bluuebunny/crossref_metadata_2025_split huggingface dataset:
Stable Li Metal Anodes via Regulating Lithium Plating/Stripping in Vertically Aligned Microchannels
Authors: Wang Shu‐Hua , Yin Ya‐Xia , Zuo Tong‐Tong , Dong Wei , Li Jin‐Yi , Shi Ji‐Lei , Zhang Chang‐Huan , Li Nian‐Wu , Li Cong‐Ju , Guo Yu‐Guo 
Published: September 2017

AbstractLi anodes have been rapidly developed in recent years owing to the rising demand for higher‐energy‐density batteries. However, the safety issues induced by dendrites hinder the practical applications of Li anodes. Here, Li metal anodes stabilized by regulating lithium plating/stripping in vertically aligned microchannels are reported. The current density distribution and morphology evolution of the Li deposits on porous Cu current collectors are systematically analyzed. Based on simulations in COMSOL Multiphysics, the tip effect leads to preferential deposition on the microchannel walls, thus taking full advantage of the lightening rod theory of classical electromagnetism for restraining growth of Li dendrites. The Li anode with a porous Cu current collector achieves an enhanced cycle stability and a higher average Coulombic efficiency of 98.5% within 200 cycles. In addition, the resultant LiFePO4/Li full battery demonstrates excellent rate capability and stable cycling performance, thus demonstrating promise as a current collector for high‐energy‐density, safe rechargeable Li batteries.
Palladium‐Catalyzed [5+1] Annulation of 2‐(1‐Arylvinyl) Anilines and α‐Diazocarbonyl Compounds toward Multi‐functionalized Quinolines
Authors: Zhu Jiawei , Hu Weiming , Sun Song , Yu Jin‐Tao , Cheng Jiang 
Published: September 2017

AbstractA palladium‐catalyzed [5+1] annulation of 2‐(1‐arylvinyl) anilines and α‐diazocarbonyl compounds has been developed, affording a series of multi‐functionalized quinolines in moderate to good yields. This procedure proceeded with the sequential insertion of N−H bond to the palladium carbene, intramolecular Heck reaction and decarboxylation steps. In this reaction, alkyl 2‐diazophenylacetates served as C1 building block, which represents a key compliment to diazo chemistry.magnified image
Designing 1,5‐Naphthyridine‐2,6‐dione‐Based Conjugated Polymers for Higher Crystallinity and Enhanced Light Absorption to Achieve 9.63% Efficiency Polymer Solar Cells
Authors: Yoon Won Sik , Kim Dong Won , Choi Min‐Woo , Park Jun‐Mo , Park Soo Young 
Published: September 2017

AbstractHighly crystalline conjugated polymers represent a key material for producing high‐performance thick‐active‐layer polymer solar cells (PSCs). However, despite their potential, a limited number of crystalline polymers are used in PSCs because of the lack of highly coplanar acceptor building blocks and insufficient light absorptivity (α < 105) of most donor (D)–acceptor (A)‐type polymers. This study reports a series of novel 3,7‐di(thiophen‐2‐yl)‐1,5‐naphthyridine‐2,6‐dione (NTDT) acceptor‐based conjugated polymers, PNTDT‐2T, PNTDT‐TT, and PNTDT‐2F2T, synthesized with 2,2′‐bithiophene (2T), thieno[3,2‐b]thiophene (TT), and 3,3′‐difluoro‐2,2′‐bithiophene (2F2T) donor units, respectively. PNTDT‐2F2T exhibits superior polymer crystallinity and a much higher absorption coefficient than those of PNTDT‐2T or PNTDT‐TT because of adequate matching between highly coplanar A (NTDT) and D (2F2T) building blocks. A bulk heterojunction solar cell based on PNTDT‐2F2T exhibits a power conversion efficiency of up to 9.63%, with a high short circuit current of 18.80 mA cm−2 and fill factor of 0.70, when a thick active layer (>200 nm) is used, without postfabrication hot processing. The findings demonstrate that the polymer crystallinity and absorption coefficient can be effectively controlled by selecting appropriate D and A building blocks, and that NTDT is a novel and versatile A building block for highly efficient thick‐active‐layer PSCs.
Bicycling suppresses abnormal beta synchrony in the Parkinsonian basal ganglia
Authors: Storzer Lena , Butz Markus , Hirschmann Jan , Abbasi Omid , Gratkowski Maciej , Saupe Dietmar , Vesper Jan , Dalal Sarang S. , Schnitzler Alfons 
Published: September 2017

