐basierte Methode vor, mit der die Disassemblierung Blockpolymer‐basierter Nanopartikel bestätigt wurde. Dabei wurden einzelne Ketten jeweils mit einem FRET‐Farbstoffpaar markiert, ehe sie nach Selbstassemblierung kovalent mit pH‐sensiblen Ketal‐Vernetzern stabilisiert wurden.
Dynamische Kopplung bei niedriger Reynoldszahl
Authors: Dey Krishna Kanti 
Published: July 2018

AbstractAktive Kolloide, bei denen kollektives und emergentes Verhalten auftritt, gewähren nützliche Einblicke in die statistische Physik von Nichtgleichgewichtssystemen. Um die Prinzipien des Energietransfers unter den Bedingungen einer niedrigen Reynoldszahl kennenzulernen, hat man Kolloidsuspensionen untersucht, die aktive Mikroschwimmer enthalten. Studien an aktiven Enzymen und metallorganischen Katalysatoren im Ångström‐Bereich belegten, dass bereits Moleküle Energie auf ihre Umgebung übertragen und dadurch die Gesamtdynamik des Systems substantiell beeinflussen können. Anhand der Diffusion von unreaktiven Tracern in einer aktiven Lösung wurde gezeigt, dass der Energietransfer in Systemen mit unterschiedlichen Schwimmern ähnlich abläuft – ungeachtet der Größe, der Art der Energieübertragung und des Antriebssystems des Schwimmers. Dieser Aufsatz diskutiert bisherige Forschungsergebnisse und die beobachteten Gemeinsamkeiten bei der dynamischen Kopplung von Schwimmern mit der Umgebung.
Intensely Photoluminescent Diamidophosphines of the Alkaline‐Earth Metals, Aluminum, and Zinc
Authors: Bestgen Sebastian , Schoo Christoph , Neumeier B. Lilli , Feuerstein Thomas J. , Zovko Christina , Köppe Ralf , Feldmann Claus , Roesky Peter W. 
Published: July 2018

AbstractThe positively charged and weakly polarizable s‐block metals commonly do not usually have phosphine ligands in molecular complexes. Herein, we report mono‐ and dinuclear small diamidophosphine complexes of the alkaline‐earth metals Mg, Ca, and Sr, which were prepared from simple precursors and a phosphine‐functionalized diamine ligand N,N‐bis(2‐(diphenyl‐phosphino)phenyl)ethane‐1,2‐diamine (PNHNHP). The alkaline‐earth metal based complexes [(PNNP)Mg]2 and [(PNNP)M(thf)3] (M=Ca, Sr), exhibit unusual coordination spheres and show bright fluorescence, both in the solid state and in solution. For comparison, the even stronger luminescent Al and Zn complexes [(PNNP)Zn]2 and [(PNNP)AlCl] were prepared. Emission lifetimes in the nanosecond range and high photoluminescence quantum yields up to 93 % are observed at room temperature.
Dissipative Self‐Assembly of Photoluminescent Silicon Nanocrystals
Authors: Grötsch Raphael K. , Angı Arzu , Mideksa Yonatan G. , Wanzke Caren , Tena‐Solsona Marta , Feige Matthias J. , Rieger Bernhard , Boekhoven Job 
Published: July 2018

AbstractSolutions of silicon nanocrystals (SiNCs) are used in a diverse range of applications because of their tunable photoluminescence, biocompatibility, and the abundance of Si. In dissipative supramolecular materials, self‐assembly of molecules or nanoparticles is driven by a chemical reaction network that irreversible consumes fuel. The properties of the emerging structures are controlled by the kinetics of the underlying chemical reaction network. Herein, we demonstrate the dissipative self‐assembly of photoluminescent SiNCs driven by a chemical fuel. A chemical reaction induces self‐assembly of the water‐soluble SiNCs. However, the assemblies are transient, and when the chemical reaction network runs out of fuel, the SiNCs disassemble. The lifetime of the assemblies is controlled by the amount of fuel added. As an application of the transient supramolecular material, we demonstrate that the platform can be used to control the delayed uptake of the nanocrystals by mammalian cells.
Nano–silica functionalized with thiol–based dendrimer as a host for gold nanoparticles: An efficient and reusable catalyst for chemoselective oxidation of alcohols
Authors: Haghshenas Kashani Sara , Landarani‐Isfahani Amir , Moghadam Majid , Tangestaninejad Shahram , Mirkhani Valiollah , Mohammadpoor‐Baltork Iraj 
Published: July 2018

