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Spectroscopic observation of iodosylarene metalloporphyrin adducts and manganese(V)-oxo porphyrin species in a cytochrome P450 analogue
Metalloporphyrin compounds are studied as models of cytochrome P450, which is capable of catalysing oxidative reactions. Here, reaction conditions are varied to allow spectroscopic observation of oxidant-metalloporphyrin adducts and metal-oxo intermediates, which may elucidate reaction mechanisms.
- Mian Guo
- , Hang Dong
- & Aiwen Lei
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Orthogonal switching of a single supramolecular complex
Orthogonal switching has been achieved in supramolecular systems, in which different responses can be triggered on demand by different stimuli. Tian et al.report host–guest heteroternary complexes with both redox- and light-responsive guests in a single, supramolecular entity.
- Feng Tian
- , Dezhi Jiao
- & Oren A. Scherman
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Tracking lithium transport and electrochemical reactions in nanoparticles
Developing next generation batteries requires better understanding of the dynamics of electrochemical reactions in working electrodes. Using a transmission electron microscope, Wanget al. develop a means to track the real time flow of lithium atoms in electrodes during the discharge of a functioning electrochemical cell.
- Feng Wang
- , Hui-Chia Yu
- & Jason Graetz
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Article
| Open AccessDetermination of monolayer-protected gold nanoparticle ligand–shell morphology using NMR
Binary mixtures of molecules on the surface of nanoparticles can arrange randomly or into different domains to form Janus, patchy or striped particles. Liuet al.show that NMR can be used to determine the ligand-shell morphology of particles coated with aliphatic and aromatic ligands.
- Xiang Liu
- , Miao Yu
- & Francesco Stellacci
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A general method for the large-scale synthesis of uniform ultrathin metal sulphide nanocrystals
Ultrathin metal sulphides are attractive components for electronic and optical devices and are promising anode materials for lithium-ion batteries. Here, a universal, soft colloidal templating strategy is employed for the large-scale synthesis of uniform, ultrathin metal sulphide nanomaterials.
- Yaping Du
- , Zongyou Yin
- & Hua Zhang
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Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer
The practical performance of lithium sulphide batteries is much less than their predicted performance because redox products dissolve over time. Su and Manthiram show that microporous carbon membranes inserted between cathode and separator localize soluble polysulphide species and improve battery cycling characteristics.
- Yu-Sheng Su
- & Arumugam Manthiram
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One-piece micropumps from liquid crystalline core-shell particles
Liquid crystal elastomers can perform mechanical motion triggered by external stimuli, and are light weight, flexible materials that may be integrated into micromechanical systems. Here they are used to fabricate a one-piece temperature-responsive micropump viaa microfluidic double-emulsion process.
- Eva-Kristina Fleischmann
- , Hsin-Ling Liang
- & Rudolf Zentel
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High strain rate deformation of layered nanocomposites
Bullet-proof materials made of nanostructured composites outperform conventional materials, yet little is known of their nanoscale response to high-speed impact. Using laser-propelled microscopic projectiles, Lee et al.directly visualize this process in layered nanocomposites.
- Jae-Hwang Lee
- , David Veysset
- & Edwin L. Thomas
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Article
| Open AccessSimilarities between protein folding and granular jamming
Granular matter is rigid when jammed, and flows under external loads. Here temperature- and force-unfolding molecular dynamics stimulations are used to demonstrate that proteins display features of jamming, characterized by a force distribution peak on folding and a slowdown of stress relaxation.
- Prasanth P Jose
- & Ioan Andricioaei
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Electrografting of calix[4]arenediazonium salts to form versatile robust platforms for spatially controlled surface functionalization
The spontaneous adsorption of alkanethiols is widely utilized to fabricate functional surfaces but gives limited stability and regularity. Mattiuzziet al. report a method that uses preorganized platforms (rigid tetrapodant calix[4]arenes), which allows further surface functionalization and spatial control.
