bluuebunny/crossref_metadata_2025_split huggingface dataset:
Superhydrophilic and Underwater Superoleophobic Poly(propylene) Nonwoven Coated with TiO2 by Atomic Layer Deposition
Authors: Li Chen , Ren Lipei , Liu Xin , Zhang Chunhua , Chen Dongzhi , Xu Weilin , Qin Yong 
Published: November 2020

AbstractTo develop an effective and convenient solution for underwater repelling oil and cleaning up oily water, TiO2 nano‐coating is deposited on the surface of poly(propylene) nonwoven (PPN) by atomic layer deposition (ALD). There is no evident change in the morphologies comparing ALD‐modified PPN with PPN except for thickness. For oils of different densities, such as 1,2‐dichloroethane, methylene chloride, chloroform, carbon tetrachloride, n‐hexane, and petroleum ether, the underwater oil contact angle and underwater oil sliding angle of ALD‐modified PPN range from 152.25° to 156.19° and 5.63° to 8.80°, respectively, exhibiting superior superhydrophilicity and underwater superoleophobicity. Notably, ALD‐modified PPN shows a high chemical stability in different solutions, such as acid, alkali, salt, and polar solvent, which even can slightly improve the underwater superoleophobicity of TiO2 nano‐coating. The excellent underwater anti‐oil property, self‐cleaning property, robust chemical resistance, and easily scaled‐up preparation process of TiO2‐coated PPN suggest great potential for practical applications in the energy, environmental protection, marine anti‐fouling, and microflow control fields.
Elucidating and Mitigating Degradation Processes in Perovskite Light‐Emitting Diodes
Authors: Andaji‐Garmaroudi Zahra , Abdi‐Jalebi Mojtaba , Kosasih Felix U. , Doherty Tiarnan , Macpherson Stuart , Bowman Alan R. , Man Gabriel J. , Cappel Ute B. , Rensmo Håkan , Ducati Caterina , Friend Richard H. , Stranks Samuel D. 
Published: November 2020

AbstractHalide perovskites have attracted substantial interest for their potential as disruptive display and lighting technologies. However, perovskite light‐emitting diodes (PeLEDs) are still hindered by poor operational stability. A fundamental understanding of the degradation processes is lacking but will be key to mitigating these pathways. Here, a combination of in operando and ex situ measurements to monitor the performance degradation of (Cs0.06FA0.79MA0.15)Pb(I0.85Br0.15)3 PeLEDs over time is used. Through device, nanoscale cross‐sectional chemical mapping, and optical spectroscopy measurements, it is revealed that the degraded performance arises from an irreversible accumulation of bromide content at one interface, which leads to barriers to injection of charge carriers and thus increased nonradiative recombination. This ionic segregation is impeded by passivating the perovskite films with potassium halides, which immobilizes the excess halide species. The passivated PeLEDs show enhanced external quantum efficiency (EQE) from 0.5% to 4.5% and, importantly, show significantly enhanced stability, with minimal performance roll‐off even at high current densities (>200 mA cm−2). The decay half‐life for the devices under continuous operation at peak EQE increases from <1 to ≈15 h through passivation, and ≈200 h under pulsed operation. The results provide generalized insight into degradation pathways in PeLEDs and highlight routes to overcome these challenges.
Defect Suppression in Oriented 2D Perovskite Solar Cells with Efficiency over 18% via Rerouting Crystallization Pathway
Authors: Yang Yi , Liu Cheng , Syzgantseva Olga A. , Syzgantseva Maria A. , Ma Shuang , Ding Yong , Cai Molang , Liu Xuepeng , Dai Songyuan , Nazeeruddin Mohammad Khaja 
Published: November 2020

AbstractVertically oriented 2D perovskites exhibit promising optoelectronic properties and intrinsic stability, but their photovoltaic application is still limited by the low power conversion efficiency (PCE) compared to 3D analogs. Here, a new crystallization pathway (RCP) is reported to suppress defects in vertically oriented 2D perovskite caused by its over‐rapid self‐assembly behavior. By controlling the specific adsorption of an ammonium halide additive on different perovskite crystal planes, the dynamic preferred growth of (111) plane is intentionally restrained, and the minority (202) planes emerge as secondary nucleation sites to stimulate the creation of large grains. As the halogen‐regulated deprotonation of ammonium proceeds, the (111) crystal plane gradually recovers its growth dominance, and a vertically oriented 2D perovskite film finally forms with high homogeneity, reduced trap density of states, and desired carrier transport/collection kinetics. Solar cells using RCP‐2D films show a highly reproducible and stable PCE reaching 18.5% with a high fill factor of 83.4%. These findings provide critical missing information on simultaneously achieving highly oriented and less defective 2D perovskite films for excellent device performance.
Azobindungsbildung auf Metalloberflächen
Authors: Meng Xiangzhi , Klaasen Henning , Viergutz Lena , Schulze Lammers Bertram , Witteler Melanie C. , Mönig Harry , Amirjalayer Saeed , Liu Lacheng , Neugebauer Johannes , Gao Hong‐Ying , Studer Armido , Fuchs Harald 
Published: November 2020

