bluuebunny/crossref_metadata_2025_split huggingface dataset:
Role of Charge Density Wave in Monatomic Assembly in Transition Metal Dichalcogenides
Authors: Feng Haifeng , Xu Zhongfei , Zhuang Jincheng , Wang Li , Liu Yani , Xu Xun , Song Li , Hao Weichang , Du Yi 
Published: February 2019

AbstractThe charge density wave (CDW) in transition metal dichalcogenides (TMDs) has drawn tremendous interest due to its potential for tailoring their surface electronic and chemical properties. Due to technical challenges, however, how the CDW could modulate the chemical behavior of TMDs is still not clear. Here, this work presents a study of applying the CDW of NbTe2, with a high transition temperature above room temperature, to generate the assembling adsorption of Sn adatoms on the surface. It is shown that highly ordered monatomic Sn adatoms with a quasi‐1D structure can be obtained under regulation by the single‐axis CDW of the substrate. In addition, the CDW modulated superlattices could in turn change the surface electronic properties from semimetallic to metallic. These results demonstrate an effective approach for tuning the surface chemical properties of TMDs by their CDWs, which could be applied in exploring them for various practical applications, such as heterogeneous catalysis, epitaxial growth of low‐dimensional materials, and future nanoelectronics.
Multistimuli Response and Polymorphism of a Novel Tetraphenylethylene Derivative
Authors: Huang Guangxi , Jiang Yuqing , Yang Sifen , Li Bing Shi , Tang Ben Zhong 
Published: February 2019

AbstractMulti‐stimuli‐responsive fluorescent molecule tetraphenylethylene (TPE) derivative 1 is synthesized, which contains a TPE skeleton and peripheries of two methoxyl groups and one carboxyl group. It shows a typical aggregation‐induced emission behavior and also exhibits fluorescence responses to pH change and amine vapors, and multicolored mechanochromic properties. The emission of 1 can be reversibly switched among blue (1p‐f, 462 nm, Φf = 7.4%), bright cyan (1p‐h, 482 nm, Φf = 82.3%), and yellow (1p‐g, 496 nm, Φf = 10.5%) with high contrast through solvent fuming, heating, or grinding. Molecule 1 occurs in four crystalline states (1c‐a, 1c‐b, 1c‐c, and 1c‐d) after crystallization from different solvents. The multicolored mechanochromic property is related to the different interactions and packing modes of molecules in the crystals. The crystals with weak fluorescent emission have characteristic porous structures and corresponding intensive XRD diffraction peaks, which are absent in the crystal with intensive fluorescent emission. The porous structures are critical for the fluorescence intensity of the molecules. Upon heating, the porous structures of crystals are damaged and fluorescence is significantly enhanced.
New Organic Electrode Materials for Ultrafast Electrochemical Energy Storage
Authors: Zhao‐Karger Zhirong , Gao Ping , Ebert Thomas , Klyatskaya Svetlana , Chen Zhi , Ruben Mario , Fichtner Maximilian 
Published: February 2019

AbstractOrganic materials are both environmentally and economically attractive as potential electrode candidates. This Research News reports on a new class of stable and electrically conductive organic electrodes based on metal porphyrins with functional groups that are capable of electrochemical polymerization, rendering the materials promising for electrochemical applications. Their structural flexibility and the unique highly conjugated macrocyclic structure allows the produced organic electrodes to act as both cathode and anode materials giving access to fast charging as well as high cycling stability. The extreme thermal and chemical stability of the porphyrin‐based organic electrodes and their chemical versatility suggest an important role for these molecular systems in the further development of novel electrochemical energy storage applications.
One‐Step Construction of Hydrophobic MOFs@COFs Core–Shell Composites for Heterogeneous Selective Catalysis
Authors: Cai Mengke , Li Yinle , Liu Qinglin , Xue Ziqian , Wang Haiping , Fan Yanan , Zhu Kelong , Ke Zhuofeng , Su Cheng‐Yong , Li Guangqin 
Published: February 2019

