bluuebunny/crossref_metadata_2025_split huggingface dataset:
Casting Nanoporous Platinum in Metal–Organic Frameworks
Authors: Gao Xiang , Pei Xiaokun , Gardner David W. , Diercks Christian S. , Lee Seungkyu , Rungtaweevoranit Bunyarat , Prevot Mathieu S. , Zhu Chenhui , Fakra Sirine , Maboudian Roya 
Published: January 2019

AbstractNanocasting based on porous templates is a powerful strategy in accessing materials and structures that are difficult to form by bottom‐up syntheses in a controlled fashion. A facile synthetic strategy for casting ordered, nanoporous platinum (NP‐Pt) networks with a high degree of control by using metal–organic frameworks (MOFs) as templates is reported here. The Pt precursor is first infiltrated into zirconium‐based MOFs and subsequently transformed to 3D metallic networks via a chemical reduction process. It is demonstrated that the dimensions and topologies of the cast NP‐Pt networks can be accurately controlled by using different MOFs as templates. The Brunauer–Emmett–Teller surface areas of the NP‐Pt networks are estimated to be >100 m2 g−1 and they exhibit excellent catalytic activities in the methanol electrooxidation reaction (MEOR). This new methodology presents an attractive route to prepare well‐defined nanoporous materials for diverse applications ranging from energy to sensing and biotechnology.
Room Temperature Commensurate Charge Density Wave in Epitaxial Strained TiTe2 Multilayer Films
Authors: Fragkos Sotirios , Sant Roberto , Alvarez Carlos , Bosak Alexei , Tsipas Polychronis , Tsoutsou Dimitra , Okuno Hanako , Renaud Gilles , Dimoulas Athanasios 
Published: January 2019

AbstractThe group IVB 2D transition metal dichalcogenides are considered to be stable in the high symmetry trigonal octahedral structure due to the lack of unpaired d‐electrons on the metal site. It is found that multilayer epitaxial TiTe2 is an exception adopting a commensurate 2 × 2 × 2 charge density wave (CDW) structure at room temperature with an ABA type of stacking as evidenced by direct lattice imaging and reciprocal space mapping. The CDW is stabilized by highly anisotropic strain imposed by the substrate with an out‐off‐plane compression which reduces the interlayer van der Waals gap increasing the coupling between TiTe2 layers. A weaker 2 × 2 CDW is also confirmed at room temperature for epitaxial monolayer TiTe2. The addition of epitaxial strained TiTe2 to the family of CDW materials will enable real world applications that take advantage of a CDW ground state at room temperature.
Simultaneously Enhanced Efficiency and Stability of Perovskite Solar Cells with TiO2@CdS Core–Shell Nanorods Electron Transport Layer
Authors: Liu Wei , Chu Liang , Liu Nanjing , Cheng Yangfeng , Wu Fan , Li Yifeng , Pu Yong , Zhang Jian , Li Xing'ao , Huang Wei 
Published: January 2019

AbstractBoth demands of stability and efficiency constitute the gargantuan barriers of perovskite solar cells (PSCs), hampering the academic communities and industrial production. Herein, it is demonstrated that, after depositing optimized CdS shell layers on TiO2 nanorod arrays (NAs) by a simple and rapid chemical bath method at room temperature, the efficiency and stability of PSCs are simultaneously enhanced. The PSCs based on TiO2/CdS core–shell NAs achieve higher power conversion efficiency up to 17.71%, compared to 15.93% of the pristine TiO2 NAs‐based cells. Especially, the stability of the PSCs is prominently improved after optimized CdS layer modification without encapsulation. The significant enhancement of both efficiency and stability are mainly ascribed to that the type‐II structure of TiO2/CdS coaxial nanorods can suppress recombination, and the oxygen vacancies on TiO2 surfaces are not directly contacted with perovskite layers. The surface modification on TiO2 NAs opens up an alternative approach toward improving the performance and stability of PSCs.
Topological Charge Inversion of Optical Vortex with Geometric Metasurfaces
Authors: Zhang Yuchao , Gao Jie , Yang Xiaodong 
Published: January 2019

