bluuebunny/crossref_metadata_2025 huggingface dataset:
Waveform Selective Surfaces
Authors: Wakatsuchi Hiroki , Long Jiang , Sievenpiper Daniel F.
Published: January 2019

The role of frequency is very important in electromagnetics since it may significantly change how a material interacts with an incident wave if the frequency spectrum varies. Here, a new kind of microwave window is demonstrated that has the unique property of controlling transmission and reflection based on not only the frequency of an incoming wave but also the waveform or pulse width. This is achieved by designing a planar periodic surface with circuit elements including diodes, which convert most of the incoming signal to zero frequency. This surface can preferentially pass or reject different kinds of signals, such as short pulses or continuous waves, even if they occur at the same frequency. Such a structure can be used, for example, to allow long communication signals to pass through, while rejecting short radar pulses in the same frequency band. It is related to the classic frequency selective surface, but adds the new dimension of waveform selectivity, which is possible only by introducing nonlinear electronics into the surface. Thus, the study is expected to provide new solutions to both fundamental and applied electromagnetic issues ranging from traditional antenna design and wireless communications to emerging areas such as cloaking, perfect lenses, and wavefront shaping.
Reticulate Dual‐Nanowire Aerogel for Multifunctional Applications: a High‐Performance Strain Sensor and a High Areal Capacity Rechargeable Anode
Authors: Wang Zhipeng , Wang Yunsong , Chen Yijun , Yousaf Muhammad , Wu Huaisheng , Cao Anyuan , Han Ray P. S.
Published: January 2019

Nanowire aerogels (NWAs) are highly versatile and used in many applications. However, most synthesized NWAs are composed of single components that may produce unsatisfactory aggregated performance in mechanical strength, conductivity, and electrochemistry. To address this issue, a reticulate dual‐nanowire aerogel (rDNWA) composed of FeS2 nanowires and carbon nanotubes (CNTs) via a simple solvothermal method is synthesized. The rDNWA possesses excellent compressibility (modulus of 1.32 MPa), good conductivity (0.65 S cm−1), and high porosity (>98%). It can be applied as a high‐performance strain sensor with good sensitivity (Gauge Factor = 1.69) and enhanced stability. It can be densified to yield a high areal capacity of 10.0 mAh cm−2 and a high mass loading of 14.4 mg cm−2 after 100 cycles. As a freestanding anode for lithium ion battery (LIB), it exhibits a high specific mass capacity of 1031 mAh g−1 after 100 cycles at a current density of 100 mA g−1 and retains it to 729 mAh g−1 at a current density of 500 mA g−1 after 400 cycles. The outstanding overall performance of the hybrid aerogel is derived from the synergistic effect of intertwined CNTs and FeS2 nanowires and can be extended to fabricate NWAs with novel multifunctional capabilities.
Chiroptical‐Conjugated Polymer/Chiral Small Molecule Hybrid Thin Films for Circularly Polarized Light‐Detecting Heterojunction Devices
Authors: Kim Na Yeon , Kyhm Jihoon , Han Hyemi , Kim Soo Jin , Ahn Jongtae , Hwang Do Kyung , Jang Ho Won , Ju Byeong‐Kwon , Lim Jung Ah
Published: January 2019

Herein, a simple and facile strategy is described to obtain chiroptically active semiconductor thin films by blending of poly(3‐alkylthiophene)s, which are conventional achiral polymer semiconductors, and 1,1′‐binaphthyl (BN), a versatile chiral molecule. As expected, the intermolecular interaction between the two materials is important to extend the chirality of the binaphthyl molecules to the hybrid films. The controlled phase separation and crystallization of poly[3‐(6‐carboxyhexyl)thiophene‐2,5‐diyl] (P3CT) and binaphthyl hybrid films result in unique heterojunction bilayer thin‐film structures that consisted of BN microcrystals at the top and a P3CT/BN mixed layer at the bottom. Such heterojunction bilayer films exhibit significantly amplified chiroptical response with weak broadened tails, which is due to the enhanced crystallization of the chiral BN molecules and formation of heteroaggregates in the hybrid films. Based on the characterization of crystalline structure and photoluminescence analysis, it is found that new electronic energy states are formed in the conduction band region of P3CTs in the P3CT/BN heteroaggregates, which contribute to chirality transfer from BN to the hybrid films. As a proof of concept, a photodiode capable of distinguishably sensing the left‐ and right‐handed circularly polarized light is successfully fabricated by using the hybrid films with the heterojunction bilayer structure.
Magnetocontrollable Droplet and Bubble Manipulation on a Stable Amphibious Slippery Gel Surface
Authors: Guo Pu , Wang Zubin , Heng Liping , Zhang Yuqi , Wang Xuan , Jiang Lei
Published: January 2019