AbstractDie Bildung von Azoverbindungen durch Redoxkreuzkupplung von Nitroarenen und Arylaminen, welche in Lösungsmittelchemie herausfordernd ist, wird durch Oberflächenchemie ermöglicht. Die Reaktionsprodukte werden mit einem kryogenen Rastertunnelmikroskop (STM) und per Röntgenphotoelektronenspektroskopie (XPS) analysiert. Durch die Verwendung gut konzipierter Vorläufer, welche eine Amino‐ und eine Nitrofunktion enthalten, werden Azopolymere durch hocheffiziente Nitro‐Amino‐Kreuzkupplung auf der Oberfläche hergestellt. Experimente mit anderen Substraten und Oberflächenorientierungen zeigen, dass die Metalloberfläche einen signifikanten Einfluss auf die Reaktionseffizienz hat. Zudem wurde herausgefunden, dass die Reaktion partiell oxidierter/reduzierter Vorläuferverbindungen in Dimerisierungsreaktionen ebenfalls stattfindet, was Licht auf den Mechanismus wirft, welcher durch DFT‐Berechnungen weiter untersucht wurde.
Hot‐Electron‐Induced Photothermal Catalysis for Energy‐Dependent Molecular Oxygen Activation
Authors: Zhang Wei , Chen Yu , Zhang Gong , Tan Xiao , Ji Qinghua , Wang Zhaowu , Liu Huijuan , Qu Jiuhui 
Published: November 2020

AbstractHot electrons activate reactants and reduce the activation energy barrier (Ea) of a reaction through electron donation. However, a comprehensive understanding of the intrinsic driving force of this electron‐donating effect is lacking, let alone the precise manipulation of electron donation processes. Herein, the essential and promotional role of hot electron energy on the electron‐donating effect was elucidated using molecular oxygen activation (MOA) as a model reaction. Through providing an available electron source to the conventional photo‐thermal conversion system, the high energy carried by hot electrons was liberated and greatly enhanced the electron donation towards the LUMO (π*) orbit of O2. The energy was also transferred to O2 and elevated the potential energy surface (PES) of MOA, which was reflected by the enhanced formation of superoxide oxygen anions. As predicted, the Ea of MOA decreased by 45.1 % and exhibited a substantial light dependence, demonstrating that MOA became energy‐efficient due to improved exploitation and conversion of photon energies.
Liquid Nanoparticles: Manipulating the Nucleation and Growth of Nanoscale Droplets
Authors: Wang Ruoxu , Han Fei , Chen Bo , Liu Lingmei , Wang Shaoyan , Zhang Hua , Han Yu , Chen Hongyu 
Published: November 2020

AbstractBy manipulating the nucleation and growth of solid materials, the synthesis of various sophisticated nanostructures has been achieved. Similar methodology, if applied to liquids, could enable the mass‐production and control of ultra‐small droplets at the scale of nanoparticles (10−18 L or below). It would be highly desirable since droplets play a fundamental role in numerous applications. Here we present a general strategy to synthesize and manipulate nanoscale droplets, similar to what has been done to solid nanoparticles in classic solution‐synthesis. It was achieved by a solute‐induced phase separation which initiates the nucleation of droplets from a homogeneous solution. These liquid nanoparticles have great potentials to be manipulated like their solid counterparts, borrowing from the vast methodologies of nanoparticle synthesis, such as burst nucleation, seeded growth, and co‐precipitation. Liquid nanoparticles also serve as a general synthetic platform, to fabricate nanoreactors, drug‐loaded carriers, and other hollow nanostructures with a variety of shell materials.
Dynamic Activation of Adsorbed Intermediates via Axial Traction for the Promoted Electrochemical CO2 Reduction
Authors: Wang Xinyue , Wang Yu , Sang Xiahan , Zheng Wanzhen , Zhang Shihan , Shuai Ling , Yang Bin , Li Zhongjian , Chen Jianmeng , Lei Lecheng , Adli Nadia Mohd , Leung Michael K. H. , Qiu Ming , Wu Gang , Hou Yang 
Published: November 2020

