bluuebunny/crossref_metadata_2025_split huggingface dataset:
Phosphonium Modification Leads to Ultrapermeable Antibacterial Polyamide Composite Membranes with Unreduced Thickness
Authors: Peng Huawen , Zhang Wen‐Hai , Hung Wei‐Song , Wang Naixin , Sun Jian , Lee Kueir‐Rarn , An Quan‐Fu , Liu Cheng‐Mei , Zhao Qiang 
Published: April 2020

AbstractWater transport rate in network membranes is inversely correlated to thickness, thus superior permeance is achievable with ultrathin membranes prepared by complicated methods circumventing nanofilm weakness and defects. Conferring ultrahigh permeance to easily prepared thicker membranes remains challenging. Here, a tetrakis(hydroxymethyl) phosphonium chloride (THPC) monomer is discovered that enables straightforward modification of polyamide composite membranes. Water permeance of the modified membrane is ≈6 times improved, give rising to permeability (permeance × thickness) one magnitude higher than state‐of‐the‐art polymer nanofiltration membranes. Meanwhile, the membrane exhibits good rejection (RNa2SO4 = 98%) and antibacterial properties under crossflow conditions. THPC modification not only improves membrane hydrophilicity, but also creates additional angstrom‐scale channels in polyamide membranes for unimpeded transport of water. This unique mechanism provides a paradigm shift in facile preparation of ultrapermeable membranes with unreduced thickness for clean water and desalination.
All Dry Bottom‐Up Assembly of Omniphobic Interfaces
Authors: Ghaleni Mahdi Mohammadi , Kaviani Shayan , Rajwade Kimya , Bavarian Mona , Perreault François , Nejati Siamak 
Published: April 2020

AbstractCreating reentrant structures on flexible and porous substrates is a significant challenge for the scalable fabrication of omniphobic membranes. The design of such membranes requires control over the surface topography and chemistry of the interfacial domains. Here, a continuous bottom‐up method, based on initiated chemical vapor deposition, is developed to enable the fabrication of flexible omniphobic membranes. The developed membranes hinder the intrusion of droplets of low surface energy liquids (e.g., ethanol) colliding with the surface at a velocity of about 2 m s−1. The stable wetting resistance of the membranes allows for the desalination of low surface energy synthetic and municipal wastewater streams.
Simultaneously Enhancing Photoluminescence Quantum Efficiency and Optical Gain of Polyfluorene via Backbone Intercalation of 2,5‐Dimethyl‐1,4‐Phenylene
Authors: Zhang Qi , Wu Yinan , Lian Shaoshan , Gao Jinxin , Zhang Sihao , Hai Gang , Sun Chen , Li Xiangchun , Xia Ruidong , Cabanillas‐Gonzalez Juan , Mo Yueqi 
Published: April 2020

AbstractSimultaneous enhancement of photoluminescence quantum efficiency (PLQE) and optical gain in semiconducting polymer films is desirable for optically‐ or electrically‐pumped organic solid‐state lasers. In this work, a simple self‐dilution effect is achieved by introducing a small amount (≈10% by weight) of 2,5‐dimethyl‐1,4‐phenylene (DP) units in the backbone of poly(9,9‐dioctylfluorene) (PFO). The resulting copolymers, compared with PFO (PLQE 39%), exhibit a significantly increased PLQE (66%) while keeping similar absorption and photoluminescence profile, concomitant with an enhancement in optical gain properties. The radiative decay rate increases sharply along with a sustaining reduction in the non‐radiative decay rate in these copolymers, following similar principle of physical dilution of a luminescent compound in solution or in a polymer matrix. Among all the copolymers, the one containing 10% DP units exhibits the lowest amplified spontaneous emission/distributed feedback laser threshold (10.9 nJ/1.4 nJ, eightfold reduction), and the highest gain coefficient (54.4 cm−1). The results demonstrate that a moderate DP/fluorene ratio can maximize the beneficial self‐dilution effects. These investigations shed light on new design strategies to achieve conjugated polymers with concurrent high PLQE and large optical gain properties.
Interface Coassembly and Polymerization on Magnetic Colloids: Toward Core–Shell Functional Mesoporous Polymer Microspheres and Their Carbon Derivatives
Authors: Pan Panpan , Zhang Tong , Yue Qin , Elzatahry Ahmed A. , Alghamdi Abdulaziz , Cheng Xiaowei , Deng Yonghui 
Published: April 2020

