Nature Chemistry Contents April 2014 Volume 6 Number 4 pp 255-370

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TABLE OF CONTENTS April 2014 Volume 6, Issue 4 Editorial Correspondence Commentary Feature Thesis Books and Arts Research Highlights Blogroll News and Views Review Articles Addendum In Your Element Subscribe   Facebook   RSS   Recommend to library   Twitter   Advertisement Nature Chemistry is 5  Nature Chemistry is now five years old! To celebrate, we look at some facts and figures relating to the manuscripts that have passed through our hands - including information about how many submissions we have received and where they came from, our referee pool, the authors and titles of published papers, as well as some citation data. Each editor has also picked out one of their favourite papers and explains why it stood out for them. Selected content free to registered users until April 22nd    Editorial Top Take five   pp255 - 257 doi:10.1038/nchem.1911 As Nature Chemistry celebrates its fifth birthday, we take a look at some of the facts and figures that underpin the story of the journal so far. Correspondence Top Contradictions in X-ray structures of intermediates in the photocycle of photoactive yellow protein   pp258 - 259 Ville R. I. Kaila, Friedrich Schotte, Hyun Sun Cho, Gerhard Hummer and Philip A. Anfinrud doi:10.1038/nchem.1898 See also: Correspondence by Jung et al. | Article by Jung et al. Reply to 'Contradictions in X-ray structures of intermediates in the photocycle of photoactive yellow protein'   pp259 - 260 Yang Ouk Jung, Jae Hyuk Lee, Joonghan Kim, Marius Schmidt, Keith Moffat et al. doi:10.1038/nchem.1897 See also: Correspondence by Kaila et al. | Article by Jung et al. Commentary Top Beyond Hofmeister   pp261 - 263 Pavel Jungwirth and Paul S. Cremer doi:10.1038/nchem.1899 Research efforts related to the Hofmeister series of salt ions have waxed and waned during its long and storied history. The past few decades have, however, witnessed a renaissance in its study, and the importance of the related solvation science is becoming ever more apparent. Feature Top A few of our favourite things   pp264 - 266 doi:10.1038/nchem.1902 To celebrate Nature Chemistry turning five years old, editors past and present each share the story of a paper that, for one reason or another, stands out from all the others they have shepherded into the journal. Thesis Top Attack of the clones   pp267 - 268 Michelle Francl doi:10.1038/nchem.1906 Michelle Francl suggests that self-plagiarism is a misleading term and that repeating yourself in publications isn't always a bad thing. Books and Arts Top Television: Pick your poison   p269 Chad Jones doi:10.1038/nchem.1909 Research Highlights Top Interlocked molecules: Triple-clipped links | Cryopreservation: In the deep freeze | Asymmetric catalysis: Separation of powers | Polymersomes: A light alteration Blogroll Top Blogroll: The human element   p271 Vittorio Saggiomo doi:10.1038/nchem.1900 News and Views Top Protein chemistry: Catalytic amyloid fibrils   pp273 - 274 Tobias Aümuller and Marcus Fändrich doi:10.1038/nchem.1904 Amyloid fibrils are formed from polypeptide chains assembled into an organized fibrillar structure. Now, it has been shown that such fibrillar structures can also bind metal ions and catalyse chemical reactions. See also: Article by Rufo et al. Reaction kinetics: Isotope effects feel the cold   pp274 - 275 Mark Brouard doi:10.1038/nchem.1903 Kinetic isotope effects are widely used to elucidate reaction mechanisms and are generally interpreted in terms of simple kinetic models. Measurements of this effect for the Penning ionization reaction between helium and dihydrogen highlight the need for a quantum description of chemical reaction rates when sub-kelvin temperatures are approached. See also: Article by Lavert-Ofir et al. Polymer synthesis: Chaining up carbon dioxide   pp276 - 277 Andrew P. Dove doi:10.1038/nchem.1907 The development of methods for efficiently using carbon dioxide in synthesis would enable chemists to tap into this abundant resource. Now, an indirect route to the copolymerization of alkenes with carbon dioxide shows how this greenhouse gas may prove useful in the search for new 'green' materials. See also: Article by Nakano et al. Metal-organic frameworks: Recognizing the unrecognizable   pp277 - 