Stabilizing Otherwise Unstable Anions with Halogen Bonding Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-18 Xinxing Zhang, Gaoxiang Liu, Sandra Ciborowski, Kit Bowen
The n→π* Interaction Acc. Chem. Res. (IF 20.268) Pub Date : 2017-07-23 00:00:00 Robert W. Newberry, Ronald T. Raines
Ni-Catalyzed Alkene Carboacylation via Amide C–N Bond Activation J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-20 James A. Walker, Kevin L. Vickerman, Jenna N. Humke, Levi M. Stanley
The Metal Drives the Chemistry: Dual Functions of Acireductone Dioxygenase Chem. Rev. (IF 47.928) Pub Date : 2017-07-21 Aditi R. Deshpande, Thomas C. Pochapsky, Dagmar Ringe
Singlet Oxygen Photophysics in Liquid Solvents: Converging on a Unified Picture Acc. Chem. Res. (IF 20.268) Pub Date : 2017-07-21 Mikkel Bregnhøj, Michael Westberg, Boris F. Minaev, Peter R. Ogilby
Isolable Bis(triarylamine) Dications: Analogues of Thiele’s, Chichibabin’s, and Müller’s Hydrocarbons Acc. Chem. Res. (IF 20.268) Pub Date : 2017-07-21 Gengwen Tan, Xinping Wang
Magnetic separation: its application in mining, waste purification, medicine, biochemistry and chemistry Chem. Soc. Rev. (IF 38.618) Pub Date : 2017-07-21 M. Iranmanesh, J. Hulliger
Asymmetric Brønsted acid catalysis with chiral carboxylic acids Chem. Soc. Rev. (IF 38.618) Pub Date : 2017-07-21 Chang Min, Daniel Seidel
Separating Proton and Electron Transfer Effects in Three-Component Concerted Proton-Coupled Electron Transfer Reactions J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Wesley D. Morris, James M. Mayer
An Assay Based on SAMDI Mass Spectrometry for Profiling Protein Interaction Domains J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Patrick T. O’Kane, Milan Mrksich
Multielectron Chemistry within a Model Nickel Metalloprotein: Mechanistic Implications for Acetyl-CoA Synthase J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Anastasia C. Manesis, Matthew J. O’Connor, Camille R. Schneider, Hannah S. Shafaat
5-Formyl- and 5-Carboxydeoxycytidines Do Not Cause Accumulation of Harmful Repair Intermediates in Stem Cells J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 René Rahimoff, Olesea Kosmatchev, Angie Kirchner, Toni Pfaffeneder, Fabio Spada, Victor Brantl, Markus Müller, Thomas Carell
Combined Theoretical and Experimental Studies of Nickel-Catalyzed Cross-Coupling of Methoxyarenes with Arylboronic Esters via C–O Bond Cleavage J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Martin C. Schwarzer, Ryosuke Konno, Takayuki Hojo, Akimichi Ohtsuki, Keisuke Nakamura, Ayaka Yasutome, Hiroaki Takahashi, Toshiaki Shimasaki, Mamoru Tobisu, Naoto Chatani, Seiji Mori
Inversion in Mg1–xNixAl2O4 Spinel: New Insight into Local Structure J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Eric C. O’Quinn, Jacob Shamblin, Brandon Perlov, Rodney C. Ewing, Joerg Neuefeind, Mikhail Feygenson, Igor Gussev, Maik Lang
Chemoselective Asymmetric Intramolecular Dearomatization of Phenols with α-Diazoacetamides Catalyzed by Silver Phosphate J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Hiroki Nakayama, Shingo Harada, Masato Kono, Tetsuhiro Nemoto
Raman Optical Activity Reveals Carotenoid Photoactivation Events in the Orange Carotenoid Protein in Solution J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Tomotsumi Fujisawa, Ryan L. Leverenz, Momoka Nagamine, Cheryl A. Kerfeld, Masashi Unno