AbstractCore–shell structured magnetic mesoporous polymer or carbon‐based microspheres not only possess the combined merits of magnetic particles and stable mesoporous shell but also provide various organic functional groups for further modification and immobilization of active sites, thus opening up more possibility for various applications. Herein, a bottom‐up soft‐templating strategy is developed to controllably synthesize core–shell magnetic mesoporous polydopamine microspheres (MMP) and their derivative magnetic mesoporous carbon (MMC) microspheres via an amphiphilic block copolymer‐directed interface assembly and polymerization (denoted as abc‐DIAP) approach. The obtained uniform MMP microspheres have a well‐defined structure consisting of magnetic core, silica middle layer and mesoporous PDA shell, uniform mesopores of 11.9 nm, high specific surface areas (235.6 m2 g−1) and rich functional groups. They show fast magnetic separation speed and superior performance in selective adsorption of Cyt.C from complex biosample solutions. Moreover, they can be in situ converted into core–shell magnetic mesoporous carbon (MMC) for efficient in‐pore immobilization of ultrafine Au nanoparticles for high‐efficiency catalytic epoxidation of styrene with high conversion (88.6%) and selectivity (90.1%) toward styrene oxide.
Molecular Basis of Ubiquitination Catalyzed by the Bacterial Transglutaminase MavC
Authors: Guan Hongxin , Fu Jiaqi , Yu Ting , Wang Zhao‐Xi , Gan Ninghai , Huang Yini , Perčulija Vanja , Li Yu , Luo Zhao‐Qing , Ouyang Songying 
Published: April 2020

AbstractThe Legionella pneumophila effector MavC is a transglutaminase that carries out atypical ubiquitination of the host ubiquitin (Ub)‐conjugation enzyme UBE2N by catalyzing the formation of an isopeptide bond between Gln40Ub and Lys92UBE2N, which leads to inhibition of signaling in the NF‐κB pathway. In the absence of UBE2N, MavC deamidates Ub at Gln40 or catalyzes self‐ubiquitination. However, the mechanisms underlying these enzymatic activities of MavC are poorly understood at the molecular level. This study reports the structure of the MavC–UBE2N–Ub ternary complex representing a snapshot of MavC‐catalyzed crosslinking of UBE2N and Ub, which reveals the way by which UBE2N–Ub binds to the Insertion and Tail domains of MavC. Based on the structural and experimental data, the catalytic mechanism for the deamidase and transglutaminase activities of MavC is proposed. Finally, by comparing the structures of MavC and MvcA, the homologous protein that reverses MavC‐induced UBE2N ubiquitination, several essential regions and two key residues (Trp255MavC and Phe268MvcA) responsible for their respective enzymatic activities are identified. The results provide insights into the mechanisms for substrate recognition and ubiquitination mediated by MavC as well as explanations for the opposite activity of MavC and MvcA in terms of regulation of UBE2N ubiquitination.
Metal‐Ion Coupled Electron Transfer Kinetics in Intercalation‐Based Transition Metal Oxides
Authors: Nikitina Victoria A. , Vassiliev Sergey Y. , Stevenson Keith J. 
Published: April 2020

