bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Rotaxane Scaffold Bearing Multiple Redox Centers: Synthesis, Surface Modification and Electrochemical Properties
Authors: Steffenhagen Marie , Latus Alina , Trinh Thi Minh Nguyet , Nierengarten Iwona , Lucas Ivan T. , Joiret Suzanne , Landoulsi Jessem , Delavaux‐Nicot Béatrice , Nierengarten Jean‐François , Maisonhaute Emmanuel 
Published: December 2017

AbstractA rotaxane scaffold incorporating two dithiolane anchoring units for the modification of gold surfaces has been functionalized with multiple copies of a redox unit, namely ferrocene. Surface modification has been first assessed at the single molecule level by atomic force microscopy (AFM) and scanning tunneling microscopy (STM) imaging, while tip enhanced Raman spectroscopy (TERS) provided the local vibrational signature of the ferrocenyl subunits of the rotaxanes grafted onto the gold surface. Finally, oxidation of the redox moieties within a rotaxane scaffold grafted onto gold microelectrodes has been investigated by ultrafast cyclic voltammetry. Intramolecular electron hopping is indeed extremely fast in this system. Moreover, the kinetics of charge injection depends on the molecular coverage due to the influence of intermolecular contacts on molecular motions.
Tetraphenylethylene Foldamers with Double Hairpin‐Turn Linkers, TNT‐Binding Mode and Detection of Highly Diluted TNT Vapor
Authors: Xiong Jia‐Bin , Feng Hai‐Tao , Wang Jin‐Hua , Zhang Chun , Li Bao , Zheng Yan‐Song 
Published: December 2017

AbstractTetraphenylethylene (TPE) foldamers with double hairpin‐turn linkers showing an aggregation‐induced emission (AIE) effect have been synthesized for the first time. A crystal structure of a foldamer–TNT complex has been obtained, enabling unprecedented direct observation of the interactions between TNT molecules and the chromophores of the foldamer. Instead of π–π stacking interactions, which have often been considered to be the key mechanism in the binding of TNT by chromophoric receptors, strong n–π interactions between the nitro groups of TNT and the aromatic rings of the foldamer have been found. Exceptionally, by addition of 1 % NaF to a suspension of the foldamer in H2O/THF (95:5), the fluorescence quenching efficiency by TNT vapor significantly increased from about 20 % to more than 90 %. Even after diluting TNT‐saturated air at 25 °C by a factor of 2×104, an obvious quenching response was observed, indicating that ultratrace TNT vapor (down to 3.4 fg per mL of air) could be detected.
Efficient Buchwald–Hartwig–Migita Cross‐Coupling for DNA Thioglycoconjugation
Authors: Probst Nicolas , Lartia Rémy , Théry Océane , Alami Mouâd , Defrancq Eric , Messaoudi Samir 
Published: December 2017

AbstractAn efficient method for the thioglycoconjugation of iodinated oligonucleotides by Buchwald–Hartwig–Migita cross‐coupling under mild conditions is reported. The method enables divergent synthesis of many different functionalized thioglycosylated ODNs in good yields, without affecting the integrity of the other A, C, and G nucleobases.
General One‐Pot Synthesis of Transition‐Metal Phosphide/Nitrogen‐Doped Carbon Hybrid Nanosheets as Ultrastable Anodes for Sodium‐Ion Batteries
Authors: Li Jingjing , Shi Liang , Gao Jingyu , Zhang Genqiang 
Published: December 2017

AbstractSodium‐ion batteries (SIBs) have been considered as promising energy storage devices in grid‐level applications, owing to their largely reduced cost compared with that of lithium‐ion batteries. However, the practical application of SIBs has been seriously hindered because of the lack of appropriate anode materials, limited by the thermodynamics perspective, which is one of the central task at current stage. Herein, we have developed a general one‐pot strategy for the synthesis of transition‐metal phosphide (TMP) based hybrid nanosheets composed of carbon‐coated TMP nanoparticles anchored to the surface of nitrogen‐doped carbon nanosheets. This facile and cost‐effective method is quite universal and holds potential to be further extended to other metal phosphide materials. Significantly, the hybrid nanosheet electrode possesses excellent sodium storage properties as anodes for SIBs, including high specific capacity, an ultra‐long cycle life and a remarkable rate performance. This work makes a significant contribution to not only the synthetic methodology of TMP–carbon two‐dimensional hybrid nanostructures, but also the application of TMP‐based anodes for high‐energy SIBs.
Synthesis, Structure, and Acidity Constants of Ligated α‐Boryl Acetic Acids
Authors: Allen Thomas H. , Horner Anthony R. , Geib Steven J. , Weber Stephen G. , Curran Dennis P. 
Published: December 2017

