bluuebunny/crossref_metadata_2025_split huggingface dataset:
Capacitive Enhancement Mechanisms and Design Principles of High‐Performance Graphene Oxide‐Based All‐Solid‐State Supercapacitors
Authors: Gao Yong , Wan Yiyang , Wei Bingqing , Xia Zhenhai 
Published: February 2018

AbstractGraphene oxide (GO)‐based all‐solid‐state supercapacitors (GO‐A3Ss) are superior over liquid electrolyte‐based supercapacitors and capable of being integrated on a single chip in various geometry shapes for the use of future smart wearable electronics field as a fast energy storage device, but their capacitance need to be improved. Here, a new approach has been developed for enhancing the capacitive capability of the supercapacitors through molecular dynamics simulations with the first‐principle input. A theoretical model of charge storage is developed to understand the unique capacitive enhancement mechanism and to predict the capacitance of the GO‐A3Ss, which agrees well with the experimental observations. A novel supercapacitor with GO and reduced graphene oxide (rGO) alternatively layered structures is designed based on the model, and its energy density is the highest among conventional supercapacitors using liquid electrolytes and all‐solid‐state supercapacitors using aerogels or hydrogels as the solid‐state electrolyte. Based on the predictions, two new types of high‐performance GO/rGO multilayered capacitors are proposed to meet different practical applications. The results of this work provide an approach for the design of high‐performance all‐solid‐state supercapacitors based on GO and rGO materials.
Confined Growth of ZIF‐8 Nanocrystals with Tunable Structural Colors
Authors: Chang Bingdong , Yang Yuanqing , Jansen Henri , Ding Fei , Mølhave Kristian , Sun Hongyu 
Published: February 2018

AbstractZeolitic imidazolate frameworks (ZIF‐8) have promising applications as sensors or catalysts due to their highly porous crystalline structures. While most of the previous studies are based on ZIF‐8 crystals either in isolated particles in aqueous environments or in a compact colloidal form, here a facile method is reported to achieve wafer‐based isolated ZIF‐8 nanocrystals to facilitate their integration in microsystems and as surface coatings for catalysis. The fabrication process includes the growth of compact zinc oxide film by atomic layer deposition that functions as the Zn source for the ZIF‐8 synthesis, and the dispersion of gold nanoparticles as inhibitors for the following crystallization transformation of ZIF‐8 crystals. By choosing the concentration of gold nanoparticles, the density of ZIF‐8 nanocrystals can be controlled and the sizes of individual ZIF‐8 crystals can be scaled down to ≈100 nm. A wide range of structural colors generated by the ZIF‐8 nanocrystals is also observed, which can be attributed to the size‐dependent resonant scattering as verified by finite‐difference time‐domain simulations and classical Mie theory. The scalable fabrication of wafer‐based ZIF‐8 nanocrystals empowered with tunable optical properties paves a new way to explore the promising applications in nanophotonics and bionanotechnology.
Optically Transparent Protective Coating for Plastics Using Dual Spray and Atmospheric Plasma Deposition
Authors: Ding Yichuan , Dong Siming , Han Jiahao , He Dongjing , Zhao Zhenlin , Dauskardt Reinhold H. 
Published: February 2018

AbstractThe successful processing of bilayer protective coatings on plastics using a combined spray and atmospheric plasma deposition method is shown. The base layer is a spray deposited coating with high adhesion using (3‐glycidyloxypropyl) trimethoxysilane and tetrapropyl zirconate (TPOZ) precursors. The top dense layer is deposited by atmospheric plasma deposition with a tetraethyl orthosilicate precursor. The coating deposition rate, chemical composition, elastic modulus, hardness, and adhesion to poly(methyl methacrylate) (PMMA) substrates are investigated. The adhesion to the polymer substrate is found to decrease with increasing TPOZ content in the precursor solution, while the elastic modulus and hardness of the base layer increase. A silane surface pretreatment of the PMMA substrate is shown to significantly increase the coating adhesion. The adhesion of the optimized coating is so high that it forces the debond interface change from adhesive failure at the coating/PMMA interface to cohesive failure within the PMMA substrate. The combined bilayer structure exhibits a >90% transparency in the visible wavelengths, eightfold increase in adhesion energy and fourfold increase in Young's modulus compared to commercial sol–gel polysiloxane coatings. The approach provides a strategy for an unprecedented combination of adhesion and mechanical properties.
A Combined Experimental and Computational Study of Gas Sensing by Cu3SnS4 Nanoparticulate Film: High Selectivity, Stability, and Reversibility for Room Temperature H2S Sensing
Authors: M Thripuranthaka , Sharma Neha , Das Tilak , Varhade Swapnil , Badadhe Satish S. , Thotiyl Musthafa Ottakam , Kabir Mukul , Ogale Satishchandra 
Published: February 2018

