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Nature Chemistry Contents July 2017 Volume 9 Number 6 pp 603 - 724

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Nature Chemistry


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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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TABLE OF CONTENTS

July 2017 Volume 9, Issue 7

Editorial
Thesis
News and Views
Articles
Erratum
Addendum
In Your Element
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Editorial

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A chemical century   p603
doi:10.1038/nchem.2815
The launch of Nature Chemistry in 2009 prompted some criticism of journal proliferation, but 100 issues later this young offender has matured into an accepted part of the publishing landscape.

Thesis

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Pasteur and the art of chirality   pp604 - 605
Joseph Gal
doi:10.1038/nchem.2790
Louis Pasteur was a scientific giant of the nineteenth century, but, as Joseph Gal asks, was his most famous contribution to the understanding of chemistry — chirality — influenced more by his artistic talents?

Identity crisis   pp606 - 607
Michelle Francl
doi:10.1038/nchem.2807
Michelle Francl reminds us that you don't need to look like Einstein to be a scientist.

News and Views

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Polycyclic aromatic hydrocarbons: Synthesis successes   pp608 - 609
Roser Valentí and Stephen M. Winter
doi:10.1038/nchem.2799
Disentangling the chemistry and physics behind reported unconventional superconductivity and exotic magnetism in alkali-intercalated PAHs has remained problematic due to the lack of phase-pure samples. Two synthetic pathways have now remedied this issue, facilitating studies of cooperative electronic properties based on carbon π-electrons.

See also: Article by Takabayashi et al. | Article by Romero et al.

Enzymatic catalysis: New functional twists for P450s   pp609 - 611
Rudi Fasan
doi:10.1038/nchem.2810
Two papers provide insight into the reactivity of cytochrome P450s. A direct link between electron donation and reactivity has been shown with a selenocysteine-ligated P450 compound I, whereas a serine-ligated P450 (P411) has been engineered to catalyse an intermolecular C–H amination via nitrene transfer.

See also: Article by Onderko et al. | Article by Prier et al.

DNA nanotechnology: Bringing lipid bilayers into shape   pp611 - 613
Stefan Howorka
doi:10.1038/nchem.2809
Lipid bilayers form the thin and floppy membranes that define the boundary of compartments such as cells. Now, a method to control the shape and size of bilayers using DNA nanoscaffolds has been developed. Such designer materials advance synthetic biology and could find use in membrane research.

See also: Article by Zhang et al.

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Articles

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Cooperative polymerization of α-helices induced by macromolecular architecture   pp614 - 622
Ryan Baumgartner, Hailin Fu, Ziyuan Song, Yao Lin and Jianjun Cheng
doi:10.1038/nchem.2712



The secondary and tertiary structure of a protein has profound implications on function and catalysis. Now, both the secondary and tertiary structures of a synthetic polymer have been utilized to catalyse the polymerization of N-carboxyanhydrides. Both the folding of the resulting polypeptides into α-helices and their macromolecular organization dramatically enhance the polymerization rate.

Characterization of a selenocysteine-ligated P450 compound I reveals direct link between electron donation and reactivity   pp623 - 628
Elizabeth L. Onderko, Alexey Silakov, Timothy H. Yosca and Michael T. Green
doi:10.1038/nchem.2781



The oxidative prowess of cytochrome P450s has been suggested to stem from the electron-donating axial ligand. Now, a selenocysteine-ligated P450 compound I has been trapped and characterized providing an avenue to examine this hypothesis. Measurements reveal that the selenolate-ligated compound I cleaves C–H bonds more rapidly than the wild-type equivalent.

See also: News and Views by Fasan

Enantioselective, intermolecular benzylic C–H amination catalysed by an engineered iron-haem enzyme   pp629 - 634
Christopher K. Prier, Ruijie K. Zhang, Andrew R. Buller, Sabine Brinkmann-Chen and Frances H. Arnold
doi:10.1038/nchem.2783



The intermolecular amination of C–H bonds is an enabling transformation for the synthesis of nitrogen-containing molecules; however, developing catalysts for this class of reactions is very challenging. Now, an iron-based enzyme for this reaction has been engineered, demonstrating that a protein can confer a difficult new function upon an otherwise unreactive base metal.