AbstractBasic hydrolyses of various ligated α‐boryl acetic acid esters provided the first ligated derivatives of the unknown compound boroacetic acid (BH2CH2CO2H). Four monoacids (L‐BH2CH2CO2H) and one diacid (L‐BH(CH2CO2H)2) were prepared with N‐heterocyclic carbene, amine, and pyridine ligands (L). The stable acids were characterized by X‐ray crystallography and acidity constant (pKa) measurements. They rank among the least acidic of all known carboxylic acids. In turn, their conjugate bases are among the strongest of all carboxylates.
Fission yeast Myo2: Molecular organization and diffusion in the cytoplasm
Authors: Friend Janice E. , Sayyad Wasim A. , Arasada Rajesh , McCormick Chad D. , Heuser John E. , Pollard Thomas D. 
Published: December 2017

AbstractMyosin‐II is required for the assembly and constriction of cytokinetic contractile rings in fungi and animals. We used electron microscopy, fluorescence recovery after photobleaching (FRAP), and fluorescence correlation spectroscopy (FCS) to characterize the physical properties of Myo2 from fission yeast Schizosaccharomyces pombe. By electron microscopy, Myo2 has two heads and a coiled‐coiled tail like myosin‐II from other species. The first 65 nm of the tail is a stiff rod, followed by a flexible, less‐ordered region up to 30 nm long. Myo2 sediments as a 7 S molecule in high salt, but aggregates rather than forming minifilaments at lower salt concentrations; this is unaffected by heavy chain phosphorylation. We used FRAP and FCS to observe the dynamics of Myo2 in live S. pombe cells and in cell extracts at different salt concentrations; both show that Myo2 with an N‐terminal mEGFP tag has a diffusion coefficient of ∼ 3 µm2 s−1 in the cytoplasm of live cells during interphase and mitosis. Photon counting histogram analysis of the FCS data confirmed that Myo2 diffuses as doubled‐headed molecules in the cytoplasm. FCS measurements on diluted cell extracts showed that mEGFP‐Myo2 has a diffusion coefficient of ∼ 30 µm2 s−1 in 50 to 400 mM KCl concentrations.
Improving the Potency of Cancer Immunotherapy by Dual Targeting of IDO1 and DNA
Authors: Fang Kun , Dong Guoqiang , Wang Hongyu , He Shipeng , Wu Shanchao , Wang Wei , Sheng Chunquan 
Published: December 2017

AbstractHerein we report the first exploration of a dual‐targeting drug design strategy to improve the efficacy of small‐molecule cancer immunotherapy. New hybrids of indoleamine 2,3‐dioxygenase 1 (IDO1) inhibitors and DNA alkylating nitrogen mustards that respectively target IDO1 and DNA were rationally designed. As the first‐in‐class examples of such molecules, they were found to exhibit significantly enhanced anticancer activity in vitro and in vivo with low toxicity. This proof‐of‐concept study has established a critical step toward the development of a novel and effective immunotherapy for the treatment of cancers.
Complete multinuclear solid‐state NMR of metal‐organic frameworks: The case of α‐Mg‐formate
Authors: Lucier Bryan E. G. , Zhang Yue , Huang Yining 
Published: December 2017

AbstractMetal‐organic frameworks (MOFs) are exciting porous materials with a growing number of applications ranging from catalysis to gas storage. Establishing logical connections between the local MOF structure and its properties is not often straightforward, however, solid‐state NMR is a sensitive probe of local structure and can be used to shed light on processes such as guest adsorption and gas motion within MOFs. As illustrated using our recent works on the microporous α‐Mg‐formate (Mg3(HCOO)6) MOF, complete multinuclear solid‐state NMR characterization of MOFs is now possible, and can provide unique insight that is not readily available through other methods. A wide variety of solid‐state NMR techniques have been employed, including direct‐excitation, cross‐polarization, fast magic‐angle spinning, and two‐dimensional experiments. New variable‐temperature 2H solid‐state NMR data of deuterated hydrogen gas within α‐Mg‐formate and the resulting detailed dynamic information is also presented, analyzed, and discussed.
Conditional survival of patients with gastric cancer who undergo curative resection: A multi‐institutional analysis in China
Authors: Wang Pengliang , Sun Zhe , Wang Wei , Deng Jingyu , Wang Zhenning , Liang Han , Zhou Zhiwei , Xu Huimian 
Published: December 2017

