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Integrated circuit-based electrochemical sensor for spatially resolved detection of redox-active metabolites in biofilms
The direct detection of metabolites secreted by cells can indicate how cellular dynamics affects population development. Here, the authors present an integrated circuit-based method for electrochemical imaging of redox-active signalling molecules with spatial resolution within bacterial colonies.
- Daniel L. Bellin
- , Hassan Sakhtah
- & Kenneth L. Shepard
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Toward atomically-precise synthesis of supported bimetallic nanoparticles using atomic layer deposition
Synthesis of supported bimetallic nanoparticles often results in mixtures containing one or two metals. Here, the authors report a highly controlled method where one metal particle is initially formed on a support and the second metal is then grown exclusively on this metal surface.
- Junling Lu
- , Ke-Bin Low
- & Jeffrey W. Elam
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Solar-induced direct biomass-to-electricity hybrid fuel cell using polyoxometalates as photocatalyst and charge carrier
The direct conversion of biomass to electricity is an important process. Here, the authors use polyoxometallates as both photocatalyst and charge carrier to generate electricity in a solar-powered hybrid fuel cell that can consume natural biomass, such as cellulose or wood powders, at low temperature.
- Wei Liu
- , Wei Mu
- & Yulin Deng
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Dynamic urea bond for the design of reversible and self-healing polymers
The design of dynamic covalent bonds is crucial to self-healing polymer materials, but the reaction normally occurs in the presence of heat or/and catalysts. Ying et al.report a catalyst-free design of dynamic urea bonds that are capable of autonomous repairing at low temperature.
- Hanze Ying
- , Yanfeng Zhang
- & Jianjun Cheng
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Revealing lithium–silicide phase transformations in nano-structured silicon-based lithium ion batteries via in situ NMR spectroscopy
Understanding structural transformations of electrodes during cycling is of significance in batteries. Here Ogata et al. develop an approach for probing (de)lithiation processes in nano-silicon by in situNMR spectroscopy, which reveals structural and kinetic insights into the lithium–silicide phase transformations.
- K. Ogata
- , E. Salager
- & C.P. Grey
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A selective and efficient electrocatalyst for carbon dioxide reduction
Electrochemical reduction of carbon dioxide to more useful products is an industrially important process. Here, the authors report a nanoporous silver catalyst that efficiently and selectively reduces carbon dioxide due to its high surface area and intrinsically high activity.
- Qi Lu
- , Jonathan Rosen
- & Feng Jiao
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Photobiocatalytic chemistry of oxidoreductases using water as the electron donor
Enzymes have been considered as biocatalysts for organic chemistry, however their broad application has been somewhat hampered by the requirement for reducing cofactors. Here, the authors demonstrate that, in the presence of titania photocatalysts, water can be used as the sacrificial electron donor.
- Maria Mifsud
- , Serena Gargiulo
- & Avelino Corma
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Hydrochromic molecular switches for water-jet rewritable paper
Office printing is popular around the world, but suffers from the relatively high cost of ink and excessive paper waste. Here the authors demonstrate an eco-friendly dye-impregnated rewritable paper that can be printed using water and erased by heating, thereby allowing simple, repeated recycling.
- Lan Sheng
- , Minjie Li
- & Sean Xiao-An Zhang
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| Open AccessDehydration and crystallization of amorphous calcium carbonate in solution and in air
The crystallization of amorphous calcium carbonate is a widely studied process. Here, the authors probe the mechanism and show that transformation to calcite is preceded by dehydration, even in solution, and that loss of the final water fraction triggers crystallization.
- Johannes Ihli
- , Wai Ching Wong
- & Fiona C. Meldrum
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Polystyrene sulphonic acid resins with enhanced acid strength via macromolecular self-assembly within confined nanospace
Solid acid catalysts allow easy separation and reduction in waste not easily achievable with mineral acids. Here the authors report polystyrene sulphonic acid resins whose acid strength and catalytic performance can be tuned by changing their morphology within a confined nanospace.
