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https://www.readbyqxmd.com/read/28212484/on-surface-site-selective-cyclization-of-corrole-radicals
#1
Stefano Tebi, Mateusz Paszkiewicz, Hazem Aldahhak, Francesco Allegretti, Sabrina Gonglach, Michael Haas, Mario Waser, Peter S Deimel, Pablo Casado Aguilar, Yi-Qi Zhang, Anthoula C Papageorgiou, David Andrew Duncan, Johannes V Barth, Wolf Gero Schmidt, Reinhold Koch, Uwe Gerstmann, Eva Rauls, Florian Klappenberger, Wolfgang Schöfberger, Stefan Müllegger
Radical cyclization is among the most powerful and versatile reactions for constructing mono- and polycyclic systems, but has, to date, remained unexplored in the context of on-surface synthesis. We report the controlled on-surface synthesis of stable corrole radicals on Ag(111) via site-specific dehydrogenation of a pyrrole N H bond in the 5,10,15-tris(pentafluoro-phenyl)-corrole triggered by annealing at 330 K under ultra-high vacuum conditions. We reveal a thermally-induced regioselective cyclization reaction mediated by a radical cascade and resolve the reaction mechanism of the pertaining cyclodefluorination reaction at the single-molecule level...
February 17, 2017: ACS Nano
https://www.readbyqxmd.com/read/28212395/delayed-apoptosis-allows-islet-%C3%AE-cells-to-implement-an-autophagic-mechanism-to-promote-cell-survival
#2
Heather L Hayes, Brett S Peterson, Jonathan M Haldeman, Christopher B Newgard, Hans E Hohmeier, Samuel B Stephens
Increased β-cell death coupled with the inability to replicate existing β-cells drives the decline in β-cell mass observed in the progression of both major forms of diabetes. Understanding endogenous mechanisms of islet cell survival could have considerable value for the development of novel strategies to limit β-cell loss and thereby promote β-cell recovery. Insulinoma cells have provided useful insight into β-cell death pathways but observations made in cell lines sometimes fail to translate to primary islets...
2017: PloS One
https://www.readbyqxmd.com/read/28212352/rta-occupancy-of-the-origin-of-lytic-replication-during-murine-gammaherpesvirus-68-reactivation-from-b-cell-latency
#3
Alexis L Santana, Darby G Oldenburg, Varvara Kirillov, Laraib Malik, Qiwen Dong, Roman Sinayev, Kenneth B Marcu, Douglas W White, Laurie T Krug
RTA, the viral Replication and Transcription Activator, is essential for rhadinovirus lytic gene expression upon de novo infection and reactivation from latency. Lipopolysaccharide (LPS)/toll-like receptor (TLR)4 engagement enhances rhadinovirus reactivation. We developed two new systems to examine the interaction of RTA with host NF-kappaB (NF-κB) signaling during murine gammaherpesvirus 68 (MHV68) infection: a latent B cell line (HE-RIT) inducible for RTA-Flag expression and virus reactivation; and a recombinant virus (MHV68-RTA-Bio) that enabled in vivo biotinylation of RTA in BirA transgenic mice...
February 16, 2017: Pathogens
https://www.readbyqxmd.com/read/28212330/synthesis-of-8-aryl-o-methylcyanidins-and-their-usage-for-dye-sensitized-solar-cell-devices
#4
Yuki Kimura, Kin-Ichi Oyama, Yasujiro Murata, Atsushi Wakamiya, Kumi Yoshida
Anthocyanins as natural pigments are colorful and environmentally compatible dyes for dye-sensitized solar cells (DSSCs). To increase the efficiency, we designed and synthesized unnatural O-methylflavonols and O-methylcyanidins that possess an aryl group at the 8-position. We synthesized per-O-methylquercetin from quercetin, then using selective demethylation prepared various O-methylquercetins. Using the Suzuki-Miyaura coupling reaction, 8-arylation of per-O-methylquercetin was achieved. Using a LiAlH₄ reduction or Clemmensen reduction, these flavonols were transformed to the corresponding cyanidin derivatives in satisfactory yields...
February 16, 2017: International Journal of Molecular Sciences
https://www.readbyqxmd.com/read/28212282/collagen-gold-nanoparticle-conjugates-for-versatile-biosensing
#5
Sarah Unser, Samuel Holcomb, ReJeana Cary, Laura Sagle
Integration of noble metal nanoparticles with proteins offers promising potential to create a wide variety of biosensors that possess both improved selectivity and versatility. The multitude of functionalities that proteins offer coupled with the unique optical properties of noble metal nanoparticles can allow for the realization of simple, colorimetric sensors for a significantly larger range of targets. Herein, we integrate the structural protein collagen with 10 nm gold nanoparticles to develop a protein-nanoparticle conjugate which possess the functionality of the protein with the desired colorimetric properties of the nanoparticles...