Smart manipulation of liquid/bubble transport has garnered widespread attention due to its potential applications in many fields. Designing a responsive surface has emerged as an effective strategy for achieving controllable transport of liquids/bubbles. However, it is still challenging to fabricate stable amphibious responsive surfaces that can be used for the smart manipulation of liquid in air and bubbles underwater. Here, amphibious slippery surfaces are fabricated using magnetically responsive soft poly(dimethylsiloxane) doped with iron powder and silicone oil. The slippery gel surface retains its magnetic responsiveness and demonstrates strong affinity for bubbles underwater but shows small and switching resistance forces with the water droplets in air and bubbles underwater, which is the key factor for achieving the controllable transport of liquids/bubbles. On the slippery gel surface, the sliding behaviors of water droplets and bubbles can be reversibly controlled by alternately applying/removing an external magnetic field. Notably, compared with slippery liquid‐infused porous surfaces, the slippery gel surface demonstrates outstanding stability, whether in air or underwater, even after 100 cycles of alternately applying/removing the magnetic field. This surface shows potential applications in gas/liquid microreactors, gas–liquid mixed fluid transportation, bubble/droplet manipulation, etc.
Graphynes for Water Desalination and Gas Separation
Authors: Qiu Hu , Xue Minmin , Shen Chun , Zhang Zhuhua , Guo Wanlin
Published: January 2019

Selective transport of mass through membranes, so‐called separation, is fundamental to many industrial applications, e.g., water desalination and gas separation. Graphynes, graphene analogs yet containing intrinsic uniformly distributed pores, are excellent candidates for highly permeable and selective membranes owing to their extreme thinness and high porosity. Graphynes exhibit computationally determined separation performance far beyond experimentally measured values of commercial state‐of‐the‐art polyamide membranes; they also offer advantages over other atomically thin membranes like porous graphene in terms of controllability in pore geometry. Here, recent progress in proof‐of‐concept computational research into various graphynes for water desalination and gas separation is discussed, and their theoretically predicted outstanding permeability and selectivity are highlighted. Challenges associated with the future development of graphyne‐based membranes are further analyzed, concentrating on controlled synthesis of graphyne, maintenance of high structural stability to withstand loading pressures, as well asthe demand for accurate computational characterization of separation performance. Finally, possible directions are discussed to align future efforts in order to push graphynes and other 2D material membranes toward practical separation applications.
Charged Metal Nanoparticles for Chemoelectronic Circuits
Authors: Zhao Xing , Guo Jiahui , Xiao Tao , Zhang Yuchun , Yan Yong , Grzybowski Bartosz A.
Published: January 2019

Although metal nanoparticles (NPs) stabilized with self‐assembled monolayers (SAMs) of various organic ligands have proven useful in applications ranging from chemical sensing, to bionanotechnology, to plasmonics and energy conversion, they have not been widely considered as suitable building blocks of electronic circuitry, largely because metals screen electric fields and prevent electrically tunable conductivity. However, when metal nanoparticles a few nanometers in size are stabilized by charged ligands and placed under bias, the counterions surrounding the NPs can redistribute and establish local electric fields that feed back into the electronic currents passing through the nanoparticles' metallic cores. Herein, the manner in which the interplay between counterion gradients and electron flows can be controlled by using different types of SAMs is discussed. This can give rise to a new class of nanoparticle‐based “chemoelectronic” logic circuits capable of sensing, processing, and ultimately reporting various chemical signals.
Carbon‐Based Metal‐Free Catalysts for Energy Storage and Environmental Remediation
Authors: Hu Chuangang , Lin Yi , Connell John W. , Cheng Hui‐Ming , Gogotsi Yury , Titirici Maria‐Magdalena , Dai Liming
Published: January 2019