ObjectiveFreezing of gait is a poorly understood symptom of Parkinson disease, and can severely disrupt the locomotion of affected patients. However, bicycling ability remains surprisingly unaffected in most patients suffering from freezing, suggesting functional differences in the motor network. The purpose of this study was to characterize and contrast the oscillatory dynamics underlying bicycling and walking in the basal ganglia.MethodsWe present the first local field potential recordings directly comparing bicycling and walking in Parkinson disease patients with electrodes implanted in the subthalamic nuclei for deep brain stimulation. Low (13–22Hz) and high (23–35Hz) beta power changes were analyzed in 22 subthalamic nuclei from 13 Parkinson disease patients (57.5 ± 5.9 years old, 4 female). The study group consisted of 5 patients with and 8 patients without freezing of gait.ResultsIn patients without freezing of gait, both bicycling and walking led to a suppression of subthalamic beta power (13–35Hz), and this suppression was stronger for bicycling. Freezers showed a similar pattern in general. Superimposed on this pattern, however, we observed a movement‐induced, narrowband power increase around 18Hz, which was evident even in the absence of freezing.InterpretationThese results indicate that bicycling facilitates overall suppression of beta power. Furthermore, movement leads to exaggerated synchronization in the low beta band specifically within the basal ganglia of patients susceptible to freezing. Abnormal ∼18Hz oscillations are implicated in the pathophysiology of freezing of gait, and suppressing them may form a key strategy in developing potential therapies. Ann Neurol 2017;82:592–601
Protein Catenation Enhances Both the Stability and Activity of Folded Structural Domains
Authors: Wang Xiao‐Wei , Zhang Wen‐Bin 
Published: September 2017

AbstractCatenanes are intriguing molecular architectures with unique properties. Herein, we report the cellular synthesis of protein catenanes containing folded structural domains, aided by synergy between p53 dimerization and SpyTag/SpyCatcher chemistry. Concatenation of green fluorescent protein (GFP) was shown to increase chemical stability without disrupting the fluorescence properties, and concatenated dihydrofolate reductase (DHFR) exhibited a melting temperature around 4 °C higher and catalytic activity around 27 % higher than the wild‐type DHFR and the cyclic/linear controls. Catenation also confers considerable proteolytic resistance on DHFR. The results suggest that catenation could enhance both the stability and activity of folded proteins, thus making topology engineering an attractive approach for tailoring protein properties without varying their native sequences.
Regioselective Transformation of Long π‐Conjugated Backbones: From Oligofurans to Oligoarenes
Authors: Gadakh Sunita , Shimon Linda J. W. , Gidron Ori 
Published: September 2017

AbstractWe demonstrate the transformation of oligofurans through sequential Diels–Alder cycloaddition reactions to provide oligoarenes in two chemical steps, regardless of the oligomer length. By this method, oligonaphthalenes containing up to six units were obtained in high yield through the formation of up to 12 new C−C bonds. The versatility of this method was demonstrated for various polyaromatic hydrocarbons. The regioselectivity of this process enabled the synthesis of a library of substituted triarylenes from a single terfuran precursor by modification of the dienophile strength and the order of addition. Overall, this study demonstrates that long oligofurans are interesting not only as organic electronic materials, but also as starting materials for the formation of various conjugated systems.
Improved Biocompatibility of Black Phosphorus Nanosheets by Chemical Modification
Authors: Qu Guangbo , Liu Wei , Zhao Yuetao , Gao Jie , Xia Tian , Shi Jianbo , Hu Ligang , Zhou Wenhua , Gao Jiejun , Wang Huaiyu , Luo Qian , Zhou Qunfang , Liu Sijin , Yu Xue‐Feng , Jiang Guibin 
Published: September 2017

AbstractBlack phosphorus nanosheets (BPs) show great potential for various applications including biomedicine, thus their potential side effects and corresponding improvement strategy deserve investigation. Here, in vitro and in vivo biological effects of BPs with and without titanium sulfonate ligand (TiL4) modification are investigated. Compared to bare BPs, BPs with TiL4 modification (TiL4@BPs) can efficiently escape from macrophages uptake, and reduce cytotoxicity and proinflammation. The corresponding mechanisms are also discussed. These findings may not only guide the applications of BPs, but also propose an efficient strategy to further improve the biocompatibility of BPs.
Effector‐Triggered Self‐Replication in Coupled Subsystems
Authors: Komáromy Dávid , Tezcan Meniz , Schaeffer Gaël , Marić Ivana , Otto Sijbren 
Published: September 2017