February 15, 2017: Sensors
https://www.readbyqxmd.com/read/28212175/advances-in-epilepsy-gene-discovery-and-implications-for-epilepsy-diagnosis-and-treatment
#6
Joseph D Symonds, Sameer M Zuberi, Michael R Johnson
PURPOSE OF REVIEW: Epilepsy genetics is shifting from the academic pursuit of gene discovery to a clinical discipline based on molecular diagnosis and stratified medicine. We consider the latest developments in epilepsy genetics and review how gene discovery in epilepsy is influencing the clinical classification of epilepsy and informing new therapeutic approaches and drug discovery. RECENT FINDINGS: Recent studies highlighting the importance of mutation in GABA receptors, NMDA receptors, potassium channels, G-protein coupled receptors, mammalian target of rapamycin pathway and chromatin remodeling are discussed...
February 15, 2017: Current Opinion in Neurology
https://www.readbyqxmd.com/read/28212156/impact-of-very-low-anti-m%C3%A3-llerian-hormone-on-pregnancy-success
#7
Alberto Pacheco, María Cruz, Juan A García-Velasco
PURPOSE OF REVIEW: Biomarkers are useful tool to help clinicians to estimate the chances of pregnancy of an infertile couple prior to assisted reproductive treatment. One proposed candidate is anti-Müllerian hormone (AMH), but its role as a predictor of reproductive success, especially in patients with low or very low levels, is under discussion. This review highlights recent findings from literature regarding to reproductive outcome in women with very low levels of AMH. RECENT FINDINGS: Although there is a general agreement about the lower pregnancy rates of patients with very low levels of AMH compared with patients with normal AMH levels, the role of AMH as a predictor of success is still under discussion...
February 15, 2017: Current Opinion in Obstetrics & Gynecology
https://www.readbyqxmd.com/read/28212094/characteristics-of-myosin-v-processivity
#8
Jun-Ping Zhang, Yi Liu, Wei Sun, Xiaoyang Zhao, Ta La, Wei-Sheng Guo
Myosin V is a processive doubled-headed biomolecular motor involved in many intracellular organelle and vesicle transport. The unidirectional movement is coupled with the adenosine triphosphate (ATP) hydrolysis and product release cycle. With the progress of experimental techniques and the enhancement of measuring directness, detailed knowledge of the motility of myosin V has been obtained.Following the ATPase cycle, the 4-state mechanochemical model of the myosin V's processive movement is used. The transitions between various states take place in a stochastic manner...
February 14, 2017: IEEE/ACM Transactions on Computational Biology and Bioinformatics
https://www.readbyqxmd.com/read/28212091/multistability-and-bifurcation-analysis-of-inhibitory-coupled-cyclic-genetic-regulatory-networks-with-delays
#9
Guang Ling, Zhi-Hong Guan, Bin Hu, Qiang Lai, Yonghong Wu
Many biological systems have the conspicuous property to present more than one stable state and diverse rhythmic behaviors. A closed relationship between these complex dynamic behaviors and cyclic genetic structures has been witnessed by pioneering works. In this paper, a typical structure of inhibitory coupled cyclic genetic networks is introduced to further enlighten this mechanism of stability and biological rhythms of living cells. The coupled networks consist two identical cyclic genetic subnetworks, which inhibit each other directly...
February 14, 2017: IEEE Transactions on Nanobioscience
https://www.readbyqxmd.com/read/28212073/a-two-time-scale-neurodynamic-approach-to-constrained-minimax-optimization
#10
Xinyi Le, Jun Wang
This paper presents a two-time-scale neurodynamic approach to constrained minimax optimization using two coupled neural networks. One of the recurrent neural networks is used for minimizing the objective function and another is used for maximization. It is shown that the coupled neurodynamic systems operating in two different time scales work well for minimax optimization. The effectiveness and characteristics of the proposed approach are illustrated using several examples. Furthermore, the proposed approach is applied for H∞ model predictive control...