- Xiaomin Zhang
- , Yaopeng Zhao
- & Qihua Yang
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Interaction of bipolaron with the H2O/O2 redox couple causes current hysteresis in organic thin-film transistors
Current hysteresis restricts the applications of organic thin-film transistors, and a mechanistic understanding is lacking despite extensive studies on it. Qu et al.demonstrate experimentally that current hysteresis is caused by an interaction between bipolaron and the water/oxygen redox couple.
- Minni Qu
- , Hui Li
- & Zhi-Jun Qiu
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| Open AccessComplex self-assembly of pyrimido[4,5-d]pyrimidine nucleoside supramolecular structures
Supramolecular self-assembly is a fundamentally important process in fields ranging from structural biology to materials chemistry. Here, the authors report the supramolecular assembly of complex nanostructures from simple nucleosides, and probe the formation process using various in situtechniques.
- Hang Zhao
- , Xiurong Guo
- & Qianming Chen
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Direct chemical conversion of graphene to boron- and nitrogen- and carbon-containing atomic layers
There is interest in hexagonal boron nitride and hexagonal boron carbonitride in electronics applications, but synthesizing them with high quality is challenging. Here, chemical vapour deposition graphene was chemically converted to hexagonal boron nitride and hexagonal boron carbonitride with both high on-off ratios and mobilities.
- Yongji Gong
- , Gang Shi
- & Pulickel M. Ajayan
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The isotopic effects of deuteration on optoelectronic properties of conducting polymers
Isotopic substitution alters the optoelectronic properties of conducting polymers, but a microscopic understanding is still missing. Shao et al.address this effect using a series of polymer isotopes that are synthesized with deuterium atoms substituted either on their backbone or side chains.
- Ming Shao
- , Jong Keum
- & Kai Xiao
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A nanocomposite superstructure of metal oxides with effective charge transfer interfaces
Mesocrystals are periodic arrangements of nanoparticles that allow for a tuning of the superstructure properties via its constituents. Here Bian et al. combine the properties of different nanocrystalline materials and fabricate a superstructure of two metal oxides with n- and p-type polarity.
- Zhenfeng Bian
- , Takashi Tachikawa
- & Tetsuro Majima
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A high-energy-density sugar biobattery based on a synthetic enzymatic pathway
Incomplete oxidation of fuels is a common problem in enzymatic fuel cells and it leads to low energy densities. Zhu et al. report the complete oxidation of sugar in an enzymatic fuel cell through a synthetic enzymatic pathway, which exhibits higher energy densities than lithium-ion batteries.
- Zhiguang Zhu
- , Tsz Kin Tam
- & Y. -H. Percival Zhang
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Self-assembled tunable networks of sticky colloidal particles
A wide diversity of surfaces patterned with microfibres is highly desirable for various applications as electrode materials. Demortière et al.develop a facile approach of producing polymer microfibres with controlled architectures via dynamic self-assembly under an alternating electric field.
- Arnaud Demortière
- , Alexey Snezhko
- & Igor S. Aranson
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Graphene etching on SiC grains as a path to interstellar polycyclic aromatic hydrocarbons formation
Although polycyclic aromatic hydrocarbons have been observed in interstellar space, their formation mechanism is still unclear. Here, Merino et al.present a proof-of-concept study that these molecules can form in a top-down route on a graphitized surface of silicon-carbide stardust.
- P. Merino
- , M. Švec
- & J.A. Martin-Gago
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Electrofluorochromism in π-conjugated ionic liquid crystals
The ability to easily modulate a material’s photoluminescent properties in response to stimuli is difficult to achieve in liquid crystals. Here the authors report ionic liquid crystals exhibiting high fluorescent quantum yields with redox-dependent photoluminescence.
- Amerigo Beneduci
- , Sante Cospito
- & Giuseppe Chidichimo
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Stereospecific ring expansion from orthocyclophanes with central chirality to metacyclophanes with planar chirality
Functionalization of carbon–carbon and unactivated carbon–hydrogen bonds is a highly desirable method to generate complex chemical structures with a minimum amount of waste. Here the authors use light and a metal catalyst to generate cyclophanes from simple starting materials.
