bluuebunny/crossref_metadata_2025_split huggingface dataset:
Comparison of Remission and Lupus Low Disease Activity State in Damage Prevention in a United States Systemic Lupus Erythematosus Cohort
Authors: Petri Michelle , Magder Laurence S. 
Published: May 2018

ObjectiveOne objective in the treatment of systemic lupus erythematosus (SLE) disease activity is to reduce long‐term rates of organ damage. We undertook this study to analyze data from a large clinical SLE cohort to compare patients achieving different levels of disease activity with respect to rates of long‐term damage.MethodsWe analyzed data from 1,356 SLE patients in the Hopkins Lupus Cohort, followed up quarterly, with 77,105 person‐months observed from 1987 to 2016. Three outcome measures were considered: clinical remission with no treatment, clinical remission on treatment, and lupus low disease activity state (LLDAS).ResultsPatients achieved LLDAS in 50% of their follow‐up months. They achieved clinical remission with no treatment or clinical remission on treatment in only 13% and 27%, respectively, of their follow‐up visits. The rates of damage consistently declined with increased percentage of prior time in either LLDAS or clinical remission on treatment. Spending a short proportion of prior time (<25%) in clinical remission on treatment was associated with a relatively low rate of damage compared to never achieving that condition (1.01 events per 10 person‐years versus 1.82 events per 10 person‐years; rate ratio 0.54, P < 0.0001). Those patients who experienced LLDAS at least 50% of the time had relatively low rates of damage (rate ratio 0.39–0.47, P < 0.0001).ConclusionLLDAS is an easier target to achieve than clinical remission on treatment and results in reduced risk of long‐term damage. However, even a small percentage of time in clinical remission on treatment was associated with reduced damage.
Epidemiology and Outcomes of Granulomatosis With Polyangiitis in Pediatric and Working‐Age Adult Populations In the United States
Authors: Panupattanapong Sirada , Stwalley Dustin L. , White Andrew J. , Olsen Margaret A. , French Anthony R. , Hartman Mary E. 
Published: May 2018

ObjectiveThe incidence and prevalence of granulomatosis with polyangiitis (GPA) in the US is not well characterized. Owing to its rarity, outcomes data in pediatric‐onset GPA are also lacking. The aims of this study were to describe the epidemiology of GPA and outcomes in GPA patients in the US, and to compare outcomes between pediatric and working‐age adult patients.MethodsA retrospective cohort study using the 2006–2014 Truven Health Analytics MarketScan Commercial Claims and Encounters Database was conducted. The incidence and prevalence rates of pediatric and adult GPA (age <65 years) were calculated. Outcomes among the 2 age groups were analyzed.ResultsA total of 5,562 cases of GPA were identified, of which 214 (3.8%) were pediatric onset and 5,348 (96.2%) were adult onset. The incidence rate of pediatric‐onset GPA was 1.8 cases per 1 million person‐years, compared to 12.8 cases per 1 million person‐years in working‐age adults. There was a slight female preponderance in both groups (63% and 53% among pediatric and adult GPA patients, respectively). Rates of hospitalization and severe infections were high in both children and working‐age adults, but children had more frequent hospitalizations (rate ratio [RR] 1.3 [95% confidence interval (95% CI) 1.1–1.4]) and 2–3‐times higher rates of leukopenia (RR 2.6 [95% CI 1.5–4.3]), neutropenia (RR 2.2 [95% CI 1.2–4.0]), and hypogammaglobulinemia (RR 3.7 [95% CI 2.0–6.4]). Time‐to‐event analyses showed no differences in the time to hospitalization, severe infection, major relapse, or end‐stage renal disease.ConclusionThis study represents the largest cohort of GPA reported to date. Pediatric GPA patients experienced more frequent hospitalizations and were more vulnerable to hematologic complications than non‐elderly adult patients.
Ring‐to‐Cage Structural Conversion via Template Effect in a Gold(I) Metallosupramolecular System
Authors: Nishiura Misa , Kojima Tatsuhiro , Igashira‐Kamiyama Asako , Konno Takumi 
Published: May 2018

