bluuebunny/crossref_metadata_2025_split huggingface dataset:
Energetic Trinitro‐ and Fluorodinitroethyl Ethers of 1,2,4,5‐Tetrazines
Authors: Chavez David E. , Parrish Damon A. , Mitchell Lauren 
Published: June 2016

AbstractSeveral new energetic ethyl ethers of 1,2,4,5‐tetrazine have been synthesized. These molecules display good thermal stability, good oxygen balance, and high densities. Included in these studies are a 2,2,2‐trinitroethoxy 1,2,4,5‐tetrazine and two fluorodinitroethoxy 1,2,4,5‐tetrazines. One of these compounds was converted into the di‐N‐oxide derivative. The sensitivity of these materials towards destructive stimuli was determined, and overall the materials show promising energetic performance properties.
Enantioselective Intramolecular C−H Insertion of Donor and Donor/Donor Carbenes by a Nondiazo Approach
Authors: Zhu Dong , Ma Jun , Luo Kui , Fu Hongguang , Zhang Li , Zhu Shifa 
Published: June 2016

AbstractThe first enantioselective intramolecular C−H insertion and cyclopropanation reactions of donor‐ and donor/donor‐carbenes by a nondiazo approach are reported. The reactions were conducted in a one‐pot manner without slow addition and provided the desired dihydroindole, dihydrobenzofuran, tetrahydrofuran, and tetrahydropyrrole derivatives with up to 99 % ee and 100 % atom efficiency.
Integration of Nine Steps into One Membrane Reactor To Produce Synthesis Gases for Ammonia and Liquid Fuel
Authors: Li Wenping , Zhu Xuefeng , Chen Shuguang , Yang Weishen 
Published: June 2016

AbstractThe synthesis of ammonia and liquid fuel are two important chemical processes in which most of the energy is consumed in the production of H2/N2 and H2/CO synthesis gases from natural gas (methane). Here, we report a membrane reactor with a mixed ionic‐electronic conducting membrane, in which the nine steps for the production of the two types of synthesis gases are shortened to one step by using water, air, and methane as feeds. In the membrane reactor, there is no direct CO2 emission and no CO or H2S present in the ammonia synthesis gas. The energy consumption for the production of the two synthesis gases can be reduced by 63 % by using this membrane reactor. This promising membrane reactor process has been successfully demonstrated by experiment.
Template Synthesis, Metalation, and Self‐Assembly of Protic Gold(I)/(NHC)2 Tectons Driven by Metallophilic Interactions
Authors: Ruiz Javier , García Lucía , Sol Daniel , Vivanco Marilín 
Published: June 2016

AbstractA new protocol for the synthesis of protic bis(N‐heterocyclic carbene) complexes of AuI by a stepwise metal‐controlled coupling of isocyanide and propargylamine is described. They are used as tectons for the construction of supramolecular architectures through metalation and self‐assembly. Notably a unique polymeric chain of CuI with alternate AuI/bis(imidazolate) bridging scaffolds and strong unsupported CuI–CuI interactions has been generated, as well as a 28‐metal‐atoms cluster containing a nanopiece of Cu2O trapped by peripheral AuI/bis(imidazolate) moieties.
A Powerful Chiral Phosphoric Acid Catalyst for Enantioselective Mukaiyama–Mannich Reactions
Authors: Zhou Fengtao , Yamamoto Hisashi 
Published: June 2016

AbstractA new BINOL‐derived chiral phosphoric acid bearing 2,4,6‐trimethyl‐3,5‐dinitrophenyl substituents at the 3,3′‐positions was developed. The utility of this chiral phosphoric acid is demonstrated by a highly enantioselective (ee up to >99 %) and diastereoselective (syn/anti up to >99:1) asymmetric Mukaiyama–Mannich reaction of imines with a wide range of ketene silyl acetals. Moreover, this method was successfully applied to the construction of vicinal tertiary and quaternary stereogenic centers with excellent diastereo‐ and enantioselectivity. Significantly, BINOL‐derived N‐triflyl phosphoramide constitutes a complementary catalyst system that allows the title reaction to be applied to more challenging imines without an N‐(2‐hydroxyphenyl) moiety.
Highly modulated bisindoles: ligands for copper‐catalyzed Sonogashira reaction
Authors: Wang Xiu , Wang Zhenhua , Wu Ya , Luo Yanlong , Zhang Guofang , Jian Yajun , Sun Huaming , Zhang Weiqiang , Gao Ziwei 
Published: June 2016

