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Nature Chemistry Contents September 2017 Volume 9 Number 9 pp 831 - 924

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Nature Reviews Chemistry is an online-only journal that provides both an introduction to chemists embarking on a new topic of investigation and thought-provoking, in-depth sections for the expert. The journal also publishes regular columns which focus on the teaching of chemistry and on the translation of research into business opportunities.

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TABLE OF CONTENTS

September 2017 Volume 9, Issue 9

Editorial
Interview
News and Views
Articles
In Your Element
 
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Editorial

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The bottom line   p831
doi:10.1038/nchem.2860
Our understanding of actinide chemistry lags behind that of the rest of the periodic table. A collection of articles in this issue highlights recent progress featuring uranium(VI) dianions bearing four U-N multiple bonds, berkelium(IV) stabilized in solution and delocalization of 5f electrons in a plutonium material.
 

Interview

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Bonding with actinides   p832
Anne Pichon
doi:10.1038/nchem.2855
Suzanne Bart from Purdue University talks to Nature Chemistry about her investigations into the chemistry of actinides, and why she finds them both challenging and rewarding.
 

News and Views

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Supported liquid metal catalysts: Popping up to the surface   pp833 - 834
Günther Rupprechter
doi:10.1038/nchem.2849
Merging the advantages of homogeneous and heterogeneous catalysts is a useful strategy for creating improved catalytic systems. Now, a concept has been developed that uses single Pd atoms — supported within liquid alloy droplets — that emerge from the droplet subsurface and interior to react with molecules approaching from the gas phase.

See also: Article by Taccardi et al.

Organometallic mechanisms: Measuring up with the early metals   pp834 - 836
Ian A. Tonks
doi:10.1038/nchem.2851
Mathematically modelling metal-ligand bonding in late transition-metal complexes has been an important tool in catalyst development — although lacking for early transition metals such as Cr and Ti. Now, a simple method for measuring ligand donor properties promises to elevate high-valent early transition metal catalysis to the same level.

See also: Article by Billow et al.

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Nature Reviews Materials is an online-only, materials science journal that provides an accurate and balanced discussion on a chosen topic, together with an authoritative voice from experienced researchers. Spanning physics, chemistry, biology and engineering, the journal publishes a broad range of Reviews and Comments from world-leading scientists.

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Articles

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Quantifying ligand effects in high-oxidation-state metal catalysis   pp837 - 842
Brennan S. Billow, Tanner J. McDaniel and Aaron L. Odom
doi:10.1038/nchem.2843



Catalysis involving high-valent metals is an important facet of modern chemistry, but tools for catalyst development in this field have lagged behind those for low-valent systems. Now, an experimental system that can accurately model and predict reactivity has been developed to aid high-valent catalyst design.
Chemical compounds
See also: News and Views by Tonks

Chelation and stabilization of berkelium in oxidation state +IV   pp843 - 849
Gauthier J.-P. Deblonde, Manuel Sturzbecher-Hoehne, Peter B. Rupert, Dahlia D. An, Marie-Claire Illy et al.
doi:10.1038/nchem.2759



Berkelium is the only transplutonium element predicted to be able to exhibit both +III and +IV oxidation states in solution. Bk(IV) has now been stabilized through chelation with a siderophore derivative. The resulting neutral coordination compound was characterized and compared with the negatively charged species obtained by chelation of neighbouring trivalent actinides.
Chemical compounds

Elucidating bonding preferences in tetrakis(imido)uranate(VI) dianions   pp850 - 855
Nickolas H. Anderson, Jing Xie, Debmalya Ray, Matthias Zeller, Laura Gagliardi et al.
doi:10.1038/nchem.2767



The field of high-valent uranium chemistry has been dominated by the linear uranyl moiety [UO2]2+ and its imido analogues. A family of tetrakis(imido)uranate dianions has now been developed that displays four uranium–nitrogen multiple bonds. Their geometry is dictated by cation coordination and steric factors rather than electronic ones.
Chemical compounds

Incipient class II mixed valency in a plutonium solid-state compound   pp856 - 861
Samantha K. Cary, Shane S. Galley, Matthew L. Marsh, David L. Hobart, Ryan E. Baumbach et al.
doi:10.1038/nchem.2777



Unlike in the d block, intervalence charge transfer is rare in the 5f block owing to localized valence electrons and poor overlap between metal and ligand orbitals. Delocalization of 5f electrons has now been observed in a Pu(III)/Pu(IV)–pyridinedicarboxylate solid-state compound. It occurs through metal-to-ligand charge transfer with both plutonium centres.
 

Gallium-rich Pd–Ga phases as supported liquid metal catalysts   pp862 - 867
N. Taccardi, M. Grabau, J. Debuschewitz, M. Distaso, M. Brandl et al.
doi:10.1038/nchem.2822



Creating systems that merge some of the advantages of both heterogeneous and molecular catalysis is a useful approach to developing improved catalysts. Following this strategy, a liquid mixture of gallium and palladium supported on porous glass has now been shown to form an active catalyst for alkane dehydrogenation that is resistant to coke formation and is thus highly stable.