AbstractElectrochemical metal‐ion intercalation systems are acknowledged to be a critical energy storage technology. The kinetics of the intercalation processes in transition‐metal based oxides determine the practical characteristics of metal‐ion batteries, such as the energy density, power, and cyclability. With the emergence of post lithium‐ion batteries, such as sodium‐ion and potassium‐ion batteries, which function predominately in nonaqueous electrolytes of special formulation and exhibit quite varied material stability with regard to their surface chemistries and reactivity with electrolytes, the practical routes for the optimization of metal‐ion battery performance become essential. Electrochemical methods offer a variety of means to quantitatively study the diffusional, charge transfer, and phase transformation rates in complex systems, which are, however, rather rarely fully adopted by the metal‐ion battery community, which slows down the progress in rationalizing the rate‐controlling factors in complex intercalation systems. Herein, several practical approaches for diagnosing the origin of the rate limitations in intercalation materials based on phenomenological models are summarized, focusing on the specifics of charge transfer, diffusion, and nucleation phenomena in redox‐active solid electrodes. It is demonstrated that information regarding rate‐determining factors can be deduced from relatively simple analysis of experimental methods including cyclic voltammetry, chronoamperometry, and impedance spectroscopy.
Alloy Anode Materials for Rechargeable Mg Ion Batteries
Authors: Niu Jiazheng , Zhang Zhonghua , Aurbach Doron 
Published: April 2020

AbstractRechargeable magnesium ion batteries are interesting as one of the alternative metal ion battery systems to lithium ion batteries due to the wide availability and accessibility of magnesium in the earth's crust. On the one hand, electrolyte solutions in which Mg metal anodes are fully reversible are not suitable for the use of high voltage/high capacity transition metal oxide cathodes due to complex surface phenomena. On the other hand, Mg metal anodes cannot work reversibly in conventional electrolyte solutions in which high voltage/high capacity Mg insertion cathodes can work because of passivation phenomena that fully block them. Replacing Mg metal with alternative anodes that can work reversibly in conventional electrolyte solutions could provide a promising route to elaborate high voltage and high capacity rechargeable Mg battery systems. Herein, the recent progress in alloy anodes based on group IIIA, IVA, VA elements is summarized. The theoretical evaluations, achievable capacities, synthetic strategies, battery test configurations, electrochemical properties, and underlying reaction mechanisms are systematically summarized and discussed. The key issues and challenges impeding their current use are identified and some valuable suggestions for their future development as practical reversible anodes for Mg batteries are provided.
The US Market for Agricultural Labor: Evidence from the National Agricultural Workers Survey
Authors: Li An , Reimer Jeffrey J. 
Published: April 2020

AbstractRecent changes in agricultural labor supply have created renewed interest in the market for farm labor. This study estimates the supply of farm labor using 1989–2016 data from the National Agricultural Workers Survey. In the preferred specification a $1 rise in wage is associated with workers supplying 0.538 more hours, all else held constant. This estimate masks changes in this relationship over time, however, as workers responded positively to wages before 2001, and reversed this relationship after 2001. Other results highlight the role of illegality, education, experience, gender, and other characteristics with respect to labor supply.
Low levels of ADAMTS‐13 with high anti‐ADAMTS‐13 antibodies during remission of immune‐mediated thrombotic thrombocytopenic purpura highly predict for disease relapse: A multi‐institutional study
Authors: Schieppati Francesca , Russo Laura , Marchetti Marina , Barcella Luca , Cefis Maurizio , Gomez‐Rosas Patricia , Caldara Gloria , Carpenedo Monica , D'Adda Mariella , Rambaldi Alessandro , Savignano Chiara , Billio Atto , Bruno Franco Massimiliano , Toschi Vincenzo , Falanga Anna 
Published: April 2020