AbstractThe topological charge (TC) inversion of optical vortex is demonstrated along the beam propagation direction by using plasmonic geometric metasurfaces with the initial wave fronts designed from the principle of caustic surface. The detailed TC inversion evolution process is observed together with the transmutation point where the vortex vanishes. The orbital angular momentum (OAM) mode distributions during the TC inversion process are studied to show the dynamic redistributions of OAM mode density between the central area and the surrounding area of the beam with the total OAM conserved. Furthermore, the TC inversion of self‐accelerating vortex beam along the parabolic trajectory is presented. The realization of controlling TC inversion of optical vortex along arbitrary beam trajectory paves the way for many applications with more complex functionalities in optical trapping and manipulation, optical sensing, quantum information and computation, and data communication.
Phase‐Separation Engineering of Glass for Drastic Enhancement of Upconversion Luminescence
Authors: Fang Zaijin , Chen Zhi , Peng Wencai , Shao Chongyun , Zheng Shupei , Hu Lili , Qiu Jianrong , Guan Bai‐Ou 
Published: January 2019

AbstractOptical gain materials are of fundamental importance for various applications, such as lasers, lighting, optical communication, microscopy, and spectroscopy. However, the requirements for high luminescence efficiency and excellent thermodynamic stability of materials are always contradictory. As a result, wide applications of optical materials in high‐temperature, high‐humidity, and high‐power laser‐irradiated environments are restricted. Here, a facile approach based on phase‐separation engineering is proposed to modulate the thermodynamic stability and enhance the luminescence efficiency of optical gain materials. It is shown that the thermodynamic stability and luminescence efficiency of the phase‐separated fluorosilicate (FS) gain glass are both enhanced dramatically when the SiO2 concentration is optimized. Owing to the confinement effect of phase‐separation network structure on active ions, the upconversion (UC) luminescence efficiency of the designed glass is 150 times higher than that of traditional FS glasses and even seven times higher than that of ZBLAN (ZrF4‐BaF2‐LaF3‐AlF3‐NaF) glass, which is the most commonly used material for UC fiber lasing applications. These intriguing properties of the glass indicate that phase‐separation engineering not only provides a powerful solution to conquer the conventional contradiction between thermodynamic stability and luminescence efficiency but also offers significant opportunities for manufacturing a wide range of optical composites with multiple functions.
An Untethered Magnetic‐ and Light‐Responsive Rotary Gripper: Shedding Light on Photoresponsive Liquid Crystal Actuators
Authors: Pilz da Cunha Marina , Foelen Yari , van Raak Roel J. H. , Murphy Jeffrey N. , Engels Tom A. P. , Debije Michael G. , Schenning Albert P. H. J. 
Published: January 2019

AbstractHere, a remotely controlled dual magneto‐ and photoresponsive soft robotic gripper is reported, capable of loading, transport, rotation, and release of cargo. The untethered soft actuator consists of a magnetically responsive polydimethylsiloxane layer containing magnetic iron powder coated onto the central region of a light‐responsive liquid crystal polymer film hosting photochromic azobenzene dyes. Light is used to trigger the actuator to autonomously grab and pick up cargo with a high degree of control. Magnetic response is employed to conduct the locomotion as magnetic guidance, allowing the gripper to have both translational freedom and rotational freedom in its locomotion, differentiating the device from other soft robotic grippers. Control can be attained even in enclosed and/or confined spaces, through solely remote actuation. Through combined video, mechanical, and thermal analyses, the actuation mechanism of the light‐responsive liquid crystal network is investigated, shedding light on the decisive role of the temperature evolution in governing both rate of motion and deformation amplitude of the light‐responsive soft actuator.
Aldolase‐Catalyzed Asymmetric Synthesis of N‐Heterocycles by Addition of Simple Aliphatic Nucleophiles to Aminoaldehydes
Authors: Roldán Raquel , Hernández Karel , Joglar Jesús , Bujons Jordi , Parella Teodor , Fessner Wolf‐Dieter , Clapés Pere 
Published: January 2019

AbstractNitrogen heterocycles are structural motifs found in many bioactive natural products and of utmost importance in pharmaceutical drug development. In this work, a stereoselective synthesis of functionalized N‐heterocycles was accomplished in two steps, comprising the biocatalytic aldol addition of ethanal and simple aliphatic ketones such as propanone, butanone, 3‐pentanone, cyclobutanone, and cyclopentanone to N‐Cbz‐protected aminoaldehydes using engineered variants of d‐fructose‐6‐phosphate aldolase from Escherichia coli (FSA) or 2‐deoxy‐d‐ribose‐5‐phosphate aldolase from Thermotoga maritima (DERATma) as catalysts. FSA catalyzed most of the additions of ketones while DERATma was restricted to ethanal and propanone. Subsequent treatment with hydrogen in the presence of palladium over charcoal, yielded low‐level oxygenated N‐heterocyclic derivatives of piperidine, pyrrolidine and N‐bicyclic structures bearing fused cyclobutane and cyclopentane rings, with stereoselectivities of 96–98 ee and 97:3 dr in isolated yields ranging from 35 to 79%.magnified image
Gravure‐Printed Flexible Perovskite Solar Cells: Toward Roll‐to‐Roll Manufacturing
Authors: Kim Young Yun , Yang Tae‐Youl , Suhonen Riikka , Välimäki Marja , Maaninen Tiina , Kemppainen Antti , Jeon Nam Joong , Seo Jangwon 
Published: January 2019