See also: News and Views by Rupprechter

Visible-light excitation of iminium ions enables the enantioselective catalytic β-alkylation of enals   pp868 - 873
Mattia Silvi, Charlie Verrier, Yannick P. Rey, Luca Buzzetti and Paolo Melchiorre
doi:10.1038/nchem.2748



Chiral iminium ions generated from an amine catalyst and enals are key organocatalytic intermediates in thermal asymmetric processes. Now, visible-light excitation of these iminium ions can turn these compounds into strong oxidants to enable enantioselective photochemical β-alkylations of enals with silanes, which are unachievable via conventional ground state pathways.
Chemical compounds

A 31-residue peptide induces aggregation of tau's microtubule-binding region in cells   pp874 - 881
Jan Stöhr, Haifan Wu, Mimi Nick, Yibing Wu, Manasi Bhate et al.
doi:10.1038/nchem.2754



The self-propagation of misfolded conformations of tau occurs in neurodegenerative diseases, including Alzheimer's disease. The microtubule-binding region, tau244-372, reproduces much of the aggregation behaviour of tau in cells and animal models. Now, it has been shown that a 31-residue peptide from tau's R3 domain forms a cross-β conformation that efficiently seeds aggregation of tau244-372 in cells.
 

Solvent-switchable continuous-breathing behaviour in a diamondoid metal–organic framework and its influence on CO2 versus CH4 selectivity   pp882 - 889
Elliot J. Carrington, Craig A. McAnally, Ashleigh J. Fletcher, Stephen P. Thompson, Mark Warren et al.
doi:10.1038/nchem.2747



Breathing metal–organic frameworks (MOFs) are functional materials whose molecular-scale pores can reversibly open and close. In contrast to typical defined structural transitions, continuous breathing has now been observed for a diamondoid MOF. Removal of two different solvents leads to two desolvated MOF polymorphs with dramatically different porosities and gas uptake properties, including CO2/CH4 selectivities. Partial desolvation introduces pressure-gated CO2 adsorption.
 

The structure and binding mode of citrate in the stabilization of gold nanoparticles   pp890 - 895
Hind Al-Johani, Edy Abou-Hamad, Abdesslem Jedidi, Cory M. Widdifield, Jasmine Viger-Gravel et al.
doi:10.1038/nchem.2752



The manner in which carboxylates bind to the surface of nanoparticles has been an important question in materials science. Now, multinuclear magnetic resonance experiments — alongside DFT calculations, XPS and TEM measurements — have elucidated the three-dimensional ligand structures of gold nanoparticles capped with various ratios of carboxylate-containing ligands, and enabled the determination of the most probable binding modes.
 

Iterative assembly line synthesis of polypropionates with full stereocontrol   pp896 - 902
Teerawut Bootwicha, Julian M. Feilner, Eddie L. Myers and Varinder K. Aggarwal
doi:10.1038/nchem.2757



Polypropionates can be grown — one carbon atom at a time — using the iterative homologation of boronic esters. This assembly line strategy was enabled through the use of enantioenriched lithiated a-chlorosilanes as masked carbinol units. Polypropionates were obtained in a fully stereocontrolled manner, including the stereochemically challenging anti–anti isomers.
Chemical compounds

Stereochemical plasticity modulates cooperative binding in a CoII12L6 cuboctahedron   pp903 - 908
Felix J. Rizzuto and Jonathan R. Nitschke
doi:10.1038/nchem.2758



An interconverting system of three distinct stereoisomers of a cuboctahedral CoII-based cage is able to regulate the binding affinities of large anionic guests. Through cooperative templation with fullerene guests, the cage converts into a desymmetrized cage that in turn exhibits positive cooperativity in binding of an icosahedral anion; this interaction is anti-cooperative in the fullerene-free parent.
 

Tyrosine sulfation modulates activity of tick-derived thrombin inhibitors   pp909 - 917
Robert E. Thompson, Xuyu Liu, Jorge Ripoll-Rozada, Noelia Alonso-García, Benjamin L. Parker et al.
doi:10.1038/nchem.2744



Tyrosine sulfation strongly enhances the inhibition of thrombin by the tick-derived anticoagulants madanin-1 and chimadanin. Protein chemical synthesis and structural studies have revealed a mode of inhibition that is unprecedented among cysteine-free anticoagulant proteins. This inhibition occurs through the recognition of the highly basic exosite II of thrombin.
 

Chlorodifluoromethane-triggered formation of difluoromethylated arenes catalysed by palladium   pp918 - 923
Zhang Feng, Qiao-Qiao Min, Xia-Ping Fu, Lun An and Xingang Zhang
doi:10.1038/nchem.2746



Chlorodifluoromethane (ClCF2H), an inexpensive and abundant industrial raw material, represents an ideal and straightforward reagent for introducing the difluoromethyl group. However, efficient approaches for activation of the typically inert ClCF2H are limited. Now, ClCF2H is employed via a difluorocarbene pathway for palladium-catalysed difluoromethylation of arylboronic acids with broad substrate scope.
Chemical compounds

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In Your Element

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Peaceful berkelium   p924
Andreas Trabesinger
doi:10.1038/nchem.2845
The first new element produced after the Second World War has led a rather peaceful life since entering the period table — until it became the target of those producing superheavy elements, as Andreas Trabesinger describes.
 

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