Hidden Oceans? Unraveling the Structure of Hydrous Defects in the Earth’s Deep Interior J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Helen Grüninger, Katherine Armstrong, Dominik Greim, Tiziana Boffa-Ballaran, Daniel J. Frost, Jürgen Senker
Computational and Experimental Studies on the Effects of Monomer Planarity on Covalent Organic Framework Formation J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Christina M. Thompson, Gino Occhialini, Gregory T. McCandless, Sampath B. Alahakoon, Victoria Cameron, Steven O. Nielsen, Ronald A. Smaldone
Sky-Blue-Emitting Dendritic Alkynylgold(III) Complexes for Solution-Processable Organic Light-Emitting Devices J. Am. Chem. Soc. (IF 13.858) Pub Date : 2017-07-21 Chin-Ho Lee, Man-Chung Tang, Yi-Chun Wong, Mei-Yee Chan, Vivian Wing-Wah Yam
Borylenes: An Emerging Class of Compounds Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Michele Soleilhavoup, Guy Bertrand
Silver-Catalyzed Oxidative C(sp3)−P Bond Formation through C−C and P−H Bond Cleavage Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Lili Li, Wenbin Huang, Lijin Chen, Jiaxing Dong, Xuebing Ma, Yungui Peng
A Direct Synthesis of Highly Substituted π-Rich Aromatic Heterocycles from Oxetanes Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Alexander R. White, Ryan A. Kozlowski, Shiou-Chuan Tsai, Christopher D. Vanderwal
Exceptionally Strong Electron-Donating Ability of Bora-Ylide Substituent vis-à-vis Silylene and Silylium Ion Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Alfredo Rosas-Sánchez, Isabel Alvarado-Beltran, Antoine Baceiredo, Nathalie Saffon-Merceron, Stéphane Massou, Vicenç Branchadell, Tsuyoshi Kato
Tight Molecular Recognition of Benzo[a]pyrene by a High-Affinity Antibody Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Andreas Eichinger, Irmgard Neumaier, Michael Pschenitza, Reinhard Niessner, Dietmar Knopp, Arne Skerra
A simple supramolecular assay for drug detection in urine Chem. Commun. (IF 6.319) Pub Date : 2017-07-21 Silvia Sonzini, Jade A. McCune, Peter Ravn, Oren A. Scherman, Christopher F. van der Walle
Using anion recognition to control the folding and unfolding of a single chain phosphorescent polymer Chem. Commun. (IF 6.319) Pub Date : 2017-07-17 Xiaofan Ji, Chenxing Guo, Xian-Sheng Ke, Xiaodong Chi, Jonathan L. Sessler
Adapting the Glaser Reaction for Bioconjugation: Robust Access to Structurally Simple, Rigid Linkers Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Anthony P. Silvestri, Philip A. Cistrone, Philip E. Dawson
Hollow and microporous triphenylamine networks post-modified with TCNE for enhanced organocathode performance Chem. Commun. (IF 6.319) Pub Date : 2017-07-14 Jaewon Choi, Eui Soon Kim, Ju Hong Ko, Sang Moon Lee, Hae Jin Kim, Yoon-Joo Ko, Seung Uk Son
Structural diversity of metal–organic self-assembly assisted by chlorine Chem. Commun. (IF 6.319) Pub Date : 2017-07-14 Lei Xie, Chi Zhang, Yuanqi Ding, Wenlong E, Chunxue Yuan, Wei Xu
Direct Alkylation of Amines with Primary and Secondary Alcohols through Biocatalytic Hydrogen Borrowing Angew. Chem. Int. Ed. (IF 11.994) Pub Date : 2017-07-21 Sarah L. Montgomery, Juan Mangas-Sanchez, Matthew P. Thompson, Godwin A. Aleku, Beatriz Dominguez, Nicholas J. Turner
A CuI/CuIII prototypical organometallic mechanism for the deactivation of an active pincer-like CuI catalyst in Ullmann-type couplings Chem. Commun. (IF 6.319) Pub Date : 2017-07-13 Mireia Rovira, Lucie Jašíková, Erik Andris, Ferran Acuña-Parés, Marta Soler, Imma Güell, Ming-Zheng Wang, Laura Gómez, Josep M. Luis, Jana Roithová, Xavi Ribas