AbstractThe exploration of novel porous core–shell materials is of great significance because of their prospectively improved performance and extensive applications in separation, energy conversion, and catalysis. Here, mesoporous metal–organic frameworks (MOFs) NH2‐MIL‐101(Fe) as a core generate a shell with mesoporous covalent organic frameworks (COFs) NUT‐COF‐1(NTU) by a covalent linking process, the composite NH2‐MIL‐101(Fe)@NTU keeping retentive crystallinity with hierarchical porosity well. Importantly, the NH2‐MIL‐101(Fe)@NTU composite shows significantly enhanced catalytic conversion and selectivity during styrene oxidation. It is mainly due to the hydrophilic MOF nanocrystals readily gathering the hydrophobic reactants styrene and boosting the radical mechanism path after combining the hydrophobic COFs shell. The synthetic strategy in this systematic study develops a new rational design for the synthesis of other core–shell MOF/COF‐based hybrid materials, which can expand the promising applications.
Rapid and reproducible characterization of sickling during automated deoxygenation in sickle cell disease patients
Authors: Rab Minke A.E. , van Oirschot Brigitte A. , Bos Jennifer , Merkx Tesy H. , van Wesel Annet C.W. , Abdulmalik Osheiza , Safo Martin K. , Versluijs Birgitta A. , Houwing Maite E. , Cnossen Marjon H. , Riedl Jurgen , Schutgens Roger E.G. , Pasterkamp Gerard , Bartels Marije , van Beers Eduard J. , van Wijk Richard 
Published: February 2019

AbstractIn sickle cell disease (SCD), sickle hemoglobin (HbS) polymerizes upon deoxygenation, resulting in sickling of red blood cells (RBCs). These sickled RBCs have strongly reduced deformability, leading to vaso‐occlusive crises and chronic hemolytic anemia. To date, there are no reliable laboratory parameters or assays capable of predicting disease severity or monitoring treatment effects. We here report on the oxygenscan, a newly developed method to measure RBC deformability (expressed as Elongation Index ‐ EI) as a function of pO2. Upon a standardized, 22 minute, automated cycle of deoxygenation (pO2 median 16 mmHg ± 0.17) and reoxygenation, a number of clinically relevant parameters are produced in a highly reproducible manner (coefficients of variation <5%). In particular, physiological modulators of oxygen affinity, such as, pH and 2,3‐diphosphoglycerate showed a significant correlation (respectively R = ‑0.993 and R = 0.980) with Point of Sickling (PoS5%), which is defined as the pO2 where a 5% decrease in EI is observed during deoxygenation. Furthermore, in vitro treatment with antisickling agents, including GBT440, which alter the oxygen affinity of hemoglobin, caused a reproducible left‐shift of the PoS, indicating improved deformability at lower oxygen tensions. When RBCs from 21 SCD patients were analyzed, we observed a significantly higher PoS in untreated homozygous SCD patients compared to treated patients and other genotypes. We conclude that the oxygenscan is a state‐of‐the‐art technique that allows for rapid analysis of sickling behavior in SCD patients. The method is promising for personalized treatment, development of new treatment strategies and could have potential in prediction of complications.
Short survival and frequent transformation in extranodal marginal zone lymphoma with multiple mucosal sites presentation
Authors: Alderuccio Juan Pablo , Zhao Wei , Desai Amrita , Ramdial Jeremy , Gallastegui Nicolas , Kimble Erik , de la Fuente Macarena I. , Husnain Muhammad , Rosenblatt Joseph D. , Alencar Alvaro J. , Schatz Jonathan H. , Moskowitz Craig H. , Chapman Jennifer R. , Vega Francisco , Reis Isildinha M. , Lossos Izidore S. 
Published: February 2019

AbstractBetween 11 and 37% of extranodal marginal zone lymphoma (EMZL) patients present with disease involvement in multiple mucosal sites (MMS). We analyzed 405 EMZL patients seen between 1995 and 2017: 265 (65.4%) patients presented with stage I disease, 49 of 309 (15.8%) patients with bone marrow involvement, and 35 of 328 (10.7%) patients with monoclonal gammopathy (MG). Forty‐three (10.6%) patients had MMS presentation, which was more frequently seen in patients aged >60 years (55.8%). Five (17.9%) of 28 MMS patients had MG. MMS patients commonly exhibited the International Prognostic Index (IPI) >2 (79.1%), Follicular Lymphoma International Prognostic Index (FLIPI) >2 (39.5%), and Mucosa‐Associated Lymphoid Tissue Lymphoma International Prognostic Index (MALT‐IPI) 2‐3 (60.5%). Both MMS presentation and MG were associated with shorter survival univariately. In multivariable Cox regression models, shorter progression‐free survival (PFS) and overall survival (OS) were observed in patients with MMS (hazard ratio [HR] = 3.08 and 2.92, respectively), age ≥60 years (HR = 1.52 and 2.45, respectively), and in patients who failed to attain a complete remission following initial therapy (HR = 3.27 and 2.13, respectively). Elevated lactate dehydrogenase was associated with shorter PFS (HR = 1.92), while anemia (HR = 2.46) was associated with shortened OS. MALT‐IPI ≥2 (HR = 2.47 and 4.75), FLIPI >2 (HR = 1.65 and 2.09), and IPI >2 (HR = 2.09 and 1.73) were associated with shorter PFS and OS, respectively. Higher grade transformation (HGT) occurred in 11 (25.6%) MMS patients with a 5‐year cumulative incidence of 13.2% (95% CI 4.7‐26.1%). EMZL patients with MMS presentation represent a novel clinical subset associated with shorter PFS, OS, and higher incidence of HGT that needs novel therapeutic approaches.
A Concise Stereoselective Synthesis of Naturally Occurring d‐Xylo‐C18‐Guggultetrol and its C2‐Epimer
Authors: Chandra Naveen , Fernandes Rodney A. 
Published: February 2019