AbstractIn living systems processes like genome duplication and cell division are carefully synchronized through subsystem coupling. If we are to create life de novo, similar control over essential processes such as self‐replication need to be developed. Here we report that coupling two dynamic combinatorial subsystems, featuring two separate building blocks, enables effector‐mediated control over self‐replication. The subsystem based on the first building block shows only self‐replication, whereas that based on the second one is solely responsive toward a specific external effector molecule. Mixing the subsystems arrests replication until the effector molecule is added, resulting in the formation of a host–effector complex and the liberation of the building block that subsequently engages in self‐replication. The onset, rate and extent of self‐replication is controlled by the amount of effector present.
CO Oxidation by Group 3 Metal Monoxide Cations Supported on [Fe(CO)4]2−
Authors: Chi Chaoxian , Qu Hui , Meng Luyan , Kong Fanchen , Luo Mingbiao , Zhou Mingfei 
Published: September 2017

AbstractInfrared photodissociation spectroscopy of mass‐selected heteronuclear cluster anions in the form of OMFe(CO)5− (M=Sc, Y, La) indicates that all these anions involve an 18‐electron [Fe(CO)4]2− building block that is bonded with the M center through two bridged carbonyl ligands. The OLaFe(CO)5− anion is determined to be a CO‐tagged complex involving a [Fe(CO)4]2−[LaO]+ anion core. In contrast, the OYFe(CO)5− anion is characterized to have a [Fe(CO)4]2−[Y(η2‐CO2)]+ structure involving a side‐on bonded CO2 ligand. The CO‐tagged complex and the [Fe(CO)4]2−[Sc(η2‐CO2)]+ isomer co‐exist for the OScFe(CO)5− anion. These observations indicate that both the ScO+ and YO+ cations supported on [Fe(CO)4]2− are able to oxidize CO to CO2. Theoretical analyses show that [Fe(CO)4]2− coordination significantly weakens the MO+ bond and decreases the energy gap of the interacting valence orbitals between MO+ and CO, leading to the CO oxidation reactions being both thermodynamically exothermic and kinetically facile.
Reaktivität eines Dihydrodiborens gegen CO: Koordination, Insertion, Spaltung und spontane Bildung eines cyclischen Alkins
Authors: Arrowsmith Merle , Böhnke Julian , Braunschweig Holger , Celik Mehmet Ali 
Published: September 2017

AbstractIn einer CO‐Atmosphäre geht das Dihydrodiboren [(cAAC)HB=BH(cAAC)] eine Koordination mit CO ein. Gleichzeitig findet eine reversible Wasserstoffmigration von einem Boratom auf das Carbenkohlenstoffatom sowie eine ebenfalls reversible CO‐Insertion in die B=B‐Bindung statt. Das Erhitzen des CO‐Addukts resultiert in zwei ungewöhnlichen Ringerweiterungsprodukten: zum einen in einer Verbindung mit einer B=C‐Bindung zu einem sechsgliedrigen 1,2‐Azaborinan‐3‐yliden, zum anderen in einem beispiellosen neungliedrigen, cyclischen Alkin als Resultat einer reduktiven CO‐Spaltung und spontaner Bildung einer C≡C‐Dreifachbindung.
Gold(III) Alkyne Complexes: Bonding and Reaction Pathways
Authors: Rocchigiani Luca , Fernandez‐Cestau Julio , Agonigi Gabriele , Chambrier Isabelle , Budzelaar Peter H. M. , Bochmann Manfred 
Published: September 2017

AbstractThe synthesis and characterization of hitherto hypothetical AuIII π‐alkyne complexes is reported. Bonding and stability depend strongly on the trans effect and steric factors. Bonding characteristics shed light on the reasons for the very different stabilities between the classical alkyne complexes of PtII and their drastically more reactive AuIII congeners. Lack of back‐bonding facilitates alkyne slippage, which is energetically less costly for gold than for platinum and explains the propensity of gold to facilitate C−C bond formation. Cycloaddition followed by aryl migration and reductive deprotonation is presented as a new reaction sequence in gold chemistry.
Patterned Colloidal Photonic Crystals
Authors: Hou Jue , Li Mingzhu , Song Yanlin 
Published: September 2017