Bisindoles (BIMs) were modulated as powerful N,N′ donor ligands for the copper‐catalyzed Sonogashira reaction. Ligand screening experiments on 11 BIM compounds found that 3,3′‐(4‐chlorophenyl)methylenebis(1‐methyl‐1H‐indole) (10%) efficiently accelerated CuCl (5%)‐catalyzed cross‐coupling of aryl iodides with terminal alkynes. A wide range of substituted aryl iodides and/or alkyl‐ and aryl‐substituted terminal alkynes were examined, leading to the corresponding coupling products with yields up to 99%. An efficient and scalable protocol for the synthesis of BIM ligands on a gram scale, with extremely low catalyst loading of o‐ClC6H4NH3+Cl−, was also developed with a reaction time of 20 min with yields up to 93%. This novel N,N′ ligand was air‐stable, easily available and highly modulated with low copper loading. Copyright © 2016 John Wiley & Sons, Ltd.
Brief Report: Anti–Eukaryotic Initiation Factor 2B Autoantibodies Are Associated With Interstitial Lung Disease in Patients With Systemic Sclerosis
Authors: Betteridge Zoe E. , Woodhead Felix , Lu Hui , Shaddick Gavin , Bunn Christopher C. , Denton Christopher P. , Abraham David J. , du Bois Roland M. , Lewis Mervyn , Wells Athol U. , McHugh Neil J. 
Published: June 2016

ObjectiveTo investigate novel systemic sclerosis (SSc) autoantibodies in autoantibody‐negative patients and establish clinical associations.MethodsSerum samples and clinical data for 548 patients with SSc were collected. Routine serologic techniques were used to test the serum samples for known SSc autoantibodies, and samples with negative results were further investigated by radiolabeled‐protein immunoprecipitation assay. Sera that immunoprecipitated a novel 30‐kd band were analyzed by indirect immunofluorescence and immunoprecipitation, using depleted cell extracts to establish a common reactivity. Mass spectrometry was performed to identify the novel autoantigen, and the results were confirmed using commercial antibodies. Sera from 426 patients with other forms of connective tissue disease, 103 with rheumatoid arthritis, 114 with idiopathic interstitial lung disease (ILD), and 150 healthy subjects were serotyped as controls.ResultsA novel autoantigen with a molecular weight of ∼30 kd was recognized by 7 sera from patients with SSc, 6 of whom had ILD, and by no controls. Six of the patients had diffuse cutaneous involvement, and 4 had overlap features with other autoimmune diseases. Immunodepletion experiments indicated that all samples targeted the same autoantigen, and mass spectrometry identified the novel autoantigen as eukaryotic initiation factor 2B (eIF2B).ConclusionWe report the identification of a novel autoantibody (anti‐eIF2B) in a small number of patients with SSc (∼1%); this autoantibody is closely associated with diffuse cutaneous manifestations and the presence of ILD.
Brief Report: Trends in Hospitalizations Due to Acute Coronary Syndromes and Stroke in Patients With Systemic Lupus Erythematosus, 1996 to 2012
Authors: Tektonidou Maria G. , Wang Zhong , Ward Michael M. 
Published: June 2016