- Naoki Ishida
- , Shota Sawano
- & Masahiro Murakami
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Diversity-oriented synthesis as a tool for identifying new modulators of mitosis
Diversity-oriented synthesis is a useful tool to synthesize libraries of structurally complex molecules. Here, the authors show the utility of this method by ultimately identifying a compound causing mitotic arrest and cancer cell death.
- Brett M. Ibbeson
- , Luca Laraia
- & David R. Spring
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Identification of a low-spin acylperoxoiron(III) intermediate in bio-inspired non-heme iron-catalysed oxidations
Hydrocarbon oxidations using non-heme iron catalysts together with hydrogen peroxide and acetic acid are synthetically useful. Here the authors characterize a low-spin acylperoxoiron(III) species that undergoes rate determining decay to an unobserved oxoiron(V) oxidant, elucidating catalyst activity.
- Williamson N. Oloo
- , Katlyn K. Meier
- & Lawrence Que
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Manipulating surface reactions in lithium–sulphur batteries using hybrid anode structures
Operation of lithium–sulphur batteries suffers from uncontrolled lithium polysulphide formation and corrosion at the anode. Huang et al.design an integrated anode structure composed of electrically connected graphite and lithium metal, which alleviates the problems and leads to high battery performance.
- Cheng Huang
- , Jie Xiao
- & Jun Liu
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| Open AccessA Diels–Alder super diene breaking benzene into C2H2 and C4H4 units
The stability of the benzene molecule reduces its tendency to react in ways that perturb the aromaticity—for example, in Diels–Alder reactions. Here the authors report a diene capable of not only inducing benzene to react under mild conditions but also of breaking apart the ring system itself.
- Yusuke Inagaki
- , Masaaki Nakamoto
- & Akira Sekiguchi
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Hydrogen evolution from a copper(I) oxide photocathode coated with an amorphous molybdenum sulphide catalyst
Photoelectrochemical water splitting may be used to produce hydrogen using abundant solar energy. Here, the authors fabricate layered films of amorphous molybdenum sulphide on copper(I) oxide and demonstrate the catalytic activity and enhanced stability of these devices made from earth-abundant materials.
- Carlos G. Morales-Guio
- , S. David Tilley
- & Xile Hu
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Highly stable organic polymer field-effect transistor sensor for selective detection in the marine environment
Field-effect transistors are widely used for environmental sensing and monitoring applications. Here, the authors present an organic field-effect transistor with the inherent advantages of low-cost and scalable fabrication, and which is sufficiently stable to be deployed in marine environments.
- Oren Knopfmacher
- , Mallory L. Hammock
- & Zhenan Bao
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Full open-framework batteries for stationary energy storage
Battery technologies are promising for grid-scale applications, but existing batteries in general operate at low rates, have limited cycle life and are expensive. Pasta et al. develop a grid-scale battery based on Prussian Blue electrodes, which shows potential in overcoming these problems.
- Mauro Pasta
- , Colin D. Wessells
- & Yi Cui
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High yield exfoliation of two-dimensional chalcogenides using sodium naphthalenide
Molybdenum disulphide may be prepared by lithiation and exfoliation; however the process requires a long lithiation and produces low yields. Here, the authors show that metal naphthalenides may be used for the intercalation, and that the resulting products are of high quality and may be inkjet-printed.
- Jian Zheng
- , Han Zhang
- & Kian Ping Loh
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A strategic approach to recharging lithium-sulphur batteries for long cycle life
Capacity degradation over extended cycles is a major problem in lithium-sulphur batteries. Here, Su et al.report a charge operation control strategy to inhibit dissolution of polysulphides leading to enhanced capacity retention over multiple cycles.
- Yu-Sheng Su
- , Yongzhu Fu
- & Arumugam Manthiram
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Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode
Understanding the oxygen reduction reaction at fuel cell cathodes requires information on adsorbed oxygenated species. Sanchez Casalongue et al. report in situidentification of oxygenated intermediates at cathodes and establish a correlation between the cathode potential and the surface speciation.
