Physical sciences articles within Nature Chemistry

Featured

  • Article |

    Although enzymes are known to use diiron centres to cleave carbon–hydrogen bonds, preparing synthetic compounds that can break these strong, stable bonds has remained notoriously difficult. Now, converting a low-spin ‘diamond core’ iron–oxo biomimetic complex into its high-spin ‘open core’ counterpart has enhanced its C–H bond cleavage ability by over a million times.

    • Genqiang Xue
    • , Raymond De Hont
    •  & Lawrence Que Jr

  • Research Highlights |

    The intercalation of potassium into a simple aromatic hydrocarbon results in a new class of organic superconductors.

    • Neil Withers

  • Research Highlights |

    A comparison of models for the sun-protection factor, transparency and production of reactive oxygen species leads to a prediction of the optimum size of titania nanoparticles for use in sunscreen.

    • Stephen Davey

  • Article |

    A wide range of porous framework materials has been assembled with a modular approach that takes advantage of prefabricated structural building units (SBUs). Now, it has been shown that functional all-inorganic frameworks can be made from a macrocyclic polyoxometalate SBU — that has a built-in aperture approximately 1 nm in diameter — linked together with redox-switchable metal ions.

    • Scott G. Mitchell
    • , Carsten Streb
    •  & Leroy Cronin

  • Article |

    Nanotubular structures made from different materials are being investigated for applications ranging from sensing to drug delivery, but controlling how they interact with ‘cargo’ molecules has proved challenging. Now, the selective uptake, precise positioning and triggered release of gold nanoparticles has been achieved with nanotubes assembled from triangular DNA building blocks.

    • Pik Kwan Lo
    • , Pierre Karam
    •  & Hanadi F. Sleiman

  • Article |

    Chiral thiols and organosulfur compounds are important in many areas of chemistry but there are relatively few methods available for their efficient enantioselective synthesis. Here, a kinetic resolution of chiral thiols is reported along with a demonstration that a concomitant desymmetrization of the acylating agent is beneficial for the selectivity of both processes.

    • Aldo Peschiulli
    • , Barbara Procuranti
    •  & Stephen J. Connon

  • Research Highlights |

    Molecular dynamics simulations have revealed important mechanistic details about how carbamate is transported from one active site to another within in an enzyme.

    • Gavin Armstrong

  • Research Highlights |

    Charge transport through electron hopping has been observed between π–π stacked perylene derivatives incorporated into DNA hairpin scaffolds.

    • Anne Pichon

  • News & Views |

    The interactions of electrons and water molecules are not just of great fundamental interest but are also studied to understand the role electrons have in damaging biomolecules. Now using ultrafast photoelectron spectroscopy, key details about the energy and lifetime of the hydrated electron in bulk and at an interface have been determined.

    • Daniel M. Neumark

  • Article |

    The existence of solvated electrons bound at the liquid/water surface has not, until now, been proved experimentally. Here, using ultrafast photoelectron spectroscopy, the existence, vertical binding energies and lifetimes of solvated electrons bound at the water-surface/vacuum interface, and in bulk solution, have been revealed.

    • Katrin R. Siefermann
    • , Yaxing Liu
    •  & Bernd Abel

  • Research Highlights |

    Thermally stable stereoisomers can be interconverted by the application of a mechanical force using ultrasound irradiation.

    • Stephen Davey

  • Research Highlights |

    A krypton difluoride coordination compound — where it acts as a ligand to a bromine atom — has been synthesized and studied.

    • Neil Withers

  • News & Views |

    The long-awaited first total synthesis of the structurally intriguing natural product palau'amine has now been achieved. The synthesis features cascade reactions and an 'across ring' stitching of a 'macropalau'amine', and sets the bar for future efforts towards an enantioselective variant.

    • Daniel Romo

  • News & Views |

    Public acceptance of the expansion of nuclear power may hinge on the safe disposal of nuclear waste. Ion exchangers that remove radioactive metals — such as caesium ions — from the waste could provide part of the answer, so a flexible-framework material that selectively grab them from solution is a step in the right direction.

    • Abraham Clearfield

  • News & Views |

    Monitoring the dynamics of a single molecule is impeded by their motion in solution, and immobilizing them without changing their properties is problematic. By using a trapping method that counteracts a molecule's Brownian motion, the complex dynamics of a fluorescent protein, allophycocyanin, have been investigated.

