Friday, June 22, 2018

Nature Chemistry Contents July 2018 Volume 10 Number 7 pp 687 - 786

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July 2018 Volume 10, Issue 7

News & Views
Amendments & Corrections
In Your Element

Calls for nominations: 2018
John Maddox Prize for Standing up for Science

Recognising the work of individuals who promote science in the face of hostility 

KACST Impact

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Ring binders    p687



Talking to Pauling’s ghost    pp688 - 689
Michelle Francl

Nature Spotlight on Hong Kong: building science innovation 

Hong Kong is maximising major scientific innovation and commercial benefits through its proximity to the research and development hubs in mainland China. Yet barriers to collaboration remain.

Access the full supplement for more 



Looking in the library    pp690 - 691
Russell Johnson

News & Views


Shaping molecular diversity    pp692 - 694
Emil S. Iqbal & Matthew C. T. Hartman

2D materials worth their salt    pp694 - 695
Artem R. Oganov

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Amino-acid-encoded biocatalytic self-assembly enables the formation of transient conducting nanostructures    pp696 - 703
Mohit Kumar, Nicole L. Ing, Vishal Narang, Nadeesha K. Wijerathne, Allon I. Hochbaum et al.

Amino acids have now been used as chemical inputs to provide control over self-assembly in semiconducting structures. This approach enables temporal control over the formation of nanostructures and consequently control over their transient electronic conductivity.



Second-generation DNA-templated macrocycle libraries for the discovery of bioactive small molecules    pp704 - 714
Dmitry L. Usanov, Alix I. Chan, Juan Pablo Maianti & David R. Liu

A second-generation DNA-templated library of 256,000 small-molecule macrocycles has been developed. The improved method was created by streamlining and integrating multiple aspects of DNA-encoded and DNA-templated library synthesis methodology. In vitro selection of the macrocycle library against insulin-degrading enzyme enabled the discovery of potent inhibitors.



Cyclization of peptides with two chemical bridges affords large scaffold diversities    pp715 - 723
Sangram S. Kale, Camille Villequey, Xu-Dong Kong, Alessandro Zorzi, Kaycie Deyle et al.

Crosslinking within peptides containing two pairs of cysteines to form chemical bridges has now been shown to provide rapid access to thousands of different macrocyclic scaffolds in libraries that are easy to synthesize, screen and decode. Applying this strategy to phage-encoded libraries yielded binders with remarkable affinities despite the small molecular mass.



Cyclometallated ruthenium catalyst enables late-stage directed arylation of pharmaceuticals    pp724 - 731
Marco Simonetti, Diego M. Cannas, Xavier Just-Baringo, Iñigo J. Vitorica-Yrezabal & Igor Larrosa

Nearly two decades after its discovery, the Ru(II)-catalysed C–H arylation of N-chelating aromatics with aryl halides was reinvestigated and a new key reaction intermediate was uncovered. A thorough mechanistic elucidation has now led to the development of a new class of catalysts with unique efficacy towards late-stage arylation of ‘real-world’ compounds.



Engineering the entropy-driven free-energy landscape of a dynamic nanoporous protein assembly    pp732 - 739
Robert Alberstein, Yuta Suzuki, Francesco Paesani & F. Akif Tezcan

Living systems rely on externally tuneable and stimuli-responsive conformational changes of proteins and protein assemblies for a wide range of essential functions. A combination of experimental and computational analyses has now enabled the fabrication of a rationally designed, synthetic, stimuli-responsive protein assembly through modulation of its free-energy landscape.



Shape-preserving transformation of carbonate minerals into lead halide perovskite semiconductors based on ion exchange/insertion reactions    pp740 - 745
Tim Holtus, Lukas Helmbrecht, Hans C. Hendrikse, Iaroslav Baglai, Sophie Meuret et al.

Biominerals feature unique and potentially useful three-dimensional structures but are often difficult to transform into functional materials. Now, a two-step ion exchange/insertion reaction has been shown to convert synthetic carbonate salts and calcium carbonate biominerals into lead halide perovskites with tunable optoelectronic properties while preserving the shapes and microstructures of the precursors.