- Hernan Sanchez Casalongue
- , Sarp Kaya
- & Hirohito Ogasawara
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A general approach to crystalline and monomodal pore size mesoporous materials
Mesoporous oxides are important materials with a range of tunable structural properties. Here, the authors report a general, inverse micelle-based method to produce crystalline mesoporous materials with monomodal pore sizes from a range of elements.
- Altug S. Poyraz
- , Chung-Hao Kuo
- & Steven L. Suib
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A very stable complex of a modified marine cyclopeptide with chloroform
Typically dispersion forces are weak interactions, and host–guest chemistry is dominated by more powerful events such as hydrogen bonding. Here, the authors show extremely high binding between a modified marine peptide and chloroform, driven by dispersion interactions with the chlorine atoms.
- Gebhard Haberhauer
- , Áron Pintér
- & Sascha Woitschetzki
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Supramolecular high-aspect ratio assemblies with strong antifungal activity
Efficient and pathogen-specific antifungal agents are required to mitigate drug resistance problems. Here the authors present a series of cationic small molecules, which are easy to isolate and characterize, and which can self-assemble to give polymer-like antifungal activity and specificity.
- Kazuki Fukushima
- , Shaoqiong Liu
- & James L. Hedrick
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Adaptive strong-field control of chemical dynamics guided by three-dimensional momentum imaging
Shaped femtosecond laser pulses can control the dynamics of chemical reactions but understanding the underlying control process is difficult. Towards this end, Wells et al.show that feedback from rapid inversion of velocity map images of photofragment ions can target specific adaptive control outcomes.
- E. Wells
- , C.E. Rallis
- & I. Ben-Itzhak
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| Open AccessStructural analysis and mapping of individual protein complexes by infrared nanospectroscopy
Mid-infrared spectroscopy offers important chemical and structural information about biological samples but diffraction prevents nanoscale studies. Amenabar et al.demonstrate Fourier transform infrared nanospectroscopy for analysing the secondary structure of protein complexes with 30 nm spatial resolution.
- Iban Amenabar
- , Simon Poly
- & Rainer Hillenbrand
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Renewable and metal-free carbon nanofibre catalysts for carbon dioxide reduction
The efficient catalysis of the electrochemical reduction of carbon dioxide is an important industrial process, usually performed by noble metal catalysts. Here the authors report a metal-free carbon nanofibre-based catalyst operating with a negligible overpotential, high current density and long-term stability.
- Bijandra Kumar
- , Mohammad Asadi
- & Amin Salehi-Khojin
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Pits confined in ultrathin cerium(IV) oxide for studying catalytic centers in carbon monoxide oxidation
Catalytic carbon monoxide oxidation is an industrially important process. Here, the authors show that ultrathin cerium(IV) oxide with surface confined pits provides an ideal platform for investigating and optimizing the role of local atomic structure on carbon monoxide adsorption and oxygen activation.
- Yongfu Sun
- , Qinghua Liu
- & Yi Xie
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Downsizing a human inflammatory protein to a small molecule with equal potency and functionality
Replicating the functionality of bioactive proteins using rationally designed small molecule mimics is both economically valuable and synthetically challenging. Here the authors develop a mimic of the inflammatory protein C3a with equal biological potency but enhanced stability and bioavailability.
- Robert C. Reid
- , Mei-Kwan Yau
- & David P. Fairlie
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A light-induced spin crossover actuated single-chain magnet
Spin-crossover complexes and single-chain magnets exhibit magnetic bistability and may be used in information storage applications. Here, the authors present a one-dimensional spin-crossover complex wherein the single-chain magnet behaviour is actuated by light-induced excited spin-state trapping.
- Tao Liu
- , Hui Zheng
- & Chunying Duan
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Giant infrared absorption bands of electrons and holes in conjugated molecules
The absorption of mid-infrared light by organic molecules is used for diagnostics and sensing purposes. Here Zamadar et al.find that mid-infrared molar absorption coefficients of conjugated molecules bearing charges, owing to polaron vibrations, are often more than one hundred times larger than those of comparable neutral molecules.