278 Krista S. Walton doi:10.1038/nchem.1910 Separating carbon monoxide from chemically similar nitrogen gas is particularly challenging. Now, a flexible porous coordination polymer has been developed that recognizes carbon monoxide over nitrogen, with structural changes in the material leading to its accelerated adsorption. Asymmetric synthesis: Cascades of catalytic selectivity   pp279 - 280 Rian D. Dewhurst and Todd B. Marder doi:10.1038/nchem.1905 A combination of catalytic asymmetric diboration of terminal alkenes and Suzuki-Miyaura cross-coupling has been exploited in the synthesis of a variety of important medicinal agents. The process overcomes a number of problems in the application of these important catalytic processes. Photonics JOBS of the week Senior research associate position in computational chemistry-biology Spanish National Research Council (CSIC) PhD Computational Spin Chemistry Max-Planck Institute for Dynamics of Complex Technical Systems Assistant professor in Analytical Chemistry Vrije Universiteit Brussel Member of academic staff / Senior Scientist (E 13 TV-L) TU Dresden PhD Studentship in Plasma Catalysis for Fuel Production University of Liverpool More Science jobs from Photonics EVENT A Celebration of Organic Chemistry 2014 22.09.14 Surrey, UK More science events from Review Top The power of ion mobility-mass spectrometry for structural characterization and the study of conformational dynamics   pp281 - 294 Francesco Lanucara, Stephen W. Holman, Christopher J. Gray and Claire E. Eyers doi:10.1038/nchem.1889 Ion mobility-mass spectrometry (IM-MS) is enhancing many areas of (bio)chemical analysis because it can separate ions both by their mass-to-charge ratio and differences in their cross-sectional area. IM-MS can be used for structural characterization, enhanced analysis of complex mixtures or to gain insights into conformational dynamics. Articles Top Diversity in the dynamical behaviour of a compartmentalized programmable biochemical oscillator   pp295 - 302 Maximilian Weitz, Jongmin Kim, Korbinian Kapsner, Erik Winfree, Elisa Franco et al. doi:10.1038/nchem.1869 Compartmentalization of complex chemical networks is an essential step towards the creation of cell-scale molecular systems. The encapsulation of a synthetic biochemical oscillating reaction system into cell-sized emulsion droplets is now demonstrated; a large variability in its oscillatory dynamics is observed, which is attributed to partitioning effects. Short peptides self-assemble to produce catalytic amyloids   pp303 - 309 Caroline M. Rufo, Yurii S. Moroz, Olesia V. Moroz, Jan Stöhr, Tyler A. Smith et al. doi:10.1038/nchem.1894 Amyloid fibril formation is often catalysed by mature fibrils or other aggregates on the fibrillization pathway; however, fibrils cannot normally catalyse other chemical reactions. Here, small seven-residue peptides designed from first principles are shown to form amyloid fibrils that can efficiently catalyse ester hydrolysis. See also: News and Views by Aumuller & Fandrich SnAP reagents for the one-step synthesis of medium-ring saturated N-heterocycles from aldehydes   pp310 - 314 Cam-Van T. Vo, Michael U. Luescher and Jeffrey W. Bode doi:10.1038/nchem.1878 The availability of facile cross-coupling protocols is sometimes blamed for the high occurrence of ‘flat’ aromatic molecules in drug-screening collections. Here, reagents are described that make possible the one-step transformation of aldehydes into medium-ring saturated N-heterocycles. The methodology has exceptional substrate scope and functional group tolerance and provides a route to heterocycles not easily prepared by other methods. Chemical compounds Stable GaX2, InX2 and TlX2 radicals   pp315 - 319 Andrey V. Protchenko, Deepak Dange, Jeffrey R. Harmer, Christina Y. Tang, Andrew D. Schwarz et al. doi:10.1038/nchem.1870 The chemistry of group 13 metals (M) is dominated by +1 and +3 oxidation states, so MX2 species are typically metal–metal-bonded dimers, M(II)2X4 or mixed-valence species M(I)M(III)X4. Now, monomeric M(II)(boryl)2 radicals have been prepared for gallium, indium and thallium. The compounds — structurally characterized by X-ray crystallography — are stable up to 130 °C and exhibit dominant metal-centred radical character. Chemical compounds Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol   