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Volume 13 Issue 4, April 2021

Ultrafast at the interface

The ubiquitous interface between water and other phases provides a unique environment where various important processes take place. For example, chemical reactions occurring at the water interface are important in biological and environmental settings and also in organic/inorganic chemistry and electrochemistry. Now, ultrafast phase-sensitive interface-selective vibrational spectroscopy has revealed that the photoionization reaction of phenol proceeds four orders of magnitude faster at the water surface than in the bulk aqueous phase. The cover shows a representation of the experiment, showing the UV, visible and IR light pulses used to monitor the photochemical change at the air–water interface.

See Kusaka et al.

Image credit: Tahei Tahara, RIKEN. Cover design: Tulsi Voralia.

Q&A

  • The career paths of Alveda Williams and Cory Valente have closely mirrored each other — perhaps surprisingly so for a straight Black woman and a gay white man with very different childhoods. They talk to Nature Chemistry about their journeys from research and development roles to Dow’s inclusion and diversity team.

    • Anne Pichon
    Q&A

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Thesis

  • Michelle Francl wonders what the future will think of her office.

    • Michelle Francl
    Thesis
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News & Views

  • The physical properties of a liquid at an interface differ from bulk solution limits, but how this affects chemical reactivity is unclear. Now, ultrafast, surface-sensitive vibrational spectroscopy has revealed that the light-induced reaction of phenol with water is four orders of magnitude faster at the water surface than in bulk.

    • Robert A. Walker
    News & Views
  • Harnessing the unique catalytic properties of enzymes for abiotic reactions is a prized goal that has inspired a variety of approaches in enzyme design and engineering. Now, the transfer hydrogenation of ketones with silanes has been reported, catalysed by a native carbonic anhydrase.

    • Hans Martin Senn
    News & Views
  • The therapeutic applications of DNAzymes are limited because of their low effectiveness in vivo. Now, a promising approach for constructing DNAzymes that show high gene-silencing efficiency in mammalian cells has been developed. This approach incorporates chemical modifications into an existing DNAzyme scaffold.

    • Yifei Zhou
    • Chuanzheng Zhou
    News & Views
  • Modelling the structure and behaviour of vesicles in cells requires liposomes with precise sizes, but producing liposomes with a narrow size distribution is challenging. An approach has now been developed to accurately size-sort liposomes in a scalable way by coating them with customized structures based on DNA nanotechnology.

    • Silvia Hernández-Ainsa
    News & Views
  • The formation of all-carbon quaternary centres is a challenging problem in organic chemistry, with far-reaching implications for functional molecule discovery. Now an inventive solution has been developed, using sulfinamides as traceless linkers for an asymmetric radical Truce–Smiles rearrangement.

    • David M. Whalley
    • Michael F. Greaney
    News & Views
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Articles

  • Reactions at the interface between water and other phases play important roles in various chemical settings. Now, ultrafast phase-sensitive interface-selective vibrational spectroscopy has revealed that the photoionization of phenol can occur four orders of magnitude faster at the water surface than in the bulk aqueous phase.

    • Ryoji Kusaka
    • Satoshi Nihonyanagi
    • Tahei Tahara
    Article
  • Enzymatic reactions involving mononuclear metal hydrides are unknown in nature, despite the prevalence of such intermediates in synthetic transition-metal catalysed reactions. Now, it has been shown that zinc-containing carbonic anhydrase enzymes can catalyse hydride transfers from silanes to ketones with high enantioselectivity and there is evidence to support the intermediacy of a mononuclear zinc hydride.

    • Pengfei Ji
    • Jeeyoung Park
    • John F. Hartwig
    Article
  • RNA-cleaving DNA enzymes (DNAzymes) have the potential to function as therapeutic agents by silencing the expression of disease-associated proteins. Xeno-nucleic acids were used to improve the catalytic activity and biological stability of a highly evolved DNAzyme known as 10–23. The enzyme exhibits a robust multiple-turnover activity in cultured mammalian cells.

    • Yajun Wang
    • Kim Nguyen
    • John C. Chaput
    Article
  • The assembly of a single configuration of an all-carbon quaternary centre within acyclic systems remains a challenge for synthetic chemists. Now, it has been shown that α-all-carbon quaternary centres can be installed in acyclic amides, with excellent levels of absolute stereocontrol, through a radical sulfinyl Truce–Smiles rearrangement.

    • Cédric Hervieu
    • Mariia S. Kirillova
    • Cristina Nevado
    Article
  • Small liposomes of uniform sizes are valuable tools for studying membrane biology and developing drug-delivery vehicles. Now, a DNA-assisted sorting technique has been shown to produce multiple species of monodispersed liposomes with mean diameters below 150 nm in a scalable manner. This approach has enabled the high-resolution analyses of curvature-dependent membrane protein activities.

    • Yang Yang
    • Zhenyong Wu
    • Chenxiang Lin
    Article
  • Solvent plays a critical role in electron-transfer reactions, but short-range solvation dynamics are challenging to observe. Now, femtosecond X-ray solution scattering has been used to directly monitor the reorganization of water upon ultrafast intramolecular electron transfer in a bimetallic complex. Coherent motions of the first-shell water molecules are observed, arising from changes in solute–solvent hydrogen bonding.

    • Elisa Biasin
    • Zachary W. Fox
    • Munira Khalil
    Article
  • On-surface dehydrogenative bond formation between sp3-hybridized carbon atoms usually requires high temperatures. Now, it has been shown that the higher homologue, silicon, can undergo dehydrogenative polymerization at room temperature on metal surfaces. This process creates well-ordered structures on Au(111) and Cu(111), with different stereoselectivity depending on the metal.

    • Lacheng Liu
    • Henning Klaasen
    • Armido Studer
    Article
  • Some metal–organic frameworks (MOFs) can promote photocatalytic hydrogen evolution and others can facilitate water oxidation, but it is difficult to combine them into a single system. Now, by confining MOFs that can promote each half-reaction within the hydrophobic and hydrophilic regions of a liposome to avoid the fast recombination of photo-generated charges, evidence for water splitting has been obtained.

    • Huihui Hu
    • Zhiye Wang
    • Cheng Wang
    Article
  • Excising hydrogen adjacent to a carbonyl group—one of the most basic and widely employed transformations in organic synthesis—is traditionally achieved using metals and/or stoichiometric oxidants. Now, it has been shown that an electrochemically driven approach removes such requirements, resulting in a more sustainable and easily scalable method with wide substrate scope.

    • Samer Gnaim
    • Yusuke Takahira
    • Phil S. Baran
    Article
  • The metathesis of carbon–carbon double bonds is an important tool in organic synthesis and now a similar reshuffling has been carried out with heavier alkene analogues featuring unsymmetrically substituted Ge=Ge double bonds. This reaction enables the synthesis of symmetric molecular digermenes as well as a polymer based on Ge=Ge repeat units.

    • Lukas Klemmer
    • Anna-Lena Thömmes
    • David Scheschkewitz
    Article
  • Although many natural products and drug molecules contain N–N linkages, the chemistry of N–N coupling is somewhat underdeveloped. Now, a nitrene-mediated intermolecular N–N coupling of dioxazolones and arylamines that relies on iridium or iron catalysis has been developed. These reactions offer a simple and efficient method for the synthesis of hydrazides from readily available precursors.

    • Hao Wang
    • Hoimin Jung
    • Gong Chen
    Article
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