AbstractImmune‐mediated thrombotic thrombocytopenic purpura (iTTP) is a life‐threatening immune‐mediated thrombotic microangiopathy. Daily therapeutic plasma exchange (TPE) and the optimized use of rituximab have strikingly improved the outcome of this disease, however the rate of disease recurrence remains high. Specific predictors of relapse in patients in remission can be relevant for an optimal patient management. In this study, we aimed to identify predictive variables of disease relapse in a multicenter cohort of 74 out of 153 iTTP patients. They were tested at different time points during remission for the levels of ADAMTS‐13 activity and autoantibody, and did not receive pre‐emptive treatment for ADAMTS‐13 activity deficiency during remission. The results showed that the association of ADAMTS13 activity ≤20% with a high anti‐ADAMTS‐13 titer at remission, and the time to response to first line treatment ≥13 days, were independent predictive factors of disease relapse. In addition, the use of rituximab in patients with exacerbation or refractoriness to TPE was significantly associated with reduced relapse rate. By Cox regression analysis, patients with ADAMTS‐13 activity ≤20% plus anti‐ADAMTS13 antibody titer ≥15 U/mL at remission had an increased risk of relapse (HR 1.98, CI 95% 1.087‐3.614; P < .02). These findings may help to outline more personalized therapeutic strategies in order to provide faster and sustained responses to first‐line iTTP treatment and prevent relapses in these patients.
Ecarin based coagulation testing
Authors: Gosselin Robert C. , Douxfils Jonathan 
Published: April 2020

AbstractEcarin is derived from venom of Echis carinatus, and will activate prothrombin into meizothrombin which will then cleave fibrinogen to result in clot formation. Ecarin based testing has been described for decades, but these assays were typically restricted to reference or speciality coagulation laboratories. This test was initially described for the assessment of direct thrombin inhibitors (eg, bivalirudin lepirudin, or argatroban) and was not affected by heparins or heparinoids. Ecarin based assays were rarely used for anticoagulation monitoring until the emergence of the direct oral thrombin inhibitor dabigatran etexilate in 2010. As this test was mentioned in the prescribing information for dabigatran etexilate, there was increased interest for use by clinical laboratories as the preferred method for assessing the anticoagulant effect of this drug. The purpose of this document is to review the current status of ecarin based assays for assessing dabigatran. This is with the understanding that these methods can also be exploited for determining the anticoagulation effect of parenteral direct thrombin inhibitors, such as argatroban and bivalirudin.
Aortic arch geometry predicts outcome in patients with Loeys–Dietz syndrome independent of the causative gene
Authors: Mariucci Elisabetta , Spinardi Luca , Stagni Silvia , Graziano Claudio , Lovato Luigi , Pacini Davide , Di Marco Luca , Careddu Lucio , Angeli Emanuela , Ciuca Cristina , Wischmeijer Anita , Gargiulo Gaetano , Donti Andrea 
Published: April 2020

AbstractThis study aimed to investigate the potential association between imaging features and cardiovascular outcomes in patients with Loeys–Dietz syndrome (LDS). We performed a retrospective cohort study of 36 patients with LDS and described cardiovascular events and imaging data. We observed different clinical courses in patients with LDS, irrespective of the causative gene. Angular or elongated aortic arch geometry correlated with aortic dissection (R = .39, p = .02), occurrence of the first cardiovascular event before 45 years of age (R = .36, p = .03), and the number of operations (R = 0.47, p = .004), but not with age (R = −.05, p = .79) or the causative gene (R = −0.04, p = .79). Relative absences of cardiovascular events at ages 20, 40, and 60 were 100, 75, and 56%, respectively, in patients with “romanesque” aortic arches, and 74, 39, and 21%, respectively, in patients with “gothic” and “elongated” aortic arches (p = .03). Angular or elongated aortic arch geometry is associated with early‐onset of disease and a worse cardiovascular outcome in LDS patients. Large multicenter studies are warranted to elucidate the impact of aortic arch morphology evaluation in clinical practice.
Chloro‐ and Trifluoromethyl Derivatives of Fullerene C82, C82Cl14 and C82(CF3)14
Authors: Tamm Nadezhda B. , Fritz Maria A. , Troyanov Sergey I. 
Published: April 2020