    • Peter Dedecker
    •  & Johan Hofkens

  • News & Views |

    Electromerism is an unfamiliar concept to many chemists and refers to molecules that are not conventional isomers but instead differ in how the electrons are distributed across their structure. A novel example of such electromers has now been demonstrated.

    • Thomas Bally

  • News & Views |

    Supramolecular gels, which rely on non-covalent interactions, are typically fragile. Now, hydrogels that possess remarkable mechanical strength combined with the ability to rapidly self-heal have been built through multiple non-covalent interactions.

    • David K. Smith

  • Editorial |

    As the saying goes, a picture is worth a thousand words, but when that picture appears on the front cover of a scientific journal, that estimate is probably a little on the low side.

  • In Your Element |

    Herbert Roesky relates how the small, highly electronegative fluorine atom unveiled the chemical reactivity of noble gases and found many practical applications. but it can also render organic compounds highly toxic or pollutants.

    • Herbert W. Roesky

  • News & Views |

    Monomers that contain masked ketene groups provide new opportunities for facile crosslinking and post-synthetic modification of polymers in a wide variety of materials applications.

    • Steve Rimmer

  • Commentary |

    Traditional scientific conferences can be costly and time-consuming, and certainly aren't 'green', with participants travelling long distances to attend. Are there advantages to meetings held in the virtual world, and can they really offer equally satisfying — or even better — experiences compared with the real world?

    • Christopher J. Welch
    • , Sanjoy Ray
    •  & Martin Leach

  • Article |

    Stepwise deuteration of protonated methane CH5+ — a fluxional structure that undergoes ‘hydrogen scrambling’ — leads to dramatic changes in the infrared spectra of the isotopologues. The spectra can be assigned using ab initio quantum simulations that account for the non-classical occupation — by H and D atoms — of topologically different sites within the molecule.

    • Sergei D. Ivanov
    • , Oskar Asvany
    •  & Stephan Schlemmer

  • Article |

    Steric, torsion, stereoelectronic and polar effects are widely used to explain and predict the stereochemical outcome of synthetic organic reactions. Here, the asymmetric distortion of the reactant is considered and used to explain the observed stereoselectivity where these accepted models are unable to provide a clear prediction.

    • Robert V. Kolakowski
    •  & Lawrence J. Williams

  • Article |

    Formic acid fuel cells require nanosized intermetallic nanoparticles as anode catalysts, but current techniques are poor at producing the small size required. Now, surface-modified ordered mesoporous carbons have been used to produce nanocrystallites as small as 1.5 nm that are extremely active catalysts.

    • Xiulei Ji
    • , Kyu Tae Lee
    •  & Linda F. Nazar

  • Article |

    A triflimide-catalysed rearrangement of N-allylhydrazones has been developed that allows for the generation of a sigma bond between two unfunctionalized sp3 carbons such that no clear marker remains for how the bond was formed. This traceless bond construction offers new avenues for convergent fragment coupling in synthetic strategies.

    • Devon A. Mundal
    • , Christopher T. Avetta Jr
    •  & Regan J. Thomson

  • Research Highlights |

    The slow oxidation of tellurium in semiconductor cadmium telluride nanoparticles, accompanied by the replacement of tellurium by sulfur, has led to CdS/CdTe nanoparticles that self-assemble under visible light into twisted nanoribbons.

    • Anne Pichon

  • Research Highlights |

    The motion of a molecule on a hot surface is investigated using molecular dynamics, revealing a regime of fast rolling and vibrational excitation.

    • Gavin Armstrong

  • Article |

    Fullerene cages that break the isolated pentagon rule are rare and often unstable. Now a range of fullerenes that feature three sequentially fused pentagons of carbon have been stabilized by chlorination.

    • Yuan-Zhi Tan
    • , Jia Li
    •  & Lan-Sun Zheng

  • Article |

    Polytheonamide B is a large non-ribosomal peptide with very high bioactivity. The synthesis described here includes the first preparation of several non-proteinogenic amino acids and a general coupling strategy for large non-natural peptides. The synthesis is a key step necessary to understand and utilize the bioactivity of this and similar compounds.

