Nature Chemistry Contents January 2018 Volume 10 Number 1 pp 1 - 110

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Advertisement Open for Submissions   A new open access, multi-and interdisciplinary journal dedicated to publishing the finest research on both microbial biofilms and microbiomes, the journal is now open for submissions.   Explore the benefits of submitting your next research article TABLE OF CONTENTS January 2018 Volume 10, Issue 1 Thesis News and Views Correction Review Articles Erratum In Your Element   Advertisement npj Clean Water: open for submissions     An open access, online-only journal, dedicated to publishing high-quality papers that describe the significant and cutting-edge research that continues to ensure the supply of clean water to populations.   Explore the benefits of submitting your next manuscript.   Subscribe   Facebook   RSS   Recommend to library   Twitter   Thesis Top Making molecular monsters   pp1 - 2 Michelle Francl doi:10.1038/nchem.2920 Michelle Francl muses on fantastic beasts of chemistry and why we try to find them.   News and Views Top Multi-electron transfer photochemistry: Caught in the act   pp3 - 4 Anna M. Beiler and Gary F. Moore doi:10.1038/nchem.2896 The accumulation of multiple redox equivalents is essential in photo-driven catalytic reactions such as solar water splitting. However, direct spectroscopic observation of a twice-oxidized species under diffuse illumination has proved elusive until now. See also: Article by Chen & Ardo Flexible molecular materials: Stressed out crystals   pp4 - 6 Bart Kahr and Michael D. Ward doi:10.1038/nchem.2913 Molecular crystals have recently started to shake their inflexible reputation. Now, copper(II) acetylacetonate needles have been shown to be very flexible, and their mechanical deformation has been assessed through materials constants using methods customarily reserved for non-molecular materials. See also: Article by Worthy et al. Water splitting: Passing the acid test   pp6 - 7 Qiushi Yin and Craig L. Hill doi:10.1038/nchem.2921 Water-oxidation catalysts that are fast and efficient in strong acid are rare even though there are several benefits for systems working at low pH. Such catalysts usually feature expensive noble metals such as ruthenium and iridum; however, an electrocatalytic system that is exceptionally efficient and based on cobalt has now been developed. See also: Article by Blasco-Ahicart et al. Chemistry JOBS of the week Senior Application Scientist Schrodinger, Inc Assistant Director, Member Relations MIT Faculty Positions Thomas Jefferson University (TJU) Transmission Electron Microscopy University of California - Irvine Postdoctoral Associate The Scripps Research Institute - Florida More Science jobs from Chemistry EVENT "6th Annual International Conference on Chemistry " 26.07.18 Athens, Greece More science events from Correction Top Correction   p7 doi:10.1038/nchem.2925   Review Top Collaborative routes to clarifying the murky waters of aqueous supramolecular chemistry   pp8 - 16 Paul S. Cremer, Amar H. Flood, Bruce C. Gibb and David L. Mobley doi:10.1038/nchem.2894 Given its ubiquity, the importance of understanding the properties of water cannot be understated. Now, stemming from discussions at a National Science Foundation-supported workshop, this Review Article highlights where there is latent chemical space for potential collaborations between the physical and supramolecular communities, both of which are interested in how molecules interact with each other in water.   Advertisement npj Quantum Materials is a new open access journal that is now open for submissions. The journal publishes broad coverage of quantum materials, their fundamental properties, fabrication and applications.   