ObjectiveCardiovascular disease (CVD) has been recognized as a major cause of morbidity in patients with systemic lupus erythematosus (SLE), but it is not clear whether increased awareness of these risks has translated into improvements in CVD morbidity at the population level. The aim of this study was to examine trends in hospitalization rates for CVD events in a representative sample of adult patients with SLE in the US from 1996 to 2012.MethodsWe used the Nationwide Inpatient Sample to estimate the rates of hospitalization for acute myocardial infarction (MI), unstable angina, and ischemic stroke from 1996 to 2012 in patients with SLE. We compared these trends with those in the general population.ResultsDuring the study years, there were an estimated 31,012 hospitalizations for acute MI, 4,160 hospitalizations for unstable angina, and 26,144 hospitalizations for ischemic stroke among patients with SLE. The rates of hospitalization for acute MI and ischemic stroke increased over time in patients with SLE, while the rates for unstable angina decreased. The rates for all 3 conditions decreased in the general population over these years, with hospitalization rates for unstable angina decreasing faster in the general population than in patients with SLE.ConclusionIncreased awareness of the burden of CVD in patients with SLE has not yet translated into decreased rates of hospitalization for acute MI or stroke. This may be due to barriers in implementation of CVD risk factor modification or to SLE‐specific risks that have not yet been identified or effectively targeted.
Elevated IgA Plasmablast Levels in Subjects at Risk of Developing Rheumatoid Arthritis
Authors: Kinslow Jennifer D. , Blum Lisa K. , Deane Kevin D. , Demoruelle M. Kristen , Okamoto Yuko , Parish Mark C. , Kongpachith Sarah , Lahey Lauren J. , Norris Jill M. , Robinson William H. , Holers V. Michael 
Published: June 2016

ObjectiveThe disease process in rheumatoid arthritis (RA) starts years before the clinical diagnosis is made, and elevated levels of disease‐specific autoantibodies can be detected during this period. Early responses to known or novel autoantigens likely drive the eventual production of pathogenic autoimmunity. Importantly, the presence of disease‐specific autoantibodies can identify individuals who are at high risk of developing RA but who do not currently have arthritis. The goal of the current study was to characterize plasmablasts from individuals at risk of developing RA.MethodsWe investigated antibody‐secreting plasmablasts derived from a well‐characterized cohort of individuals who were at risk of developing RA, based on RA‐related serum autoantibody positivity, as compared to patients with early (<1 year) seropositive RA as well as healthy control subjects. The plasmablast antibody repertoires of at‐risk subjects were analyzed using DNA barcode–based methods with paired heavy‐ and light‐chain gene sequencing. Cells were single‐cell sorted, the cell‐ and plate‐specific DNA barcodes were sequentially added, and next‐generation sequencing was performed.ResultsTotal plasmablast levels were similar in the antibody‐positive (1%) and control (0.4–1.6%) groups. However, increased frequencies of IgA+ versus IgG+ plasmablasts were observed in the antibody‐positive group (39% IgA+ and 37% IgG+) as compared to other groups (1–9% IgA+ and 71‐87% IgG+). Paired antibody sequences from antibody‐positive subjects revealed cross‐isotype clonal families and similar sequence characteristics in the IgA and IgG plasmablast repertoires. Antibody‐positive individuals also demonstrated elevated serum levels of IgA isotype anti–cyclic citrullinated peptide 3 antibodies.ConclusionThe IgA plasmablast dominance in these antibody‐positive individuals suggests that a subset of RA‐related autoantibodies may arise from mucosal immune responses and may be involved in early disease pathogenesis in individuals who are at risk of developing RA.
A Novel Mechanism for Generating the Interferon Signature in Lupus: Opsonization of Dead Cells by Complement and IgM
Authors: Zhuang Haoyang , Han Shuhong , Li Yi , Kienhöfer Deborah , Lee Pui , Shumyak Stepan , Meyerholz Richard , Rosadzinski Krzysztof , Rosner Danielle , Chan Annie , Xu Yuan , Segal Mark , Sobel Eric , Yang Li‐Jun , Hoffmann Markus H. , Reeves Westley H. 
Published: June 2016

