bluuebunny/crossref_metadata_2025_split huggingface dataset:
Emerging Functional Porous Polymeric and Carbonaceous Materials for Environmental Treatment and Energy Storage
Authors: Zheng Bingna , Lin Xidong , Zhang Xingcai , Wu Dingcai , Matyjaszewski Krzysztof 
Published: November 2019

AbstractThe demand for practical and cost‐effective environmental treatment and energy storage materials is exploding. Porous polymeric and carbonaceous materials have attracted tremendous interest on account of their well‐developed porosity and tunable surface chemistry. Functionalization of pore structures further enhances their properties for environmental treatment and energy storage. Herein, the procedures for functionalization of porous structures are introduced, including predesign and postsynthetic strategies. Subsequently, the important advancements of emerging porous polymers for environmental treatment in sorption (e.g., organic micropollutant adsorption, heavy metal ion removal, radionuclide extraction, and oil absorption) and membrane separation (e.g., aqueous micropollutant separation, organic solvent nanofiltration, desalination and pervaporation), as well as for energy storage ranging from the electrodes and separators of batteries to supercapacitor electrodes are highlighted. Moreover, given the combined merits of high intrinsic conductivity, porosity, and physicochemical stability, novel polymer‐based porous carbons for energy storage are also highlighted. Key functionalization chemistry for each application is discussed and an in‐depth understanding of the structure–property relationships of these functional porous materials is provided. Finally, the challenges and perspectives of emerging functional porous polymeric and carbonaceous materials for environmental treatment and energy storage are proposed.
High‐Performance Quantum‐Dot Light‐Emitting Diodes Using NiOx Hole‐Injection Layers with a High and Stable Work Function
Authors: Lin Jian , Dai Xingliang , Liang Xiaoyong , Chen Desui , Zheng Xuerong , Li Yifei , Deng Yunzhou , Du Hui , Ye Yuxun , Chen Dong , Lin Chen , Ma Luying , Bao Qinye , Zhang Haibing , Wang Linjun , Peng Xiaogang , Jin Yizheng 
Published: November 2019

AbstractSolution‐processed oxide thin films are actively pursued as hole‐injection layers (HILs) in quantum‐dot light‐emitting diodes (QLEDs), aiming to improve operational stability. However, device performance is largely limited by inefficient hole injection at the interfaces of the oxide HILs and high‐ionization‐potential organic hole‐transporting layers. Solution‐processed NiOx films with a high and stable work function of ≈5.7 eV achieved by a simple and facile surface‐modification strategy are presented. QLEDs based on the surface‐modified NiOx HILs show driving voltages of 2.1 and 3.3 V to reach 1000 and 10 000 cd m−2, respectively, both of which are the lowest among all solution‐processed LEDs and vacuum‐deposited OLEDs. The device exhibits a T95 operational lifetime of ≈2500 h at an initial brightness of 1000 cd m−2, meeting the commercialization requirements for display applications. The results highlight the potential of solution‐processed oxide HILs for achieving efficient‐driven and long‐lifetime QLEDs.
Sustainable Membrane Production through Polyelectrolyte Complexation Induced Aqueous Phase Separation
Authors: Baig Muhammad Irshad , Durmaz Elif Nur , Willott Joshua D. , de Vos Wiebe M. 
Published: November 2019

AbstractNonsolvent induced phase separation (NIPS) is the most common approach to produce polymeric membranes. Unfortunately, NIPS relies heavily on aprotic organic solvents like N‐methyl‐pyrrolidone. These solvents are unsustainable, repro‐toxic for humans and are therefore becoming increasingly restricted within the European Union. A new and sustainable method, aqueous phase separation (APS), is reported that eliminates the use of organic solvents. A homogeneous solution of two polyelectrolytes, the strong polyanion poly(sodium 4‐styrenesulfonate) (PSS) and the weak polycation poly(allylamine hydrochloride) (PAH), is prepared at high pH, where PAH is uncharged. Immersing a film of this solution in a low pH bath charges the PAH and results in a controlled precipitation, forming a porous water‐insoluble polyelectrolyte complex, a membrane. Pore sizes can be tuned from micrometers to just a few nanometers, and even to dense films, simply by tuning the polyelectrolyte concentrations, molecular weights, and by changing the salinity of the bath. This leads to excellent examples of microfiltration, ultrafiltration, and nanofiltration membranes. Polyelectrolyte complexation induced APS is a viable and sustainable approach to membrane production that provides excellent control over membrane properties and even allows new types of separations.
Self‐Assembling of Conductive Interlayer‐Expanded WS2 Nanosheets into 3D Hollow Hierarchical Microflower Bud Hybrids for Fast and Stable Sodium Storage
Authors: Hu Xiang , Liu Yangjie , Li Junwei , Wang Genxiang , Chen Junxiang , Zhong Guobao , Zhan Hongbing , Wen Zhenhai 
Published: November 2019

