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ACS Central Science

Prachi Patel
No abstract text is available yet for this article.
February 22, 2017: ACS Central Science
Wei Liu, Weiyang Li, Denys Zhuo, Guangyuan Zheng, Zhenda Lu, Kai Liu, Yi Cui
Lithium metal based batteries represent a major challenge and opportunity in enabling a variety of devices requiring high-energy-density storage. However, dendritic lithium growth has limited the practical application of lithium metal anodes. Here we report a nanoporous, flexible and electrochemically stable coating of silica@poly(methyl methacrylate) (SiO2@PMMA) core-shell nanospheres as an interfacial layer on lithium metal anode. This interfacial layer is capable of inhibiting Li dendrite growth while sustaining ionic flux through it, which is attributed to the nanoscaled pores formed among the nanospheres...
February 22, 2017: ACS Central Science
Mao Chen, Yuwei Gu, Awaneesh Singh, Mingjiang Zhong, Alex M Jordan, Santidan Biswas, LaShanda T J Korley, Anna C Balazs, Jeremiah A Johnson
Light-initiated additive manufacturing techniques typically rely on layer-by-layer addition or continuous extraction of polymers formed via nonliving, free radical polymerization methods that render the final materials "dead" toward further monomer insertion; the polymer chains within the materials cannot be reactivated to induce chain extension. An alternative "living additive manufacturing" strategy would involve the use of photocontrolled living radical polymerization to spatiotemporally insert monomers into dormant "parent" materials to generate more complex and diversely functionalized "daughter" materials...
February 22, 2017: ACS Central Science
Roberta Lentini, Noël Yeh Martín, Michele Forlin, Luca Belmonte, Jason Fontana, Michele Cornella, Laura Martini, Sabrina Tamburini, William E Bentley, Olivier Jousson, Sheref S Mansy
Artificial cells capable of both sensing and sending chemical messages to bacteria have yet to be built. Here we show that artificial cells that are able to sense and synthesize quorum signaling molecules can chemically communicate with V. fischeri, V. harveyi, E. coli, and P. aeruginosa. Activity was assessed by fluorescence, luminescence, RT-qPCR, and RNA-seq. Two potential applications for this technology were demonstrated. First, the extent to which artificial cells could imitate natural cells was quantified by a type of cellular Turing test...
February 22, 2017: ACS Central Science
Ariel L Furst, Alexander C Hoepker, Matthew B Francis
Endocrine disrupting compounds are found in increasing amounts in our environment, originating from pesticides, plasticizers, and pharmaceuticals, among other sources. Although the full impact of these compounds is still under study, they have already been implicated in diseases such as obesity, diabetes, and cancer. The list of chemicals that disrupt normal hormone function is growing at an alarming rate, making it crucially important to find sources of contamination and identify new compounds that display this ability...
February 22, 2017: ACS Central Science
Chang Liu, J C Yves Le Blanc, Bradley B Schneider, Jefry Shields, James J Federico, Hui Zhang, Justin G Stroh, Gregory W Kauffman, Daniel W Kung, Christian Ieritano, Evan Shepherdson, Mitch Verbuyst, Luke Melo, Moaraj Hasan, Dalia Naser, John S Janiszewski, W Scott Hopkins, J Larry Campbell
The microsolvated state of a molecule, represented by its interactions with only a small number of solvent molecules, can play a key role in determining the observable bulk properties of the molecule. This is especially true in cases where strong local hydrogen bonding exists between the molecule and the solvent. One method that can probe the microsolvated states of charged molecules is differential mobility spectrometry (DMS), which rapidly interrogates an ion's transitions between a solvated and desolvated state in the gas phase (i...
February 22, 2017: ACS Central Science
Timothy M Swager
No abstract text is available yet for this article.
February 22, 2017: ACS Central Science
Miriam L Diamond
No abstract text is available yet for this article.