AbstractA unique example of a ring‐to‐cage structural conversion in a multinuclear gold(I) coordination system with d‐penicillamine (d‐H2pen) is reported. The reaction of [Au2Cl2(dppe)] (dppe=1,2‐bis(diphenylphosphino)ethane) with d‐H2pen in a 1:1 ratio gave [Au4(dppe)2(d‐pen)2] ([1]), in which two [Au2(dppe)]2+ units are linked by two d‐pen S atoms in a cyclic form so as to have two bidentate‐N,O coordination arms. The subsequent reaction of [1] with Cu(OTf)2 afforded [Au4Cu(dppe)2(d‐pen)2]2+ ([2]2+), in which a CuII ion is chelated by the two coordination arms in [1] to form an AuI4CuII bicyclic metallocage. A similar reaction using Cu(NO3)2 was accompanied by the ring expansion of [1] to [Au8(dppe)4(d‐pen)4], leading to the production of [Au8Cu2(dppe)4(d‐pen)4]4+ ([3]4+). In [3]4+, two CuII ions are each chelated by the two coordination arms to form an AuI8CuII2 tricyclic metallocage, accommodating a nitrate ion. The use of Ni(NO3)2 or Ni(OAc)2 instead of Cu(NO3)2 commonly gave a tricyclic metallocage of [Au8Ni2(dppe)4(d‐pen)4]4+ ([4]4+), but a water molecule was accommodated inside the AuI8NiII2 metallocage.
Hypoglycemic Effects of a Polysaccharide from Tetrastigma hemsleyanum Diels & Gilg in Alloxan‐Induced Diabetic Mice
Authors: Ru Yi , Chen Xiao , Xu Jie , Huang Lihong , Jiang Miaoshan , Guo Longhua , Lin Zhenyu , Qiu Bin , Wong Kwok‐Yin 
Published: May 2018

Tetrastigma hemsleyanum Diels & Gilg, a well‐known traditional Chinese medicine, possesses antitumor and anti‐inflammatory activity, etc. However, the anti‐diabetic effect has not been determined. In our present study, a water‐soluble polysaccharide, named THP with molecular weight of 93 307 Da, was isolated from T. hemsleyanum by DEAE‐52 ion‐exchange and Sephadex G‐100 chromatography. It contains rhamnose, arabinose, mannose, glucose, and galactose in the molar ratio of 0.07:0.14:0.38:0.21:0.31. Then anti‐diabetic effects of THP were examined by treating alloxan‐induced diabetic mice with different doses (100, 200, and 300 mg/kg) of THP orally. The results showed that THP could decrease the blood glucose, TC, TG, LDL‐C levels, increase the body weight, HDL‐C, insulin levels, and enhance the activities of antioxidant enzyme system in alloxan‐induced diabetic mice. Furthermore, the histopathological examination of pancreas, liver, and kidney indicated that THP could protect and reverse β‐cells in diabetic mice with low damage to liver and kidney, which suggests that THP may stimulate pancreatic release of insulin and can be an effectively potential candidate for diabetes mellitus.
Coordination‐Assisted Bioorthogonal Chemistry: Orthogonal Tetrazine Ligation with Vinylboronic Acid and a Strained Alkene
Authors: Eising Selma , Xin Bo‐Tao , Kleinpenning Fleur , Heming Jurriaan J. A. , Florea Bogdan I. , Overkleeft Herman S. , Bonger Kimberly M. 
Published: May 2018

AbstractBioorthogonal chemistry can be used for the selective modification of biomolecules without interfering with any other functionality that might be present. Recent developments in the field include orthogonal bioorthogonal reactions to modify multiple biomolecules simultaneously. During our research, we observed that the reaction rates for the bioorthogonal inverse‐electron‐demand Diels–Alder (iEDDA) reactions between nonstrained vinylboronic acids (VBAs) and dipyridyl‐s‐tetrazines were exceptionally higher than those between VBAs and tetrazines bearing a methyl or phenyl substituent. As VBAs are mild Lewis acids, we hypothesised that coordination of the pyridyl nitrogen atom to the boronic acid promoted tetrazine ligation. Herein, we explore the molecular basis and scope of VBA–tetrazine ligation in more detail and benefit from its unique reactivity in the simultaneous orthogonal tetrazine labelling of two proteins modified with VBA and norbornene, a widely used strained alkene. We further show that the two orthogonal iEDDA reactions can be performed in living cells by labelling the proteasome by using a nonselective probe equipped with a VBA and a subunit‐selective VBA bearing a norbornene moiety.
Discovery of the Tiancilactone Antibiotics by Genome Mining of Atypical Bacterial Type II Diterpene Synthases
Authors: Dong Liao‐Bin , Rudolf Jeffrey D. , Deng Ming‐Rong , Yan Xiaohui , Shen Ben 
Published: May 2018