AbstractTransition‐metal dichalcogenides have emerged as promising anodes of sodium ion batteries (SIBs). Their practical SIB application calls for an easy‐to‐handle synthetic technique capable of fabricating favorable properties with high conductivity and stable structure. Here, a solvothermal strategy is reported for bottom‐up self‐assembling of nanoflowers' building block, i.e., conductive interlayer‐expanded 2D WS2 nanosheets thanks to in situ interlayer modification by nitrogen‐doped carbon matrix, into 3D hollow microflower bud‐like hybrids (H‐WS2@NC). The 3D nano/microhierarchical hollow structures are constructed by conductive interlayer‐expanded WS2 nanosheets' building blocks, providing abundant channels facilitating mass transport/electrons transfer, robust protection layer to avoid the direct contact between WS2 nanosheets and electrolyte, sufficient inner space for accommodating volume variation, and decreased ions diffusion energy barrier for accelerating electrochemical kinetics, as revealed by density functional theory calculations. As such, the 3D H‐WS2@NC hybrids exhibit quite attractive sodium storage performance with high reversible capacity, superior rate capability, and impressively long cycling life. The 3D H‐WS2@NC is further verified as anode of sodium‐ion full cell pairing with Na3V2(PO4)3/rGO cathode, delivering a stable reversible capacity of 296 mAh g−1 at 0.5 A g−1 with high energy density of 128 Wh kg−1total at a power density of 386 W kg−1total.
Spatial Collection in Colloidal Quantum Dot Solar Cells
Authors: Ouellette Olivier , Lesage‐Landry Antoine , Scheffel Benjamin , Hoogland Sjoerd , García de Arquer F. Pelayo , Sargent Edward H. 
Published: November 2019

AbstractIn thin‐film photovoltaic (PV) research and development, it is of interest to determine where the chief losses are occurring within the active layer. Herein, a method is developed and presented by which the spatial distribution of charge collection, operando, is ascertained, and its application in colloidal quantum dot (CQD) solar cells is demonstrated at a wide range of relevant bias conditions. A systematic computational method that relies only on knowledge of measured optical parameters and bias‐dependent external quantum efficiency spectra is implemented. It is found that, in CQD PV devices, the region near the thiol‐treated hole‐transport layer suffers from low collection efficiency, as a result of bad band alignment at this interface. The active layer is not fully depleted at short‐circuit conditions, and this accounts for the limited short‐circuit current of these CQD solar cells. The high collection efficiency outside of the depleted region agrees with a diffusion length on the order of hundreds of nanometers. The method provides a quantitative tool to study the operating principles and the physical origins of losses in CQD solar cells, and can be deployed in thin‐film solar cell device architectures based on perovskites, organics, CQDs, and combinations of these materials.
Visual Appearance of Chiral Nematic Cellulose‐Based Photonic Films: Angular and Polarization Independent Color Response with a Twist
Authors: Chan Chun Lam Clement , Bay Mélanie M. , Jacucci Gianni , Vadrucci Roberto , Williams Cyan A. , van de Kerkhof Gea T. , Parker Richard M. , Vynck Kevin , Frka‐Petesic Bruno , Vignolini Silvia 
Published: November 2019