- Alice Mattiuzzi
- , Ivan Jabin
- & Corinne Lagrost
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Article
| Open AccessUltra-precise insertion of functional monomers in chain-growth polymerizations
Copolymers prepared by controlled radical chain-growth polymerizations usually contain ill-defined monomer sequences. Here, successive feeds of donor and acceptor comonomers are used to control the primary structure of the synthesized copolymers with very high accuracy.
- Mirela Zamfir
- & Jean-François Lutz
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Article
| Open AccessSn-Beta zeolites with borate salts catalyse the epimerization of carbohydrates via an intramolecular carbon shift
Epimerization of carbohydrates to rare sugars yields products that have potential applications as anti-viral drugs or chiral building blocks. Here, Sn-Beta zeolite in the presence of sodium tetraborate is shown to catalyze the selective epimerization of aldoses in aqueous media.
- William R. Gunther
- , Yuran Wang
- & Yuriy Román-Leshkov
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Lightweight nanoporous metal hydroxide-rich zeotypes
Nanoporous zeotypes have applications as catalysts and in gas separation, but they are usually produced as moderately dense silicates and aluminosilicates with relatively low capacities for gas uptake. Here, zeotype structures are reported with very low densities and high total specific pore volumes.
- Benjamin T.R. Littlefield
- & Mark T. Weller
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Highly stable Pt monolayer on PdAu nanoparticle electrocatalysts for the oxygen reduction reaction
Platinum is used as a cathode in fuel cells but undergoes dissolution during potential changes, hindering commercial application in electric vehicles. Sasakiet al.report a new class of stable electrocatalysts that consist of platinum monolayers on palladium–gold alloy nanoparticles.
- Kotaro Sasaki
- , Hideo Naohara
- & Radoslav R. Adzic
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Protein encapsulation within synthetic molecular hosts
Protein encapsulation in molecular cages has the potential to alter protein function and aid crystallization. Here, ubiquitin is encapsulated within a giant coordination cage; the protein is attached to a bidentate ligand, and the cage self-assembles upon addition of capping ligands and Pd(II) ions.
- Daishi Fujita
- , Kosuke Suzuki
- & Makoto Fujita
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Monodisperse conjugated polymer particles by Suzuki–Miyaura dispersion polymerization
Well-defined, monodisperse colloids of semiconducting polymers are required as new photonic and optoelectronic materials. Here, a Suzuki–Miyaura dispersion polymerization is used to produce monodisperse sub-micrometer particles of a range of semiconducting polymers.
- Alexander J.C. Kuehne
- , Malte C. Gather
- & Joris Sprakel
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Article
| Open AccessQuasiparticles and Fermi liquid behaviour in an organic metal
The physical properties of organic metals have generally been described in terms of a highly correlated Luttinger liquid. Using angle-resolved photoelectron spectroscopy, Kisset al. measure the Fermi surface of (BEDT-TTF)3Br(pBIB), and find that, in contrast to other systems, it can be described as a Fermi liquid.
- T. Kiss
- , A. Chainani
- & S. Shin
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Computational design of self-assembling register-specific collagen heterotrimers
The computational prediction of complex protein architectures has been used to design globular proteins, but the folding of collagen triple helices is difficult to predict. Here, a sequence-based scoring function for triple helix is developed and used to select sequences likely to self-assemble with high stability.
- Jorge A. Fallas
- & Jeffrey D. Hartgerink
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Quantifying through-space charge transfer dynamics in π-coupled molecular systems
The charge-transfer characteristics of conjugated molecules are important in determining their electronic properties. Using resonant photoemission spectroscopy, Batraet al. quantify the through-space charge transfer in two model conjugated systems with femtosecond resolution.
- Arunabh Batra
- , Gregor Kladnik
- & Latha Venkataraman
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Fabrication of flexible and freestanding zinc chalcogenide single layers
Ultrathin inorganic materials hold promise for a variety of applications, including flexible electronics. This work presents a fabrication method that permits the synthesis of large and flexible freestanding layers of zinc selenide that display a high-photocurrent density.