Abstractd‐Gluconic acid δ‐lactone has served as an economical and commercially available key chiral template for a concise 7‐step stereoselective synthesis of d‐xylo‐ and d‐lyxo‐configured guggultetrols. The key steps involved are a one‐pot conversion of d‐gluconic acid δ‐lactone to γ‐vinyl‐β‐hydroxy‐γ‐lactone, a chain extension through a Grignard reaction and a diastereoselective Sharpless asymmetric dihydroxylation.
Second‐Sphere Biomimetic Multipoint Hydrogen‐Bonding Patterns to Boost CO2 Reduction of Iron Porphyrins
Authors: Gotico Philipp , Boitrel Bernard , Guillot Régis , Sircoglou Marie , Quaranta Annamaria , Halime Zakaria , Leibl Winfried , Aukauloo Ally 
Published: February 2019

AbstractInspired by nature's orchestra of chemical subtleties to activate and reduce CO2, we have developed a family of iron porphyrin derivatives in to which we have introduced urea groups functioning as multipoint hydrogen‐bonding pillars on the periphery of the porphyrinic ring. This structure closely resembles the hydrogen‐bond stabilization scheme of the carbon dioxide (CO2) adduct in the carbon monoxide dehydrogenase (CODH). We found that such changes to the second coordination sphere significantly lowered the overpotential for CO2 reduction in this family of molecular catalysts and importantly increased the CO2 binding rate while maintaining high turnover frequency (TOF) and selectivity. Entrapped water molecules within the molecular clefts were found to be the source of protons for the CO2 reduction.
Achieving High Affinity and Selectivity for Asymmetric Dimethylarginine by Putting a Lid on a Box
Authors: Mullins Alexandria G. , Pinkin Nicholas K. , Hardin Joshua A. , Waters Marcey L. 
Published: February 2019

AbstractThe methylation states of Lys and Arg represent a particularly challenging set of targets to distinguish selectively in water using synthetic receptors. To date, trimethyllysine (Kme3) is the only post translational modification (PTM) of the eight possible methylation states of Lys and Arg that can be recognized selectively. Here, we report the first synthetic receptor capable of selectively recognizing asymmetric dimethylarginine (Rme2a). This was achieved by using a biased dynamic combinatorial chemistry (DCC) library to generate a receptor mimicking the 5‐sided box‐like shape of Rme2 reader proteins, a feature that has been hypothesized to impart selectivity. Additionally, we synthesized a thioether‐linked analogue of the resulting receptor to provide a novel scaffold with maintained selectivity but greater stability. This work introduces strategies that can be applied towards achieving selectivity based on subtle differences in hydrophilic guests in aqueous solutions.
pH‐Responsive Pillar[6]arene‐based Water‐Soluble Supramolecular Hexagonal Boxes
Authors: Kaizerman‐Kane Dana , Hadar Maya , Tal Noam , Dobrovetsky Roman , Zafrani Yossi , Cohen Yoram 
Published: February 2019

AbstractWe describe the preparation of the first water‐soluble pH‐responsive supramolecular hexagonal boxes (SHBs) based on multiple charge‐assisted hydrogen bonds between peramino‐pillar[6]arenes 2 with the molecular “lid” mellitic acid (1 a). The interaction between 2 and 1 a, as well as the other “lids” pyromellitic and trimesic acids (1 b and 1 c, respecively) were studied by a combination of experimental and computational methods. Interestingly, the addition of 1 a to the complexes of the protonated form of pillar[6]arene 2, that is, 3, with bis‐sulfonate 4 a or 4 b, immediately led to guest escape along with the formation of closed 1 a22 supramolecular boxes. Moreover, the process of the openning and closing of the supramolecular boxes along with threading and escaping of the guests, respectively, was found to be reversible and pH‐responsive. This study paves the way for the easy and modular preparation of different SHBs that may have myriad applications.
Resonance‐Mediated Below‐Threshold Delayed Photoemission and Non‐Franck–Condon Photodissociation of Cold Oxyallyl Anions
Authors: Albeck Yishai , Lunny Katharine G. , Benitez Yanice , Shin Ashley J. , Strasser Daniel , Continetti Robert E. 
Published: February 2019

