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Nature Chemistry

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https://www.readbyqxmd.com/read/28430205/controlled-membrane-translocation-provides-a-mechanism-for-signal-transduction-and-amplification
#1
Matthew J Langton, Flore Keymeulen, Maria Ciaccia, Nicholas H Williams, Christopher A Hunter
Transmission and amplification of chemical signals across lipid bilayer membranes is of profound significance in many biological processes, from the development of multicellular organisms to information processing in the nervous system. In biology, membrane-spanning proteins are responsible for the transmission of chemical signals across membranes, and signal transduction is often associated with an amplified signalling cascade. The ability to reproduce such processes in artificial systems has potential applications in sensing, controlled drug delivery and communication between compartments in tissue-like constructs of synthetic vesicles...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430203/photoredox-activation-of-carbon-dioxide-for-amino-acid-synthesis-in-continuous-flow
#2
Hyowon Seo, Matthew H Katcher, Timothy F Jamison
Although carbon dioxide (CO2) is highly abundant, its low reactivity has limited its use in chemical synthesis. In particular, methods for carbon-carbon bond formation generally rely on two-electron mechanisms for CO2 activation and require highly activated reaction partners. Alternatively, radical pathways accessed via photoredox catalysis could provide new reactivity under milder conditions. Here we demonstrate the direct coupling of CO2 and amines via the single-electron reduction of CO2 for the photoredox-catalysed continuous flow synthesis of α-amino acids...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430199/control-over-differentiation-of-a-metastable-supramolecular-assembly-in-one-and-two-dimensions
#3
Tomoya Fukui, Shinnosuke Kawai, Satoko Fujinuma, Yoshitaka Matsushita, Takeshi Yasuda, Tsuneaki Sakurai, Shu Seki, Masayuki Takeuchi, Kazunori Sugiyasu
Molecular self-assembly under kinetic control is expected to yield nanostructures that are inaccessible through the spontaneous thermodynamic process. Moreover, time-dependent evolution, which is reminiscent of biomolecular systems, may occur under such out-of-equilibrium conditions, allowing the synthesis of supramolecular assemblies with enhanced complexities. Here we report on the capacity of a metastable porphyrin supramolecular assembly to differentiate into nanofibre and nanosheet structures. Mechanistic studies of the relationship between the molecular design and pathway complexity in the self-assembly unveiled the energy landscape that governs the unique kinetic behaviour...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430197/g-quadruplex-organic-frameworks
#4
Yi-Lin Wu, Noah E Horwitz, Kan-Sheng Chen, Diego A Gomez-Gualdron, Norman S Luu, Lin Ma, Timothy C Wang, Mark C Hersam, Joseph T Hupp, Omar K Farha, Randall Q Snurr, Michael R Wasielewski
Two-dimensional covalent organic frameworks often π stack into crystalline solids that allow precise spatial positioning of molecular building blocks. Inspired by the hydrogen-bonded G-quadruplexes found frequently in guanine-rich DNA, here we show that this structural motif can be exploited to guide the self-assembly of naphthalene diimide and perylene diimide electron acceptors end-capped with two guanine electron donors into crystalline G-quadruplex-based organic frameworks, wherein the electron donors and acceptors form ordered, segregated π-stacked arrays...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430196/organocatalytic-stereoselective-8-2-and-6-4-cycloadditions
#5
Rasmus Mose, Gert Preegel, Jesper Larsen, Sofie Jakobsen, Eva Høgh Iversen, Karl Anker Jørgensen
Cycloadditions that involve more than six π electrons are termed higher-order cycloadditions and are an excellent tool for solving complex synthetic challenges, as they provide direct access to polycyclic scaffolds that contain medium-sized rings. They have interesting synthetic potential for the discovery of new bioactive molecules and in natural product synthesis. It is peculiar that stereocontrolled [8+2] and [6+4] cycloadditions have been largely neglected for the past 50 years. Here we demonstrate a cross-dienamine activation of 2-cyclopentenone and the unprecedented endocyclic linear-dienamine activation of 2-cyclohexenones and 2-cycloheptenones...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430195/a-stable-compound-of-helium-and-sodium-at-high-pressure
#6
Xiao Dong, Artem R Oganov, Alexander F Goncharov, Elissaios Stavrou, Sergey Lobanov, Gabriele Saleh, Guang-Rui Qian, Qiang Zhu, Carlo Gatti, Volker L Deringer, Richard Dronskowski, Xiang-Feng Zhou, Vitali B Prakapenka, Zuzana Konôpková, Ivan A Popov, Alexander I Boldyrev, Hui-Tian Wang