February 22, 2017: ACS Central Science
Sivaprakash Shanmugam, Jiangtao Xu, Cyrille Boyer
No abstract text is available yet for this article.
February 22, 2017: ACS Central Science
Mitch Jacoby
No abstract text is available yet for this article.
February 22, 2017: ACS Central Science
Xavier Gómez-Santacana, Silvia Pittolo, Xavier Rovira, Marc Lopez, Charleine Zussy, James A R Dalton, Adèle Faucherre, Chris Jopling, Jean-Philippe Pin, Francisco Ciruela, Cyril Goudet, Jesús Giraldo, Pau Gorostiza, Amadeu Llebaria
Phenylazopyridines are photoisomerizable compounds with high potential to control biological functions with light. We have obtained a series of phenylazopyridines with light dependent activity as negative allosteric modulators (NAM) of metabotropic glutamate receptor subtype 5 (mGlu5). Here we describe the factors needed to achieve an operational molecular photoisomerization and its effective translation into in vitro and in vivo receptor photoswitching, which includes zebrafish larva motility and the regulation of the antinociceptive effects in mice...
January 25, 2017: ACS Central Science
Jan-Stefan Völler, Morana Dulic, Ulla I M Gerling-Driessen, Hernan Biava, Tobias Baumann, Nediljko Budisa, Ita Gruic-Sovulj, Beate Koksch
Fluorine being not substantially present in the chemistry of living beings is an attractive element in tailoring novel chemical, biophysical, and pharmacokinetic properties of peptides and proteins. The hallmark of ribosome-mediated artificial amino acid incorporation into peptides and proteins is a broad substrate tolerance, which is assumed to rely on the absence of evolutionary pressure for efficient editing of artificial amino acids. We used the well-characterized editing proficient isoleucyl-tRNA synthetase (IleRS) from Escherichia coli to investigate the crosstalk of aminoacylation and editing activities against fluorinated amino acids...
January 25, 2017: ACS Central Science
Sheng-Ying Hsieh, Jeffrey W Bode
Redox neutral photocatalytic transformations often require careful pairing of the substrates and photoredox catalysts in order to achieve a catalytic cycle. This can limit the range of viable transformations, as we recently observed in attempting to extend the scope of the photocatalytic synthesis of N-heterocycles using silicon amine protocol (SLAP) reagents to include starting materials that require higher oxidation potentials. We now report that the inclusion of Lewis acids in photocatalytic reactions of organosilanes allows access to a distinct reaction pathway featuring an Ir(III)*/Ir(IV) couple instead of the previously employed Ir(III)*/Ir(II) pathway, enabling the transformation of aromatic and aliphatic aldehydes to thiomorpholines and thiazepanes...
January 25, 2017: ACS Central Science
Brian J Smith, Lucas R Parent, Anna C Overholts, Peter A Beaucage, Ryan P Bisbey, Anton D Chavez, Nicky Hwang, Chiwoo Park, Austin M Evans, Nathan C Gianneschi, William R Dichtel
Covalent organic frameworks (COFs) are two- or three-dimensional (2D or 3D) polymer networks with designed topology and chemical functionality, permanent porosity, and high surface areas. These features are potentially useful for a broad range of applications, including catalysis, optoelectronics, and energy storage devices. But current COF syntheses offer poor control over the material's morphology and final form, generally providing insoluble and unprocessable microcrystalline powder aggregates. COF polymerizations are often performed under conditions in which the monomers are only partially soluble in the reaction solvent, and this heterogeneity has hindered understanding of their polymerization or crystallization processes...
January 25, 2017: ACS Central Science
Weidong Zhou, Yutao Li, Sen Xin, John B Goodenough
A reversible plating/stripping of a dendrite-free metallic-sodium anode with a reduced anode/ceramic interfacial resistance is created by a thin interfacial interlayer formed in situ or by the introduction of a dry polymer film. Wetting of the sodium on the interfacial interlayer suppresses dendrite formation and growth at different discharge/charge C-rates. All-solid-state batteries were obtained with a high cycling stability and Coulombic efficiency at 65 °C.