Sign up for article e-alerts>>>   Articles Top Direct observation of sequential oxidations of a titania-bound molecular proxy catalyst generated through illumination of molecular sensitizers   pp17 - 23 Hsiang-Yun Chen and Shane Ardo doi:10.1038/nchem.2892 Photosynthesis uses sunlight to oxidize or reduce reaction centres multiple times and prepare them for multiple-electron-transfer reactions. Now, it has been shown that a molecular proxy for a multiple-electron-transfer electrocatalyst can be oxidized twice by dye molecules when both are anchored to a mesoporous TiO2 thin film and excited with low-intensity visible light. Chemical compounds See also: News and Views by Beiler & Moore Polyoxometalate electrocatalysts based on earth-abundant metals for efficient water oxidation in acidic media   pp24 - 30 Marta Blasco-Ahicart, Joaquín Soriano-López, Jorge J. Carbó, Josep M. Poblet and J. R. Galan-Mascaros doi:10.1038/nchem.2874 Electrochemical water oxidation in acidic media is a promising water-splitting technique, but typically requires noble metal catalysts. Now, two polyoxometalate salts based on earth-abundant metals have shown excellent catalytic performance for the oxygen evolution reaction. The barium salt of a cobalt-phosphotungstate polyanion outperformed the state-of-the-art IrO2 catalyst at pHs lower than 1. See also: Article by Seo et al. Chromophore twisting in the excited state of a photoswitchable fluorescent protein captured by time-resolved serial femtosecond crystallography   pp31 - 37 Nicolas Coquelle, Michel Sliwa, Joyce Woodhouse, Giorgio Schirò, Virgile Adam et al. doi:10.1038/nchem.2853 Providing detailed structural descriptions of the ultrafast photochemical events that occur in light-sensitive proteins is key to their understanding. Now, excited-state structures in the reversibly switchable fluorescent protein rsEGFP2 have been solved by time-resolved crystallography using an X-ray laser. These structures enabled the design of a mutant with improved photoswitching quantum yields.   Bioinspired chemical synthesis of monomeric and dimeric stephacidin A congeners   pp38 - 44 Ken Mukai, Danilo Pereira de Sant'Ana, Yasuo Hirooka, Eduardo V. Mercado-Marin, David E. Stephens et al. doi:10.1038/nchem.2862 The biosynthesis of secondary metabolites such as stephacidin A and its congeners continues to intrigue both biochemists and synthetic chemists. Now, a laboratory chemical synthesis of these natural products has been achieved based on a bioinspired synthetic strategy, which may provide key insights into the possible biosynthesis of these captivating molecules. Chemical compounds Dynamic covalent chemistry enables formation of antimicrobial peptide quaternary assemblies in a completely abiotic manner   pp45 - 50 James F. Reuther, Justine L. Dees, Igor V. Kolesnichenko, Erik T. Hernandez, Dmitri V. Ukraintsev et al. doi:10.1038/nchem.2847 Despite advances in peptide synthesis techniques, explicit control over the quaternary structure of synthetic peptides has remained elusive. Now, the dynamic covalent chemistry of hydrazide- and aldehyde-containing peptides has now been shown to enable the formation of unique quaternary structures with topological diversity. Using this method, oligomers were assembled into complex structures showing dramatic enhancements of antimicrobial effectiveness versus Staphylococcus Aureus.   Designing cooperatively folded abiotic uni- and multimolecular helix bundles   pp51 - 57 Soumen De, Bo Chi, Thierry Granier, Ting Qi, Victor Maurizot et al. doi:10.1038/nchem.2854 Rationally designed arrays of hydrogen bonds between aromatic oligoamide segments have now been shown to generate abiotic helix-turn-helix and unexpected dimeric and trimeric helix bundle motifs. These structures show kinetic and thermodynamic stability, and cooperative folding in nonpolar solvents.   Organocatalytic asymmetric arylation of indoles enabled by azo groups   pp58 - 64 Liang-Wen Qi, Jian-Hui Mao, Jian Zhang and Bin Tan doi:10.1038/nchem.2866 The use of activating and directing groups can dramatically alter the course of a reaction. Now, it has been shown that an azo group can effectively perform as both in chiral phosphoric-acid catalysed formal nucleophilic aromatic substitution of azobenzene derivatives with indoles, affording axially chiral arylindoles with excellent enantioselectivities. Chemical compounds Atomic resolution of structural changes in elastic crystals of copper(II) acetylacetonate   pp65 - 69 Anna Worthy, Arnaud Grosjean, Michael C. Pfrunder, Yanan Xu, Cheng Yan et al. doi:10.1038/nchem.2848 Crystals are typically thought to be brittle and fragile materials, but needles of copper(II) acetylacetonate have