Owing to their high earth‐abundance, eco‐friendliness, high electrical conductivity, large surface area, structure tunability at the atomic/morphological levels, and excellent stability in harsh conditions, carbon‐based metal‐free materials have become promising advanced electrode materials for high‐performance pseudocapacitors and metal–air batteries. Furthermore, carbon‐based nanomaterials with well‐defined structures can function as green catalysts because of their efficiency in advanced oxidation processes to remove organics in air or from water, which reduces the cost for air/water purification and avoids cross‐contamination by eliminating the release of heavy metals/metal ions. Here, the research and development of carbon‐based catalysts in supercapacitors and batteries for clean energy storage as well as in air/water treatments for environmental remediation are reviewed. The related mechanistic understanding and design principles of carbon‐based metal‐free catalysts are illustrated, along with the challenges and perspectives in this emerging field.
Phytochrome‐Based Extracellular Matrix with Reversibly Tunable Mechanical Properties
Authors: Hörner Maximilian , Raute Katrin , Hummel Barbara , Madl Josef , Creusen Guido , Thomas Oliver S. , Christen Erik H. , Hotz Natascha , Gübeli Raphael J. , Engesser Raphael , Rebmann Balder , Lauer Jasmin , Rolauffs Bernd , Timmer Jens , Schamel Wolfgang W. A. , Pruszak Jan , Römer Winfried , Zurbriggen Matias D. , Friedrich Christian , Walther Andreas , Minguet Susana , Sawarkar Ritwick , Weber Wilfried
Published: January 2019

Interrogation and control of cellular fate and function using optogenetics is providing revolutionary insights into biology. Optogenetic control of cells is achieved by coupling genetically encoded photoreceptors to cellular effectors and enables unprecedented spatiotemporal control of signaling processes. Here, a fast and reversibly switchable photoreceptor is used to tune the mechanical properties of polymer materials in a fully reversible, wavelength‐specific, and dose‐ and space‐controlled manner. By integrating engineered cyanobacterial phytochrome 1 into a poly(ethylene glycol) matrix, hydrogel materials responsive to light in the cell‐compatible red/far‐red spectrum are synthesized. These materials are applied to study in human mesenchymal stem cells how different mechanosignaling pathways respond to changing mechanical environments and to control the migration of primary immune cells in 3D. This optogenetics‐inspired matrix allows fundamental questions of how cells react to dynamic mechanical environments to be addressed. Further, remote control of such matrices can create new opportunities for tissue engineering or provide a basis for optically stimulated drug depots.
An Ultra‐Shapeable, Smart Sensing Platform Based on a Multimodal Ferrofluid‐Infused Surface
Authors: Ahmed Abdelsalam , Hassan Islam , Mosa Islam M. , Elsanadidy Esraa , Sharafeldin Mohamed , Rusling James F. , Ren Shenqiang
Published: January 2019

The development of wearable, all‐in‐one sensors that can simultaneously monitor several hazard conditions in a real‐time fashion imposes the emergent requirement for a smart and stretchable hazard avoidance sensing platform that is stretchable and skin‐like. Multifunctional sensors with these features are problematic and challenging to accomplish. In this context, a multimodal ferrofluid‐based triboelectric nanogenerator (FO‐TENG), featuring sensing capabilities to a variety of hazard stimulus such as a strong magnetic field, noise level, and falling or drowning is reported. The FO‐TENG consists of a deformable elastomer tube filled with a ferrofluid, as a triboelectric layer, surrounded by a patterned copper wire, as an electrode, endowing the FO‐TENG with excellent waterproof ability, conformability, and stretchability (up to 300%). In addition, The FO‐TENG is highly flexible and sustains structural integrity and detection capability under repetitive deformations, including bending and twisting. This FO‐TENG represents a smart multifaceted sensing platform that has a unique capacity in diverse applications including hazard preventive wearables, and remote healthcare monitoring.
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

Nanocasting 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

The 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

Both 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

The 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

Optical 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

Here, 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

Nitrogen 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%.

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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

Recent 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

An 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

The 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

Crafting 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

Aluminiumbatteriesysteme 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

Escherichia 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

A 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

Background

Prenatal 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.

Methods

We 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.

Results

Nearly 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.

Conclusion

This 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.
Development and validation of a risk scoring system based on baseline angiographic results by visual estimation for risk prEdiction of side‐branch OccLusion in coronary bifurcation InterVEntion: The baseline V‐RESOLVE score
Authors: He Yuan , Zhang Dong , Yin Dong , Zhu Chenggang , Feng Lei , Song Chenxi , Chen Changzhe , Feng Lei , Dou Kefei
Published: January 2019

Objective

We aimed to adapt the visual estimation for Risk prEdiction of side‐branch OccLusion in coronary bifurcation interVEntion (V‐RESOLVE) score to enable risk prediction for side‐branch (SB) occlusion using only baseline coronary angiogram data.

Background

The V‐RESOLVE score, which comprises angiographic factors at baseline and after lesion preparation, is a validated tool for predicting SB occlusion risk in coronary bifurcation intervention.

Methods

To develop and validate the new scoring system, we used data pertaining to 1,545 patients and another 1,286 consecutive patients. Baseline V‐RESOLVE was derived from V‐RESOLVE by replacing the two pre‐stenting angiographic factors with the corresponding preprocedural characteristics, while maintaining the scoring standard itself. We evaluated the diagnostic performance of baseline V‐RESOLVE for predicting SB occlusion and preformed risk stratification with characterization of non‐high‐risk and high‐risk lesions.

