Latest Research

  • Article |

    The M-cluster in the active site of nitrogenase is derived from an 8Fe core assembled via coupling and rearrangement of two [Fe4S4] clusters concomitant with the insertion of an interstitial carbon and a ninth sulfur. Now, by combining synthetic [Fe4S4] clusters and assembly with a protein template, it has been shown that sulfite gives rise to the ninth sulfur that is inserted into the nitrogenase cofactor after the radical SAM-dependent carbide insertion and cofactor core rearrangement.

    • Kazuki Tanifuji
    • , Chi Chung Lee
    • , Nathaniel S. Sickerman
    • , Kazuyuki Tatsumi
    • , Yasuhiro Ohki
    • , Yilin Hu
    •  & Markus W. Ribbe
  • Article |

    Collision-induced spin–orbit transitions involve multiple interaction potentials and are by nature non-adiabatic, complicating both their experimental and theoretical study. Crossed-beam experiments and non-Born–Oppenheimer quantum calculations for inelastic collisions of carbon atoms with helium atoms, down to energies corresponding to temperatures below 10 K, have now been performed. Quantum-dynamical resonances predicted by theory were experimentally detected.

    • Astrid Bergeat
    • , Simon Chefdeville
    • , Michel Costes
    • , Sébastien B. Morales
    • , Christian Naulin
    • , Uzi Even
    • , Jacek Kłos
    •  & François Lique
  • Article |

    Scattering of molecules at low temperature that are prepared in single quantum states illuminates the mechanism of rotationally inelastic collisions and reveals the reorientation of partner molecules. By correlating each outgoing partial wave with the incoming waves, partial-wave analysis of the scattering angular distribution determines the dominant short- and long-range anisotropies of the interaction potential.

    • William E. Perreault
    • , Nandini Mukherjee
    •  & Richard N. Zare
  • Article |

    Molecular collisions can lead to the absorption of incident light even for transitions that are spectroscopically forbidden for the isolated molecules. Now the electronic–vibrational transitions of O2 have been theoretically studied and, contrary to textbook knowledge, it is shown that the absorption mechanism and the spectral line shape depend on the collision partner, oxygen or nitrogen.

    • Tijs Karman
    • , Mark A. J. Koenis
    • , Agniva Banerjee
    • , David H. Parker
    • , Iouli E. Gordon
    • , Ad van der Avoird
    • , Wim J. van der Zande
    •  & Gerrit C. Groenenboom
  • Article |

    The biosynthesis of the [FeFe] hydrogenase active site H-cluster requires several Fe–S proteins that perform poorly understood reactions. Now, a reaction intermediate trapped in the enzyme HydG is shown to contain a [(Cys)Fe(CO)(CN)] species identified as the first organometallic Fe moiety en route to the catalytic H-cluster.

    • Guodong Rao
    • , Lizhi Tao
    • , Daniel L. M. Suess
    •  & R. David Britt
  • Article |

    The phase in which a crystal exists can have a direct influence over its properties; however, it is usually difficult to control during synthesis. Now it has been shown that micrometre-sized metallic 1T′-MoS2- and 1T′-MoSe2-layered crystals can be prepared in high phase purity on a large scale, and that they display promising electrocatalytic activity towards the hydrogen evolution reaction.

    • Yifu Yu
    • , Gwang-Hyeon Nam
    • , Qiyuan He
    • , Xue-Jun Wu
    • , Kang Zhang
    • , Zhenzhong Yang
    • , Junze Chen
    • , Qinglang Ma
    • , Meiting Zhao
    • , Zhengqing Liu
    • , Fei-Rong Ran
    • , Xingzhi Wang
    • , Hai Li
    • , Xiao Huang
    • , Bing Li
    • , Qihua Xiong
    • , Qing Zhang
    • , Zheng Liu
    • , Lin Gu
    • , Yonghua Du
    • , Wei Huang
    •  & Hua Zhang
  • Article |

    Mg-based batteries possess potential advantages over their lithium counterparts; however, the use of reversible oxidation-resistant, carbonate-based electrolytes has been hindered because of their undesirable electrochemical reduction reactions. Now, by engineering a Mg2+-conductive artificial interphase on a Mg electrode surface, which prevents such reactivity, highly reversible Mg deposition/stripping in carbonate-based electrolytes has been demonstrated.

    • Seoung-Bum Son
    • , Tao Gao
    • , Steve P. Harvey
    • , K. Xerxes Steirer
    • , Adam Stokes
    • , Andrew Norman
    • , Chunsheng Wang
    • , Arthur Cresce
    • , Kang Xu
    •  & Chunmei Ban
  • Article |

    Peptide macrocycles are uniquely suited to engage some challenging biological targets, such as protein–protein interactions. Inspired by the ‘C–H’ cross-linked peptide natural products, a highly efficient and generally applicable strategy for constructing cyclophane-braced peptide macrocycles has been developed. The strategy is based on palladium-catalysed intramolecular C(sp3)–H arylation reactions.