now been shown to be flexible enough to be reversibly tied into a knot. Mechanistic investigations using synchrotron X-ray diffraction determined that the elastic bending occurs through rotation of the molecules within the crystal lattice. See also: News and Views by Kahr & Ward Synthetic nat- or ent-steroids in as few as five chemical steps from epichlorohydrin   pp70 - 77 Wan Shin Kim, Kang Du, Alan Eastman, Russell P. Hughes and Glenn C. Micalizio doi:10.1038/nchem.2865 Steroids are arguably the most well studied and successful class of natural-product-inspired pharmaceuticals, yet step-economical and enantiospecific de novo synthesis remains challenging. Now, it is shown that the combination of metallacycle-mediated annulative cross-coupling and vinyl cyclopropane rearrangement chemistry can be used to deliver a variety of partially aromatic synthetic steroids in a concise, flexible and enantiospecific fashion. Chemical compounds Self-assembly of polyhedral metal–organic framework particles into three-dimensional ordered superstructures   pp78 - 84 Civan Avci, Inhar Imaz, Arnau Carné-Sánchez, Jose Angel Pariente, Nikos Tasios et al. doi:10.1038/nchem.2875 Colloidal particles of metal–organic frameworks (ZIF-8 and UiO-66) with different polyhedral shapes can self-assemble into well-ordered, porous three-dimensional superstructures. These superstructures function as photonic crystals, with a photonic band gap that depends on the size of the MOF particles and shifts upon the sorption of guests within their pores.   Late-stage chemoselective functional-group manipulation of bioactive natural products with super-electrophilic silylium ions   pp85 - 90 Trandon A. Bender, Philippa R. Payne and Michel R. Gagné doi:10.1038/nchem.2863 Determining the structure­–activity relationships for complex structures can be quite challenging, but it is often the method by which many natural products are optimized for use as drugs. Now, the combination of a fluoroaryl borane catalyst, a phosphine additive and a silane reducing agent enables the late-stage selective modification of complex bioactive natural products in order to provide rapid access to a wide array of structures, and therefore functions. Chemical compounds Predicting DNA hybridization kinetics from sequence   pp91 - 98 Jinny X. Zhang, John Z. Fang, Wei Duan, Lucia R. Wu, Angela W. Zhang et al. doi:10.1038/nchem.2877 The rate constant of DNA hybridization varies over several orders of magnitude and is affected by temperature and DNA sequence. A machine-learning algorithm that is capable of accurately predicting hybridization rate constants has now been developed. Tests with this algorithm showed that over 90% of predictions were correct to within a factor of three.   Mechanism-based enhancement of scope and enantioselectivity for reactions involving a copper-substituted stereogenic carbon centre   pp99 - 108 Jaehee Lee, Suttipol Radomkit, Sebastian Torker, Juan del Pozo and Amir H. Hoveyda doi:10.1038/nchem.2861 Although organocopper compounds are well known in organic chemistry, only recently has a set of catalytic reactions emerged that involve intermediates containing a copper-substituted stereogenic carbon centre. Now, a mechanistic study demonstrates that a better understanding of this distinction offers ways to address significant limitations in scope and enantioselectivity, explaining why unexpected variations in selectivity can occur. Chemical compounds Erratum Top Erratum: Glucose-responsive insulin by molecular and physical design   p109 Naveed A. Bakh, Abel B. Cortinas, Michael A. Weiss, Robert S. Langer, Daniel G. Anderson et al. doi:10.1038/nchem.2898   In Your Element Top Terbium glows green   p110 Geng Deng doi:10.1038/nchem.2914 Geng Deng relates how terbium, a garden-variety lanthanide, has found its way into our daily lives owing to its green fluorescence.   Top Natureevents is a fully searchable, multi-disciplinary database designed to maximise exposure for events organisers. The contents of the Natureevents Directory are now live. The digital version is available here. Find the latest scientific conferences, courses, meetings and symposia on natureevents.com. 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