Helium is generally understood to be chemically inert and this is due to its extremely stable closed-shell electronic configuration, zero electron affinity and an unsurpassed ionization potential. It is not known to form thermodynamically stable compounds, except a few inclusion compounds. Here, using the ab initio evolutionary algorithm USPEX and subsequent high-pressure synthesis in a diamond anvil cell, we report the discovery of a thermodynamically stable compound of helium and sodium, Na2He, which has a fluorite-type structure and is stable at pressures >113 GPa...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430194/engineering-genetic-circuit-interactions-within-and-between-synthetic-minimal-cells
#7
Katarzyna P Adamala, Daniel A Martin-Alarcon, Katriona R Guthrie-Honea, Edward S Boyden
Genetic circuits and reaction cascades are of great importance for synthetic biology, biochemistry and bioengineering. An open question is how to maximize the modularity of their design to enable the integration of different reaction networks and to optimize their scalability and flexibility. One option is encapsulation within liposomes, which enables chemical reactions to proceed in well-isolated environments. Here we adapt liposome encapsulation to enable the modular, controlled compartmentalization of genetic circuits and cascades...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430193/self-propelled-supramolecular-nanomotors-with-temperature-responsive-speed-regulation
#8
Yingfeng Tu, Fei Peng, Xiaofeng Sui, Yongjun Men, Paul B White, Jan C M van Hest, Daniela A Wilson
Self-propelled catalytic micro- and nanomotors have been the subject of intense study over the past few years, but it remains a continuing challenge to build in an effective speed-regulation mechanism. Movement of these motors is generally fully dependent on the concentration of accessible fuel, with propulsive movement only ceasing when the fuel consumption is complete. Here we report a demonstration of control over the movement of self-assembled stomatocyte nanomotors via a molecularly built, stimulus-responsive regulatory mechanism...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430192/a-monodisperse-transmembrane-%C3%AE-helical-peptide-barrel
#9
Kozhinjampara R Mahendran, Ai Niitsu, Lingbing Kong, Andrew R Thomson, Richard B Sessions, Derek N Woolfson, Hagan Bayley
The fabrication of monodisperse transmembrane barrels formed from short synthetic peptides has not been demonstrated previously. This is in part because of the complexity of the interactions between peptides and lipids within the hydrophobic environment of a membrane. Here we report the formation of a transmembrane pore through the self-assembly of 35 amino acid α-helical peptides. The design of the peptides is based on the C-terminal D4 domain of the Escherichia coli polysaccharide transporter Wza. By using single-channel current recording, we define discrete assembly intermediates and show that the pore is most probably a helix barrel that contains eight D4 peptides arranged in parallel...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430191/activating-lattice-oxygen-redox-reactions-in-metal-oxides-to-catalyse-oxygen-evolution
#10
Alexis Grimaud, Oscar Diaz-Morales, Binghong Han, Wesley T Hong, Yueh-Lin Lee, Livia Giordano, Kelsey A Stoerzinger, Marc T M Koper, Yang Shao-Horn
Understanding how materials that catalyse the oxygen evolution reaction (OER) function is essential for the development of efficient energy-storage technologies. The traditional understanding of the OER mechanism on metal oxides involves four concerted proton-electron transfer steps on metal-ion centres at their surface and product oxygen molecules derived from water. Here, using in situ (18)O isotope labelling mass spectrometry, we provide direct experimental evidence that the O2 generated during the OER on some highly active oxides can come from lattice oxygen...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430190/tuning-underwater-adhesion-with-cation-%C3%AF-interactions
#11
Matthew A Gebbie, Wei Wei, Alex M Schrader, Thomas R Cristiani, Howard A Dobbs, Matthew Idso, Bradley F Chmelka, J Herbert Waite, Jacob N Israelachvili
Cation-π interactions drive the self-assembly and cohesion of many biological molecules, including the adhesion proteins of several marine organisms. Although the origin of cation-π bonds in isolated pairs has been extensively studied, the energetics of cation-π-driven self-assembly in molecular films remains uncharted. Here we use nanoscale force measurements in combination with solid-state NMR spectroscopy to show that the cohesive properties of simple aromatic- and lysine-rich peptides rival those of the strong reversible intermolecular cohesion exhibited by adhesion proteins of marine mussel...