- Yongfu Sun
- , Zhihu Sun
- & Yi Xie
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A non-syn-gas catalytic route to methanol production
Methanol is an important industrial chemical and liquid fuel, and is usually produced by the syn-gas route from natural gas. Wuet al. develop a new catalytic process that directly converts ethylene glycol, derived from biomass or fossil fuels, to methanol in hydrogen using a Pd/Fe2O3co-precipitated catalyst.
- Cheng-Tar Wu
- , Kai Man Kerry Yu
- & Shik Chi Edman Tsang
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Naphthol radical couplings determine structural features and enantiomeric excess of dalesconols in Daldinia eschscholzii
The dalesconol natural products are biosynthesised in an enantiomeric excess of 67%, rather than as a single enantiomer or a racemate. Tanet al. report that this unusual enantioselectivity is a result of the dominance of particular conformers of naphthol dimer intermediates.
- Wei Fang
- , Shen Ji
- & Ren Xiang Tan
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Hygro-responsive membranes for effective oil–water separation
Membrane-based technologies to separate oil–water mixtures are energy-intensive, suffer from fouling or cannot separate a wide range of mixtures. Now, a new membrane is reported that is superhydrophilic and superoleophobic, and can separate a range of oil–water mixtures with high efficiency, without an external energy source.
- Arun K. Kota
- , Gibum Kwon
- & Anish Tuteja
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Article |
Stirring competes with chemical induction in chiral selection of soft matter aggregates
Chirality can be induced both by physical forces and by chemical induction processes. Here, a self-assembled system is reported in which chiral selection is controlled by the combined action of a chiral dopant and vortical stirring, which can act either constructively or destructively.
- Núria Petit-Garrido
- , Josep Claret
- & Francesc Sagués
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Biomimetic layer-by-layer assembly of artificial nacre
Nacre is an organic–inorganic composite biomaterial, which consists of an ordered multilayer structure of crystalline calcium carbonate platelets separated by porous organic layers. Finnemoreet al. present a route to artificial nacre which mimics the natural layer-by-layer biosynthesis.
- Alexander Finnemore
- , Pedro Cunha
- & Ullrich Steiner
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Article
| Open AccessPatterning symmetry in the rational design of colloidal crystals
Patchy colloids are colloidal particles with chemically or physically patterned surfaces that result in complex interactions arising between them. By means of numerical simulations, Romano and Sciortino show that suitably tailored patches can induce the crystallization of patchy colloids into specific crystal structures.
- Flavio Romano
- & Francesco Sciortino
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Article
| Open AccessAmbient-stable tetragonal phase in silver nanostructures
Crystallization of noble metal atoms usually leads to the thermodynamically stable face-centred cubic phase. Sunet al. show that internal strain in silver nanoparticles leads to lattice distortion and a stable body-centred tetragonal phase.
- Yugang Sun
- , Yang Ren
- & Dean J. Miller
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Article
| Open AccessStructural correlations in the generation of polaron pairs in low-bandgap polymers for photovoltaics
The electronic and optical properties of polymer semiconductors are largely dictated by their chemical structure. This study examines the nature of the photoexcited states generated in donor–acceptor polymers, and uncovers the dynamics of polaron pairs generation and recombination.
- Raphael Tautz
- , Enrico Da Como
- & Ullrich Scherf
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Microporous metal-organic framework with potential for carbon dioxide capture at ambient conditions
Metal-organic frameworks are promising candidates for capturing and sequestering carbon dioxide. Chen and co-workers report a metal-organic framework that exhibits high uptake of carbon dioxide at ambient conditions, and is a potentially useful adsorbent for post-combustion carbon dioxide capture.
- Shengchang Xiang
- , Yabing He
- & Banglin Chen
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Self-assembling subnanometer pores with unusual mass-transport properties
Molecular systems with rigid macrocyclic backbones self-assemble into synthetic nanopores that mimic the mass-transport characteristics of biological channels. Zhouet al. produce self-assembling hydrophobic nanopores that mediate highly selective transmembrane ion transport and highly efficient transmembrane water permeability.