AbstractSeveral binary sulfides are used for sensing of gases such as NH3, NO2, and H2, but not for H2S, especially at room temperature, because of the relative inactivity of metal sulfide surface bonds for this gas. The situation can be entirely different in the ternary case, however, due to the possible synergy of interactions involving dual cation surface chemistry. This is borne out by the present work wherein the Cu3SnS4 material, the Cu‐rich ternary sulfide used for the first time in the gas sensing context, not only senses H2S at room temperature but also remarkably does so with high selectivity and stability. Thus, a combined experimental and computer modeling study on the use of nanocrystalline orthorhombic Cu3SnS4 phase is reported for H2S sensing. The material shows sensitivity for a wide range of H2S concentrations (from 10 to 2000 ppm). The performance of the sensing device fabricated on Kapton substrate remains intact even after several days and multiple bending cycles. Importantly, these experimental findings are consistent with the results of density functional theory calculations for binding energies for different gases, namely, H2S, NO2, NH3, and CO, on Cu3SnS4 surface.
Multiple Synergistic Toughening Graphene Nanocomposites through Cadmium Ions and Cellulose Nanocrystals
Authors: Gao Yuan , Xu Hanjie , Cheng Qunfeng 
Published: February 2018

AbstractRobust and functional graphene‐based nanocomposites are attractive in flexible electric devices. Herein, a strong and conductive bioinspired graphene‐based nanocomposite is demonstrated via multiple synergistic toughening effect from graphene oxide (GO), cellulose nanocrystals (CNC), and cadmium ion (Cd2+). The multiple synergistic toughening effect can be realized from building blocks of 2D GO nanosheets and 1D CNC, interface interactions of hydrogen bonding from CNC and ionic bonding from Cd2+, resulting in integrated graphene‐based nanocomposites with high strength, and toughness as well as electrical conductivity. This ternary synthetic graphene‐based nanocomposite possessing outstanding physical properties provides a clear vision in the application of flexible electric devices. Furthermore, this bioinspired strategy could also serve as a guideline for the development of high‐performance graphene‐based nanocomposites in the future.
Graphene Tunable Plasmon–Phonon Coupling in Mid‐IR Complementary Metamaterial
Authors: Chen Nan , Hasan Dihan , Ho Chong Pei , Lee Chengkuo 
Published: February 2018

AbstractMetamaterial‐based plasmonics has become an overwhelming research field due to its enormous potential and versatility in molecular sensing, imaging, and nonlinear optics. This work presents a new tunable plasmonic platform on which the metamaterial resonance is coupled with infrared vibrational bond in the presence of graphene electrostatic modulation. The maximum electric field enhancement factor induced by mode coupling is 14 and the quality factor (Q‐factor) of phonon mode is increased approximately by fourfold. The graphene electrostatic modulation based on the parallel‐plate capacitor configuration enables a wavelength shift of 1.57 nm V−1, resonance intensity and Q‐factor modulation depth of 103.34% and 70%, respectively. Metamaterial based plasmon polariton perfectly matched with phonon mode yields the highest Q‐factor of 40. However, this perfectly matched resonance appears to be prohibitively “switched off” in the electrostatic tuning, which is reported for the first time. Mode splitting investigation reveals the largest coupling strength of 8.1 meV (1.96 THz) that results in the insensitivity to the perturbation caused by graphene modulation. Finally, an averaged sensitivity of 1.677 µm RIU−1 and a tunable figure of merit are reported, depicting the versatility of this platform for multiplexed sensing applications in various conditions.
Flexible and Transparent Organic Phototransistors on Biodegradable Cellulose Nanofibrillated Fiber Substrates
Authors: Park Junsu , Seo Jung‐Hun , Yeom Seung‐Won , Yao Chunhua , Yang Vina W. , Cai Zhiyong , Jhon Young Min , Ju Byeong‐Kwon 
Published: February 2018