ObjectiveIn vitro studies suggest that the type I interferon (IFN) signature seen in most lupus patients results from Fcγ receptor–mediated uptake of nucleic acid–containing immune complexes by plasmacytoid dendritic cells and engagement of endosomal Toll‐like receptors. The aim of this study was to reexamine the pathogenesis of the IFN signature in vivo.MethodsLupus was induced in mice by injecting pristane. Some mice were treated with normal immunoglobulin or with cobra venom factor to deplete complement. The IFN signature was evaluated by polymerase chain reaction. The IFN signature also was determined in C4‐deficient patients and control subjects.ResultsWild‐type C57BL/6 mice with pristane‐induced lupus developed a strong IFN signature, which was absent in immunoglobulin‐deficient (μMT), C3−/−, and CD18−/− mice. Intravenous infusion of normal IgM, but not IgG, restored the IFN signature in μMT mice, and the IFN signature in wild‐type mice was inhibited by depleting complement, suggesting that opsonization by IgM and complement is involved in IFN production. Consistent with that possibility, the levels of “natural” IgM antibodies reactive with dead cells were increased in pristane‐treated wild‐type mice compared with untreated controls, and in vivo phagocytosis of dead cells was impaired in C3‐deficient mice. To examine the clinical relevance of these findings, we identified 10 C4‐deficient patients with lupus‐like disease and compared them with 152 C4‐intact patients and 21 healthy controls. In comparison with C4‐intact patients, C4‐deficient patients had a different clinical/serologic phenotype and lacked the IFN signature.ConclusionThese studies define previously unrecognized roles of natural IgM, complement, and complement receptors in generating the IFN signature in lupus.
Sulfur Confined in Sub‐Nanometer‐Sized 2 D Graphene Interlayers and Its Electrochemical Behavior in Lithium–Sulfur Batteries
Authors: Du Wen‐Cheng , Zhang Juan , Yin Ya‐Xia , Guo Yu‐Guo , Wan Li‐Jun 
Published: June 2016

AbstractMicrospace‐confined sulfur molecules as cathodes for lithium–sulfur (Li−S) batteries have shown great significance in both scientific and technical aspects. A study of different microspace‐confined sulfur will not only promote the advancement of Li−S batteries but also arouse a wide interest in sulfur chemistry and related applications. Herein, we choose two‐dimensional (2D) graphene interlayer as host and construct 2D space‐confined sulfur model systems by simple intercalation chemistry of graphite oxide. Two routes, including solvothermal method and interlamellar reaction approach, are developed, and sulfur can be easily intercalated into sub‐nanometer‐sized graphene interlayers, forming a graphene confined sulfur structure. The 2D space‐confined sulfur can work well in a carbonate‐based electrolyte and show similar electrochemical behaviors of small sulfur molecules, indicating the special molecular form of sulfur in graphene layers. The 2D space‐confined sulfur concept will be helpful for further understanding the electrochemical character of confined sulfur molecules and designing a high‐performance sulfur cathode.
Neuropeptide derivatives to regulate the reproductive axis: Kisspeptin receptor (KISS1R) ligands and neurokinin‐3 receptor (NK3R) ligands
Authors: Oishi Shinya , Fujii Nobutaka 
Published: June 2016

ABSTRACTRecent research has indicated pivotal roles for neuropeptides and their cognate receptors in reproductive physiology. Kisspeptins are RF‐amide neuropeptides that stimulate gonadotropin‐releasing hormone (GnRH) neurons in the hypothalamus. Neurokinin B (NKB) is a member of the tachykinin family of neuropeptides and positively regulates pulsatile GnRH secretion. These peptides are coexpressed in kisspeptin/NKB/Dyn (KNDy) neurons of the arcuate nucleus, where they contribute to the regulation of puberty onset and other reproductive functions. In this review, the design of peptide ligands for the kisspeptin (KISS1R) and neurokinin‐3 (NK3R) receptors are described. © 2016 Wiley Periodicals, Inc. Biopolymers (Pept Sci) 106: 588–597, 2016.
Marital status and survival in patients with gastric cancer
Authors: Jin Jie‐Jie , Wang Wei , Dai Fa‐Xiang , Long Zi‐Wen , Cai Hong , Liu Xiao‐Wen , Zhou Ye , Huang Hua , Wang Ya‐Nong 
Published: June 2016