pp320 - 324 Felix Studt, Irek Sharafutdinov, Frank Abild-Pedersen, Christian F. Elkjær, Jens S. Hummelshøj et al. doi:10.1038/nchem.1873 A Ni-Ga catalyst that reduces CO2 to methanol at ambient pressure has been discovered through a descriptor-based computational analysis, and has been shown experimentally to be particularly active and selective. This represents a first step towards the development of small-scale low-pressure processes for CO2 reduction to methanol from distributed hydrogen production. Copolymerization of carbon dioxide and butadiene via a lactone intermediate   pp325 - 331 Ryo Nakano, Shingo Ito and Kyoko Nozaki doi:10.1038/nchem.1882 Radical polymerization of a metastable lactone intermediate — formed from carbon dioxide and butadiene using a palladium catalyst — produces a high-CO2-content (29 wt%) polymer. This approach circumvents the thermodynamic and kinetic barriers typically associated with direct copolymerization of carbon dioxide and olefins, and can also be applied to one-pot co- and terpolymerization of carbon dioxide and 1,3-butadienes. Chemical compounds See also: News and Views by Dove Observation of the isotope effect in sub-kelvin reactions   pp332 - 335 Etay Lavert-Ofir, Yuval Shagam, Alon B. Henson, Sasha Gersten, Jacek Klos et al. doi:10.1038/nchem.1857 In cold chemistry, quantum phenomena in reactants' translational motion lead to the temporary trapping of reactants in a collisional complex. It is now shown that this metastable complex is responsible for a dramatic quantum kinetic isotope effect as observed in Penning ionization reactions at low temperatures. See also: News and Views by Brouard The oxidative inactivation of FeFe hydrogenase reveals the flexibility of the H-cluster   pp336 - 342 Vincent Fourmond, Claudio Greco, Kateryna Sybirna, Carole Baffert, Po-Hung Wang et al. doi:10.1038/nchem.1892 FeFe hydrogenases, the enzymes that oxidize or produce H2, are inactivated under oxidizing conditions. Here, it is shown that this inactivation results from H2 binding to coordination positions that are normally blocked by intrinsic CO ligands. This flexibility of the active site prevents irreversible oxidative damage. Side-chain control of porosity closure in single- and multiple-peptide-based porous materials by cooperative folding   pp343 - 351 C. Martí-Gastaldo, D. Antypov, J. E. Warren, M. E. Briggs, P. A. Chater et al. doi:10.1038/nchem.1871 A family of dipeptide-based metal–organic frameworks has been shown to respond to the presence of guests in a cooperative manner controlled by one amino acid residue. When the linker features a serine residue, guest removal enables the formation of hydrogen bonds between the residue's side-chains, causing a conformational change that closes the MOF's porous domain. Palladium-triggered deprotection chemistry for protein activation in living cells   pp352 - 361 Jie Li, Juntao Yu, Jingyi Zhao, Jie Wang, Siqi Zheng et al. doi:10.1038/nchem.1887 Restoring a protein's function in response to specific stimuli can enable a signalling pathway to be activated and the effect monitored over time. Here, a chemical rescue strategy for restoring protein function inside live cells is described, in which palladium catalysts are used to deprotect a propargylcarbamate group of a lysine analogue. Time-resolved observations of water oxidation intermediates on a cobalt oxide nanoparticle catalyst   pp362 - 367 Miao Zhang, Moreno de Respinis and Heinz Frei doi:10.1038/nchem.1874 The conversion of water to oxygen is an essential process for both natural and artificial photosynthesis. Important intermediates in the stepwise mechanism of water oxidation on the surface of cobalt oxide have now been spectroscopically identified, providing key insights for the development of higher-efficiency catalysts made from Earth-abundant materials. Addendum Top Addendum: Discrimination of epimeric glycans and glycopeptides using IM-MS and its potential for carbohydrate sequencing   p368 P. Both, A. P. Green, C. J. Gray, R. Sardzik, J. Voglmeir et al. doi:10.1038/nchem.1901 In Your Element Top Extricating erbium   p370 Claude Piguet doi:10.1038/nchem.1908 Claude Piguet reflects on the history of erbium, which is very much intertwined with its rare earth cousins yttrium, ytterbium and terbium. 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