AbstractHigh‐temperature chlorination of a HPLC fraction containing fullerene C82 resulted in the isolation and X‐ray structure elucidation of the first chloro derivative of IPR C82, C82(3)Cl14. High‐temperature trifluoromethylatiion of a higher fullerene mixture followed by HPLC separation allowed the isolation and structural characterization of a new CF3 derivative, C82(3)(CF3)14. The addition patterns of C82(3)Cl14 and C82(3)(CF3)12–18 are discussed in terms of the formation of stabilizing substructures on a fullerene cage such as isolated C=C bonds and benzenoid rings.
Bridging Therapy or IV Thrombolysis in Minor Stroke with Large Vessel Occlusion
Authors: Seners Pierre , Perrin Claire , Lapergue Bertrand , Henon Hilde , Debiais Séverine , Sablot Denis , Girard Buttaz Isabelle , Tamazyan Ruben , Preterre Cécile , Laksiri Nadia , Mione Gioia , Arquizan Caroline , Lucas Ludovic , Baron Jean‐Claude , Turc Guillaume ,   MINOR‐STROKE Collaborators
Published: April 2020

ObjectiveWhether bridging therapy (intravenous thrombolysis [IVT] followed by endovascular treatment) is superior to IVT alone in minor stroke with large vessel occlusion (LVO) is unknown.MethodsMulticentric retrospective observational study including, in intention‐to‐treat, consecutive IVT‐treated minor strokes (National Institutes of Health Stroke Scale [NIHSS] ≤ 5) with LVO, with or without additional mechanical thrombectomy. Propensity‐score (inverse probability of treatment weighting) was used to reduce baseline between‐groups differences. The primary outcome was excellent outcome, that is, modified Rankin score 0 to 1 at 3 months follow‐up.ResultsOverall, 598 patients were included (214 and 384 in the bridging therapy and IVT groups, respectively). Following propensity‐score weighting, the distribution of baseline clinical and radiological variables was similar across the two patient groups. Compared with IVT alone, bridging therapy was not associated with excellent outcome (odds ratio [OR] = 0.96; 95% confidence interval [CI] = 0.75–1.24; p = 0.76), but was associated with symptomatic intracranial hemorrhage (OR = 3.01; 95% CI = 1.77–5.11; p < 0.0001). Occlusion site was a strong modifier of the effect of bridging therapy on outcome (pinteraction < 0.0001), with bridging therapy associated with higher odds of excellent outcome in proximal M1 (OR = 3.26; 95% CI = 1.67–6.35; p = 0.0006) and distal M1 (OR = 1.69; 95% CI = 1.01–2.82; p = 0.04) occlusions, but with lower odds of excellent outcome for M2 (OR = 0.53; 95% CI = 0.38–0.75; p = 0.0003) occlusions. Bridging therapy was associated with higher rates of symptomatic intracranial hemorrhage in M2 occlusions only (OR = 4.40; 95% CI = 2.20–8.83; p < 0.0001).InterpretationAlthough overall outcomes were similar in intended bridging therapy as compared to intended IVT alone in minor strokes with LVO, our results suggest that intended bridging therapy may be beneficial in M1 occlusions, whereas the benefit–risk profile may favor IVT alone in M2 occlusions. ANN NEUROL 2020 ANN NEUROL 2020;88:160–169
On‐Surface Synthesis of Cumulene‐Containing Polymers via Two‐Step Dehalogenative Homocoupling of Dibromomethylene‐Functionalized Tribenzoazulene
Authors: Urgel José I. , Di Giovannantonio Marco , Eimre Kristjan , Lohr Thorsten G. , Liu Junzhi , Mishra Shantanu , Sun Qiang , Kinikar Amogh , Widmer Roland , Stolz Samuel , Bommert Max , Berger Reinhard , Ruffieux Pascal , Pignedoli Carlo A. , Müllen Klaus , Feng Xinliang , Fasel Roman 
Published: April 2020