AbstractRegulating the local environment and structure of metal center coordinated by nitrogen ligands (M‐N4) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M‐N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni‐N4‐O/C). The Ni‐N4‐O/C electrocatalyst exhibited excellent CO2RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at −0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from −0.5 to −1.1 V. The superior CO2RR activity is due to the Ni‐N4‐O active moiety composed of a Ni‐N4 site with an additional oxygen atom that induces an axial traction effect.
Reduktion und Umlagerung eines Bor(I)‐Carbonylkomplexes
Authors: Rang Maximilian , Fantuzzi Felipe , Arrowsmith Merle , Krummenacher Ivo , Beck Eva , Witte Robert , Matler Alexander , Rempel Anna , Bischof Tobias , Radacki Krzysztof , Engels Bernd , Braunschweig Holger 
Published: November 2020

AbstractBei der Einelektronenreduktion eines durch eine cyclisches (Alkyl)(amino)carben (CAAC) stabilisierten Arylborylen‐Carbonylkomplexes erfolgt die Bildung eines dimeren Borylketyl‐Radikalanions, bedingt durch eine intramolekulare Arylmigration zum CO Kohlenstoffatom. Computergestützte Analyse liefert Hinweise auf eine radikalanionische [(CAAC)B(CO)Ar].− Zwischenstufe. Weiterführende Reduktion des entstandenen Komplexes liefert ein hoch nukleophiles (Boranyliden)methanolat.
Kinetic Barriers and Microscopic Mechanisms of Noble Gas Adsorption by Nanoporous γ‐Mg(BH4)2 Obtained by Means of Sub‐Second X‐Ray Diffraction
Authors: Dovgaliuk Iurii , Senkovska Irena , Li Xiao , Dyadkin Vadim , Filinchuk Yaroslav , Chernyshov Dmitry 
Published: November 2020

AbstractGas adsorption by porous frameworks sometimes results in structure “breathing”, “pores opening/closing”, “negative gas adsorption”, and other phenomena. Time‐dependent diffraction can address both kinetics of the guest uptake and structural response of the host framework. Using sub‐second in situ powder X‐ray diffraction, three intracrystalline diffusion scenarios have been evaluated from the isothermal kinetics of Ar, Kr, and Xe adsorption by nanoporous γ‐Mg(BH4)2. These scenarios are dictated by two possible simultaneous transport mechanisms: diffusion through the intra‐ (i) and interchannel apertures (ii) of γ‐Mg(BH4)2 crystal structure. The contribution of (i) and (ii) changes depending on the kinetic diameter of the noble gas molecule and temperature regime. The lowest single activation barrier for the smallest Ar suggests equal diffusion of the atoms trough both pathways. Contrary, for the medium sized Kr we resolve the contributions of two parallel transport mechanisms, which tentatively can be attributed to the smaller barrier of the migration paths via the channel like pores and the higher barrier for the diffusion via narrow aperture between these channels. The largest Xe atoms diffuse only along 1D channels and show the highest single activation barrier.
Azo bond formation on metal surfaces
Authors: Meng Xiangzhi , Klaasen Henning , Viergutz Lena , Schulze Lammers Bertram , Witteler Melanie C. , Mönig Harry , Amirjalayer Saeed , Liu Lacheng , Neugebauer Johannes , Gao Hong‐Ying , Studer Armido , Fuchs Harald 
Published: November 2020

AbstractThe formation of azo compounds via redox cross‐coupling of nitroarenes and arylamines, challenging in solution phase chemistry, is achieved by on‐surface chemistry. Reaction products are analyzed with a cryogenic scanning tunneling microscope (STM) and X‐ray photoelectron spectroscopy (XPS). By using well‐designed precursors containing both an amino and a nitro functionality, azo polymers are prepared on surface via highly efficient nitro‐amino cross‐coupling. Experiments conducted on other substrates and surface orientations reveal that the metal surface has a significant effect on the reaction efficiency. The reaction was further found to proceed from partially oxidized/reduced precursors in dimerization reactions, shedding light on the mechanism that was studied by DFT calculations.
Supramolecular Bait to Trigger Non‐Equilibrium Co‐Assembly and Clearance of Aβ42
Authors: Wu Te‐Haw , Lai Rai‐Hua , Yao Chun‐Nien , Juang Jyh‐Lyh , Lin Shu‐Yi 
Published: November 2020