AbstractRecent advances in perovskite solar cells (PSCs) have resulted in greater than 23% efficiency with superior advantages such as flexibility and solution‐processability, allowing PSCs to be fabricated by a high‐throughput and low‐cost roll‐to‐roll (R2R) process. The development of scalable deposition processes is crucial to realize R2R production of flexible PSCs. Gravure printing is a promising candidate with the benefit of direct printing of the desired layer with arbitrary shape and size by using the R2R process. Here, flexible PSCs are fabricated by gravure printing. Printing inks and processing parameters are optimized to obtain smooth and uniform films. SnO2 nanoparticles are uniformly printed by reducing surface tension. Perovskite layers are successfully formed by optimizing the printing parameters and subsequent antisolvent bathing. 2,2′,7,7′‐Tetrakis‐(N,N‐di‐4‐methoxyphenylamino)‐9,9′‐spirobifluorene is also successfully printed. The all‐gravure‐printed device exhibits 17.2% champion efficiency, with 15.5% maximum power point tracking efficiency for 1000 s. Gravure‐printed flexible PSCs based on a two‐step deposition of perovskite layer are also demonstrated. Furthermore, a R2R process based on the gravure printing is demonstrated. The champion efficiency of 9.7% is achieved for partly R2R‐processed PSCs based on a two‐step fabrication of the perovskite layer.
pH‐Controlled Multiple Interconversion between Cucurbit[7]uril‐Based Molecular Shuttle, [3]Pseudorotaxane and [2]Pseudorotaxane
Authors: Shi Hao , Zhang Kun , Lin Rui‐Lian , Sun Wen‐Qi , Chu Xiang‐Feng , Liu Xin‐Hua , Liu Jing‐Xin 
Published: January 2019

AbstractAn axle molecule 12+ containing one viologen nucleus and two identical p‐toluic acid sides was synthesized. The sequential binding of the Q[7] wheels to the 12+ axle leads to the formation of a molecular shuttle and then a homowheel, [3]pseudorotaxane. The [3]pseudorotaxane can reversibly transform to [2]pseudorotaxane by acid‐base control. On the other hand, the initially formed molecular shuttle can also transform to [2]pseudorotaxane directly and reversibly under pH control. As a whole, a molecular shuttle and [3]/[2]pseudorotaxanes constructed a pH‐controlled multiple interconvertible system.
Spontaneous and Fast Molecular Motion at Room Temperature in the Solid State
Authors: Alam Parvej , Leung Nelson L. C. , Cheng Yanhua , Zhang Haoke , Liu Junkai , Wu Wenjie , Kwok Ryan T. K. , Lam Jacky W. Y. , Sung Herman H. Y. , Williams Ian D. , Tang Ben Zhong 
Published: January 2019

AbstractThe development of molecular machines requires new building blocks which are easy to characterize and visualize to realize a complexity comparable to their natural counterparts such as biological enzymes. Furthermore, with the desire to build functional nanobots capable of navigating living organisms, it is necessary that the building blocks show mobility even in the solid state. Herein we report a system which is emissive in the amorphous state but is non‐fluorescent in the crystalline state due to the formation of extensive π‐π interactions. This dual nature could be exploited for easy visualization of its solid‐state molecular rearrangement. The emission of the amorphous film was quenched as the molecules spontaneously formed π‐π interactions even in the solid state. Scratching the non‐emissive film destroyed the interactions and restored the emission of the film. The emission quickly disappeared with an average lifetime of 20 s as the compound reformed the π‐network even at room temperature.
DNA‐Decorated, Helically Twisted Nanoribbons: A Scaffold for the Fabrication of One‐Dimensional, Chiral, Plasmonic Nanostructures
Authors: Golla Murali , Albert Shine K. , Atchimnaidu Siriki , Perumal Devanathan , Krishnan Nithiyanandan , Varghese Reji 
Published: January 2019