January 25, 2017: ACS Central Science
Hang Chu, Joel M Smith, Jakob Felding, Phil S Baran
Total syntheses of the complex, highly oxygenated sesquiterpenes thapsigargin (1) and nortrilobolide (2) are presented. Access to analogues of these promising bioactive natural products has been limited to tedious isolation and semisynthetic efforts. Elegant prior total syntheses demonstrated the feasibility of creating these entitites in 36-42 step processes. The currently reported route proceeds in a scalable and more concise fashion by utilizing two-phase terpene synthesis logic. Salient features of the work include application of the classic photosantonin rearrangement and precisely choreographed installation of the multiple oxygenations present on the guaianolide skeleton...
January 25, 2017: ACS Central Science
Bryan S Matsuura, Patrick Kölle, Dirk Trauner, Regina de Vivie-Riedle, Robin Meier
Aplydactone (1) is a brominated ladderane sesquiterpenoid that was isolated from the sea hare Aplysia dactylomela together with the chamigranes dactylone (2) and 10-epi-dactylone (3). Given the habitat of A. dactylomela, it seems likely that 1 is formed from 2 through a photochemical [2 + 2] cycloaddition. Here, we disclose a concise synthesis of 1, 2, and 3 that was guided by excited state theory and relied on several highly stereoselective transformations. Our experiments and calculations confirm the photochemical origin of 1 and explain why it is formed as the sole isomer...
January 25, 2017: ACS Central Science
Zhanyong Li, Aaron W Peters, Varinia Bernales, Manuel A Ortuño, Neil M Schweitzer, Matthew R DeStefano, Leighanne C Gallington, Ana E Platero-Prats, Karena W Chapman, Christopher J Cramer, Laura Gagliardi, Joseph T Hupp, Omar K Farha
Zr-based metal-organic frameworks (MOFs) have been shown to be excellent catalyst supports in heterogeneous catalysis due to their exceptional stability. Additionally, their crystalline nature affords the opportunity for molecular level characterization of both the support and the catalytically active site, facilitating mechanistic investigations of the catalytic process. We describe herein the installation of Co(II) ions to the Zr6 nodes of the mesoporous MOF, NU-1000, via two distinct routes, namely, solvothermal deposition in a MOF (SIM) and atomic layer deposition in a MOF (AIM), denoted as Co-SIM+NU-1000 and Co-AIM+NU-1000, respectively...
January 25, 2017: ACS Central Science
Liam J O'Connor, Ishna N Mistry, Sarah L Collins, Lisa K Folkes, Graham Brown, Stuart J Conway, Ester M Hammond
Azide-containing compounds have broad utility in organic synthesis and chemical biology. Their use as powerful tools for the labeling of biological systems in vitro has enabled insights into complex cellular functions. To date, fluorogenic azide-containing compounds have primarily been employed in the context of click chemistry and as sensitive functionalities for hydrogen sulfide detection. Here, we report an alternative use of this functionality: as fluorogenic probes for the detection of depleted oxygen levels (hypoxia)...
January 25, 2017: ACS Central Science
Jean-Louis Do, Tomislav Friščić
The past decade has seen a reawakening of solid-state approaches to chemical synthesis, driven by the search for new, cleaner synthetic methodologies. Mechanochemistry, i.e., chemical transformations initiated or sustained by mechanical force, has been advancing particularly rapidly, from a laboratory curiosity to a widely applicable technique that not only enables a cleaner route to chemical transformations but offers completely new opportunities in making and screening for molecules and materials. This Outlook provides a brief overview of the recent achievements and opportunities created by mechanochemistry, including access to materials, molecular targets, and synthetic strategies that are hard or even impossible to access by conventional means...
January 25, 2017: ACS Central Science
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