AbstractIn living systems, non‐equilibrium states that control the assembly‐disassembly of cellular components underlie the gradual complexification of life, whereas in nonliving systems, most molecules follow the laws of thermodynamic equilibrium to sustain dynamic consistency. Little is known about the roles of non‐equilibrium states of interactions between supramolecules in living systems. Here, a non‐equilibrium state of interaction between supramolecular lipopolysaccharide (LPS) and Aβ42, an aggregate‐prone protein that causes Alzheimer's disease (AD), was identified. Structurally, Aβ42 presents a specific groove that is recognized by the amphiphilicity of LPS bait in a non‐equilibrium manner. Functionally, the transient complex elicits a cellular response to clear extracellular Aβ42 deposits in neuronal cells. Since the impaired clearance of toxic Aβ42 deposits correlates with AD pathology, the non‐equilibrium LPS and Aβ42 could represent a useful target for developing AD therapeutics.
Chiral Molecular Propellers of Triarylborane Ammonia Adducts
Authors: Kemper Michael , Engelage Elric , Merten Christian 
Published: November 2020

AbstractChiral molecular propeller conformations have been induced to various triaryl structures including trityl derivatives and triaryl boranes. For borane–amine adducts, such induced propeller chirality has not been reported yet due to the low energy barrier for racemization in common triarylboranes such as B(C6H5)3 or B(C6F5)3. Herein, we demonstrate that point chirality in side chains of chiral triarylborane–ammonia adducts, which feature intramolecular hydrogen bonds in addition to the dative N→B bond, can efficiently be transferred to triarylborane propeller chirality. Employing X‐ray crystallography and ECD/VCD spectroscopy for structural characterizations, we investigate three examples with different steric demands of the incorporated chiral alkoxy side groups. We elucidate the conformational preferences of the molecular propellers. Furthermore, we show that computationally predicted conformational preferences obtained for the isolated, only implicitly solvated molecules are actually opposite to the experimentally observed ones.
Reduction and Rearrangement of a Boron(I) Carbonyl Complex
Authors: Rang Maximilian , Fantuzzi Felipe , Arrowsmith Merle , Krummenacher Ivo , Beck Eva , Witte Robert , Matler Alexander , Rempel Anna , Bischof Tobias , Radacki Krzysztof , Engels Bernd , Braunschweig Holger 
Published: November 2020

AbstractThe one‐electron reduction of a cyclic (alkyl)(amino)carbene (CAAC)‐stabilized arylborylene carbonyl complex yields a dimeric borylketyl radical anion, resulting from an intramolecular aryl migration to the CO carbon atom. Computational analyses support the existence of a [(CAAC)B(CO)Ar].− radical anion intermediate. Further reduction leads to a highly nucleophilic dianionic (boraneylidene)methanolate.
Mg‐Pillared LiCoO2: Towards Stable Cycling at 4.6 V
Authors: Huang Yangyang , Zhu Yongcheng , Fu Haoyu , Ou Mingyang , Hu Chenchen , Yu Sijie , Hu Zhiwei , Chen Chien‐Te , Jiang Gang , Gu Hongkai , Lin He , Luo Wei , Huang Yunhui 
Published: November 2020

AbstractLiCoO2 is used as a cathode material for lithium‐ion batteries, however, cationic/anodic‐redox‐induced unstable phase transitions, oxygen escape, and side reactions with electrolytes always occur when charging LiCoO2 to voltages higher than 4.35 V, resulting in severe capacity fade. Reported here is Mg‐pillared LiCoO2. Dopant Mg ions, serving as pillars in the Li‐slab of LiCoO2, prevent slab sliding in a delithiated state, thereby suppressing unfavorable phase transitions. Moreover, the resulting Li‐Mg mixing structure at the surface of Mg‐pillared LiCoO2 is beneficial for eliminating the cathode‐electrolyte interphase overgrowth and phase transformation in the close‐to‐surface region. Mg‐pillared LiCoO2 exhibits a high capacity of 204 mAh g−1 at 0.2 C and an enhanced capacity retention of 84 % at 1.0 C over 100 cycles within the voltage window of 3.0–4.6 V. In contrast, pristine LiCoO2 has a capacity retention of 14 % within the same voltage window.
Effects of varying melt flow rates on laser melt‐electrospinning of low‐density polyethylene nanofibers
Authors: Zakaria Mohammad , Shibahara Kanta , Bhuiyan Anamul Hoque , Nakane Koji 
Published: November 2020

