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August 2018 Volume 10, Issue 8

News & Views
Amendments & Corrections
In Your Element



Abiogenesis and the reverse Hofmeister effect    pp797 - 798
Bruce C. Gibb

News & Views


The naked truth about K+ selectivity    pp799 - 800
Ben Corry

Scissoring genes with light    pp800 - 801
Aleksandar P. Ivanov & Joshua B. Edel

Optimizing orthogonality    pp802 - 803
William S. C. Ngai & Peng R. Chen

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Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process    pp804 - 812
Irina Yarulina, Kristof De Wispelaere, Simon Bailleul, Joris Goetze, Mike Radersma et al.

As of yet, no clear structure–performance descriptors have been developed to tune the catalytic activity of zeolitic methanol-to-olefin catalysts. Now it has been shown that introducing Lewis acidity into Brønsted acidic zeolites boosts their performance. Although Brønsted acidity is found to define propylene selectivity, Lewis acidity is responsible for prolonging lifetime.



Direct knock-on of desolvated ions governs strict ion selectivity in K+ channels    pp813 - 820
Wojciech Kopec, David A. Köpfer, Owen N. Vickery, Anna S. Bondarenko, Thomas L. C. Jansen et al.

That K+ channels conduct K+ ions at near-diffusion limited rates, but block the passage of smaller Na+ ions, creates an apparent contradiction. Now, atomistic simulations and free-energy calculations are used to show that both K+ permeation and ion selectivity are governed by the direct knock-on of completely desolvated ions in the channels’ selectivity filter.



Site-selective photoinduced cleavage and profiling of DNA by chiral semiconductor nanoparticles    pp821 - 830
Maozhong Sun, Liguang Xu, Aihua Qu, Peng Zhao, Tiantian Hao et al.

Genome editing relies on engineered nucleases to change an organism’s DNA, but has not yet been achieved using abiotic materials. Now, chiral cysteine-capped CdTe nanoparticles are found to specifically recognize and, following photoirradiation, cut between bases T and A at the GATATC restriction site in DNA with over 90 base pairs.



Mutually orthogonal pyrrolysyl-tRNA synthetase/tRNA pairs    pp831 - 837
Julian C. W. Willis & Jason W. Chin

Pyrrolysyl-tRNA synthetase(PylRS)/PyltRNACUA pairs that lack the N-terminal domain but are active and orthogonal are discovered, and pairs that are mutually orthogonal to existing PylRS/PyltRNACUA pairs are developed. Mutually orthogonal PylRS/PyltRNA pairs are combined to genetically encode the incorporation of distinct ncAAs into proteins synthesized in E. coli.



The domino hexadehydro-Diels–Alder reaction transforms polyynes to benzynes to naphthynes to anthracynes to tetracynes (and beyond?)    pp838 - 844
Xiao Xiao & Thomas R. Hoye

Properly designed polyyne substrates are shown to undergo efficient cascades of thermal cycloaddition reactions initiated by (rate-limiting) benzyne formation. Proceeding through naphthyne, anthracyne or tetracyne intermediates, rapid access to highly fused, polycyclic aromatic compounds can be achieved.



Infrared spectroscopy reveals multi-step multi-timescale photoactivation in the photoconvertible protein archetype dronpa    pp845 - 852
Sergey P. Laptenok, Agnieszka A. Gil, Christopher R. Hall, Andras Lukacs, James N. Iuliano et al.

Understanding the mechanism of photoconversion in fluorescent proteins is essential to optimizing applications in imaging and optogenetics. It has now been demonstrated that photoconversion in the photoswitchable protein dronpa follows a multi-step mechanism, with both chromophore and protein structural dynamics occurring on multiple timescales from picoseconds to hundreds of microseconds.



Polyyne formation via skeletal rearrangement induced by atomic manipulation    pp853 - 858
Niko Pavliček, Przemyslaw Gawel, Daniel R. Kohn, Zsolt Majzik, Yaoyao Xiong et al.