Highly regio-, diastereo- and enantioselective deracemization of axially chiral 3-alkylideneoxindoles Chem. Commun. (IF 6.319) Pub Date : 2017-07-12 Hongjiang Mei, Lili Lin, Lifeng Wang, Li Dai, Xiaohua Liu, Xiaoming Feng
Unveiling the synergistic effect of polysulfide additive and MnO2 hollow spheres in evolving a stable cyclic performance in Li–S batteries Chem. Commun. (IF 6.319) Pub Date : 2017-07-12 Syed Abdul Ahad, P. Ragupathy, Soojy Ryu, Hyun-Wook Lee, Do Kyung Kim
Radiofluorination of a NHC–PF5 adduct: toward new probes for 18F PET imaging Chem. Commun. (IF 6.319) Pub Date : 2017-07-11 Boris Vabre, Kantapat Chansaenpak, Mengzhe Wang, Hui Wang, Zibo Li, François P. Gabbaï
Copper-catalyzed Mannich-type oxidative β-functionalization of tertiary amines Chem. Commun. (IF 6.319) Pub Date : 2017-07-10 Min-Jie Zhou, Shou-Fei Zhu, Qi-Lin Zhou
Highly efficient enantioselective liquid–liquid extraction of 1,2-amino-alcohols using SPINOL based phosphoric acid hosts Chem. Sci. (IF 8.668) Pub Date : 2017-07-21 Erik B. Pinxterhuis, Jean-Baptiste Gualtierotti, Hero J. Heeres, Johannes G. de Vries, Ben L. Feringa
Potent mechanism-based sirtuin-2-selective inhibition by an in situ-generated occupant of the substrate-binding site, “selectivity pocket” and NAD+-binding site Chem. Sci. (IF 8.668) Pub Date : 2017-07-21 Paolo Mellini, Yukihiro Itoh, Hiroki Tsumoto, Ying Li, Miki Suzuki, Natsuko Tokuda, Taeko Kakizawa, Yuri Miura, Jun Takeuchi, Maija Lahtela-Kakkonen, Takayoshi Suzuki
Perhydrohelicenes and other diamond-lattice based hydrocarbons: the choreography of inversion Chem. Sci. (IF 8.668) Pub Date : 2017-07-17 Roger W. Alder, Craig P. Butts, Richard B. Sessions
Temporal switching of an amphiphilic self-assembly by a chemical fuel-driven conformational response Chem. Sci. (IF 8.668) Pub Date : 2017-07-11 Krishnendu Jalani, Shikha Dhiman, Ankit Jain, Subi J. George
The m6A methylation perturbs the Hoogsteen pairing-guided incorporation of an oxidized nucleotide Chem. Sci. (IF 8.668) Pub Date : 2017-07-06 Shaoru Wang, Yanyan Song, Yafen Wang, Xin Li, Boshi Fu, Yinong Liu, Jiaqi Wang, Lai Wei, Tian Tian, Xiang Zhou
Structures of the CRISPR genome integration complex Science (IF 37.205) Pub Date : 2017-07-20 00:00:00 Addison V. Wright, Jun-Jie Liu, Gavin J. Knott, Kevin W. Doxzen, Eva Nogales, Jennifer A. Doudna
CRISPR-Cas systems depend on the Cas1-Cas2 integrase to capture and integrate short foreign DNA fragments into the CRISPR locus, enabling adaptation to new viruses. We present crystal structures of Cas1-Cas2 bound to both donor and target DNA in intermediate and product integration complexes, as well as a cryo-electron microscopy structure of the full CRISPR locus integration complex including the accessory protein Integration Host Factor (IHF). The structures show unexpectedly that indirect sequence recognition dictates integration site selection by favoring deformation of the repeat and the flanking sequences. IHF binding bends the DNA sharply, bringing an upstream recognition motif into contact with Cas1 to increase both the specificity and efficiency of integration. These results explain how the Cas1-Cas2 CRISPR integrase recognizes a sequence-dependent DNA structure to ensure site-selective CRISPR array expansion during the initial step of bacterial adaptive immunity.