    • Masayuki Inoue
    • , Naoki Shinohara
    •  & Shigeru Matsuoka

  • Research Highlights |

    The reversible conversion between guanine-based extended ribbons and macrocyclic G-quartets has been directly observed at a liquid–solid interface by scanning tunnelling microscopy.

    • Anne Pichon

  • Research Highlights |

    Positive charges lower, and negative charges raise the freezing temperature of supercooled water on a pyroelectric surface, as well as affecting at which interface nucleation takes place.

    • Gavin Armstrong

  • Review Article |

    The field of organocatalysis has grown rapidly in the past decade to become, along with metal catalysis and biocatalysis, a third pillar of asymmetric catalysis. Here, progress in the use of organocatalytic cascade reactions for total synthesis is reviewed. The elegance and efficiency of such cascades mean that they have emerged as a powerful tool in synthetic organic chemistry.

    • Christoph Grondal
    • , Matthieu Jeanty
    •  & Dieter Enders

  • Research Highlights |

    A Brønsted acid co-catalyst is the key to the synthesis of furans by alkene cross-metathesis.

    • Laura Croft

  • Research Highlights |

    Exposing supramolecular filaments to X-rays results in spontaneous and reversible crystalline ordering.

    • Neil Withers

  • News & Views |

    A linear molecule containing three bipyridine ligands can be wrapped around a single metal-ion template to form an open-knot complex. The loose ends of the knot can be 'tied' together through esterification or olefin-metathesis reactions to form closed knots that do not unravel when the metal template is removed.

    • Edward E. Fenlon

  • Article |

    The movement of oxygen ions through materials is important in electrolytes and separation membranes, but is rare at lower temperatures. Two different low-temperature diffusion pathways are revealed during the reduction process of CaFeO2.5 to CaFeO2. The two pathways are significantly different, resulting in anisotropy.

    • Satoru Inoue
    • , Masanori Kawai
    •  & Yuichi Shimakawa

  • Article |

    The uptake of ammonia by a covalent–organic framework (COF) containing a high density of Lewis-acidic boron sites has been found to be significantly greater than that exhibited by other state-of-the-art porous materials. The ammonia can be removed by heating under vacuum and the structural integrity of the COF is maintained during adsorption/desorption cycles.

    • Christian J. Doonan
    • , David J. Tranchemontagne
    •  & Omar M. Yaghi

  • Article |

    The synthesis of interlocked compounds such as catenanes and rotaxanes has undergone much development in recent years, but molecular knots are still relatively hard to make. It has now been shown that a linear bipyridine oligomer can fold around a single zinc-ion template to form a complex that can be cyclized to give a molecular trefoil knot.

    • Jun Guo
    • , Paul C. Mayers
    •  & Christopher A. Hunter

  • Article |

    A methodology for describing local electronic transmission through bridging molecules between metallic electrodes is presented. Its application to simple alkane, phenyl and cross-conjugated systems highlights an unexpected number of cases whereby ‘through space’, rather than ‘through bond’ terms dominate and that interference effects coincide with the reversal of ring currents.

    • Gemma C. Solomon
    • , Carmen Herrmann
    •  & Mark A. Ratner

  • Research Highlights |

    Silicon-based polymers have been assembled into honeycomb films that exhibit good flexibility, stability and thermal conductivity, showing great promise for industrial applications.

    • Anne Pichon

  • Research Highlights |

    Replacing readily hydrolysable ester linkages with amides in a natural adjuvant has resulted in not only more stable, but significantly more active and less toxic analogues.

    • Georgia Tsoukala

  • News & Views |

    The use of conventional computers to calculate molecular properties is hindered by the exponential increase in computational cost on increasing the size of the molecules studied. Using quantum computers could be the solution and the initial steps are now being taken.

    • Kenneth R. Brown

  • News & Views |

    Quantum tunnelling can at times be the cause of kinetic isotope effects, and in these cases conventional wisdom has been that molecules with isotopes of larger mass will react more slowly. New calculations, however, predict that sometimes the reverse should be true.

    • Barry K. Carpenter

  • News & Views |

    Chemical reactions of fullerenes and metallofullerenes lined up inside single-walled carbon nanotubes can be monitored at the atomic scale inside an aberration-corrected transmission electron microscope.

    • Mauricio Terrones

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