A molecular multi-gene classifier for disease diagnostics    pp746 - 754
Randolph Lopez, Ruofan Wang & Georg Seelig

Gene expression profiling remains cost-prohibitive and challenging to implement in a clinical setting. Now, a molecular computation strategy for classifying complex gene expression signatures has been developed. Classification occurs through a series of molecular interactions between RNA inputs and engineered DNA probes designed to implement a relevant linear classification model.



Controlling Pd(iv) reductive elimination pathways enables Pd(ii)-catalysed enantioselective C(sp3)−H fluorination    pp755 - 762
Hojoon Park, Pritha Verma, Kai Hong & Jin-Quan Yu

Metal-catalysed enantioselective fluorination of C(sp3)–H bonds is an attractive method for preparing chiral organofluorines, but the challenge of achieving both enantioselectivity and reductive elimination selectivity remains unsolved. Now, it has been demonstrated that a chiral amino amide transient directing group can serve as a ligand for a palladium catalyst that promotes both enantioselective C(sp3)–H insertion and C(sp3)–F-selective reductive elimination.



Harvesting multiple electron–hole pairs generated through plasmonic excitation of Au nanoparticles    pp763 - 769
Youngsoo Kim, Jeremy G. Smith & Prashant K. Jain

Multi-electron redox reactions are kinetically sluggish; however, plasmonic nanoparticles have shown promise as multi-electron reduction catalysts. Now, the principles that govern the harvesting of multiple electron–hole pairs from plasmonically excited gold nanoparticle photocatalysts are elucidated, providing a general foundation for the plasmonic catalysis of challenging multi-electron, multi-proton chemistry, such as N2 fixation and CO2 reduction.



Catalytic promiscuity enabled by photoredox catalysis in nicotinamide-dependent oxidoreductases    pp770 - 775
Kyle F. Biegasiewicz, Simon J. Cooper, Megan A. Emmanuel, David C. Miller & Todd K. Hyster

Enzymes are powerful catalysts for chemical synthesis because they are capable of providing unparalleled levels of selectivity; however, in nature they only catalyse a limited collection of reactions. Now, it has been shown that non-natural reactions that proceed via free-radical intermediates can be catalysed with high selectivity by using an exogenous photoredox catalyst in conjunction with enzymes.



Two-dimensional Na–Cl crystals of unconventional stoichiometries on graphene surface from dilute solution at ambient conditions    pp776 - 779
Guosheng Shi, Liang Chen, Yizhou Yang, Deyuan Li, Zhe Qian et al.

The common form of salt has a 1:1 ratio of Na+ and Cl; however, species that deviate from this can be found under extreme conditions, such as high pressure. Now, as a result of cation–π interactions that promote ion–surface adsorption, Na2Cl and Na3Cl have been observed as two-dimensional crystals on graphene at ambient conditions.



Identification and characterization of diverse coherences in the Fenna–Matthews–Olson complex    pp780 - 786
Erling Thyrhaug, Roel Tempelaar, Marcelo J. P. Alcocer, Karel Žídek, David Bína et al.

The implications of coherence signals for the transfer of energy within the Fenna–Matthews–Olson complex of photosynthetic green sulfur bacteria is a well debated topic. Now, polarization-controlled 2D spectroscopy — aided by vibronic exciton modelling — has enabled the characterization of all such coherences and determination of their physical origins; while electronic coherences dephase extremely rapidly, ground- and excited-state vibrational coherences dominate.



Enrichment-triggered prodrug activation demonstrated through mitochondria-targeted delivery of doxorubicin and carbon monoxide    pp787 - 794
Yueqin Zheng, Xingyue Ji, Bingchen Yu, Kaili Ji, David Gallo et al.

A new concept for targeted drug delivery based on enrichment triggered prodrug activation has been developed. Without enrichment, the activation reaction is sluggish; however, following enrichment, the increased concentration enhances the activation reaction rate, thereby leading to the release of the payload. The same approach can be used in antibody–drug conjugate applications.



Amendments & Corrections


Publisher Correction: Ribosomal synthesis and folding of peptide-helical aromatic foldamer hybrids    p795
Joseph M. Rogers, Sunbum Kwon, Simon J. Dawson, Pradeep K. Mandal, Hiroaki Suga et al.

In Your Element


The oganesson odyssey    p796
Kit Chapman

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