Atomic manipulation was used to control the reductive rearrangement of 1,1-dibromo alkenes to acetylenes on a NaCl surface at 5 K, and the stages of the reaction were visualized with atomic resolution using AFM. Polyynes ranging from triyne to octayne were prepared in this way, and STM was used to map their frontier orbitals and determine their transport gaps.



Non-aqueous homogenous biocatalytic conversion of polysaccharides in ionic liquids using chemically modified glucosidase    pp859 - 865
Alex P. S. Brogan, Liem Bui-Le & Jason P. Hallett

As a consequence of high chemical resistance and low solubility in conventional solvents, deconstructing biomass into fuels and other useful chemical building blocks remains a challenge. Now, through enzyme modification and ionic liquid solvents, it is possible to homogeneously biocatalytically convert cellulose to sugars at a rate 30 times greater than is achievable in water.



Complementary site-selectivity in arene functionalization enabled by overcoming the ortho constraint in palladium/norbornene catalysis    pp866 - 872


Electrophilic aromatic substitution (EAS) favours arene functionalization at positions meta to electron-withdrawing groups and para to electron-donating groups. Now, with a class of bridgehead-modified norbonene derivatives that can overcome the ortho constraint typical in palladium/norbornene catalysis, arene functionalization with site-selectivity complementary to EAS approaches can be achieved.



A human MUTYH variant linking colonic polyposis to redox degradation of the [4Fe4S]2+ cluster    pp873 - 880
Kevin J. McDonnell, Joseph A. Chemler, Phillip L. Bartels, Elizabeth O’Brien, Monica L. Marvin et al.

The [4Fe4S]2+ cluster-containing DNA-repair enzyme MUTYH helps safeguard the integrity of Watson–Crick base pairing and the human genetic code. The MUTYH [4Fe4S]2+ cluster mediates DNA redox signalling and DNA lesion identification. Now, a MUTYH pathologic variant associated with catastrophic [4Fe4S]2+ cluster redox degradation, impairment of DNA signalling and human colonic tumorigenesis has been identified.



Accelerating proton-coupled electron transfer of metal hydrides in catalyst model reactions    pp881 - 887
Tianfei Liu, Meiyuan Guo, Andreas Orthaber, Reiner Lomoth, Marcus Lundberg et al.

A series of tungsten hydride complexes have been synthesized to mimic a proton-coupled electron transfer (PCET) step undergone by metal–hydride intermediates during solar fuel catalysis. It is shown that, by incorporating proton-accepting bases into the second coordination sphere, their PCET oxidation mechanism changes and its rate increases by several orders of magnitude.



Approaching sub-ppm-level asymmetric organocatalysis of a highly challenging and scalable carbon–carbon bond forming reaction    pp888 - 894
Han Yong Bae, Denis Höfler, Philip S. J. Kaib, Pinar Kasaplar, Chandra Kanta De et al.

Chiral tertiary aldols are encountered in a variety of biologically relevant molecules. Making these valuable compounds directly from unbiased ketones has proven to be extremely challenging. Now it has been shown that sub-ppm levels of in situ generated silylium-based organic Lewis acid catalysts can give quantitative product formation in very high enantiopurity through a Mukaiyama aldol reaction.



Amendments & Corrections


Author Correction: Hidden hassium    p895
Michael A. Tarselli

Author Correction: Dynamic actuation of glassy polymersomes through isomerization of a single azobenzene unit at the block copolymer interface    p895
Mijanur Rahaman Molla, Poornima Rangadurai, Lucas Antony, Subramani Swaminathan, Juan J. de Pablo et al.

Author Correction: Foldamers wave to the ribosome    p896
Alanna Schepartz

Publisher Correction: Structure–performance descriptors and the role of Lewis acidity in the methanol-to-propylene process    p897
Irina Yarulina, Kristof De Wispelaere, Simon Bailleul, Joris Goetze, Mike Radersma et al.

In Your Element


The realities of radium    p898
Vikki Cantrill

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