AbstractThis work demonstrates flexible, transparent phototransistors that can detect visible light with nontoxic organic active materials on biodegradable substrates toward environment‐friendly electronics. The molybdenum trioxide (MoO3)‐buffered indium zinc oxide as high‐performance hole injector and transparent electrodes is applied for the first time to organic phototransistors on cellulose nanofibrillated fiber substrates to achieve more than 70% of transmittance in the visible range (400–750 nm) while showing high conductivity under multiple bendings. Excellent electrical switching characteristics are obtained from transistors using a pentacene active layer with a saturation mobility value of 1.40 cm2 V−1 s−1. The phototransistors, which can detect visible light and perform in two operation modes, exhibit a maximum responsivity of 54.8 A W−1 and a photosensitivity of 24.4 under white light illumination at an intensity of 0.12 mW cm−2. Moreover, the devices show a stable operation during mechanical bending tests with radii ranging from 100 to 5 mm and cyclic bending tests of up to 2000 cycles at a fixed radius of 5 mm. The results suggest that these flexible phototransistors with properties of transparency and biodegradability have considerable potential for use in low‐cost and eco‐friendly disposable sensor systems.
Water‐Soluble Sulfo‐Fluorous Affinity (SOFA) Tag‐Assisted Enzymatic Synthesis of Oligosaccharides
Authors: Hou Kai‐Ling , Chiang Pei‐Yun , Lin Chien‐Hung , Li Ben‐Yuan , Chien Wei‐Ting , Huang Yu‐Ting , Yu Ching‐Ching , Lin Chun‐Cheng 
Published: February 2018

AbstractHerein, we report a bifunctional sulfo‐fluorous affinity (SOFA) tag‐assisted enzymatic synthesis and purification strategy for the facile preparation of bioactive glycans using fluorous solid‐phase extraction (FSPE). The incorporation of a sulfonate moiety onto the heavy fluorous tag significantly increases its water solubility, which allows the broad use of the inherently hydrophobic fluorous tag in aqueous buffers. In addition, the SOFA tag contains a photocleavable linker, enabling the easy release of amino‐functionalized oligosaccharides by UV irradiation. The SOFA tag was used in the synthesis of both negatively charged and neutral glycans to demonstrate its broad utility as an acceptor toward six different glycosyltransferases, significantly improving the feasibility of the preparation of complex glycans using FSPE. All the reactions were performed in an aqueous buffer, a minimum amount of methanol was used to purify the products, and the SOFA tag was easily recovered after photo‐irradiation. Thus, the entire synthetic process is environmentally benign.magnified image
H2S Sensing and Splitting on Atom‐Functionalized Carbon Nanotubes: A Theoretical Study
Authors: Liao Ting , Kou Liangzhi , Du Aijun , Chen Lingna , Cao Can , Sun Ziqi 
Published: February 2018

AbstractStrategies that can manipulate the electronic and chemical properties of carbon nanotubes (CNT) to meet a target application are challenging, and the introduction of atom functionalization is one path toward this goal. Herein, two types of Fe‐atom‐functionalized CNTs, Fe‐adsorbed CNTs (Fe@CNT) and Fe‐welded CNTs, the latter is a new hybrid material combining the merits of both carbon nanotubes and functional welding metals, are examined in terms of their sensitivity toward detecting hydrogen sulfide (H2S) and their selective activity toward chemically converting H2S into valuable fuel resources, for example, elemental sulfur and H2, in the framework of density functional theory (DFT) and the non‐equilibrium Green's function (NEGF) method. The catalytic center formed by the metal and the neighboring under‐coordinated carbon atoms in the Fe‐welded CNT provide an easy pathway for the splitting reaction of H2S molecules and sheds light on the design of efficient atom‐functionalized nanomaterials for other challenging chemical reactions.
Analytical Modeling of Organic–Inorganic CH3NH3PbI3 Perovskite Resistive Switching and its Application for Neuromorphic Recognition
Authors: Ren Yanyun , Milo Valerio , Wang Zhongqiang , Xu Haiyang , Ielmini Daniele , Zhao Xiaoning , Liu Yichun 
Published: February 2018

AbstractThis paper presents an analytical model of resistive switching in organic–inorganic CH3NH3PbI3 perovskite. It is interpreted that the resistive switching phenomenon is due to the formation/rupture of iodine vacancy‐based conductive filament (CF) propagating in both vertical and lateral directions. Set and reset processes are explained in the model by the evolution of the CF length and radius driven by electrical and thermal forces. The model‐based simulation results can describe the experimental results, providing an estimate of several switching parameters such as the activation energy of iodine vacancy migration and the CF diameter. Learning in a two‐transistor/one‐resistor synapse structure is demonstrated by simulations. Finally, the neuromorphic recognition of multiple patterns is demonstrated through a two‐layer neural network consisting of 5625 presynaptic neurons and four postsynaptic neurons.
Mutual Destruction of Deep Lung Tumor Tissues by Nanodrug‐Conjugated Stealth Mesenchymal Stem Cells
Authors: Kim Sang‐Woo , Lee Yeon Kyung , Hong Jeong Hee , Park Jun‐Young , Choi Young‐Ae , Lee Dong Un , Choi Jungil , Sym Sun Jin , Kim Sang‐Hyun , Khang Dongwoo 
Published: February 2018