AbstractColloidal photonic crystals (PCs) have been well developed because they are easy to prepare, cost‐effective, and versatile with regards to modification and functionalization. Patterned colloidal PCs contribute a novel approach to constructing high‐performance PC devices with unique structures and specific functions. In this review, an overview of the strategies for fabricating patterned colloidal PCs, including patterned substrate‐induced assembly, inkjet printing, and selective immobilization and modification, is presented. The advantages of patterned PC devices are also discussed in detail, for example, improved detection sensitivity and response speed of the sensors, control over the flow direction and wicking rate of microfluidic channels, recognition of cross‐reactive molecules through an array‐patterned microchip, fabrication of display devices with tunable patterns, well‐arranged RGB units, and wide viewing‐angles, and the ability to construct anti‐counterfeiting devices with different security strategies. Finally, the perspective of future developments and challenges is presented.
Low‐Temperature Reductive Aminolysis of Carbohydrates to Diamines and Aminoalcohols by Heterogeneous Catalysis
Authors: Pelckmans Michiel , Vermandel Walter , Van Waes Frederik , Moonen Kristof , Sels Bert F. 
Published: September 2017

AbstractShort amines, such as ethanolamines and ethylenediamines, are important compounds in today's bulk and fine chemicals industry. Unfortunately, current industrial manufacture of these chemicals relies on fossil resources and requires rigorous safety measures when handling explosive or toxic intermediates. Inspired by the elegant working mechanism of aldolase enzymes, a novel heterogeneously catalyzed process—reductive aminolysis—was developed for the efficient production of short amines from carbohydrates at low temperature. High‐value bio‐based amines containing a bio‐derived C2 carbon backbone were synthesized in one step with yields up to 87 C%, in the absence of a solvent and at a temperature below 405 K. A wide variety of available primary and secondary alkyl‐ and alkanolamines can be reacted with the carbohydrate to form the corresponding C2‐diamine. The presented reductive aminolysis is therefore a promising strategy for sustainable synthesis of short, acyclic, bio‐based amines.
Biocompositional and thermodecompositional analysis of South African agro‐waste corncob and husk towards production of biocommodities
Authors: Awosusi Ayotunde A. , Ayeni Augustine O. , Adeleke R. , Daramola Michael O. 
Published: September 2017

AbstractBiocompositional and thermodecompositional analyses of locally abundant agro‐wastes of South African corn were evaluated for their potential utilization as biocommodities via thermochemical and bioconversion processing. Corncob of Zea mays Zama star (white) & PAN 6Q‐252 (yellow) hybrid as well as the ear husks of South African sweet corn, Z. mays var. Saccharata were utilized in the beneficiation process. Proximate and elemental analyses were conducted to check for the moisture content, the ash content, the volatile matter, and the elemental composition of the agro‐waste samples. In addition, the thermal property of the waste, the surface chemistry and the calorific values were investigated using thermogravimetric analysis, Fourier‐transform infrared (FTIR) spectroscopy and bomb calorimetric technique, respectively. Significant amounts of alkali metals (Li, Na, and K) were found in the corn cob samples, and heavy metals such as thorium and uranium were detected in the ear husks, indicating that the biomass might not be suitable for use in thermochemical process. However, a relatively high volatile matter content recorded for the waste samples supports their use in thermochemical process with improved yield per gram of feed. These and other findings such as the high calorific value of the cob samples and the relatively low lignin‐to‐sugar ratio of the waste confirm previous reports regarding their suitability as feedstocks in thermo‐processing and bioprocessing. With the exception of the moisture content in ear husks, the minimal variation in the physicochemical property of the waste samples substantiates their suitability for co‐processing without major upsets in process kinetics. Results of other investigations such as the thermodecompositional behavior of the waste samples and the surface chemistry further shed light on the physicochemical property of the locally sourced lignocellulosic biomass waste samples. © 2017 Curtin University and John Wiley & Sons, Ltd.
The Incidence and Prevalence of Systemic Lupus Erythematosus in New York County (Manhattan), New York: The Manhattan Lupus Surveillance Program
Authors: Izmirly Peter M. , Wan Isabella , Sahl Sara , Buyon Jill P. , Belmont H. Michael , Salmon Jane E. , Askanase Anca , Bathon Joan M. , Geraldino‐Pardilla Laura , Ali Yousaf , Ginzler Ellen M. , Putterman Chaim , Gordon Caroline , Helmick Charles G. , Parton Hilary 
Published: September 2017