AbstractAlthough genome mining has advanced the identification, discovery, and study of microbial natural products, the discovery of bacterial diterpenoids continues to lag behind. Herein, we report the identification of 66 putative producers of novel bacterial diterpenoids, and the discovery of the tiancilactone (TNL) family of antibiotics, by genome mining of type II diterpene synthases that do not possess the canonical DXDD motif. The TNLs, which are broad‐spectrum antibiotics with moderate activities, are produced by both Streptomyces sp. CB03234 and Streptomyces sp. CB03238 and feature a highly functionalized diterpenoid skeleton that is further decorated with chloroanthranilate and γ‐butyrolactone moieties. Genetic manipulation of the tnl gene cluster resulted in TNL congeners, which provided insights into their biosynthesis and structure–activity relationships. This work highlights the biosynthetic potential that bacteria possess to produce diterpenoids and should inspire continued efforts to discover terpenoid natural products from bacteria.
Comparative Study of Li4Ti5O12 Composites Prepared withPristine, Oxidized, and Surfactant‐Treated Multiwalled Carbon Nanotubes for High‐Power Hybrid Supercapacitors
Authors: Lee Geon‐Woo , Kim Myeong‐Seong , Jeong Jun Hui , Roh Ha‐Kyung , Roh Kwang Chul , Kim Kwang‐Bum 
Published: May 2018

AbstractIn hybrid supercapacitors, lithium‐ion battery (LIB)‐type intercalation materials have slower reaction kinetics than electrical double‐layer‐capacitor‐type carbonaceous materials. Thus, it is of prime importance to improve the rate capability of LIB‐type intercalation materials to achieve high energy density as well as high power density from hybrid supercapacitors. In this study, we report Li4Ti5O12/pristine multiwalled carbon nanotube (LTO/P‐MWCNT) composites with high rate capability and demonstrate their anode application for high‐power hybrid supercapacitors. For comparison, two additional LTO composites are prepared by using oxidized MWCNTs and surfactant‐treated MWCNTs through a similar spray‐drying process. The LTO/P‐MWCNT composite shows superior rate capability over the other two composites, owing to the high electrical conductivity of pristine MWCNTs. The hybrid supercapacitor composed of a LTO/P‐MWCNT anode and an activated carbon cathode delivers an energy density of 70.9 Wh kg−1 at a power density of 0.03 kW kg−1 and a maximum power density of 21.8 kW kg−1 is achieved at an energy density of 24.3 Wh kg−1. Furthermore, the hybrid supercapacitor exhibits excellent cycling stability. These salient results provide further impetus to the use of MWCNTs in the design and synthesis of high‐rate oxide‐based composites with efficient lithium‐ion transport and high electrical conductivity for high‐power hybrid supercapacitors and high‐power LIBs.
Selective Photooxidation of Sulfides Catalyzed by Bis‐cyclometalated IrIII Photosensitizers Bearing 2,2′‐Dipyridylamine‐Based Ligands
Authors: Vaquero Mónica , Ruiz‐Riaguas Alba , Martínez‐Alonso Marta , Jalón Félix A. , Manzano Blanca R. , Rodríguez Ana M. , García‐Herbosa Gabriel , Carbayo Arancha , García Begoña , Espino Gustavo 
Published: May 2018