AbstractLung cancer is a highly malignant tumor, and targeted delivery of anti‐cancer drugs to deep lung tumor tissue remains a challenge in drug design. Here, it is demonstrated that bone marrow mesenchymal stem cells armed with nanodrugs are highly targeted and mutually destructive with malignant lung cancer cells and successfully eradicate lung tumors tissues. Using this approach, the current clinical dose of anti‐cancer drugs for the treatment of malignant lung tumors can be decreased by more than 100‐fold without triggering immunotoxicity.
Sequentially Triggered Nanoparticles with Tumor Penetration and Intelligent Drug Release for Pancreatic Cancer Therapy
Authors: He Xi , Chen Xinli , Liu Lisha , Zhang Yu , Lu Yifei , Zhang Yujie , Chen Qinjun , Ruan Chunhui , Guo Qin , Li Chao , Sun Tao , Jiang Chen 
Published: February 2018

AbstractPancreatic ductal adenocarcinoma (PDAC) is the most aggressive malignancy with a five year survival rate of <5%. The aberrant expression of extracellular matrix (ECM) in the tumor stroma forms a compact physical barrier, which that leads to insufficient extravasation and penetration of nanosized therapies. To overcome the severe resistance of PDAC to conventional therapies, a sequentially triggered nanoparticle (aptamer/cell‐penetrating peptide‐camptothecin prodrug, i.e., Apt/CPP‐CPTD NPs) with tumor penetration and intelligent drug release profile is designed. An ECM component (tenescin‐C) targeting aptamer (GBI‐10) is modified onto stroma‐permeable cell‐penetrating peptide (CPP) for the in vivo CPP camouflage and PDAC‐homing. In PDAC stroma, tenascin‐C can detach GBI‐10 from CPP and exposed CPP can facilitate further PDAC penetration and tumor cell endocytosis. After being endocytosed into PDAC cells, intracellular high redox potential can further trigger controlled chemodrug release. Apt/CPP‐CPTD NPs show both deep penetration in vitro 3D PDAC spheroids and in vivo tumor sections. The relatively mild in vitro cytotoxicity and excellent in vivo antitumor efficacy proves the improved PDAC targeting drug delivery and decreased systemic toxicity. The design of ECM‐redox sequentially triggered stroma permeable NPs may provide a practical approach for deep penetration of PDAC and enhanced drug delivery efficacy.
Novel climates reverse carbon uptake of atmospherically dependent epiphytes: Climatic constraints on the iconic boreal forest lichen Evernia mesomorpha
Authors: Smith Robert J. , Nelson Peter R. , Jovan Sarah , Hanson Paul J. , McCune Bruce 
Published: February 2018

Premise of the StudyChanging climates are expected to affect the abundance and distribution of global vegetation, especially plants and lichens with an epiphytic lifestyle and direct exposure to atmospheric variation. The study of epiphytes could improve understanding of biological responses to climatic changes, but only if the conditions that elicit physiological performance changes are clearly defined.MethodsWe evaluated individual growth performance of the epiphytic lichen Evernia mesomorpha, an iconic boreal forest indicator species, in the first year of a decade‐long experiment featuring whole‐ecosystem warming and drying. Field experimental enclosures were located near the southern edge of the species’ range.Key ResultsMean annual biomass growth of Evernia significantly declined 6 percentage points for every +1°C of experimental warming after accounting for interactions with atmospheric drying. Mean annual biomass growth was 14% in ambient treatments, 2% in unheated control treatments, and −9% to −19% (decreases) in energy‐added treatments ranging from +2.25 to +9.00°C above ambient temperatures. Warming‐induced biomass losses among persistent individuals were suggestive evidence of an extinction debt that could precede further local mortality events.ConclusionsChanging patterns of warming and drying would decrease or reverse Evernia growth at its southern range margins, with potential consequences for the maintenance of local and regional populations. Negative carbon balances among persisting individuals could physiologically commit these epiphytes to local extinction. Our findings illuminate the processes underlying local extinctions of epiphytes and suggest broader consequences for range shrinkage if dispersal and recruitment rates cannot keep pace.
High‐Throughput Kinetic Analysis for Target‐Directed Covalent Ligand Discovery
Authors: Craven Gregory B. , Affron Dominic P. , Allen Charlotte E. , Matthies Stefan , Greener Joe G. , Morgan Rhodri M. L. , Tate Edward W. , Armstrong Alan , Mann David J. 
Published: February 2018