Optical imaging of surface chemistry and dynamics in confinement Science (IF 37.205) Pub Date : 2017-07-20 00:00:00 Carlos Macias-Romero, Igor Nahalka, Halil I. Okur, Sylvie Roke
We imaged the interfacial structure and dynamics of water in a microscopically confined geometry in three dimensions and on millisecond time scales with a 3D structurally illuminated wide-field second harmonic microscope. Image contrast reports on the orientational order of interfacial water, induced by charge-dipole interactions between water molecules and surface charges. The images were converted into surface potential maps. Spatially resolved surface acid dissociation constant pKa,s values were determined for the silica deprotonation reaction by following pH induced chemical changes on the curved and confined surfaces of a glass micro-capillary immersed in aqueous solutions. These values ranged from 2.3 to 10.7 along the wall of a single capillary, because of surface heterogeneities. Water molecules that rotate along an oscillating external electric field were also imaged.
Cash for carbon: A randomized trial of payments for ecosystem services to reduce deforestation Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Seema Jayachandran, Joost de Laat, Eric F. Lambin, Charlotte Y. Stanton, Robin Audy, Nancy E. Thomas
We evaluated a program of payments for ecosystem services in Uganda that offered forest-owning households annual payments of 70,000 Ugandan shillings per hectare if they conserved their forest. The program was implemented as a randomized controlled trial in 121 villages, 60 of which received the program for 2 years. The primary outcome was the change in land area covered by trees, measured by classifying high-resolution satellite imagery. We found that tree cover declined by 4.2% during the study period in treatment villages, compared to 9.1% in control villages. We found no evidence that enrollees shifted their deforestation to nearby land. We valued the delayed carbon dioxide emissions and found that this program benefit is 2.4 times as large as the program costs.
Ratchet-like polypeptide translocation mechanism of the AAA+ disaggregase Hsp104 Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Stephanie N. Gates, Adam L. Yokom, JiaBei Lin, Meredith E. Jackrel, Alexandrea N. Rizo, Nathan M. Kendsersky, Courtney E. Buell, Elizabeth A. Sweeny, Korrie L. Mack, Edward Chuang, Mariana P. Torrente, Min Su, James Shorter, Daniel R. Southworth
Hsp100 polypeptide translocases are conserved members of the AAA+ family (adenosine triphosphatases associated with diverse cellular activities) that maintain proteostasis by unfolding aberrant and toxic proteins for refolding or proteolytic degradation. The Hsp104 disaggregase from Saccharomyces cerevisiae solubilizes stress-induced amorphous aggregates and amyloids. The structural basis for substrate recognition and translocation is unknown. Using a model substrate (casein), we report cryo–electron microscopy structures at near-atomic resolution of Hsp104 in different translocation states. Substrate interactions are mediated by conserved, pore-loop tyrosines that contact an 80-angstrom-long unfolded polypeptide along the axial channel. Two protomers undergo a ratchet-like conformational change that advances pore loop–substrate interactions by two amino acids. These changes are coupled to activation of specific nucleotide hydrolysis sites and, when transmitted around the hexamer, reveal a processive rotary translocation mechanism and substrate-responsive flexibility during Hsp104-catalyzed disaggregation.
Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Sunghun Choi, Tae-woo Kwon, Ali Coskun, Jang Wook Choi
Lithium-ion batteries with ever-increasing energy densities are needed for batteries for advanced devices and all-electric vehicles. Silicon has been highlighted as a promising anode material because of its superior specific capacity. During repeated charge-discharge cycles, silicon undergoes huge volume changes. This limits cycle life via particle pulverization and an unstable electrode-electrolyte interface, especially when the particle sizes are in the micrometer range. We show that the incorporation of 5 weight % polyrotaxane to conventional polyacrylic acid binder imparts extraordinary elasticity to the polymer network originating from the ring sliding motion of polyrotaxane. This binder combination keeps even pulverized silicon particles coalesced without disintegration, enabling stable cycle life for silicon microparticle anodes at commercial-level areal capacities.