Results

The area under the receiver operating characteristic curves was similar between baseline V‐RESOLVE and V‐RESOLVE (0.735 vs 0.756, P = 0.191), with good calibration for baseline V‐RESOLVE (Hosmer‐Lemeshow P = 0.714). Upon categorization by the baseline V‐RESOLVE score, high‐risk lesions (score: 14–43) demonstrated significantly higher rate of SB occlusion than did non‐high‐risk lesions (score: 0–13) (17.31% vs 4.74%, P < 0.01). Considering the V‐RESOLVE‐based risk stratification as reference, baseline V‐RESOLVE had an integrated discrimination index of −1.81% (P = 0.052), and net reclassification improvement of −3.34% (P = 0.509). Upon validation, baseline V‐RESOLVE provided satisfactory diagnostic performance and risk stratification.

Conclusions

Baseline V‐RESOLVE predicts SB occlusion in coronary bifurcation intervention based solely on the preprocedural angiographic results.
Angiographic predictors of adverse outcomes after percutaneous coronary intervention in patients with radiation associated coronary artery disease
Authors: Reed Grant W. , Rossi Jeffrey E. , Masri Ahmad , Griffin Brian P. , Ellis Stephen G. , Kapadia Samir R. , Desai Milind Y.
Published: January 2019

Objectives

To determine procedural predictors of long‐term outcomes for patients with radiation associated coronary artery disease (CAD) treated with percutaneous coronary intervention (PCI).

Background

Patients who develop CAD after external beam radiation therapy (XRT) for cancer are at high‐risk for adverse events following PCI. It is unknown if specific angiographic features can predict outcomes in this population.

Methods

This is an observational study of 157 patients with malignancy who received XRT prior to PCI. Rates of major adverse cardiovascular and cerebrovascular events (MACCEs; all‐cause mortality, myocardial infarction, repeat revascularization, or stroke) were compared across patient characteristics over time with the Cox proportional hazards and Kaplan–Meier's analyses.

Results

During follow‐up of 5.4 ± 4.5 years, 91 (58%) patients had MACCE. On Kaplan–Meier's analysis of angiographic characteristics, MACCE was more frequent in patients with at least moderate target vessel calcification (P = 0.023), ostial stenosis (P = 0.049), target vessel diameter ≥ 3.0 mm (P = 0.018), a SYNTAX score ≥ the median of 11 (P = 0.014), or bare metal stenting (BMS)/balloon angioplasty (BA) compared to drug‐eluting stenting (DES) (P = 0.006). Cardiac death was more frequent in patients with SYNTAX score ≥ 11 (P = 0.028) or BMS (P = 0.043). After multivariable adjustment for both angiographic and clinical characteristics, independent predictors of MACCE were BMS placement (P = 0.013), chronic kidney disease ≥ stage 3 (P = 0.019), New York Heart Association (NYHA) heart failure class ≥3 (P = 0.034), and SYNTAX score ≥ 11 (P = 0.041).

Conclusions

In patients previously exposed to XRT treated with PCI, independent angiographic predictors of MACCE include SYNTAX score ≥ 11 and BMS placement, suggestive that DES should be preferred in this population.
Sutureless repair of spontaneous coronary dissection with free wall rupture and cardiac tamponade
Authors: Gannon Michael P. , Graver L. Michael , Singh Avneet
Published: January 2019

Left ventricular free wall rupture is a feared complication of acute myocardial infarction typically presenting with cardiogenic shock. We present a case of spontaneous coronary artery dissection with free wall rupture and cardiac tamponade in an uncommon demographic. Friable myocardial tissue frequently precludes suture technique making biological glue repair a suitable option.
β‐MnO2/Metal–Organic Framework Derived Nanoporous ZnMn2O4 Nanorods as Lithium‐Ion Battery Anodes with Superior Lithium‐Storage Performance
Authors: Pang Fang , Hou Shuang , Wang Pu , Liu Miao , Luo Yizhen , Zhao Lingzhi
Published: January 2019