AbstractA new family of heteroleptic bis‐cyclometalated IrIII complexes with formula [Ir(
)2(
)]Cl (
=2‐phenylpyridinate and
=2,2′‐dipyridylamine or N‐benzylated 2,2′‐dipyridylamines, were synthesized, characterized, and successfully used as photosensitizers in the catalytic photooxidation of an array of dialkyl, dibenzyl, alkyl aryl, and diaryl sulfides, as well as sulfur‐containing amino acids. Furthermore, the reactions proceeded with optimal chemoselectivity, and atom economy under mild conditions. Experimental observations support a dual mechanism in which singlet oxygen and superoxide are the actual oxidants.
Nucleophilic Influences and Origin of the SN2 Allylic Effect
Authors: Galabov Boris , Koleva Gergana , Schaefer Henry F. , Allen Wesley D. 
Published: May 2018

AbstractThe potential energy surfaces for the SN2 reactions of allyl and propyl chlorides with 21 anionic and neutral nucleophiles was studied by using ωB97X‐D/6‐311++G(3df,2pd) computations. The “allylic effect” on SN2 barriers was observed for all reactions, and compared with propyl substrates, the energy barriers differed by −0.2 to −4.5 kcal mol−1 in the gas phase. Strong correlations of the SN2 net activation barriers with cation affinities, proton affinities, and electrostatic potentials at nuclei demonstrated the powerful influence of electrostatic interactions on these reactions. For the reactions of anionic (but not neutral) nucleophiles with allyl chloride, some of the incoming negative charge (0.2–18 %) migrated into the carbon chains, which would provide secondary stabilization of the SN2 transition states. Activation strain analysis provided additional insight into the allylic effect by showing that the energy of geometric distortion for the reactants to reach the SN2 transition state was smaller for each allylic reaction than for its propyl analogue. In many cases, the interaction energies between the substrate and nucleophile in this analysis were more favorable for propyl chloride reactions, but this compensation did not overcome the predominant strain energy effect.
Fabrication of Photonic Bandgap Materials by Shifting Double Frameworks
Authors: Sheng Qingqing , Mao Wenting , Han Lu , Che Shunai 
Published: May 2018

AbstractBiological organisms have evolved over millions of years to generate tremendously complex structures on a nanometer to micrometer scale. Among them, a range of three‐dimensional (3D) biological photonic structures with minimal surface or constant mean curvature surfaces have been discovered in the wing scales of insects, attracting a great deal of interest because of their unique optical properties, such as structural color, antireflection, light collection, and photonic band gaps. Single‐diamond and single‐gyroid surface structures are considered to be excellent photonic crystals with complete band gaps. Although the corresponding bicontinuous architectures have been synthesized by self‐assembly, single‐framework structures are thermodynamically unfavorable and have been only achieved by physical fabrications and the alternating gyroid method. The production of materials derived from the thermodynamically stable double‐framework structures provides a feasible solution for their chemical construction. This concept article highlights the significant progress in understanding 3D photonic structures by shifting double‐frameworks to form low‐symmetry structures, the physical properties of which can be greatly altered. Specifically, a complete photonic band gap can be achieved via a shifted double‐diamond structure composed of materials with high dielectric contrast and high refractive index. We believe this concept will provide new insights in interdisciplinary research areas including the study of photonic structures, the self‐assembly of amphiphilic molecules and the formation of biological architectures.
A Cyclometalated IrIII Complex as a Lysosome‐Targeted Photodynamic Therapeutic Agent for Integrated Imaging and Therapy in Cancer Cells
Authors: Sudheesh Karivachery V. , Jayaram Prasad S. , Samanta Animesh , Bejoymohandas Kochan S. , Jayasree Ramapurath S. , Ajayaghosh Ayyappanpillai 
Published: May 2018