In this paper, we present the synthesis of Au nanoparticles supported on nanosilica thiol based dendrimer, nSTDP. The catalyst was prepared by reduction of HAuCl4 with NaBH4 in the presence of nSTDP. The resulting Aunp–nSTDP materials were characterized by FT–IR and UV–vis spectroscopic methods, SEM, TEM, TGA, XPS and ICP analyses. The characterization of the catalyst showed that Au nanoparticles with the size of 2–6 nm are homogeneously distributed on the nSTDP dendrimer with a catalyst loading of about 0.19 mmol/g of catalyst. The Aunp–nSTDP catalyst was used in the oxidation of alcohols with tert–butyl hydroperoxide (TBHP) as oxidant. The influence of vital reaction parameters such as solvent, oxidant and amount of catalyst on the oxidation of alcohols was investigated. These reactions were best performed in an acetonitrile/water mixture (3:2) in the presence of 0.76 mol% of the catalyst on the basis of the Au content at 80 °C under atmospheric pressure of air to afford the desired products in high yields (80–93% for benzyl alcohols). The Aunp–nSTDP catalyst exhibited a high selectivity toward the corresponding aldehyde and ketone (up to 100%). Reusabiliy and stability tests demonstrated that the Aunp–nSTDP catalyst can be recycled with a negligible loss of its activity. Also this catalytic exhibited a good chemoselectivity in the oxidation of alcohols.
MoP/Al2O3 as a novel catalyst for sulfur‐resistant methanation
Authors: Wang Baowei , Zhao Jun , Meng Dajun , Li Zhenhua , Xu Yan , Ma Xinbin 
Published: July 2018

We reported γ‐alumina supported molybdenum phosphide (MoP) catalysts as a novel catalyst for sulfur‐resistant methanation reaction. The precursors of the catalyst were prepared by impregnation method and the effect of reduction temperatures (550 °C, 600 °C, 650 °C) of the precursors for sulfur‐resistant methanation was examined. The results indicated catalyst obtained by lower reduction temperature delivered better sulfur‐resistant methanation performance. Meanwhile, the influence of H2/CO ratios and H2S content was also investigated. The results indicated that high H2/CO ratio and low H2S content was favorable for methanation of MoP catalysts. The catalysts were characterized by N2 adsorption–desorption, XRD, XPS and TEM. The results confirmed that the MoP phase was formed on all the catalysts and the physicochemical properties of the samples influenced the performance for sulfur‐resistant methanation.
Enhanced Cleavage at Abasic Sites within Clustered Lesions in Nucleosome Core Particles
Authors: Yang Kun , Greenberg Marc M. 
Published: July 2018

AbstractClustered lesions are a hallmark of γ‐radiolysis, but are produced by other damaging agents as well. Bistranded clustered lesions are precursors to double‐strand breaks and are challenging to repair, thus making them an especially deleterious form of DNA damage. An abasic site (AP) is an alkaline‐labile lesion frequently present in clustered lesions. Strand scission at an AP site is accelerated ≈100‐fold in nucleosome core particles (NCPs). We examined how AP reactivity was affected within clustered lesions in NCPs. The rate constant of strand scission is increased as much as 2.5‐fold in the presence of a proximal abasic site or thymidine glycol in the complementary strand. A proximal mispair has a similar effect on AP reactivity. Increased AP reactivity within a clustered lesion correlates with decreased UV melting temperatures of the corresponding duplexes compared to one containing an isolated abasic site. However, the thermodynamics of duplex melting do not correlate with AP reactivity within different clustered lesions. Overall, increased AP reactivity within clustered lesions is attributed to greater access of histone proteins to the lesion due to decreased duplex stability.
Hybrid Molecular Container Based on Glycoluril and Triptycene: Synthesis, Binding Properties, and Triggered Release
Authors: Liu Wenjin , Lu Xiaoyong , Xue Weijian , Samanta Soumen K. , Zavalij Peter Y. , Meng Zihui , Isaacs Lyle 
Published: July 2018

AbstractWe designed and synthesized a “hybrid” molecular container 1, which is structurally related to both cucurbit[n]uril (CB[n]) and pillar[n]arene type receptors. Receptor 1 was fully characterized by 1H NMR, 13C NMR, IR, MS and X‐ray single crystal diffraction. The self‐association behavior, host–guest recognition properties of 1, and the [salt] dependence of Ka were investigated in detail by 1H NMR and isothermal titration calorimetry (ITC). Optical transmittance and TEM measurements provide strong evidence that receptor 1 undergoes co‐assemble with amphiphilic guest C10 in water to form supramolecular bilayer vesicles (diameter 25.6±2.7 nm, wall thickness ≈3.5 nm) that can encapsulate the hydrophilic anticancer drug doxorubicin (DOX) and the hydrophobic dye Nile red (NR). The release of encapsulated DOX or NR from the vesicles can be triggered by hexamethonium (8 c) or spermine (10) which leads to the disruption of the supramolecular vesicles.
Redox‐Active Chiroptical Switching in Mono‐ and Bis‐Iron Ethynylcarbo[6]helicenes Studied by Electronic and Vibrational Circular Dichroism and Resonance Raman Optical Activity
Authors: Shen Chengshuo , Srebro‐Hooper Monika , Weymuth Thomas , Krausbeck Florian , Navarrete Juan T. López , Ramírez Francisco J. , Nieto‐Ortega Belén , Casado Juan , Reiher Markus , Autschbach Jochen , Crassous Jeanne 
Published: July 2018

AbstractIntroducing one or two alkynyl–iron moieties onto a carbo[6]helicene results in organometallic helicenes (2 a,b) that display strong chiroptical activity combined with efficient redox‐triggered switching. The neutral and oxidized forms have been studied in detail by electronic and vibrational circular dichroism, as well as by Raman optical activity (ROA) spectroscopy. The experimental results were analyzed and spectra were assigned with the help of first‐principles calculations. In particular, a recently developed method for ROA calculations under resonance conditions has been used to study the intricate resonance effects on the ROA spectrum of mono‐iron ethynylhelicene 2 a.