AbstractThe ultimate functionality and applicability of polymeric nanofibers are mainly to subject on its diameter. This study explores the influence of melt flow rates (MFRs) of low‐density polyethylene (LDPE) on the diameter of laser melt electrospun nanofibers. Ethylene‐vinyl alcohol (EVOH) copolymer was added to the nonpolar LDPE as a spinning aid. After electrospinning, the EVOH was removed from LDPE/EVOH blend fiber by treating with isopropanol/water solution and LDPE nanofiber was obtained with a diameter of only 190 ± 85 nm for the highest MFR. A linear diameter reduction was observed for pure LDPE and EVOH removed LDPE fiber with the increase of MFR. However, a slight diameter increment was reported for the LDPE/EVOH blend fiber with higher MFR due to the improved melt viscosity of the component. A massive diameter decrement was found after EVOH removal from the blended fiber, resulting in the renovation of microfiber to a stable nanoscale dimension.
Study on the damage behavior of carbon fiber composite after low‐velocity impact under hygrothermal aging
Authors: Zhou Song , Jia Yao Xiong , Xu Liang , Wang Lei , Hui Li 
Published: November 2020

AbstractIn this article, T800 carbon fiber/epoxy resin composite was subjected to hygrothermal aging. By analyzing the mass change, surface morphology before and after aging, infrared spectra, and dynamic mechanical properties, the effect of hygrothermal aging on the composite properties was studied. The hygrothermal aging of the composite after low‐velocity impact, the effects of environmental factors on the damaged area, and the post‐impact compression properties of composites were studied. The results showed that the saturation moisture absorption rate of the composite after aging (71°C constant temperature) was 0.88%. Upon increasing the impact energy, an indentation appeared before the inflection point at 35 J. When the impact energy was less than 15 J, aging did not affect invisible damage. Above this, the damaged area and number of internal cracks and defects in the composite were increased. After aging, the compressive strength of composite laminates with impact damage decreased obviously. During the aging stage, the residual compressive strength of the sample was the lowest in the moisture saturated state, and hygrothermal aging had little effect on the compression failure mode after impact.
Choice bracketing and experience‐based choice
Authors: Hadar Liat , Danziger Shai , Morwitz Vicki G. 
Published: November 2020

AbstractWe examine how choice bracketing affects expected value maximization in experience‐based choice. Experience‐based choices are a series of individual choices made sequentially, for which feedback follows each choice, and are thus naturally bracketed narrowly. Previous research broadly bracketed multiple experience‐based choices for decision makers by aggregating the choices (such that each choice pertained to multiple individual choices) or by reducing feedback frequency. We find that decision makers prompted to actively broad‐bracket experience‐based choices in the presence of immediate feedback on individual choices (which prompts narrow bracketing) are more likely to choose expected value maximizing options than decision makers prompted to narrow‐bracket these choices. This pattern replicated across four studies, using different manipulations of choice bracketing, forms of feedback (partial or full), payoffs (hypothetical or incentive‐compatible payoff), subject populations, and when the choices and outcome distribution involved prices or time. We discuss the theoretical and practical implications of our findings.
How potassium came to be the dominant biological cation: of metabolism, chemiosmosis, and cation selectivity since the beginnings of life
Authors: Korolev Nikolay 
Published: November 2020

AbstractIn the cytoplasm of practically all living cells, potassium is the major cation while sodium dominates in the media (seawater, extracellular fluids). Both prokaryotes and eukaryotes have elaborate mechanisms and spend significant energy to maintain this asymmetric K+/Na+ distribution. This essay proposes an original line of evidence to explain how bacteria selected potassium at the very beginning of the evolutionary process and why it remains essential for eukaryotes.
Sequential change point detection for high‐dimensional data using nonconvex penalized quantile regression
Authors: Ratnasingam Suthakaran , Ning Wei 
Published: November 2020

AbstractIn this paper, a sequential change point detection method is developed to monitor structural change in smoothly clipped absolute deviation (SCAD) penalized quantile regression (SPQR) models. The asymptotic properties of the test statistic are derived from the null and alternative hypotheses. In order to improve the performance of the SPQR method, we propose a post‐SCAD penalized quantile regression estimator (P‐SPQR) for high‐dimensional data. We examined the finite sample properties of the proposed methods via Monte Carlo studies under different scenarios. A real data application is provided to demonstrate the effectiveness of the method.