AbstractOrganelle‐targeted photosensitizers (PSs) having luminescence properties are potential theranostic agents for simultaneous luminescence imaging and photodynamic therapy. Herein, we report a water‐soluble luminescent cyclometalated IrIII complex, Ir‐Bp‐Ly, as a lysosome‐targeted theranostic probe. Ir‐Bp‐Ly exhibits exceptional photophysical properties, with good triplet‐state quantum yield (0.90), singlet oxygen generation quantum yield (0.71 at pH 4), and long lifetime (1.47 μs). Interestingly, Ir‐Bp‐Ly localizes mostly in lysosomes due to the presence of morpholine units, suggesting its potential use as a lyso‐tracker. Ir‐Bp‐Ly displays a notable PDT effect in C6 glioma cells, efficiently generating reactive oxygen species owing to close proximity between the energy levels of its triplet state and those of molecular oxygen (3O2). The mechanism of cell death has been studied through caspase‐3/7 and flow cytometry analyses, which clearly established the apoptotic pathway.
Multi‐Valent Group 14 Chalcogenide Architectures from Ionic Liquids: 0D‐{[Cs@SnII4(GeIV4Se10)4]7−} and 2D‐{[SnII(GeIV4Se10)]2−}
Authors: Santner Silke , Wolff Alexander , Ruck Michael , Dehnen Stefanie 
Published: May 2018

AbstractIn order to explore if and how salts comprising polycations and salts comprising polyanions might interact, the [AlBr4]− salt of the [Pt@Bi10]4+ cluster cation was added to the reaction mixture for the synthesis of the supersphere cluster anion [Ge24Sn36Se132]24− from Cs4[Ge4Se10]⋅H2O and SnCl4⋅5 H2O under ionothermal conditions at 120 °C. Indeed, the reaction yields two new compounds, depending on the cation of the used ionic liquid. Apparently, the polycation is not retained under the given conditions, but it acts as a reductant affording SnII. In a (C4C1C1im)+‐based ionic liquid mixture, a unique supertetrahedral anion is obtained that embeds a Cs+ cation, 0D‐{[Cs@SnII4(GeIV4Se10)4]7−}, while (C4C1im)+ cations stabilize an unprecedented ternary layered anion, 2D‐{[SnII(GeIV4Se10)]2−}. Test reactions with common sources of SnII did not afford the new compounds, indicating the necessity of an in situ reduction, for which the polycation seems appropriate.
Sulfides and Disulfides of s‐Triazine: Potential Thermal Thiyl Radical Generators
Authors: Höhne Carl‐Christoph , Posern Christian , Böhme Uwe , Kroke Edwin 
Published: May 2018

AbstractA series of aliphatic and aromatic thioethers and dithioethers of s‐triazine were synthesised to study their thermal properties, in particular the thermally induced thiyl radical generation ability. Four symmetric s‐triazine sulfides of the type (RS)3C3N3, namely 2,4,6‐tris(phenylthio)‐ (1), 2,4,6‐tris(para‐tolylthio)‐ (3), 2,4,6‐tris(ethylthio)‐ (5) and 2,4,6‐tris(tert‐butylthio)‐1,3,5‐triazine (7), as well as four symmetric s‐triazine disulfides of the type (RSS)3C3N3, namely 2,4,6‐tris(phenyldithio)‐ (2), 2,4,6‐tris(para‐tolyldithio)‐ (4), 2,4,6‐tris(ethyldithio)‐ (6) and 2,4,6‐tris(tert‐butyldithio)‐1,3,5‐triazine (8) were synthesised. All compounds were comprehensively characterised by 1H and 13C NMR, infrared and Raman spectroscopy as well as elemental analyses. Single‐crystal X‐ray diffraction analyses of 1, 2 and 5 are discussed. The thermal behaviour was studied by thermogravimetric analyses coupled with mass spectrometry (TGA‐MS) and quantum chemical calculations. Limiting oxygen index (LOI) flammability tests showed that the disulfides are the most promising radical generators, and are most likely suitable flame retardants for selected polymers.
Synthesis and Pharmacological Evaluation of Enantiomerically Pure GluN2B Selective NMDA Receptor Antagonists
Authors: Börgel Frederik , Szermerski Marina , Schreiber Julian A. , Temme Louisa , Strutz‐Seebohm Nathalie , Lehmkuhl Kirstin , Schepmann Dirk , Ametamey Simon M. , Seebohm Guiscard , Schmidt Thomas J. , Wünsch Bernhard 
Published: May 2018