May 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430206/transmembrane-signalling-membrane-messengers
#12
Scott L Cockroft
No abstract text is available yet for this article.
April 21, 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430204/dark-times
#13
Bruce C Gibb
No abstract text is available yet for this article.
April 21, 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430202/cation-%C3%AF-interactions-mimicking-mussel-mechanics
#14
Henrik Birkedal
No abstract text is available yet for this article.
April 21, 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430201/sending-a-message-to-the-other-side
#15
EDITORIAL
(no author information available yet)
No abstract text is available yet for this article.
April 21, 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430200/tin-can
#16
Michael A Tarselli
No abstract text is available yet for this article.
April 21, 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28430198/helium-chemistry-react-with-nobility
#17
Maosheng Miao
No abstract text is available yet for this article.
April 21, 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28485398/atomically-precise-organomimetic-cluster-nanomolecules-assembled-via-perfluoroaryl-thiol-snar-chemistry
#18
Elaine A Qian, Alex I Wixtrom, Jonathan C Axtell, Azin Saebi, Dahee Jung, Pavel Rehak, Yanxiao Han, Elamar Hakim Moully, Daniel Mosallaei, Sylvia Chow, Marco S Messina, Jing Yang Wang, A Timothy Royappa, Arnold L Rheingold, Heather D Maynard, Petr Král, Alexander M Spokoyny
The majority of biomolecules are intrinsically atomically precise, an important characteristic that enables rational engineering of their recognition and binding properties. However, imparting a similar precision to hybrid nanoparticles has been challenging because of the inherent limitations of existing chemical methods and building blocks. Here we report a new approach to form atomically precise and highly tunable hybrid nanomolecules with well-defined three-dimensionality. Perfunctionalization of atomically precise clusters with pentafluoroaryl-terminated linkers produces size-tunable rigid cluster nanomolecules...
April 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28338692/computational-design-of-self-assembling-cyclic-protein-homo-oligomers
#19
Jorge A Fallas, George Ueda, William Sheffler, Vanessa Nguyen, Dan E McNamara, Banumathi Sankaran, Jose Henrique Pereira, Fabio Parmeggiani, T J Brunette, Duilio Cascio, Todd R Yeates, Peter Zwart, David Baker
Self-assembling cyclic protein homo-oligomers play important roles in biology, and the ability to generate custom homo-oligomeric structures could enable new approaches to probe biological function. Here we report a general approach to design cyclic homo-oligomers that employs a new residue-pair-transform method to assess the designability of a protein-protein interface. This method is sufficiently rapid to enable the systematic enumeration of cyclically docked arrangements of a monomer followed by sequence design of the newly formed interfaces...
April 2017: Nature Chemistry
https://www.readbyqxmd.com/read/28338691/surfactant-free-single-layer-graphene-in-water
#20
George Bepete, Eric Anglaret, Luca Ortolani, Vittorio Morandi, Kai Huang, Alain Pénicaud, Carlos Drummond
Dispersing graphite in water to obtain true (single-layer) graphene in bulk quantity in a liquid has been an unreachable goal for materials scientists in the past decade. Similarly, a diagnostic tool to identify solubilized graphene in situ has been long awaited. Here we show that homogeneous stable dispersions of single-layer graphene (SLG) in water can be obtained by mixing graphenide (negatively charged graphene) solutions in tetrahydrofuran with degassed water and evaporating the organic solvent. In situ Raman spectroscopy of these aqueous dispersions shows all the expected characteristics of SLG...
April 2017: Nature Chemistry
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