AbstractHydroxypropyl cellulose (HPC) is a biocompatible cellulose derivative capable of self‐assembling into a lyotropic chiral nematic phase in aqueous solution. This liquid crystalline phase reflects right‐handed circular polarized light of a specific color as a function of the HPC weight fraction. Here, it is demonstrated that, by introducing a crosslinking agent, it is possible to drastically alter the visual appearance of the HPC mesophase in terms of the reflected color, the scattering distribution, and the polarization response, resulting in an exceptional matte appearance in solid‐state films. By exploiting the interplay between order and disorder, a robust and simple methodology toward the preparation of polarization and angular independent color is developed, which constitutes an important step toward the development of real‐world photonic colorants.
Ternary Organic Solar Cells with Efficiency >16.5% Based on Two Compatible Nonfullerene Acceptors
Authors: Song Jiali , Li Chao , Zhu Lei , Guo Jing , Xu Jinqiu , Zhang Xuning , Weng Kangkang , Zhang Kangning , Min Jie , Hao Xiaotao , Zhang Yuan , Liu Feng , Sun Yanming 
Published: November 2019

AbstractA ternary structure has been demonstrated as being an effective strategy to realize high power conversion efficiency (PCE) in organic solar cells (OSCs); however, general materials selection rules still remain incompletely understood. In this work, two nonfullerene small‐molecule acceptors 3TP3T‐4F and 3TP3T‐IC are synthesized and incorporated as a third component in PM6:Y6 binary blends. The photovoltaic behaviors in the resultant ternary OSCs differ significantly, despite the comparable energy levels. It is found that incorporation of 15% 3TP3T‐4F into the PM6:Y6 blend results in facilitating exciton dissociation, increasing charge transport, and reducing trap‐assisted recombination. All these features are responsible for the enlarged PCE of 16.7% (certified as 16.2%) in the PM6:Y6:3TP3T‐4F ternary OSCs, higher than that (15.6%) in the 3TP3T‐IC containing ternary devices. The performance differences are mainly ascribed to the compatibility between the third component and the host materials. The 3TP3T‐4F guest acceptor exhibits an excellent compatibility with Y6, tending to form well‐mixed phases in the ternary blend without disrupting the favored bicontinuous transport networks, whereas 3TP3T‐IC displays a morphological incompatibility with Y6. This work highlights the importance of considering the compatibility for materials selection toward high‐efficiency ternary organic OSCs.
Surface‐2D/Bulk‐3D Heterophased Perovskite Nanograins for Long‐Term‐Stable Light‐Emitting Diodes
Authors: Han Tae‐Hee , Lee Jin‐Wook , Choi Yung Ji , Choi Chungseok , Tan Shaun , Lee Sung‐Joon , Zhao Yepin , Huang Yu , Kim Dongho , Yang Yang 
Published: November 2019

AbstractAlthough metal halide perovskite (MHP) light‐emitting diodes (LEDs) have demonstrated great potential in terms of electroluminescence efficiency, the operational stability of MHP LEDs currently remains the biggest bottleneck toward their practical usage. Well‐confined excitons/charge carriers in a dielectric/quantum well based on conventional spatial or potential confinement approaches substantially enhance radiative recombination in MHPs, but an increased surface‐to‐volume ratio and multiphase interfaces likely result in a high degree of surface or interface defect states, which brings about a critical environmentally/operationally vulnerable point on LED stability. Here, an effective solution is suggested to mitigate such drawbacks using strategically designed surface‐2D/bulk‐3D heterophased MHP nanograins for long‐term‐stable LEDs. The 2D surface‐functionalized MHP renders significantly reduced trap density, environmental stability, and an ion‐migration‐immune surface in addition to a fast radiative recombination owing to its spatially and potentially confined charge carriers, simultaneously. As a result, heterophased MHP LEDs show substantial improvement in operational lifetime (T50: >200 h) compared to conventional pure 3D or quasi‐2D counterparts (T50: < 0.2 h) as well as electroluminescence efficiency (surface‐2D/bulk‐3D: ≈7.70 ph per el% and pure 3D: ≈0.46 ph per el%).
Interfacial Engineering of W2N/WC Heterostructures Derived from Solid‐State Synthesis: A Highly Efficient Trifunctional Electrocatalyst for ORR, OER, and HER
Authors: Diao Jinxiang , Qiu Yu , Liu Shuangquan , Wang Weitao , Chen Kai , Li Hailong , Yuan Wenyu , Qu Yunteng , Guo Xiaohui 
Published: November 2019