- Xibin Zhou
- , Guande Liu
- & Bing Gong
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Stereoselectivity and electrostatics in charge-transfer Mn- and Cs-TCNQ4 networks on Ag(100)
The crystallization of a racemate on a surface can lead to crystals with a unit cell containing both enantiomers, or to the separation of enantiomers into crystals of single-handedness. This study shows that manganese co-absorbed with a quinone derivative leads to achiral islands, while co-absorption with caesium gives chiral islands.
- Nasiba Abdurakhmanova
- , Andrea Floris
- & Klaus Kern
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An ultrafast nickel–iron battery from strongly coupled inorganic nanoparticle/nanocarbon hybrid materials
Fast rechargeable batteries made from low-cost and abundant electrode materials are attractive for energy storage. Wanget al. develop an ultrafast Ni–Fe battery with carbon/inorganic hybrid electrodes in which the charge and discharge rates are nearly 1,000-fold higher than traditional Ni–Fe batteries.
- Hailiang Wang
- , Yongye Liang
- & Hongjie Dai
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Dynamic Jahn–Teller effect in the parent insulating state of the molecular superconductor Cs3C60
Expanded alkali fullerides are molecular superconductors with a Mott parent insulating state. Kluppet al.use infrared spectroscopy to detect the molecular Jahn–Teller distortion of fulleride ions and establish its relevance to strongly correlated superconductivity.
- Gyöngyi Klupp
- , Péter Matus
- & Kosmas Prassides
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Enantioselective synthesis of a chiral nitrogen-doped buckybowl
Nitrogen-doped fullerenes and carbon nanotubes have been produced, but the synthesis of nitrogen-doped buckybowls, is an unsolved challenge. Tanet al. report an enantioselective synthesis of triazasumanene, and show that nitrogen doping leads to deeper bowl structures than in all-carbon buckybowls.
- Qitao Tan
- , Shuhei Higashibayashi
- & Hidehiro Sakurai
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Article
| Open AccessUsing light transmission to watch hydrogen diffuse
Understanding hydrogen diffusion in metals is a challenge because of limited access to spatial evolution of the concentration profiles. Using time- and spatially resolved optical measurements, Palssonet al. determine the diffusion rate of hydrogen by directly monitoring its transit through a vanadium thin film.
- Gunnar K. Pálsson
- , Andreas Bliersbach
- & Björgvin Hjörvarsson
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Digital quantum simulation of the statistical mechanics of a frustrated magnet
Geometrically frustrated spin systems are a class of statistical mechanical models that have received widespread attention, especially in condensed matter physics. This study experimentally demonstrates a quantum information processor that can simulate the behaviour of such frustrated spin system.
- Jingfu Zhang
- , Man-Hong Yung
- & Jonathan Baugh
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Orbital switching in a frustrated magnet
Thed orbitals of transition metal compounds influence their crystallographic and physical properties. This study reports a unique structural transition in single crystals of the S=1/2 kagomé antiferromagnet, volborthite, whereby an unpaired electron 'switches' from one dorbital to another upon cooling.
- Hiroyuki Yoshida
- , Jun-ichi Yamaura
- & Zenji Hiroi
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Unsupported boron–carbon σ-coordination to platinum as an isolable snapshot of σ-bond activation
σ-Complexes of transition metals are key intermediates in metal-mediated bond activation, but have traditionally been isolable only when chelating or when one of the participating atoms is hydrogen. Here, a complex is isolated with an unsupported borirene ligand bound not through the unsaturated C=C bond, but exclusively via a B–C single bond.
- Holger Braunschweig
- , Peter Brenner
- & Alfredo Vargas
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Closed network growth of fullerenes
The formation mechanisms of fullerenes remain unclear. This study shows that fullerenes self-assemble through a closed network growth mechanism in which atomic carbon and C2are incorporated into the growing closed cages.
- Paul W. Dunk
- , Nathan K. Kaiser
- & Harold W. Kroto
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Article
| Open AccessSwitching of macroscopic molecular recognition selectivity using a mixed solvent system
Self-assembly via molecular recognition events is used in the production of functionalized materials. This Article reports that the macroscopic assembly of polyacrylamide gels can be controlled by changing the composition of a mixed solvent system.