Photoinduced decarboxylative borylation of carboxylic acids Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Alexander Fawcett, Johan Pradeilles, Yahui Wang, Tatsuya Mutsuga, Eddie L. Myers, Varinder K. Aggarwal
The conversion of widely available carboxylic acids into versatile boronic esters would be highly enabling for synthesis. We found that this transformation can be effected by illuminating the N-hydroxyphthalimide ester derivative of the carboxylic acid under visible light at room temperature in the presence of the diboron reagent bis(catecholato)diboron. A simple workup allows isolation of the pinacol boronic ester. Experimental evidence suggests that boryl radical intermediates are involved in the process. The methodology is illustrated by the transformation of primary, secondary, and tertiary alkyl carboxylic acids as well as a diverse range of natural-product carboxylic acids, thereby demonstrating its broad utility and functional group tolerance.
Bismuthene on a SiC substrate: A candidate for a high-temperature quantum spin Hall material Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 F. Reis, G. Li, L. Dudy, M. Bauernfeind, S. Glass, W. Hanke, R. Thomale, J. Schäfer, R. Claessen
Quantum spin Hall materials hold the promise of revolutionary devices with dissipationless spin currents but have required cryogenic temperatures owing to small energy gaps. Here we show theoretically that a room-temperature regime with a large energy gap may be achievable within a paradigm that exploits the atomic spin-orbit coupling. The concept is based on a substrate-supported monolayer of a high–atomic number element and is experimentally realized as a bismuth honeycomb lattice on top of the insulating silicon carbide substrate SiC(0001). Using scanning tunneling spectroscopy, we detect a gap of ~0.8 electron volt and conductive edge states consistent with theory. Our combined theoretical and experimental results demonstrate a concept for a quantum spin Hall wide-gap scenario, where the chemical potential resides in the global system gap, ensuring robust edge conductance.
Remobilization of crustal carbon may dominate volcanic arc emissions Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Emily Mason, Marie Edmonds, Alexandra V. Turchyn
The flux of carbon into and out of Earth’s surface environment has implications for Earth’s climate and habitability. We compiled a global data set for carbon and helium isotopes from volcanic arcs and demonstrated that the carbon isotope composition of mean global volcanic gas is considerably heavier, at –3.8 to –4.6 per mil (), than the canonical mid-ocean ridge basalt value of –6.0. The largest volcanic emitters outgas carbon with higher 13C and are located in mature continental arcs that have accreted carbonate platforms, indicating that reworking of crustal limestone is an important source of volcanic carbon. The fractional burial of organic carbon is lower than traditionally determined from a global carbon isotope mass balance and may have varied over geological time, modulated by supercontinent formation and breakup.
Chiral Majorana fermion modes in a quantum anomalous Hall insulator–superconductor structure Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Qing Lin He, Lei Pan, Alexander L. Stern, Edward C. Burks, Xiaoyu Che, Gen Yin, Jing Wang, Biao Lian, Quan Zhou, Eun Sang Choi, Koichi Murata, Xufeng Kou, Zhijie Chen, Tianxiao Nie, Qiming Shao, Yabin Fan, Shou-Cheng Zhang, Kai Liu, Jing Xia, Kang L. Wang
Majorana fermion is a hypothetical particle that is its own antiparticle. We report transport measurements that suggest the existence of one-dimensional chiral Majorana fermion modes in the hybrid system of a quantum anomalous Hall insulator thin film coupled with a superconductor. As the external magnetic field is swept, half-integer quantized conductance plateaus are observed at the locations of magnetization reversals, giving a distinct signature of the Majorana fermion modes. This transport signature is reproducible over many magnetic field sweeps and appears at different temperatures. This finding may open up an avenue to control Majorana fermions for implementing robust topological quantum computing.