Nanoporous ZnMn2O4 nanorods have been successfully synthesized by calcining β‐MnO2/ZIF‐8 precursors (ZIF‐8 is a type of metal–organic framework). If measured as an anode material for lithium‐ion batteries, the ZnMn2O4 nanorods exhibit an initial discharge capacity of 1792 mA h g−1 at 200 mA g−1, and an excellent reversible capacity of 1399.8 mA h g−1 after 150 cycles (78.1 % retention of the initial discharge capacity). Even at 1000 mA g−1, the reversible capacity is still as high as 998.7 mA h g−1 after 300 cycles. The remarkable lithium‐storage performance is attributed to the one‐dimensional nanoporous structure. The nanoporous architecture not only allows more lithium ions to be stored, which provides additional interfacial lithium‐storage capacity, but also buffers the volume changes, to a certain degree, during the Li+ insertion/extraction process. The results demonstrate that nanoporous ZnMn2O4 nanorods with superior lithium‐storage performance have the potential to be candidates for commercial anode materials in lithium‐ion batteries.
One‐Step Fabrication of Bio‐Compatible Coordination Complex Film on Diverse Substrates for Ternary Flexible Memory
Authors: Sun Wu‐Ji , Zhao Yong‐Yan , Zhou Jin , Cheng Xue‐Feng , He Jing‐Hui , Lu Jian‐Mei
Published: January 2019

Recently, resistance random access memories (RRAMs) have been studied extensively, because the demand for information storage is increasing. However, it remains challenging to obtain a flexible device because the active materials involved need to be nontoxic, nonpolluting, distortion‐tolerable, and biodegradable as well adhesive to diverse flexible substrates. In this paper, tannic acid (TA) and an iron ion (FeIII) coordination complex were employed as the active layer in a sandwich‐like (Al/active layer/substrate) device to achieve memory performance. A nontoxic, biocompatible TA‐FeIII coordination complex was synthesized by a one‐step self‐assembly solution method. The retention time of the TA‐FeIII memory performance was up to 15 000 s, the yield up to 53 %. Furthermore, the TA‐FeIII coordination complex can form a high‐quality film and shows stable ternary memory behavior on various flexible substrates, such as polyethylene terephthalate (PET), polyimide (PI), printer paper, and leaf. The device can be degraded by immersing it in vinegar solution. Our work will broaden the application of organic coordination complexes in flexible memory devices with diverse substrates.
Probing the Proton‐Coupled Electron‐Transfer (PCET) Reactivity of a Cross‐Conjugated Cruciform Chromophore by Redox‐State‐Dependent Fluorescence
Authors: Wagner Conrad , Hübner Olaf , Kaifer Elisabeth , Himmel Hans‐Jörg
Published: January 2019

Proton‐coupled electron transfer (PCET) reactions are of great importance in synthetic chemistry and in biology, but the acquisition of kinetic information for these reactions is often difficult. Herein, we report the synthesis of a new PCET reagent, showing redox‐state dependent fluorescence, by merging the concept of cross‐conjugated cruciform chromophores with the strategy of imposing redox activity and Brønsted basicity to aromatic compounds by substitution with guanidino groups. The compound is isolated and characterized in all stable states—reduced, twofold and fourfold protonated and twofold oxidized—and then applied in PCET reactions by using its redox‐state dependent fluorescence signal for kinetic measurements.
Evaluation of medial division of the medial geniculate (MGM) and posterior intralaminar nucleus (PIN) inputs to the rat auditory cortex, amygdala, and striatum
Authors: Smith Philip H. , Uhlrich Daniel J. , Manning Karen A.
Published: January 2019

The medial division of the medial geniculate (MGM) and the posterior intralaminar nucleus (PIN) are association nuclei of the auditory thalamus. We made tracer injections in these nuclei to evaluate/compare their presynaptic terminal and postsynaptic target features in auditory cortex, amygdala and striatum, at the light and electron microscopic levels. Cortical labeling was concentrated in Layer 1 but in other layers distribution was location‐dependent. In cortical areas designated dorsal, primary and ventral (AuD, Au1, AuV) terminals deep to Layer 1 were concentrated in infragranular layers and sparser in the supragranular and middle layers. In ectorhinal cortex (Ect), distributions below Layer 1 changed with concentrations in supragranular and middle layers. In temporal association cortex (TeA) terminal distributions below Layer 1 was intermediate between AuV/1/D and Ect. In amygdala and striatum, terminal concentrations were higher in striatum but not as dense as in cortical Layer 1. Ultrastructurally, presynaptic terminal size was similar in amygdala, striatum or cortex and in all cortical layers. Postsynaptically MGM/PIN terminals everywhere synapsed on spines or small distal dendrites but as a population the postsynaptic structures in cortex were larger than those in the striatum. In addition, primary cortical targets of terminals were larger in primary cortex than in area Ect. Thus, although postsynaptic size may play some role in changes in synaptic influence between areas it appears that terminal size is not a variable used for that purpose. In auditory cortex, cortical subdivision‐dependent changes in the terminal distribution between cortical layers may also play a role.