- Yongtai Zheng
- , Akihito Hashidzume
- & Akira Harada
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Review Article |
Electrochemical tunnelling sensors and their potential applications
Quantum-mechanical tunnelling currents across nanometre-scale gaps between electrodes are sensitive to the medium in the gap. Albrecht reviews progress towards using tunnelling currents to probe single-molecule processes, and in biosensor and sequencing applications.
- T. Albrecht
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Article |
Tuning the magneto-structural properties of non-porous coordination polymers by HCl chemisorption
Tuning the properties of responsive materials by applying an external stimulus could lead to their application as chemical switches or molecular sensors. Coronadoet al. develop a non-porous one-dimensional coordination polymer, the magnetic properties of which undergo drastic changes on chemisorption of gaseous HCl.
- Eugenio Coronado
- , Mónica Giménez-Marqués
- & Lee Brammer
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Article |
Local chiral symmetry breaking in triatic liquid crystals
Studying the structures of dense colloidal systems of anisotropic Brownian particles provides insight into fundamental processes like protein crystallization. Zhaoet al. study the phases of two-dimensional triatic liquid crystals and find that one of them exhibits local chiral-symmetry breaking.
- Kun Zhao
- , Robijn Bruinsma
- & Thomas G. Mason
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Article |
Non-polydimethylsiloxane devices for oxygen-free flow lithography
Flow lithography is used to synthesize microparticles but relies on polydimethylsiloxane microchannels for oxygen to permeate and inhibit polymerization near channel interfaces. Now, non-polydimethylsiloxane devices have been developed, which allow oxygen-free lithography, increasing the capabilities of flow lithography.
- Ki Wan Bong
- , Jingjing Xu
- & Patrick S. Doyle
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Article |
First enantioseparation and circular dichroism spectra of Au38 clusters protected by achiral ligands
Clusters of gold atoms protected with achiral thiolates can display chirality, and such chiral nanoparticles could open new possibilities in catalysis and sensing. Here, the first separation of the enantiomers of a gold cluster, protected by achiral thiolates, Au38(SCH2CH2Ph)24, is achieved.
- Igor Dolamic
- , Stefan Knoppe
- & Thomas Bürgi
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Article |
Prominent electrochromism through vacancy-order melting in a complex oxide
Electrochromic materials reversibly change their colour upon application of an electric field. Seidelet al. measure the optical properties of doped bismuth ferrite and report the largest electrochromic response for an inorganic material, which they attribute to the melting of oxygen-vacancy ordering.
- J. Seidel
- , W. Luo
- & R. Ramesh
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Article |
Bilayer order in a polycarbazole-conjugated polymer
Conjugated polymers are promising materials for organic photovoltaic solar cells. By usingin situgrazing incidence wide-angle X-ray diffraction, Ocko and collaborators report the formation of a new type of crystalline arrangement in a conjugated polymer material known as PCDTBT.
- Xinhui Lu
- , Htay Hlaing
- & Benjamin M. Ocko
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Article |
Binary colloidal structures assembled through Ising interactions
The assembly of microscopic particles into macroscopic structures may allow the fabrication of complex materials, but general strategies to provide a wide variety of structures are lacking. Khalilet al. develop a colloidal assembly system, which can be tuned to provide over 20 different pre-programmed structures.
- Karim S. Khalil
- , Amanda Sagastegui
- & Benjamin B. Yellen
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Article
| Open AccessGiant regular polyhedra from calixarene carboxylates and uranyl
Self-assembly of multi-component systems can be used to construct discrete, well-defined, nanoscopic-sized cages. Pasqualeet al. report the self-assembly of conical-shaped carboxylic acid derivatives of calix[4]arene and calix[5]arene, and the uranyl cation UO22+into octahedral and icosahedral anionic metallocages.
- Sara Pasquale
- , Sara Sattin
- & Javier de Mendoza
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