See also: News and Views by Fasan

π-electron S = ½ quantum spin-liquid state in an ionic polyaromatic hydrocarbon   pp635 - 643
Yasuhiro Takabayashi, Melita Menelaou, Hiroyuki Tamura, Nayuta Takemori, Takashi Koretsune et al.
doi:10.1038/nchem.2764



Cooperative electronic properties that arise purely from carbon π-electrons can lead to unconventional superconductivity and quantum magnetism. New packing architectures have now been established in two caesium-intercalated polyaromatic hydrocarbons, CsPhenanthrene and Cs2Phenanthrene, both strongly correlated multi-orbital Mott insulators. The frustrated magnetic topology in CsPhenanthrene also renders it a spin-½ quantum spin liquid candidate.

See also: Article by Romero et al. | News and Views by Valenti & Winter

Redox-controlled potassium intercalation into two polyaromatic hydrocarbon solids   pp644 - 652
F. Denis Romero, M. J. Pitcher, C. I. Hiley, G. F. S. Whitehead, S. Kar et al.
doi:10.1038/nchem.2765



Reports of superconductivity in KxPicene spurred interest in alkali-intercalated polyaromatic hydrocarbon (PAH) compounds, but their compositions and structures have remained unclear. Now crystalline K2Pentacene and K2Picene — neither of which are superconducting — have been prepared by mild synthesis. Structural analysis shows that the cation sites arise within the molecular layers from reorientation of the PAHs within a herringbone packing.

See also: Article by Takabayashi et al. | News and Views by Valenti & Winter

Placing and shaping liposomes with reconfigurable DNA nanocages   pp653 - 659
Zhao Zhang, Yang Yang, Frederic Pincet, Marc C. Llaguno and Chenxiang Lin
doi:10.1038/nchem.2802



Controlling liposome shape, arrangement and dynamics is important for biophysical studies and synthetic biology applications. Now, using a family of reconfigurable DNA nanocages as templates, spherical, tubular, toroidal and helical liposomes with predefined geometry have been produced. DNA-guided membrane fusion and bending is also demonstrated.

See also: News and Views by Howorka

Probing the early stages of photoreception in photoactive yellow protein with ultrafast time-domain Raman spectroscopy   pp660 - 666
Hikaru Kuramochi, Satoshi Takeuchi, Kento Yonezawa, Hironari Kamikubo, Mikio Kataoka et al.
doi:10.1038/nchem.2717



Photoreceptors play an essential role in determining the fate of subsequent biological reactions, however, tracking their structural evolution on ultrafast timescales has been challenging. Now, photoactive yellow protein has been studied using time-domain Raman spectroscopy with sub-7-femtosecond pulses, revealing the ultrafast rearrangement of its hydrogen-bonding structure and also the structure of the first photocycle intermediate.

A synthetic ion transporter that disrupts autophagy and induces apoptosis by perturbing cellular chloride concentrations   pp667 - 675
Nathalie Busschaert, Seong-Hyun Park, Kyung-Hwa Baek, Yoon Pyo Choi, Jinhong Park et al.
doi:10.1038/nchem.2706



A squaramide-based anion transporter has now been shown to cause changes in the lysosomal pH leading to impairment of lysosomal enzyme activity and disruption of autophagic processes. The study provides the first experimental evidence that synthetic ion transporters can both disrupt autophagy and induce apoptosis.

One-thousand-fold enhancement of high field liquid nuclear magnetic resonance signals at room temperature   pp676 - 680
Guoquan Liu, Marcel Levien, Niels Karschin, Giacomo Parigi, Claudio Luchinat et al.
doi:10.1038/nchem.2723



The analysis of complex (bio)molecules by NMR spectroscopy is often complicated by limitations in sensitivity. Now, it has been shown that 13C NMR signals are strongly enhanced in solution by resonant microwave irradiation of a nitroxide polarizer. This method exhibits up to one-thousand-fold improvements in sensitivity, which stands to greatly improve the detail with which small molecules and metabolites can be studied.