ObjectiveThe Manhattan Lupus Surveillance Program (MLSP) is a population‐based registry designed to determine the prevalence of systemic lupus erythematosus (SLE) in 2007 and the incidence from 2007 to 2009 among residents of New York County (Manhattan), New York, and to characterize cases by race/ethnicity, including Asians and Hispanics, for whom data are lacking.MethodsWe identified possible SLE cases from hospital records, rheumatologist records, and administrative databases. Cases were defined according to the American College of Rheumatology (ACR) classification criteria, the Systemic Lupus International Collaborating Clinics (SLICC) classification criteria, or the treating rheumatologist's diagnosis. Rates among Manhattan residents were age‐standardized, and capture–recapture analyses were conducted to assess case underascertainment.ResultsBy the ACR definition, the age‐standardized prevalence and incidence rates of SLE were 62.2 and 4.6 per 100,000 person‐years, respectively. Rates were ∼9 times higher in women than in men for prevalence (107.4 versus 12.5) and incidence (7.9 versus 1.0). Compared with non‐Hispanic white women (64.3), prevalence was higher among non‐Hispanic black (210.9), Hispanic (138.3), and non‐Hispanic Asian (91.2) women. Incidence rates were higher among non‐Hispanic black women (15.7) compared with non‐Hispanic Asian (6.6), Hispanic (6.5), and non‐Hispanic white (6.5) women. Capture–recapture adjustment increased the prevalence and incidence rates (75.9 and 6.0, respectively). Alternate SLE definitions without capture–recapture adjustment revealed higher age‐standardized prevalence and incidence rates (73.8 and 6.2, respectively, by the SLICC definition and 72.6 and 5.0 by the rheumatologist definition) than the ACR definition, with similar patterns by sex and race/ethnicity.ConclusionThe MLSP confirms findings from other registries on disparities by sex and race/ethnicity, provides new estimates among Asians and Hispanics, and provides estimates using the SLICC criteria.
New Saharan wind observations reveal substantial biases in analysed dust‐generating winds
Authors: Roberts Alexander J. , Marsham John H. , Knippertz Peter , Parker Douglas J. , Bart Mark , Garcia‐Carreras Luis , Hobby Matthew , McQuaid James B. , Rosenberg Philip D. , Walker Daniel 
Published: September 2017

AbstractFor the remote Sahara, the Earth's largest dust source, there has always been a near‐absence of data for evaluating models. Here, new observations from the Fennec project are used along with Sahelian data from the African Monsoon Multidisciplinary Analysis (AMMA) to give an unprecedented evaluation of dust‐generating winds in the European Centre for Medium‐Range Weather Forecasts ERA‐Interim reanalysis (ERA‐I). Consistent with past studies, near‐surface, high‐speed winds are lacking in ERA‐I and the diurnal variability is under‐represented. During the summer monsoon season, correlations of ERA‐I with observed wind‐speed are low (∼0.35 in Sahel and 0.25–0.4 in the Sahara). Fennec data show for the first time that: (1) correlations are reduced even in the Sahara, not directly influenced by the monsoon, (2) the systematic underestimation of observed winds by ERA‐I in the summertime Sahel extends into the central Sahara: potentially explaining the failure of global models to capture the observed global dust maximum that occurs over the summertime Sahara (such as CMIP5), and demonstrates that modelled winds must be improved if they are to capture this key feature of the climatology.
Systematic optimization of L‐tryptophan riboswitches for efficient monitoring of the metabolite in Escherichia coli
Authors: Jang Sungho , Jung Gyoo Yeol 
Published: September 2017

AbstractRiboswitches form a class of genetically encoded sensor‐regulators and are considered as promising tools for monitoring various metabolites. Functional parameters of a riboswitch, like dynamic or operational range, should be optimized before the riboswitch is implemented in a specific application for monitoring the target molecule efficiently. However, optimization of a riboswitch was not straightforward and required detailed studies owing to its complex sequence‐function relationship. Here, we present three approaches for tuning and optimization of functional parameters of a riboswitch using an artificial L‐tryptophan riboswitch as an example. First, the constitutive expression level was adjusted to control the dynamic range of an L‐tryptophan riboswitch. The dynamic range increased as the constitutive expression level increased. Then, the function of a riboswitch‐encoded protein was utilized to connect the regulatory response of the riboswitch to another outcome for amplifying the dynamic range. Riboswitch‐mediated control of the host cell growth enabled the amplification of the riboswitch response. Finally, L‐tryptophan aptamers with different dissociation constants were employed to alter the operational range of the riboswitch. The dose‐response curve was shifted towards higher L‐tryptophan concentrations when an aptamer with higher dissociation constant was employed. All strategies were effective in modifying the distinct functional parameters of the L‐tryptophan riboswitch, and they could be easily applied to optimization of other riboswitches owing to their simplicity.