AbstractTo determine the eutomers of potent GluN2B‐selective N‐methyl‐d‐aspartate (NMDA) receptor antagonists with a 3‐benzazepine scaffold, 7‐benzyloxy‐3‐(4‐phenylbutyl)‐2,3,4,5‐tetrahydro‐1H‐3‐benzazepin‐1‐ols (S)‐2 and (R)‐2 were separated by chiral HPLC. Hydrogenolysis and subsequent methylation of the enantiomerically pure benzyl ethers of (S)‐2 and (R)‐2 provided the enantiomeric phenols (S)‐3 and (R)‐3 [3‐(4‐phenylbutyl)‐2,3,4,5‐tetrahydro‐1H‐3‐benzazepine‐1,7‐diol] and methyl ethers (S)‐4 and (R)‐4. All enantiomers were obtained with high enantiomeric purity (≥99.7 % ee). The absolute configurations were determined by CD spectroscopy. R‐configured enantiomers turned out to be the eutomers in receptor binding studies and two‐electrode voltage clamp experiments. The most promising ligand of this compound series is the R‐configured phenol (R)‐3, displaying high GluN2B affinity (Ki=30 nm), high inhibition of ion flux (IC50=61 nm), and high cytoprotective activity (IC50=93 nm). Whereas the eudismic ratio in the receptor binding assay is 25, the eudismic ratio in the electrophysiological experiment is 3.
An Asymmetrical Cyanine Dye Nanoparticles for Small Vessel Photoacoustic Imaging In Vivo
Authors: Li Yunzheng , Xiong Jialiang , Shao Zixing , Ai Yongjian , Hua Ruimao , Luo Guoan , Liang Qionglin 
Published: May 2018

AbstractA novel asymmetrical cyanine dye (TR) with NIR absorption at 970 nm was synthesized and applied in photoacoustic imaging (PAI) in vivo for the first time. The advantages of asymmetrical structure in PAI was demonstrated with DFT calculation and verified by related experiments. BSA was selected as the matrix to encapsulate TR‐BSA nanoparticles (TR‐NPs) which was investigated as a PAI agent. Exceptional performance of TR‐NPs was shown in Balb/c rats caudal vein model; the details could be clearly displayed and identified at a 0.1 mm scale.
Tuning the Optical and Self‐Assembly Properties of Diketopyrrolopyrrole Semicarbazone Derivatives through Hydrogen Bonding
Authors: Militzer Swann , Tran Thi My Phuong , Mésini Philippe J. , Ruiz‐Carretero Amparo 
Published: May 2018

AbstractHydrogen bonds are great noncovalent interactions for guiding self‐assembly processes in organic semiconductors. Their presence in molecular structures allows to modify their aggregation state by changing the solvent, concentration and temperature. Here we show that just by functionalizing simple thiophene‐capped diketopyrrolopyrrole derivatives with semicarbazone units, the optical and self‐assembly properties can be tuned while controlling the formation of hydrogen bonding. The appearance of J‐type aggregates upon hydrogen‐bond formation made possible to vary the energy band gaps and supramolecular structures formed in solution and on thin films.
An autonomic‐computing approach on mapping threads to multi‐cores for software transactional memory
Authors: Zhou Naweiluo , Delaval Gwenaël , Robu Bogdan , Rutten Éric , Méhaut Jean‐François 
Published: May 2018

SummaryA parallel program needs to manage the trade‐off between the time spent in synchronisation and computation. This trade‐off is significantly affected by its parallelism degree. A high parallelism degree may decrease computing time while increasing synchronisation cost. Furthermore, thread placement on processor cores may impact program performance, as the data access time can vary from one core to another due to intricacies of the underlying memory architecture. Alas, there is no universal rule to decide thread parallelism and its mapping to cores from an offline view, especially for a program with online behaviour variation. Moreover, offline tuning is less precise. We present our work on dynamic control of thread parallelism and mapping. We address concurrency issues via Software Transactional Memory (STM). STM bypasses locks to tackle synchronisation through transactions. Autonomic computing offers designers a framework of methods and techniques to build autonomic systems with well‐mastered behaviours. Its key idea is to implement feedback control loops to design safe, efficient, and predictable controllers, which enable monitoring and adjusting controlled systems dynamically while keeping overhead low. We implement feedback control loops to automate management of threads and diminish program execution time.