AbstractCumulene compounds are notoriously difficult to prepare and study because their reactivity increases dramatically with the increasing number of consecutive double bonds. In this respect, the emerging field of on‐surface synthesis provides exceptional opportunities because it relies on reactions on clean metal substrates under well‐controlled ultrahigh‐vacuum conditions. Here we report the on‐surface synthesis of a polymer linked by cumulene‐like bonds on a Au(111) surface via sequential thermally activated dehalogenative C−C coupling of a tribenzoazulene precursor equipped with two dibromomethylene groups. The structure and electronic properties of the resulting polymer with cumulene‐like pentagon–pentagon and heptagon–heptagon connections have been investigated by means of scanning probe microscopy and spectroscopy methods and X‐ray photoelectron spectroscopy, complemented by density functional theory calculations. Our results provide perspectives for the on‐surface synthesis of cumulene‐containing compounds, as well as protocols relevant to the stepwise fabrication of carbon–carbon bonds on surfaces.
Reversible Ligand‐Gated Ion Channel via Interconversion between Hollow Single Helix and Intertwined Double Helix
Authors: Bai Dongya , Yan Tengfei , Wang Shi , Wang Yanbo , Fu Jiya , Fang Xiaomin , Zhu Junyan , Liu Junqiu 
Published: April 2020

AbstractLigand responsiveness is one of the typical mechanisms in biological organization to trigger sophisticated channel switching. Here, we report a new type of helical trimer which can undergo transition between a hollow single helix and an intertwined double helix with no cavity by complexation and decomplexation of Cu ions. In addition, the one dimensional (1D) hollow helical tubes spontaneously generated from single helices via π‐π interactions embedded into the lipid bilayers and displayed satisfactory channel stability and efficiency. With the addition of CuIions and further extraction with ammonia, the disassembly and reassembly of 1D hollow helical tubes gave rise to the reversible switching of channel activity in situ inside the bilayers. The synthetic helical system provides the first model of reversible ligand‐gated ion channel by means of dynamic transition between single and double helices, which will be available for developing intelligent artificial nanochannels for potential biological and medicinal applications.
Modular and Versatile Trans‐Encoded Genetic Switches
Authors: Paul Avishek , Warszawik Eliza M. , Loznik Mark , Boersma Arnold J. , Herrmann Andreas 
Published: April 2020

AbstractCurrent bacterial RNA switches suffer from lack of versatile inputs and are difficult to engineer. We present versatile and modular RNA switches that are trans‐encoded and based on tRNA‐mimicking structures (TMSs). These switches provide a high degree of freedom for reengineering and can thus be designed to accept a wide range of inputs, including RNA, small molecules, and proteins. This powerful approach enables control of the translation of protein expression from plasmid and genome DNA.
Reply to the Comment on “Realization of Lewis Basic Sodium Anion in the NaBH3− Cluster”
Authors: Liu Gaoxiang , Fedik Nikita , Martinez‐Martinez Chalynette , Ciborowski Sandra M. , Zhang Xinxing , Boldyrev Alexander I. , Bowen Kit H. 
Published: April 2020

AbstractWe reply to the comment by S. Pan and G. Frenking who challenged our interpretation of the Na−:→BH3 dative bond in the recently synthesized NaBH3− cluster. Our conclusion remains the same as that in our original paper (https://doi.org/10.1002/anie.201907089 and https://doi.org/10.1002/ange.201907089). This conclusion is additionally supported by the energetic pathways and NBO charges calculated at UCCSD and CASMP2(4,4) levels of theory. We also discussed the suitability of the Laplacian of electron density (QTAIM) and Adaptive Natural Density Partitioning (AdNDP) method for bond type assignment. It seems that AdNDP yields more sensible results. This discussion reveals that the complex realm of bonding is full of semantic inconsistencies, and we invite experimentalists and theoreticians to elaborate this topic and find solutions incorporating different views on the dative bond.