AbstractTo meet the practical demand of overall water splitting and regenerative metal–air batteries, highly efficient, low‐cost, and durable electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) are required to displace noble metal catalysts. In this work, a facile solid‐state synthesis strategy is developed to construct the interfacial engineering of W2N/WC heterostructures, in which abundant interfaces are formed. Under high temperature (800 °C), volatile CNx species from dicyanodiamide are trapped by WO3 nanorods, followed by simultaneous nitridation and carbonization, to form W2N/WC heterostructure catalysts. The resultant W2N/WC heterostructure catalysts exhibit an efficient and stable electrocatalytic performance toward the ORR, OER, and HER, including a half‐wave potential of 0.81 V (ORR) and a low overpotential at 10 mA cm−2 for the OER (320 mV) and HER (148.5 mV). Furthermore, a W2N/WC‐based Zn–air battery shows outstanding high power density (172 mW cm−2). Density functional theory and X‐ray absorption fine structure analysis computations reveal that W2N/WC interfaces synergistically facilitate transport and separation of charge, thus accelerating the electrochemical ORR, OER, and HER. This work paves a novel avenue for constructing efficient and low‐cost electrocatalysts for electrochemical energy devices.
Plasmonic Color Laser Printing inside Transparent Gold Nanodisk‐Embedded Poly(dimethylsiloxane) Matrices
Authors: Cui Ximin , Zhu Xiaolong , Shao Lei , Wang Jianfang , Kristensen Anders 
Published: November 2019

AbstractPlasmonic color generation from metal nanostructures has attracted intensive attention because of their excellence in achieving high spatial resolution, strong color contrast, and long‐term durability. The limited area of plasmonic patterns anchored on substrates and produced by current top‐down methods, however, severely restricts the advanced developments and potential applications in structural color display. Herein a robust method for realizing the laser printing of plasmonic colors inside transparent gold nanodisk‐embedded poly(dimethylsiloxane) matrices is presented. It is found that various colors can not only be easily generated by embedding gold nanodisks of different sizes, but also finely varied by adjusting the laser pulse intensity during printing. It is further demonstrated that multiple color layers can be laser‐printed at different depths. Stereoscopic images in the 3D matrices are laser‐printed with sizes as large as 12 × 15 mm2 and a resolution of 4600 dots per inch.
Appropriate Nonlocal Hydrodynamic Models for the Characterization of Deep‐Nanometer Scale Plasmonic Scatterers
Authors: Kupresak Mario , Zheng Xuezhi , Vandenbosch Guy A. E. , Moshchalkov Victor V. 
Published: November 2019

AbstractThe interaction between light and plasmonic systems with deep‐nanometer characteristics, which is essentially governed by quantum mechanical effects, has been extensively studied by the nonlocal hydrodynamic approach. Several hydrodynamic models, supplemented by additional boundary conditions, have been introduced in order to describe the collective motion of the free electron gas in metals. Four hydrodynamic models, namely the hard wall hydrodynamic model (HW‐HDM), the curl‐free hydrodynamic model, the shear forces hydrodynamic model, and the quantum hydrodynamic model (Q‐HDM), are thoroughly investigated. The investigation studies the mode structure (the natural modes or, in quantum optics, the quasi‐normal modes) of the spherical core–shell topology, which is complemented by the plane wave response from the system. The results of the above hydrodynamic models are also compared with those of the specular reflection method. It is demonstrated that the choice of a particular hydrodynamic model strongly affects the natural frequencies and modes in the mode structure of the topology and thus drastically modifies the simulated fields in the near and far regions. Contrary to HW‐HDM and Q‐HDM, the other two hydrodynamic models fail to predict the particles’ response accurately, showing artifactual mode hybridization.
Glass Transition and Crystallization in Hexagonal Boron Nitride: Crucial Role of Orientational Order
Authors: Ravinder R. , Garg Prateet , Krishnan N. M. Anoop 
Published: November 2019

AbstractWhile extensive studies have been carried out on 2D crystals, their disordered counterpart, namely 2D glasses, remain poorly explored. Using molecular dynamics simulation, it is demonstrated that hexagonal boron nitride (h‐BN) can exhibit crystallization and glass transition. Similar to archetypical glasses, it is observed that the glassy structures are disordered, marked by the absence of any long‐range order while exhibiting some short‐range order. Further, the structures obtained are stable in three dimensions, confirming the realistic nature of the 2D glasses. Interestingly, it is observed that the orientational order of the h‐BN structure with respect to density as well as ground state enthalpy follows a master curve for both crystallization and glass transition, revealing thermally accessible regions for the structure. Further, the standard deviation of orientational order provides information about the spatial heterogeneity in the structure, the rearrangement of which results in the formation of crystal/glass. This suggests that the orientational order may play a crucial role in controlling the propensity for crystallization/glass transition in systems having directional bonds.
All‐Optical Switchable Vanadium Dioxide Integrated Coding Metasurfaces for Wavefront and Polarization Manipulation of Terahertz Beams
Authors: Li Jie , Yang Yue , Li Jining , Zhang Yating , Zhang Zhang , Zhao Hongliang , Li Fuyu , Tang Tingting , Dai Haitao , Yao Jianquan 
Published: November 2019