Rapid heteroatom transfer to arylmetals utilizing multifunctional reagent scaffolds   pp681 - 688
Hongyin Gao, Zhe Zhou, Doo-Hyun Kwon, James Coombs, Steven Jones et al.
doi:10.1038/nchem.2672



The direct transfer of primary amino and hydroxyl groups to arylmetals in a scalable and environmentally friendly fashion remains a formidable synthetic challenge. Here, it is demonstrated that bench-stable N–H and N–alkyl oxaziridines can be used as efficient multifunctional reagents, without deprotonation, for the direct primary amination and hydroxylation of (hetero)arylmetals.
Chemical compounds

Hypersensitive dual-function luminescence switching of a silver-chalcogenolate cluster-based metal–organic framework   pp689 - 697
Ren-Wu Huang, Yong-Sheng Wei, Xi-Yan Dong, Xiao-Hui Wu, Chen-Xia Du et al.
doi:10.1038/nchem.2718



The properties of discrete species can sometimes be improved by fixing them into extended materials. This strategy has now been applied to silver(I) chalcogenide/chalcogenolate clusters, resulting in a metal–organic framework with enhanced stability and fluorescent sensing capabilities. Crystallographic analysis allows precise structural determination of guest binding, which is responsible for both emission turn-off and multicoloured turn-on.

Post-translational modification of ribosomally synthesized peptides by a radical SAM epimerase in Bacillus subtilis   pp698 - 707
Alhosna Benjdia, Alain Guillot, Pauline Ruffié, Jérôme Leprince and Olivier Berteau
doi:10.1038/nchem.2714



Radical SAM enzymes are versatile enzymes catalysing chemically challenging reactions. Now, a radical SAM enzyme that post-translationally modifies ribosomally synthesized peptides to contain D-amino acids has been discovered in Bacillus subtilis, and its mechanism has been deciphered. These peptides, called epipeptides, efficiently inhibit bacterial growth.

Observation of electron-transfer-mediated decay in aqueous solution   pp708 - 714
Isaak Unger, Robert Seidel, Stephan Thürmer, Marvin N. Pohl, Emad F. Aziz et al.
doi:10.1038/nchem.2727



Electron-transfer-mediated decay (ETMD) is a recently discovered type of electronic relaxation that involves the refilling of a core hole by an electron from a neighbouring species. It has now been observed in LiCl solution, when previously it had only been seen in rare-gas clusters. Spectra generated during ETMD are observed to be sensitive to the immediate environment of the initially ionized ion.

A polymer nanoparticle with engineered affinity for a vascular endothelial growth factor (VEGF165)   pp715 - 722
Hiroyuki Koide, Keiichi Yoshimatsu, Yu Hoshino, Shih-Hui Lee, Ai Okajima et al.
doi:10.1038/nchem.2749



Abiotic hydrogel polymer nanoparticles with affinity for a key vascular endothelial growth factor (VEGF165) have now been developed. This high-protein affinity was engineered by carefully controlling the amount and the substitution pattern of sulfated N-acetylglucosamines and the inclusion of a hydrophobic group in the monomer.

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Addendum

Top

Addendum: Aldehydes as alkyl carbanion equivalents for additions to carbonyl compounds   p723
Haining Wang, Xi-Jie Dai and Chao-Jun Li
doi:10.1038/nchem.2805

In Your Element

Top

Frantically forging fermium   p724
Brett F. Thornton and Shawn C. Burdette
doi:10.1038/nchem.2806
Brett F. Thornton and Shawn C. Burdette relate how element 100 was first identified in a nuclear weapons test, but that was classified information, so researchers had to 'discover' it again using other methods.

Erratum

Top

Erratum: Tuning underwater adhesion with cation-π interactions   p723
Matthew A. Gebbie, Wei Wei, Alex M. Schrader, Thomas R. Cristiani, Howard A. Dobbs et al.
doi:10.1038/nchem.2813

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