AbstractThe objective of this study is to examine the impact of marital status on incidence of metastasis at diagnosis, receipt of surgery, and cause‐specific survival (CSS) in patients with gastric cancer (GC). Research data is extracted from The Surveillance, Epidemiology, and End Results (SEER) database, and 18,196 patients diagnosed with GC from 2004 to 2010 are involved. Effects of marital status on incidence of metastasis at diagnosis, receipt of surgery, and CSS are determined using multivariable logistic regression and multivariable Cox regression models, as appropriate. Single GC patients have a higher incidence of metastasis at diagnosis than married patients, while the differences between divorced/separated patients or widowed patients and married patients are not significant. Among those without distant metastasis, single patients, divorced/separated patients, and widowed patients are much less likely to accept surgery compared with married patients. Finally, in the whole group of 18,196 GC patients, single patients, divorced/separated patients, and widowed patients have shorter CSS compared with married patients, even in each of the TNM stage. Marriage had a protective effect against undertreatment and cause‐specific mortality (CSM) in GC. Spousal support may contribute to higher rate of surgery receipt and better survival in patients with GC.
Effects of propolis and gamma‐cyclodextrin on intestinal neoplasia in normal weight and obese mice
Authors: Cho Youngjin , Gutierrez Linda , Bordonaro Michael , Russo Daniel , Anzelmi Frank , Hooven Jayde T. , Cerra Carmine , Lazarova Darina L. 
Published: June 2016

AbstractObesity is associated with colorectal cancer (CRC). This effect might be attributed to adipokine‐supported signaling. We have established that propolis suppresses survival signaling in CRC cells in vitro; therefore, we ascertained the ability of a propolis supplement to modulate intestinal neoplastic development in C57BL/6J‐ApcMin/+/J mice in the lean and obese state. To induce obesity, mice were fed with a Western diet containing 40% fat. Since the propolis supplement includes gamma‐cyclodextrin, the interventions included diets supplemented with or without gamma‐cyclodextrin. The animals were administered the following diets: (1) control diet, (2) control diet/gamma‐cyclodextrin, (3) control diet/propolis, (4) Western diet, (5) Western diet/gamma‐cyclodextrin, and (6) Western diet/propolis. Western diet, resulting in obesity, accelerated neoplastic progression, as evidenced by the larger size and higher grade dysplasia of the neoplasms. In the context of normal weight, gamma‐cyclodextrin and propolis affected neoplastic progression, as determined by the size of the lesions and their grade of dysplasia. A statistically significant decrease in the number of adenomas was detected in mice fed a control diet with the propolis supplement (61.8 ± 10.6 vs. 35.3 ± 7.6, P = 0.008). Although there was no significant difference in the polyp numbers between the six groups, the mice with the lowest number and size of adenomas were those fed a Western diet with gamma‐cyclodextrin. This unexpected outcome might be explained by the increased levels of apoptosis detected in the intestinal tissues of these obese mice. We posit that butyrate derived from the metabolism of gamma‐cyclodextrin may contribute to the decreased neoplastic burden in the context of obesity; however, future studies are required to address this possibility.
Monochorionic–diamniotic discordant growth in a twin pregnancy with one fetus affected by Ebstein's anomaly of tricuspid leaflets
Authors: Fukami Tatsuya , Goto Maki , Matsuoka Sakiko , Sorano Sumire , Tohyama Atsushi , Yamamoto Hiroko , Nakamura Sumie , Matsuoka Ryoei , Tsujioka Hiroshi , Eguchi Fuyuki 
Published: June 2016

Key Clinical MessageOur patient was diagnosed as having discordant twin growth with Ebstein's anomaly in the larger fetus. Cardiac function was deteriorated in accordance with progression of gestational age. Our observation indicated cardiac failure of the larger fetus. The most important issue in this situation is management of the timing of delivery.
Semihydrogenation of Propyne over Cerium Oxide Nanorods, Nanocubes, and Nano‐Octahedra: Facet‐Dependent Parahydrogen‐Induced Polarization
Authors: Zhao Evan W. , Xin Yan , Hagelin‐Weaver Helena E. , Bowers Clifford R. 
Published: June 2016