Experimentally realized mechanochemistry distinct from force-accelerated scission of loaded bonds Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Sergey Akbulatov, Yancong Tian, Zhen Huang, Timothy J. Kucharski, Qing-Zheng Yang, Roman Boulatov
Stretching polymer chains accelerates dissociation of a variety of internal covalent bonds, to an extent that correlates well with the force experienced by the scissile bond. Recent theory has also predicted scenarios in which applied force accelerates dissociation of unloaded bonds and kinetically strengthens strained bonds. We report here unambiguous experimental validation of this hypothesis: Detailed kinetic measurements demonstrate that stretching phosphotriesters accelerates dissociation of the unloaded phosphorus-oxygen bond orthogonal to the pulling axis, whereas stretching organosiloxanes inhibits dissociation of the aligned loaded silicon-oxygen bonds. Qualitatively, the outcome is determined by phosphoester elongation and siloxane contraction along the pulling axis in the respective rate-determining transition states. Quantitatively, the results agree with a simple mechanochemical kinetics model.
Tailored semiconductors for high-harmonic optoelectronics Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Murat Sivis, Marco Taucer, Giulio Vampa, Kyle Johnston, André Staudte, Andrei Yu. Naumov, D. M. Villeneuve, Claus Ropers, P. B. Corkum
The advent of high-harmonic generation in gases 30 years ago set the foundation for attosecond science and facilitated ultrafast spectroscopy in atoms, molecules, and solids. We explore high-harmonic generation in the solid state by means of nanostructured and ion-implanted semiconductors. We use wavelength-selective microscopic imaging to map enhanced harmonic emission and show that the generation medium and the driving field can be locally tailored in solids by modifying the chemical composition and morphology. This enables the control of high-harmonic technology within precisely engineered solid targets. We demonstrate customized high-harmonic wave fields with wavelengths down to 225 nanometers (ninth-harmonic order of 2-micrometer laser pulses) and present an integrated Fresnel zone plate target in silicon, which leads to diffraction-limited self-focusing of the generated harmonics down to 1-micrometer spot sizes.
An organic-inorganic perovskite ferroelectric with large piezoelectric response Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Yu-Meng You, Wei-Qiang Liao, Dewei Zhao, Heng-Yun Ye, Yi Zhang, Qionghua Zhou, Xianghong Niu, Jinlan Wang, Peng-Fei Li, Da-Wei Fu, Zheming Wang, Song Gao, Kunlun Yang, Jun-Ming Liu, Jiangyu Li, Yanfa Yan, Ren-Gen Xiong
Molecular piezoelectrics are highly desirable for their easy and environment-friendly processing, light weight, low processing temperature, and mechanical flexibility. However, although 136 years have passed since the discovery in 1880 of the piezoelectric effect, molecular piezoelectrics with a piezoelectric coefficient d33 comparable with piezoceramics such as barium titanate (BTO; ~190 picocoulombs per newton) have not been found. We show that trimethylchloromethyl ammonium trichloromanganese(II), an organic-inorganic perovskite ferroelectric crystal processed from aqueous solution, has a large d33 of 185 picocoulombs per newton and a high phase-transition temperature of 406 kelvin (K) (16 K above that of BTO). This makes it a competitive candidate for medical, micromechanical, and biomechanical applications.
Hydraulic control of tuna fins: A role for the lymphatic system in vertebrate locomotion Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Vadim Pavlov, Benyamin Rosental, Nathaniel F. Hansen, Jody M. Beers, George Parish, Ian Rowbotham, Barbara A. Block
The lymphatic system in teleost fish has genetic and developmental origins similar to those of the mammalian lymphatic system, which is involved in immune response and fluid homeostasis. Here, we show that the lymphatic system of tunas functions in swimming hydrodynamics. Specifically, a musculo-vascular complex, consisting of fin muscles, bones, and lymphatic vessels, is involved in the hydraulic control of median fins. This specialization of the lymphatic system is associated with fish in the family Scombridae and may have evolved in response to the demand for swimming and maneuvering control in these high-performance species.