AbstractCrafting of chiral plasmonic nanostructures is extremely important and challenging. DNA‐directed organization of nanoparticle on a chiral template is the most appealing strategy for this purpose. Herein, we report a supramolecular approach for the design of DNA‐decorated, helically twisted nanoribbons through the amphiphilicity‐driven self‐assembly of a new class of amphiphiles derived from DNA and hexaphenylbenzene (HPB). The ribbons are self‐assembled in a lamellar fashion through the hydrophobic interactions of HPB. The transfer of molecular chirality of ssDNA into the HPB core results in the bias of one of the chiral propeller conformations for HPB and induces a helical twist into the lamellar packing, and leads to the formation of DNA‐wrapped nanoribbons with M‐helicity. The potential of the ribbon to act as a reversible template for the 1D chiral organization of plasmonic nanomaterials through DNA hybridization is demonstrated.
Die wiederaufladbare Aluminiumbatterie: Möglichkeiten und Herausforderungen
Authors: Yang Huicong , Li Hucheng , Li Juan , Sun Zhenhua , He Kuang , Cheng Hui‐Ming , Li Feng 
Published: January 2019

AbstractAluminiumbatteriesysteme werden infolge der geringen Kosten und der hohen volumetrischen Kapazität von Aluminiummetall sowie der hohen Sicherheit des gesamten Batteriesystems als eine mögliche Ergänzung für aktuelle Lithiumbatterien betrachtet. Bis dahin müssen jedoch z. B. die Verwendung von ionischen Flüssigkeiten als Elektrolyte, in denen AlCl4− anstelle von Al3+ vorliegt, verschiedene Interkalationsreagenzien, der langsame Diffusionsprozess im Feststoff sowie der rasche Kapazitätsverlust beim Zyklieren in Aluminiumbatterien gründlich untersucht werden. Um den Blick für die Möglichkeiten und Herausforderungen dieser neuartigen Aluminiumbatterien zu öffnen, diskutiert dieser Aufsatz die Reaktionsmechanismen sowie die Schwierigkeiten, die durch den dreiwertigen Ladungsträger in Elektrolyten, Elektroden und an den Elektroden‐Elektrolyt‐Grenzflächen verursacht werden. Wir möchten mit diesem Aufsatz Wissenschaftler und Ingenieure dazu anregen, zuverlässigere Aluminiumbatterien zu entwickeln.
Directed Evolution of a Bacterial Laccase (CueO) for Enzymatic Biofuel Cells
Authors: Zhang Lingling , Cui Haiyang , Zou Zhi , Garakani Tayebeh Mirzaei , Novoa‐Henriquez Catalina , Jooyeh Bahareh , Schwaneberg Ulrich 
Published: January 2019

AbstractEscherichia coli's copper efflux oxidase (CueO) has rarely been employed in the cathodic compartment of enzymatic biofuel cells (EBFCs) due to its low redox potential (0.36 V vs. Ag/AgCl, pH 5.5) towards O2 reduction. Herein, directed evolution of CueO towards a more positive onset potential was performed in an electrochemical screening system. An improved CueO variant (D439T/L502K) was obtained with a significantly increased onset potential (0.54 V), comparable to that of high‐redox‐potential fungal laccases. Upon coupling with an anodic compartment, the EBFC exhibited an open‐circuit voltage (Voc) of 0.56 V. Directed enzyme evolution by tailoring enzymes to application conditions in EBFCs has been validated and might, in combination with molecular understanding, enable future breakthroughs in EBFC performance
Syntheses, characterization, powder X‐ray diffraction analysis and antibacterial and antioxidant activities of triphenylantimony(V) heteroleptic derivatives containing substituted oximes and morpholine dithiocarbamate
Authors: Beniwal Savita , Kumar Ashok , Chhimpa Sunil , John P.J. , Singh Yashpal , Sharma Jyoti 
Published: January 2019