AbstractThe photoexcitation of cold oxyallyl anions was studied below the adiabatic detachment threshold at a photon energy of 1.60 eV. Photodetachment was observed through two product channels, delayed electron emission from a long‐lived anionic state and dissociative photodetachment via absorption of a second photon. The former produced stable neutral C3H4O, while the latter resulted in the concerted elimination of CO+C2H4 products. The neutral oxyallyl singlet state has a barrier‐free route to cyclopropanone as well as zwitterionic character with a large charge separation and dipole moment. The role of long‐lived dipole‐bound resonances built on the singlet state below the detachment threshold is discussed. These results provide one of the first observations of delayed photoemission in a small cold molecular radical anion, a consequence of the complex electronic structure of the neutral diradical, and provide an example of resonance‐mediated control of the photodissociation processes.
Wolff Rearrangement of Oxidatively Generated α‐Oxo Gold Carbenes: An Effective Approach to Silylketenes
Authors: Zheng Yang , Zhang Junqi , Cheng Xinpeng , Xu Xinfang , Zhang Liming 
Published: February 2019

AbstractGold‐catalyzed oxidations of alkynes by N‐oxides offer direct access to reactive α‐oxo gold carbene intermediates from benign and readily available alkynes instead of hazardous diazo carbonyl compounds. Despite various versatile synthetic methods developed based on this strategy, one of the hallmarks of α‐oxo carbene/carbenoid chemistry, that is, the Wolff rearrangement, has not been realized in this context. This study discloses the first examples that show the Wolff rearrangement can be readily realized by α‐oxo gold carbenes oxidatively generated from TBS‐terminated alkynes (TBS=tert‐butyldimethylsilyl). The thus‐generated silylketenes can be either isolated pure or subsequently trapped by various internal or external nucleophiles in one pot to afford α‐silylated carboxylic acids, their derivatives, or TBS‐substituted allenes.
Reliability assessment for load‐sharing systems with exponential components using statistical expansion as a correction
Authors: Xu Jianyu , Xie Min , Hu Qingpei 
Published: February 2019

AbstractAmong recent system models, one specific type of system is generally used to model the dependence among components. Components are connected parallel in such systems as they fail one by one and are supposed to share the system work load. The model is thus referred to as the load‐sharing system model. Despite the availability of extensive reliability assessment methods for different systems, load‐sharing systems have not received enough attention from the scholars who have studied reliability assessment so far. Load‐sharing systems are generally designed for high levels of reliability. Therefore, tests for such systems can be expensive and time consuming. Limitation on resources always leads to small test sample sizes. This increases the difficulties associated with obtaining an accurate and robust system reliability assessment result. This paper proposes a novel assessment method for a certain type of load‐sharing system with components following exponential lifetime distributions. Based on the parameter estimation of the system reliability model, we introduce the Winterbottom‐Cornish‐Fisher asymptotic expansion method for implementing a correction of normal approximation. We demonstrate the accuracy of our method through a series of examples and simulation studies.
Bauwerksuntersuchungen und Belastungsversuche an der Fuldatalbrücke Bergshausen
Authors: Höhl Patrick , Schüßler Svenja , Rudolf Martin , Lauterbach Andre 
Published: February 2019

AbstractParallel zu der Nachrechnung in den Stufen 1–3 wurden im Jahr 2016 an der Fuldatalbrücke Bergshausen umfangreiche Bauwerksuntersuchungen durchgeführt.Bei der Fuldatalbrücke Bergshausen handelt es sich um eine siebenfeldrige Talbrücke im Zuge der BAB 44, die südlich der Stadt Kassel das Fuldatal überspannt. Die ca. 700 m lange Stahlbrücke besteht aus zwei Teilbauwerken, die in den Jahren 1962 und 1971 fertiggestellt wurden.Es wurden zahlreiche Materialproben am Grundwerkstoff, an den Nieten und an den Pfeilern entnommen, um im Labor die mechanisch‐technologischen Kennwerte zu ermitteln. Nach statistischer Auswertung konnten angepasste Materialkennwerte für die statischen Berechnungen angesetzt werden.In zwei nächtlichen Vollsperrungen wurden an beiden Überbauten Belastungsversuche unter definierter Verkehrsbelastung durchgeführt. Dabei wurden Dehnungen und Beschleunigungen gemessen und anschließend mit den rechnerischen Ergebnissen abgeglichen. Die Auswertung der Messergebnisse diente insbesondere zur Kalibrierung des Berechnungsmodells.Der Bestand wurde bereichsweise sehr detailliert vermessen, unter anderem mittels 3‐D‐Laserscan.Der Gesamtplanungsauftrag hat die Anhebung der Tragfähigkeit für die verbleibenden zwölf Jahre Restlebensdauer zum Ziel. Die im Bericht erläuterten Untersuchungsergebnisse flossen in den Planungsprozess dieser Ertüchtigung ein.
Bayesian personalized treatment selection strategies that integrate predictive with prognostic determinants
Authors: Ma Junsheng , Stingo Francesco C. , Hobbs Brian P. 
Published: February 2019