BACKGROUNDConditional survival estimates, which take into consideration the changing risk with increasing survival time, provide a dynamic survival probability and more accurate survival information for clinician decision making. The objective of the current study was to evaluate the conditional disease‐specific survival (DSS) for patients with gastric cancer who underwent curative surgery in China.METHODSIn total, 7658 patients with gastric cancer from a multi‐institutional cohort in China were included in the analyses. Actuarial DSS was estimated using the Kaplan‐Meier method. Three‐year conditional DSS (CDS3) of patients who had already survived for x years was estimated as CDS3 = DSS(x + 3)/DSS(x). Cox proportional hazards regression analyses were used to identify the factors related to DSS.RESULTSThe 1‐year, 3‐year, and 5‐year actuarial DSS rates were 88.2%, 64.5%, and 54.6%, respectively. By using CDS estimates, the probabilities that patients would remain alive for an additional 3 years given that they had already survived for 1, 3, and 5 years were 66.6%, 80.2%, and 88.3%, respectively. Patients who had unfavorable tumor characteristics diagnosed initially at surgery had the greatest improvement in CDS and the largest survival gap between actuarial DSS and CDS.CONCLUSIONSThe current results indicate that CDS estimates for Chinese patients with gastric cancer who underwent surgery were dynamic and increased with time elapsed. Patients who had unfavorable tumor characteristics had the greatest improvement in CDS. This valuable information could provide more a precise evaluation of long‐term prognosis and may serve as an important prognostic index in clinical practice. Cancer 2018;124:916‐24. © 2017 American Cancer Society.
Clinical impact of sedentary behaviors in adult survivors of acute lymphoblastic leukemia: A report from the St. Jude Lifetime Cohort study
Authors: Howell Carrie R. , Wilson Carmen L. , Ehrhardt Matthew J. , Partin Robyn E. , Kaste Sue C. , Lanctot Jennifer Q. , Pui Ching‐Hon , Robison Leslie L. , Hudson Melissa M. , Ness Kirsten K. 
Published: December 2017

BACKGROUNDSedentary behaviors are associated with poor health outcomes in the general population, but their clinical impact on adult survivors of childhood acute lymphoblastic leukemia (ALL) has not been characterized to date. In the current study, we described the prevalence of sedentary behaviors in survivors of ALL and examined associations between time spent sedentary and body composition and onset of cardiovascular disease (CVD) risk factors.METHODSParticipants' self‐reported screen time (eg, television, computer) and activity as measured by accelerometer were used to determine activity time (sedentary, light activity, and moderate or vigorous physical activity). The percentage of time spent in each activity was compared between 331 survivors of ALL and 330 controls. Associations between time sedentary and body composition were evaluated in survivors using linear regression models. Cox proportional hazard models were used to examine the association between time sedentary at baseline and CVD risk factor onset during follow‐up.RESULTSSurvivors spent approximately 65% of their time sedentary, 32% in light activity, and 2% in moderate or vigorous physical activity compared with 67% (P = .04), 30% (P<.01), and 3% (P<.01), respectively, in controls. Among survivors, percentage lean body mass decreased by 1.0% ± 0.4% (P = .01) per 10% increase in time sedentary. Survivors who were sedentary ≥60% per day were found to be at an increased risk of high total cholesterol (hazard ratio, 2.52; 95% confidence interval, 1.12‐5.64) and any CVD risk factor (hazard ratio, 1.96; 95% confidence interval, 1.16‐3.30).CONCLUSIONSSedentary behavior is associated with low lean mass and CVD risk factor development and should be limited in survivors of childhood ALL. Cancer 2018;124:1036‐43. © 2017 American Cancer Society.
Effects of estrogen replacement therapy on the myelin sheath ultrastructure of myelinated fibers in the white matter of middle‐aged ovariectomized rats
Authors: He Qi , Luo Yanmin , Lv Fulin , Xiao Qian , Chao Fenglei , Qiu Xuan , Zhang Lei , Gao Yuan , Xiu Yun , Huang Chunxia , Tang Yong 
Published: December 2017