AbstractCysteine‐reactive small molecules are used as chemical probes of biological systems and as medicines. Identifying high‐quality covalent ligands requires comprehensive kinetic analysis to distinguish selective binders from pan‐reactive compounds. Quantitative irreversible tethering (qIT), a general method for screening cysteine‐reactive small molecules based upon the maximization of kinetic selectivity, is described. This method was applied prospectively to discover covalent fragments that target the clinically important cell cycle regulator Cdk2. Crystal structures of the inhibitor complexes validate the approach and guide further optimization. The power of this technique is highlighted by the identification of a Cdk2‐selective allosteric (type IV) kinase inhibitor whose novel mode‐of‐action could be exploited therapeutically.
Alkenylation of C(sp3)−H Bonds by Zincation/Copper‐Catalyzed Cross‐Coupling with Iodonium Salts
Authors: Liu Chuan , Wang Qiu 
Published: February 2018

Abstractα‐Vinylation of phosphonates, phosphine oxides, sulfones, sulfonamides, and sulfoxides has been achieved by selective C−H zincation and copper‐catalyzed C(sp3)−C(sp2) cross‐coupling reaction using vinylphenyliodonium salts. The vinylation transformation proceeds in high efficiency and stereospecificity under mild reaction conditions. This zincative cross‐coupling reaction represents a general alkenylation strategy, which is also applicable for α‐alkenylation of esters, amides, and nitriles in the synthesis of β,γ‐unsaturated carbonyl compounds.
Hydrophilie als bestimmender Faktor des Stealth‐Effekts von Polyphosphoester‐funktionalisierten Nanoträgern
Authors: Simon Johanna , Wolf Thomas , Klein Katja , Landfester Katharina , Wurm Frederik R. , Mailänder Volker 
Published: February 2018

AbstractDie Anbindung von Polymeren, besonders von Polyethylenglycol (PEG), ist eine effektive Methode, um die Plasma‐Halbwertszeit von Wirkstoffträgern zu verlängern. Dieser Effekt wird der allgemeinen Abnahme der Proteinadsorption auf hydrophilen Oberflächen zusammen mit der Adsorption spezifischer Proteine zugeschrieben, jedoch sind die molekularen Ursachen für den Erfolg von PEG und anderer hydrophiler Polymere weitgehend unbekannt. Um diesen Stealth‐Effekt der Polymerhülle besser kontrollieren zu können, wurden Polyphosphoester‐beschichtete Nanocarrier mit definiert hydrophilen Eigenschaften hergestellt. Dabei zeigte sich, dass der LogP‐Wert der Copolymere die Zusammensetzung der Proteinkorona sowie die Zellinteraktionen beeinflusst. Trotz signifikanter Änderung der hydrophilen Eigenschaften bleibt die Gesamtmenge der aus dem Blut adsorbierten Proteine auf den Nanocarriern gleich, während sich die Zusammensetzung der Proteinkorona verändert. Dies unterstreicht die Bedeutung der Proteinklassen in der Proteinkorona und deren Einfluss auf die zelluläre Aufnahme.
A Highly Active N‐Heterocyclic Carbene Manganese(I) Complex for Selective Electrocatalytic CO2 Reduction to CO
Authors: Franco Federico , Pinto Mara F. , Royo Beatriz , Lloret‐Fillol Julio 
Published: February 2018

AbstractWe report here the first purely organometallic fac‐[MnI(CO)3(bis‐MeNHC)Br] complex with unprecedented activity for the selective electrocatalytic reduction of CO2 to CO, exceeding 100 turnovers with excellent faradaic yields (ηCO≈95 %) in anhydrous CH3CN. Under the same conditions, a maximum turnover frequency (TOFmax) of 2100 s−1 was measured by cyclic voltammetry, which clearly exceeds the values reported for other manganese‐based catalysts. Moreover, the addition of water leads to the highest TOFmax value (ca. 320 000 s−1) ever reported for a manganese‐based catalyst. A MnI tetracarbonyl intermediate was detected under catalytic conditions for the first time.