AbstractThe evolution of “informatics” technologies has the potential to generate massive databases, but the extent to which personalized medicine may be effectuated depends on the extent to which these rich databases may be utilized to advance understanding of the disease molecular profiles and ultimately integrated for treatment selection, necessitating robust methodology for dimension reduction. Yet, statistical methods proposed to address challenges arising with the high‐dimensionality of omics‐type data predominately rely on linear models and emphasize associations deriving from prognostic biomarkers. Existing methods are often limited for discovering predictive biomarkers that interact with treatment and fail to elucidate the predictive power of their resultant selection rules. In this article, we present a Bayesian predictive method for personalized treatment selection that is devised to integrate both the treatment predictive and disease prognostic characteristics of a particular patient's disease. The method appropriately characterizes the structural constraints inherent to prognostic and predictive biomarkers, and hence properly utilizes these complementary sources of information for treatment selection. The methodology is illustrated through a case study of lower grade glioma. Theoretical considerations are explored to demonstrate the manner in which treatment selection is impacted by prognostic features. Additionally, simulations based on an actual leukemia study are provided to ascertain the method's performance with respect to selection rules derived from competing methods.
Entrepreneurial orientation and engagement of Pakistani small and medium enterprises in sustainable development practices: Mediating role of knowledge management
Authors: Iqbal Zeeshan , Malik Maimoona 
Published: February 2019

AbstractThis research aims to shed light on the association between entrepreneurial behavior of small and medium enterprises (SMEs) and their engagement in sustainable development (SD) practices with the mediation of knowledge management (KM). In order to examine the engagement of SMEs in SD, researchers used resource‐based view of the firm as theoretical lens and specifically, analyzed the effects of entrepreneurial orientation (EO) and KM. The self‐administrated research questionnaires were distributed among the senior management of SMEs, located in major cities of Pakistan, by using convenient sampling technique. The Partial least squares‐structural equation modeling (PLS‐SEM) approach was applied, by using SmartPLS software, to test the formulated hypotheses. The study results revealed that EO is positively associated with the KM. Furthermore, KM is positively and significantly associated with the engagement of SMEs in SD practices, particularly regarding the environment, human resource management, and community and local development. Finally, the KM powerfully mediates the associations between EO and engagement of SMEs in SD practices. The overall findings concluded that entrepreneurial‐oriented firms are more likely to engage in the mechanism of KM and SD. The research implications, limitations, and directions for future research were also discussed.
Quantified or nonquantified: How quantification affects consumers' motivation in goal pursuit
Authors: Zhang Yu‐dong , Li Dong‐jin , Zhang Chu‐bing , Zhang Hui‐long 
Published: February 2019

AbstractBeing exposed to more data and devices with tracking functions than ever, quantification is concerned by an increasing number of consumers. The self‐reflection from data may raise consumers' awareness of their own goals to better modify their behaviors. This paper describes consumers' reaction to quantification and confirms its motivational effect in goal pursuit. First, we investigate the motivational effect of quantification and reveal its internal mechanism from the individual–community perspective. Results show that quantification can promote consumers' goal pursuit motivation. A quantified (vs. nonquantified) way to track progress in pursuit of a goal can strengthen consumers' self‐empowerment (individual level) and difference‐insight (community level), thus enhancing the goal pursuit motivation. Second, we explore the moderating effect of some factors on the motivational effect of quantification. Results confirm that self‐empowerment can be enhanced with high data–color consistency, and difference‐insight can be increased with low outcome–process consistency. Third, we identify the validity of various data presentation modes. Using the interactive progress framing (to date with to go) together with the several subunits mode to deliver data in different progress stages is found to be an effective way to promote consumers' goal pursuit motivation.