    • Xuekai Zhang
    • , Gang Lu
    • , Meng Sun
    • , Madhu Mahankali
    • , Yanfei Ma
    • , Mingming Zhang
    • , Wangde Hua
    • , Yuting Hu
    • , Qingbing Wang
    • , Jinghuo Chen
    • , Gang He
    • , Xiangbing Qi
    • , Weijun Shen
    • , Peng Liu
    •  & Gong Chen
  • Article |

    A second-generation DNA-templated library of 256,000 small-molecule macrocycles has been developed. The improved method was created by streamlining and integrating multiple aspects of DNA-encoded and DNA-templated library synthesis methodology. In vitro selection of the macrocycle library against insulin-degrading enzyme enabled the discovery of potent inhibitors.

    • Dmitry L. Usanov
    • , Alix I. Chan
    • , Juan Pablo Maianti
    •  & David R. Liu
  • Article |

    Molecules that mimic the charge surface of B-DNA could enable the inhibition of DNA processive enzymes. Now, helically folded aromatic oligoamide scaffolds have been synthesized that display anions at positions similar to that of B-DNA phosphates. These foldamer mimics can recognize some DNA binding proteins and inhibit enzymes such as HIV integrase and topoisomerase 1.

    • Krzysztof Ziach
    • , Céline Chollet
    • , Vincent Parissi
    • , Panchami Prabhakaran
    • , Mathieu Marchivie
    • , Valentina Corvaglia
    • , Partha Pratim Bose
    • , Katta Laxmi-Reddy
    • , Frédéric Godde
    • , Jean-Marie Schmitter
    • , Stéphane Chaignepain
    • , Philippe Pourquier
    •  & Ivan Huc
  • Article |

    Cell-to-cell variation in gene expression creates a need for techniques that characterize expression at the level of individual cells. Now, a technique for characterizing mRNA expression has been developed. The technique uses the intracellular self-assembly of magnetic nanoparticles to quantitate RNA levels at the single-cell level.

    • Mahmoud Labib
    • , Reza M. Mohamadi
    • , Mahla Poudineh
    • , Sharif U. Ahmed
    • , Ivaylo Ivanov
    • , Ching-Lung Huang
    • , Maral Moosavi
    • , Edward H. Sargent
    •  & Shana O. Kelley
  • Article |

    Nanocatalysts can undergo various dynamic phenomena that affect their activity, such as restructuring and spillover. Now, using spatially and temporally resolved imaging of individual catalytic reactions, cooperative communication between different sites within single palladium- and gold-based nanocatalysts, and between different nanocatalysts, has been observed during three distinct catalytic reactions.

    • Ningmu Zou
    • , Xiaochun Zhou
    • , Guanqun Chen
    • , Nesha May Andoy
    • , Won Jung
    • , Guokun Liu
    •  & Peng Chen
  • Article |

    Mapping energy landscapes has proved to be a powerful approach for studying reaction mechanisms. Now, this strategy has been applied to determine the activation energies and entropies that characterize the molecular steps in the misfolding and aggregation of the amyloid-β peptide, revealing striking differences between the thermodynamic signatures of primary and secondary nucleation.

    • Samuel I. A. Cohen
    • , Risto Cukalevski
    • , Thomas C. T. Michaels
    • , Anđela Šarić
    • , Mattias Törnquist
    • , Michele Vendruscolo
    • , Christopher M. Dobson
    • , Alexander K. Buell
    • , Tuomas P. J. Knowles
    •  & Sara Linse
  • Review Article |

    Phytochemicals exhibit great pharmaceutical importance despite their low abundance in nature. The microbial biosynthesis of complex phytochemicals offers one route to increase their availability and production. This Review discusses recent strategies to reconstruct plant biosynthetic pathways that have not been fully elucidated; enhance plant enzyme activity; and enhance overall reaction efficiency of multi-enzyme pathways.

    • Sijin Li
    • , Yanran Li
    •  & Christina D. Smolke
  • Perspective |

    Organic synthesis is a rate-limiting factor in drug discovery, so the pharmaceutical industry heavily relies on academic research. This Perspective highlights some of the most pressing challenges to be overcome from the industrial viewpoint — such as the development of reactions tolerating specific functionalities — and encourages stronger industry–academia relationships.

    • David C. Blakemore
    • , Luis Castro
    • , Ian Churcher
    • , David C. Rees
    • , Andrew W. Thomas
    • , David M. Wilson
    •  & Anthony Wood
  • Article |

    Halogen bonding is known to get stronger with increasing halogen polarizability, but some trends of the periodic table break down for heavy elements owing to relativistic effects. Now, through distribution coefficient measurements and relativistic quantum mechanical calculations, AtI has been shown to form stronger halogen bonds than I2—meaning that astatine conforms to the trend.