AbstractElectromagnetic metasurfaces are artificial 2D structures with sub‐wavelength size and have achieved a variety of functions. Coding metasurfaces or programmable metasurfaces are special phase‐manipulation type metasurfaces, which can be used for dynamic electromagnetic modulation and information processing in microwave band. However, programmable or tunable coding metasurfaces in terahertz band are still rare. All‐optical switchable coding metasurfaces based on vanadium dioxide (VO2) hybrid resonators are proposed for dynamic modulation of terahertz waves. The C‐shaped metal–VO2 hybrid resonators are switched from anisotropic structures to quasi‐isotropic ones due to insulator–metal transition of VO2, resulting in great attenuation of conversion efficiency for linearly polarized waves and Pancharatnam–Berry phase for circularly polarized waves. Based on this principle, several coding metasurfaces are shown for efficient and simultaneous switching of wavefront and polarization state of terahertz beams, including linearly and circularly polarized waves. It is worth mentioning that a new method for switchable shared‐aperture metasurfaces is also proposed, in which only a part of the unit cells are integrated with VO2 and tunable. This new scheme promotes the applications of terahertz coding metasurfaces such as high‐speed terahertz communication.
Application of the ESMACS Binding Free Energy Protocol to a Multi‐Binding Site Lactate Dehydogenase A Ligand Dataset
Authors: Wright David W. , Husseini Fouad , Wan Shunzhou , Meyer Christophe , van Vlijmen Herman , Tresadern Gary , Coveney Peter V. 
Published: November 2019

AbstractOver the past two decades, the use of fragment‐based lead generation has become a common, mature approach to identify tractable starting points in chemical space for the drug discovery process. This approach naturally involves the study of the binding properties of highly heterogeneous ligands. Such datasets challenge computational techniques to provide comparable binding free energy estimates from different binding modes. The performance of a range of statistically robust ensemble‐based binding free energy calculation protocols, called ESMACS (enhanced sampling of molecular dynamics with approximation of continuum solvent), is evaluated. Ligands designed to target two binding pockets in the lactate dehydogenase, a target protein, which vary in size, charge, and binding mode, are studied. When compared to experimental results, excellent statistical rankings are obtained across this highly diverse set of ligands. In addition, three approaches to account for entropic contributions are investigated: 1) normal mode analysis, 2) weighted solvent accessible surface area (WSAS), and 3) variational entropy. Normal mode analysis and WSAS correlate strongly with each other—although the latter is computationally far cheaper—but do not improve rankings. Variational entropy corrects exaggerated discrimination of ligands bound in different pockets but creates three outliers which reduce the quality of the overall ranking.
Electrochemical Mechanics of Metal Thin Films: Charge‐Induced Reversible Surface Stress for Actuation
Authors: Cheng Chuan , Grant Patrick S. , Lührs Lukas 
Published: November 2019

AbstractThe intrinsic charge‐induced surface stress of Ni thin films during electrochemical reactions with an alkaline electrolyte is measured in situ. Surface stresses induced by H absorption/desorption, α‐Ni(OH)2 formation, capacitive double‐layer charging, the α‐ to β‐Ni(OH)2 transformation, and β‐Ni(OH)2/β‐NiOOH redox reactions are identified, and each provided additive contributions to the overall stress state. Surface stresses are magnified in high‐surface‐area nanoporous Ni because local stress‐relaxation mechanisms are restricted when compared to a smooth Ni film. Ni film reversible tensile/compressive surface stresses correlate with anodic/cathodic potential scanning but with an opposite trend to that of a less reactive Au film. Surface stresses in the Ni films are up to 40 times that of Au films and suggest the possibility of using controlled surface‐stress generation for electrochemical actuation.