Triphenylantimony(V) heteroleptic derivatives containing substituted oximes and morpholine dithiocarbamate of the type Ph3Sb[R(R′)C:NO]2[S2CN(CH2CH2)2O] (where R = ─C6H5, R′ = ─CH3 (I); R = ─C6H4CH3, R′ = ─CH3 (II); R = ─C6H4Cl, R′ = ─CH3 (III); R = ─C6H4Br, R′ = ─CH3 (IV); R = ─C6H4OH, R′ = ─H (V); R(R′)C = CCH2(CH2)3CH2 (VI)) were synthesized by successive substitution reactions of triphenylantimony(V) dibromide with the sodium salt of substituted oximes and morpholine dithiocarbamate in unimolar ratio. All these newly synthesized derivatives were characterized using physicochemical and elemental analyses and tentative structures have been proposed on the basis of infrared, (1H, 13C) NMR and liquid chromatography–mass spectra. Spectral data revealed that the oxime behaves in a monodentate manner whereas morpholine dithiocarbamate behaves in an anisobidentate manner and thus distorted octahedral geometry has been proposed for these derivatives. Nanometric particle size (ca 25 nm) and monoclinic crystal system have been determined using power X‐ray diffraction data of two representative derivatives. Furthermore, these newly synthesized derivatives were screened against two bacteria, Bacillus subtilis (Gram‐positive) and Escherichia coli (Gram‐negative), to evaluate their antibacterial potential. Derivative VI exhibited maximum zone of inhibition (30 mm) against E. coli. Additionally two derivatives (I and II) were tested for their antioxidant potential, with derivative II exhibiting higher antioxidant potential (233 μM g−1). Structure–activity relationships were also investigated.
GIS method to design and assess the transportation performance of a decentralized biorefinery supply system and comparison with a centralized system: case study in southern Quebec, Canada
Authors: Lemire Pierre‐Olivier , Delcroix Benoit , Audy Jean‐François , Labelle François , Mangin Patrice , Barnabé Simon 
Published: January 2019

AbstractA decentralized supply chain that integrates biomass depots as an intermediate pre‐processing hub may be an efficient way to obtain stable and dense non‐food carbohydrate commodities that are economically transportable over long distances. This paper presents an integrated geographic information systems (GIS) method based on transport optimization to design and compare the performance of a decentralized versus a centralized biorefinery supply system. The method determines the suitable locations, allocations, sizing, and number of depots according to different demand location scenarios. The method is exemplified by a real case study in southern Quebec. In the design, the biomass depot generates raw sugar, shipped to the biorefinery, and co‐products that are used on site without transportation as animal feed and bioenergy. This diversification strategy provided by a joint production permits savings amounting to two‐thirds of the tonnage on the second transportation arc. The results present the average travel time performance in minutes in different scenarios. In the centralized configuration, the optimized stand‐alone biorefinery location scenario is 45% (59 min) and 58% (100 min) more efficient in terms of transportation than the two biorefineries located in existing industrial parks. However, the latter have a decentralized configuration that is more efficient than their centralized equivalents. In the decentralized configuration, depending on farmer participation, the biorefineries located in the existing industrial park have a transportation performance 16–42% (27–55 min) that is more efficient than their respective centralized configuration. Smaller depots and the use of numerous depots tend to reduce the average impedance as biomass availability increases. This is due to the economies of transportation related to a denser and more meshed network. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd
Characterizing adverse prenatal and postnatal experiences in children
Authors: Lebel Catherine A. , McMorris Carly A. , Kar Preeti , Ritter Chantel , Andre Quinn , Tortorelli Christina , Gibbard W. Ben 
Published: January 2019

BackgroundPrenatal and postnatal adversities, including prenatal alcohol exposure (PAE), prenatal exposure to other substances, toxic stress, lack of adequate resources, and postnatal abuse or neglect, often co‐occur. These exposures can have cumulative effects, or interact with each other, leading to worse outcomes than single exposures. However, given their complexity and heterogeneity, exposures can be difficult to characterize. Clinical services and research often overlook additional exposures and attribute outcomes solely to one factor.MethodsWe propose a framework for characterizing adverse prenatal and postnatal exposures and apply it to a cohort of 77 children. Our approach considers type, timing, and frequency to quantify PAE, other prenatal substance exposure, prenatal toxic stress, postnatal threat (harm or threat of harm), and postnatal deprivation (failure to meet basic needs) using a 4‐point Likert‐type scale. Postnatal deprivation and harm were separated into early (<24 months of age) and late (≥24 months) time periods, giving seven exposure variables. Exposures were ascertained via health records, child welfare records, interviews with birth parents, caregivers, and/or close family/friends.ResultsNearly all children had co‐occurring prenatal exposures, and two‐thirds had both prenatal and postnatal adversities. Children with high PAE were more likely to experience late postnatal adversities, and children with other prenatal substance exposure were more likely to have early postnatal deprivation. Postnatal adversities were more likely to co‐occur.ConclusionThis framework provides a comprehensive picture of a child's adverse exposures, which can inform assessment and intervention approaches and policy and will be useful for future research.