AbstractThe effects of estrogen replacement therapy (ORT) on white matter and the myelin sheath ultrastructure in the white matter of middle‐aged ovariectomized (OVX) rats were investigated in this study. Middle‐aged rats were ovariectomized and divided into a placebo replacement (OVX + O) group and an estrogen replacement (OVX + E) group. Then, the Morris water maze, electron microscope techniques, and stereological methods were used to investigate the effects of ORT on spatial learning capacity, white matter volume and the myelin sheath ultrastructure in the white matter. We found that the spatial learning capacity of the OVX + E rats was significantly improved compared with that of the OVX + O rats. When compared with that of OVX + O rats, the total volume of the myelin sheaths in the white matter of the OVX + E rats was significantly increased by 27%, and the difference between the outer perimeter and inner perimeter of the myelin sheaths of the white matter in the OVX + E rats increased significantly by 12.6%. The myelinated fibers with mean diameters of 1.2–1.4 μm were significantly longer (46.1%) in the OVX + E rats; the difference between the mean diameter of myelinated fibers and the mean diameter of axons (0–0.4 μm) was significantly increased by 21.6% in the OVX + E rats. These results suggested that ORT had positive protective effects on the spatial learning ability and on the myelin sheath ultrastructure in the white matter of middle‐aged OVX rats.
Preparation and Electrochemical Properties of NiCo2O4 Nanospinels Supported on Graphene Derivatives as Earth‐Abundant Oxygen Bifunctional Catalysts
Authors: Kumar Kavita , Loupias Lola , Canaff Christine , Morisset Sophie , Pronier Stéphane , Morais Cláudia , Habrioux Aurélien , Napporn Teko W. , Kokoh K. Boniface 
Published: December 2017

AbstractThis work reports on the facile synthesis and characterisation of a non‐precious‐metal bifunctional catalyst for oxygen reduction and evolution reactions (ORR and OER). A few‐layer reduced graphene oxide‐supported NiCo2O4 catalyst is prepared using a rapid and easy two‐step method of synthesis. It consists of the solvothermal poyl(vinylpyrrolidone)‐assisted assembly of metal complexes onto few‐layer graphene followed by a calcination step aiming at converting metal complexes into the spinel phase. Using this synthesis approach, the most active material demonstrates an outstanding activity towards the OER and ORR, making it one of the best bifunctional catalysts of these reactions ever reported. This composite catalyst exhibits improved bifunctional behaviour with a low reversibility criterion of 746 mV. The ORR process follows a four‐electron pathway and the hydroxyl selectivity is higher than those with pure reduced graphene oxide or NiCo2O4 materials, showing the synergistic effect between the two phases. Moreover, the high activity of this composite catalyst is confirmed by comparing its performance with those obtained on other cobaltite catalysts prepared using a different synthesis method, or those obtained using a different graphene‐based support.
Validation of X‐ray Wavefunction Refinement
Authors: Woińska Magdalena , Jayatilaka Dylan , Dittrich Birger , Flaig Ralf , Luger Peter , Woźniak Krzysztof , Dominiak Paulina M. , Grabowsky Simon 
Published: December 2017

AbstractThe front cover artwork is provided by the group of Prof. Krzysztof Woźniak, Dr. Paulina M. Dominiak, and Dr. Magdalena Woińska. The image shows X‐ray wavefunction refinement as a method of electron density reconstruction (symbolized by a jigsaw puzzle), which allows to obtain accurate and precise molecular geometries as well as properties of electron density, and to perform data quality evaluations. Read the full text of the article at 10.1002/cphc.201700810.
Magnetic Interaction Observed in Hetero Biradical Derivatives Containing a 2,2,5,5‐Tetramethylpyrrolin‐1‐yloxyl Unit as a Localized Spin Center
Authors: Takahashi Yusuke , Miura Youhei , Yoshioka Naoki 
Published: December 2017