Bidirectional eukaryotic DNA replication is established by quasi-symmetrical helicase loading Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Gideon Coster, John F. X. Diffley
Bidirectional replication from eukaryotic DNA replication origins requires the loading of two ring-shaped minichromosome maintenance (MCM) helicases around DNA in opposite orientations. MCM loading is orchestrated by binding of the origin recognition complex (ORC) to DNA, but how ORC coordinates symmetrical MCM loading is unclear. We used natural budding yeast DNA replication origins and synthetic DNA sequences to show that efficient MCM loading requires binding of two ORC molecules to two ORC binding sites. The relative orientation of these sites, but not the distance between them, was found to be critical for MCM loading in vitro and origin function in vivo. We propose that quasi-symmetrical loading of individual MCM hexamers by ORC and directed MCM translocation into double hexamers acts as a unifying mechanism for the establishment of bidirectional replication in archaea and eukaryotes.
Epigenetic plasticity and the hallmarks of cancer Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 William A. Flavahan, Elizabeth Gaskell, Bradley E. Bernstein
Chromatin and associated epigenetic mechanisms stabilize gene expression and cellular states while also facilitating appropriate responses to developmental or environmental cues. Genetic, environmental, or metabolic insults can induce overly restrictive or overly permissive epigenetic landscapes that contribute to pathogenesis of cancer and other diseases. Restrictive chromatin states may prevent appropriate induction of tumor suppressor programs or block differentiation. By contrast, permissive or "plastic" states may allow stochastic oncogene activation or nonphysiologic cell fate transitions. Whereas many stochastic events will be inconsequential "passengers," some will confer a fitness advantage to a cell and be selected as "drivers." We review the broad roles played by epigenetic aberrations in tumor initiation and evolution and their potential to give rise to all classic hallmarks of cancer.
Comment on “The [4Fe4S] cluster of human DNA primase functions as a redox switch using DNA charge transport” Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Andrey G. Baranovskiy, Nigar D. Babayeva, Yinbo Zhang, Luis Blanco, Youri I. Pavlov, Tahir H. Tahirov
O’Brien et al. (Research Article, 24 February 2017, eaag1789) proposed a novel mechanism of primase function based on redox activity of the iron-sulfur cluster buried inside the C-terminal domain of the large primase subunit (p58C). Serious problems in the experimental design and data interpretation raise concerns about the validity of the conclusions.
Response to Comments on “The [4Fe4S] cluster of human DNA primase functions as a redox switch using DNA charge transport” Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Elizabeth O’Brien, Marilyn E. Holt, Matthew K. Thompson, Lauren E. Salay, Aaron C. Ehlinger, Walter J. Chazin, Jacqueline K. Barton
Baranovskiy et al. and Pellegrini argue that, based on structural data, the path for charge transfer through the [4Fe4S] domain of primase is not feasible. Our manuscript presents electrochemical data directly showing charge transport through DNA to the [4Fe4S] cluster of a primase p58C construct and a reversible switch in the DNA-bound signal with oxidation/reduction, which is inhibited by mutation of three tyrosine residues. Although the dispositions of tyrosines differ in different constructs, all are within range for microsecond electron transfer.
Comment on “The [4Fe4S] cluster of human DNA primase functions as a redox switch using DNA charge transport” Science (IF 37.205) Pub Date : 2017-07-21 00:00:00 Luca Pellegrini
O’Brien et al. (Research Article, 24 February 2017, eaag1789) report that the iron-sulfur cluster of primase has a redox role in enzyme activity. Their analysis is based on a partially misfolded structure of the iron-sulfur cluster domain of primase. In the correctly folded structure, two of the three tyrosines putatively involved in electron transfer, Y345 and Y347, contact the RNA/DNA helix, providing an alternative explanation for the data of O’Brien et al.
Cycloaddition reactions of enoldiazo compounds Chem. Soc. Rev. (IF 38.618) Pub Date : 2017-07-20 00:00:00 Qing-Qing Cheng, Yongming Deng, Marianne Lankelma, Michael P. Doyle
Impact of the Metallic Crystalline Structure on the Properties of Nanocrystals and Their Mesoscopic Assemblies Acc. Chem. Res. (IF 20.268) Pub Date : 2017-07-20 00:00:00 Marie-Paule Pileni
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