AbstractThe pairwise selectivity of hydrogenation is a fundamental quantity in hydrogenation catalysis that underpins the NMR signal enhancement achievable by parahydrogen‐induced polarization (PHIP). Herein, we show how the crystal facet dependence of the pairwise selectivity of the semihydrogenation of propyne, when interpreted in the context of recent DFT calculations, can reveal new details about the hydrogenation mechanism. The pairwise selectivity of propyne hydrogenation is strongly shape dependent, which reflects the surface atom arrangements exposed on the different facets of CeO2 nanocrystals. In this first demonstration of a catalyst shape dependence of PHIP, an unprecedented pairwise selectivity of 8.1 % is observed over oxygen‐deficient facets of rods, whereas oxygen‐rich octahedra facets deliver only 1.6 % selectivity. The PHIP data are consistent with a concerted addition pathway through a six‐membered‐ring transition state, as predicted in the DFT study.
A Red to Near‐IR Fluorogen: Aggregation‐Induced Emission, Large Stokes Shift, High Solid Efficiency and Application in Cell‐Imaging
Authors: Wang Yi Jia , Shi Yang , Wang Zhaoyang , Zhu Zhenfeng , Zhao Xinyuan , Nie Han , Qian Jun , Qin Anjun , Sun Jing Zhi , Tang Ben Zhong 
Published: June 2016

AbstractA tetraphenylethene (TPE) derivative modified with the strong electron acceptor 2‐dicyano‐methylene‐3‐cyano‐4,5,5‐trimethyl‐2,5‐dihydrofuran (TCF) was obtained in high yield by a simple two‐step reaction. The resultant TPE‐TCF showed evident aggregation‐induced emission (AIE) features and pronounced solvatochromic behavior. Changing the solvent from apolar cyclohexane to highly polar acetonitrile, the emission peak shifted from 560 to 680 nm (120 nm redshift). In an acetonitrile solution and in the solid powder, the Stokes shifts are as large as 230 and 190 nm, respectively. The solid film emits red to near‐IR (red‐NIR) fluorescence with an emission peak at 670 nm and a quantum efficiency of 24.8 %. Taking the advantages of red‐NIR emission and high efficiency, nanoparticles (NPs) of TPE‐TCF were fabricated by using tat‐modified 1,2‐distearoylsn‐glycero‐3‐phosphor‐ethanol‐amine‐N‐[methoxy‐(polyethyl‐eneglycol)‐2000] as the encapsulation matrix. The obtained NPs showed perfect membrane penetrability and high fluorescent imaging quality of cell cytoplasm. Upon co‐incubation with 4,6‐diamidino‐2‐phenylindole (DAPI) in the presence of tritons, the capsulated TPE‐TCF nanoparticles could enter into the nucleus and displayed similar staining properties to those of DAPI.
Synthesis of a Pentacene‐Type Silaborin via Double Dehydrogenative Cyclization of 1,4‐Diboryl‐2,5‐disilylbenzene
Authors: Hirofuji Tatsuya , Ikeda Toshiaki , Haino Takeharu , Yamamoto Yohsuke , Kawachi Atsushi 
Published: June 2016

AbstractA new pentacene‐type silaborin, in which three benzene rings are bridged by silicon and boron atoms, has been synthesized and characterized by using NMR spectroscopy and X‐ray crystallographic analysis. The precursor, 1,4‐bis(dimesitylboryl)‐2,5‐bis(phenylsilyl)benzene (4), was prepared by stepwise introduction of a silyl group and a boryl group to a benzene ring starting from 1,4‐dibromobenzene. Double cyclization of 4 proceeds by a H‐Mes exchange and a B‐H/C‐H dehydrogenative condensation to afford pentacene‐type silaborin 5. X‐ray crystal structure analysis reveals that 5 adopts a bent structure rather than a planar one. UV/Vis spectra and DFT calculations for 5 reveal a lowering of the LUMO energy level compared with corresponding anthracene‐type 3.