AbstractThe magneto‐structural correlation of hetero biradical derivatives containing a 2,2,5,5‐tetramethylpyrrolin‐1‐yloxyl unit as a localized spin center and a verdazyl or nitronyl nitroxide radical is reported. The magnetic susceptibility measurement revealed that the verdazyl attached biradical 1 exhibits ferromagnetic interaction, whereas antiferromagnetic interaction is observed for nitronyl nitroxide attached biradical 2. An EPR study in toluene glass matrix suggests that both 1 and 2 have a ground triplet state. DFT calculations predict that there is intramolecular ferromagnetic interaction for both biradicals. The computation also suggests that the intramolecular magnetic interaction is weaker with larger dihedral angle between pyrroline ring and verdazyl ring/O−N−C−N−O plane of nitronyl nitroxide. The computations of model compounds 3 and 4 suggest that spin polarization on vinylic moiety without distribution of SOMO might be an essential condition for the intramolecular ferromagnetic interaction.
A Strategy for the Simultaneous Synthesis of Methallyl Alcohol and Diethyl Acetal with Sn‐β
Authors: Hu Wenda , Wan Yan , Zhu Lili , Cheng Xiaojie , Wan Shaolong , Lin Jingdong , Wang Yong 
Published: December 2017

AbstractInvited for this month′s cover is the group of Yong Wang at Xiamen University. The cover picture shows a strategy to simultaneously produce two important chemicals, namely, methallyl alcohol and diethyl acetal from methacrolein in ethanol solvent at low temperature on Beta zeolites modified by tin (Sn‐β catalysts). The Full Paper itself is available at 10.1002/cssc.201701435.
Memristor‐enhanced humanoid robot control system – Part I: Theory behind the novel memcomputing paradigm
Authors: Ascoli A. , Baumann D. , Tetzlaff R. , Chua L. O. , Hild M. 
Published: December 2017

SummaryMyon is a humanoid robot where each joint is controlled independently by a supervised bio‐inspired artificial neural network inducing the correction of a number of distinct actions depending on the excitation. One of the control strategies, which the network, located within a certain joint, may implement, allows a controlled motion of the limb connected to the joint from a stable state up to a prescribed height and the maintenance of the new position afterwards. The original approach adopted for this control operation is stable and robust but results in slow and energy‐inefficient limb movements. This work proposes a novel, low‐power, time‐efficient and adaptive memristor‐centred control strategy for the aforementioned robot action. The idea is based upon the exploitation of the combined ability of memristors to store and process data in the same physical location. The part I paper sets the theoretic foundations for the memcomputing paradigm to robot motion control, while the part II manuscript shall demonstrate its benefits over the original approach in terms of energy, and speed, and the inheritance from the standard strategy of a good level of adaptability to changes in the limb load on the basis of the analysis of circuit‐theoretic models adopting an ideal and a real memristor, respectively. Copyright © 2017 John Wiley & Sons, Ltd.
Atomic mass tag of bismuth‐209 for increasing the immunoassay multiplexing capacity of mass cytometry
Authors: Han Guojun , Chen Shih‐Yu , Gonzalez Veronica D. , Zunder Eli R. , Fantl Wendy J. , Nolan Garry P. 
Published: December 2017

AbstractMass cytometry (or CyTOF) is an atomic mass spectrometry‐based single‐cell immunoassay technology, which has provided an increasingly systematic and sophisticated view in basic biological and clinical studies. Using elemental reporters composed of stable heavy metal isotopes, more than 50 cellular parameters are measured simultaneously. However, this current multiplexing does not meet the theoretical capability of CyTOF instrumentation with 135 detectable channels, primarily due to the limitation of available chemistries for conjugating elemental mass tags to affinity reagents. To address this issue, we develop herein additional metallic mass tag based on bismuth‐209 (209 Bi) for efficient conjugation to monoclonal antibody. This enables the use of an addtional channel m/z = 209 of CyTOF for single‐cell immunoassays. Bismuth has nearly the same charge‐to‐radius ratio as lanthanide elements; thus, bismuth(III) cations (209Bi3+) could coordinate with DTPA chelators in the same geometry of O‐ and N‐donor groups as that of lanthanide. In this report, the coordination chemistry of 209Bi3+ with DTPA chelators and Maxpar® X8 polymers were investigated in details. Accordingly, the protocols of conjugating antibody with bismuth mass tag were provided. A method based on UV‐Vis absorbance at 280 nm of 209Bi3+‐labeling DTPA complexes was developed to evaluate the stoichiometric ratio of 209Bi3+ cations to the conjugated antibody. Side‐by‐side single‐cell analysis experiments with bismuth‐ and lanthanide‐tagged antibodies were carried out to compare the analytical sensitivities. The measurement accuracy of bismuth‐tagged antibody was validated within in vitro assay using primary human natural killer cells. Furthermore, bismuth‐tagged antibodies were successfully employed in cell cycle measurements and high‐dimensional phenotyping immunoassays. © 2017 International Society for Advancement of Cytometry