- Matibur Zamadar
- , Sadayuki Asaoka
- & John R. Miller
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The N-terminal domains of spider silk proteins assemble ultrafast and protected from charge screening
Web spiders synthesize silk fibres at high speed, assisted by a self-associating protein domain, but the molecular details are not yet understood. Here, the authors use an engineered fluorescence probe in combination with mutagenesis to reveal the underlying kinetics and side chain contributions.
- Simone Schwarze
- , Fabian U. Zwettler
- & Hannes Neuweiler
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| Open AccessConjugated organic framework with three-dimensionally ordered stable structure and delocalized π clouds
Covalent organic frameworks can utilize π-stacking interactions for the formation of ordered, layered frameworks. Here, the authors report an ordered framework with tailored π-interactions resulting in periodic ordering in three dimensions, which leads to enhanced stability and electronic properties.
- Jia Guo
- , Yanhong Xu
- & Donglin Jiang
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| Open AccessAtomically precise edge chlorination of nanographenes and its application in graphene nanoribbons
Chemical functionalization of graphene is a useful method for modulating its properties, although this is limited by a lack of control and resulting in poorly defined structures. Here the authors report the atomically precise chlorination of nanographenes and apply the methods to graphene nanoribbons.
- Yuan-Zhi Tan
- , Bo Yang
- & Klaus Müllen
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Article
| Open AccessEfficient and tunable white-light emission of metal–organic frameworks by iridium-complex encapsulation
Although many metal–organic frameworks are luminescent, few are capable of white-light emission. Here, the authors incorporate a yellow-emitting guest molecule into the cavities of a blue-emitting metal–organic framework, and tune the composition to emit white light with relatively high quantum yield.
- Chun-Yi Sun
- , Xin-Long Wang
- & Jing Li
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Probing single- to multi-cell level charge transport in Geobacter sulfurreducens DL-1
Microbial fuels cells present a way of generating electricity using the natural metabolism of microorganisms. Here the authors carry out single-cell current measurements ofGeobacter sulfurreducensDL-1 to determine the upper limits of microbial fuel cell performance.
- Xiaocheng Jiang
- , Jinsong Hu
- & Justin C. Biffinger
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Surface tension and contact with soft elastic solids
Solid contacts on a microscopic level are widely described by a classical contact mechanics theory. Here Styleet al.show that this theory breaks down when a small particle adheres to a soft surface where a fluid-like behaviour is observed because of the predominant role played by surface tension.
- Robert W. Style
- , Callen Hyland
- & Eric R. Dufresne
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Functionalization of the living diatom Thalassiosira weissflogii with thiol moieties
Biomineralization processes have inspired the design of synthetic silica structures in vitro. Here, the authors use a living diatom to fabricate organo-silica constructs and are able to incorporate thiol moieties into the diatom frustule without the loss of nano-scale architectural features.
- Yvonne Lang
- , Francisco del Monte
- & Abhay Pandit
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Nanorings and rods interconnected by self-assembly mimicking an artificial network of neurons
Molecularly interconnected networks are the building blocks for molecular circuits in nanoelectronic devices, but a mass production with tunable properties is difficult. Escárcega–Bobadilla et al.develop an approach to form interconnected self-assembled nano-rings, which resemble a network of neurons.
- Martha V. Escárcega-Bobadilla
- , Gustavo A. Zelada-Guillén
- & Arjan W. Kleij
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| Open AccessConfinement of pyridinium hemicyanine dye within an anionic metal-organic framework for two-photon-pumped lasing
Two-photon-pumped dye lasers are useful for applications such as biological imaging; however, loss processes reduce their efficiency. Here, metal-organic frameworks, into which the laser dye is incorporated, demonstrate enhanced laser operation because losses such as dye aggregation-caused quenching are reduced.
- Jiancan Yu
- , Yuanjing Cui
- & Guodong Qian
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