    • Ning Guo
    • , Rémi Maurice
    • , David Teze
    • , Jérôme Graton
    • , Julie Champion
    • , Gilles Montavon
    •  & Nicolas Galland
  • Article |

    Encoded display of multiple chemical elements on a constant macrocyclic scaffold could mimick antibody–antigen recognition. A chemical library constructed using this approach enabled the identification of specific binders against a variety of protein targets, including difficult targets, such as TNF.

    • Yizhou Li
    • , Roberto De Luca
    • , Samuele Cazzamalli
    • , Francesca Pretto
    • , Davor Bajic
    • , Jörg Scheuermann
    •  & Dario Neri
  • Article |

    The extent to which peptide synthesis by the ribosome can tolerate the inclusion of non-peptidic components is not clear. Yet such hybrids would expand the range of ribosomally synthesized structures. Now it has been shown that tRNAs acylated by aromatic foldamers can initiate the ribosomal synthesis of non-cyclic and cyclic foldamer–peptide hybrid molecules. The oligo-aryl segments contain folding information that can control peptide conformation in the hybrids.

    • Joseph M. Rogers
    • , Sunbum Kwon
    • , Simon J. Dawson
    • , Pradeep K. Mandal
    • , Hiroaki Suga
    •  & Ivan Huc
  • Article |

    Isotope effects provide deep insight into mechanisms of chemical and biochemical processes. Now, it has been shown that the pattern of isotopic substitution of the isomerizing bond of the retinal chromophore in the visual pigment rhodopsin significantly alters the reaction quantum yield—revealing a vibrational phase-dependent isotope effect.

    • C. Schnedermann
    • , X. Yang
    • , M. Liebel
    • , K. M. Spillane
    • , J. Lugtenburg
    • , I. Fernández
    • , A. Valentini
    • , I. Schapiro
    • , M. Olivucci
    • , P. Kukura
    •  & R. A. Mathies
  • Article |

    Inspired by the post-translational modifications of polypeptides widespread in biological systems, the one-pot synthesis of biohybrid materials was engineered within Escherichia coli using a recombinant expression and post-translational lipidation. The fatty-acid-modified elastin-like polypeptides (FAMEs) prepared, which comprise peptide-amphiphile segments prone to self-assembly fused to a thermally responsive elastin-like polypeptide, exhibit temperature-triggered hierarchical assembly.

    • Davoud Mozhdehi
    • , Kelli M. Luginbuhl
    • , Joseph R. Simon
    • , Michael Dzuricky
    • , Rüdiger Berger
    • , H. Samet Varol
    • , Fred C. Huang
    • , Kristen L. Buehne
    • , Nicholas R. Mayne
    • , Isaac Weitzhandler
    • , Mischa Bonn
    • , Sapun H. Parekh
    •  & Ashutosh Chilkoti
  • Article |

    The construction of dynamic protein–DNA nano-assemblies suitable for modulating protein proximities and activities has now been demonstrated. This approach uses DNA strand displacement and can enable control of enzyme activity to be programmed using logic gates. As a demonstration, a split enzyme capable of activating a prodrug is triggered is by cancer-specific miRNAs.

    • Rebecca P. Chen
    • , Daniel Blackstock
    • , Qing Sun
    •  & Wilfred Chen
  • Article |

    Heterometallic nanomaterials in unusual crystal phases that are impossible to form in the bulk state can show interesting physical and chemical properties. Here, crystal-phase heterostructured 4H/fcc Au nanowires are used as seeds to epitaxially grow a variety of binary and ternary hybrid noble metal nanostructures on the phase boundary.

    • Qipeng Lu
    • , An-Liang Wang
    • , Yue Gong
    • , Wei Hao
    • , Hongfei Cheng
    • , Junze Chen
    • , Bing Li
    • , Nailiang Yang
    • , Wenxin Niu
    • , Jie Wang
    • , Yifu Yu
    • , Xiao Zhang
    • , Ye Chen
    • , Zhanxi Fan
    • , Xue-Jun Wu
    • , Jinping Chen
    • , Jun Luo
    • , Shuzhou Li
    • , Lin Gu
    •  & Hua Zhang
  • Article |

    Even though the Grotthuss mechanism was proposed two centuries ago, it is still unclear why proton transfer via the hydroxide ion is slower than that via hydronium. Advanced ab initio molecular dynamics simulations now show that it is because proton transfer via hydroxide is less temporally correlated than transfer via hydronium.

    • Mohan Chen
    • , Lixin Zheng
    • , Biswajit Santra
    • , Hsin-Yu Ko
    • , Robert A. DiStasio Jr
    • , Michael L. Klein
    • , Roberto Car
    •  & Xifan Wu