March 2017: IEEE Transactions on Neural Networks and Learning Systems
https://www.readbyqxmd.com/read/28212072/neural-network-based-solutions-for-stochastic-optimal-control-using-path-integrals
#11
Karthikeyan Rajagopal, Sivasubramanya Nadar Balakrishnan, Jerome R Busemeyer
In this paper, an offline approximate dynamic programming approach using neural networks is proposed for solving a class of finite horizon stochastic optimal control problems. There are two approaches available in the literature, one based on stochastic maximum principle (SMP) formalism and the other based on solving the stochastic Hamilton-Jacobi-Bellman (HJB) equation. However, in the presence of noise, the SMP formalism becomes complex and results in having to solve a couple of backward stochastic differential equations...
March 2017: IEEE Transactions on Neural Networks and Learning Systems
https://www.readbyqxmd.com/read/28212063/conflict-resolution-styles-as-mediators-of-female-child-sexual-abuse-experience-and-heterosexual-couple-relationship-satisfaction-and-stability-in-adulthood
#12
Ashlee E Knapp, Darin J Knapp, Cameron C Brown, Jeffry H Larson
Trauma from female incestuous child sexual abuse may result in negative psychological consequences affecting adult relationships. This study explored relational consequences of incestuous child sexual abuse, focusing on conflict resolution styles, relationship satisfaction, and relationship stability. Using the RELATionship Evaluation dataset, 457 heterosexual couples in which female partners experienced incestuous child sexual abuse were compared to a group of 1,827 couples with no sexual abuse history. Analyses tested differences in the frequencies of reported conflict resolution styles for incestuous child sexual abuse and non-incestuous child sexual abuse groups, the mediating effects of conflict resolution styles on the relationship between incestuous child sexual abuse, and self- and partner-reported relationship satisfaction and stability...
January 2017: Journal of Child Sexual Abuse
https://www.readbyqxmd.com/read/28212037/coupled-thermodynamic-and-kinetic-changes-in-the-electrochemistry-of-ferrocenyl-monolayers-induced-by-light
#13
Ying Yang, Simone Ciampi, John Justin Gooding
We report on the light-induced systematic changes to the thermodynamics and kinetics of ferrocene units attached to a n-type silicon(100) photoelectrode. Both the reaction rate, as well as the energetics of the charge transfer, are simultaneously affected by changes to the intensity of the incident light. Cyclic voltammetry shows that increases in intensity of illumination can drive the redox process toward less positive potentials, with a downhill shift in E1/2 of ca. 160 mV by increasing light intensity from 3 to 94 mW cm-2...
February 17, 2017: Langmuir: the ACS Journal of Surfaces and Colloids
https://www.readbyqxmd.com/read/28212027/ferromagnetic-coupling-in-the-heterospin-bis-catecholato-manganese-iv-complex-with-pyridine-substituted-by-nitronyl-nitroxide
#14
Michael P Bubnov, Irina A Teplova, Eugenia A Kopylova, Konstantin A Kozhanov, Artem S Bogomyakov, Marina V Petrova, Vitaly A Morozov, Victor I Ovcharenko, Vladimir K Cherkasov
A new bis(3,6-di-tert-butyl-catecholato)manganese complex with two 4-NIT-Py ligands was synthesized and characterized [4-NIT-Py = pyridine substituted at position 4 with nitronyl-nitroxide radical, 2-(pyridin-4-yl)-4,4,5,5-tetramethyl-4,5-dihydro-1H-imidazole-3-oxide-1-oxyl]. X-ray diffraction indicated an octahedral environment of the manganese atom with a trans arrangement of ligands. Bonds lengths in the inner coordination core of the metal and in the chelate cycles that are representative of the charge distribution between the metal and ligands displayed a Mn(IV)(Cat(2-))2 charge distribution...
February 17, 2017: Inorganic Chemistry
https://www.readbyqxmd.com/read/28212025/advances-in-tip-enhanced-near-field-raman-microscopy-using-nanoantennas
#15
Xian Shi, Nicolás Coca-López, Julia Janik, Achim Hartschuh
Tip-enhanced near-field Raman microscopy spectroscopy is a scanning probe technique that is capable of providing vibrational spectroscopic information on single nanoobjects and surfaces at (sub-) nanometer spatial resolution and high detection sensitivity. In this review, we first illustrate the physical principle of optical nanoantennas used in tip-enhanced near-field Raman microscopy and tip-enhanced Raman scattering (TERS) to efficiently couple light to Raman excitations on nanometer length scales. Although the antennas' electric near-field distributions are commonly understood to determine the spatial resolution, recent experiments showing subnanometer-resolved optical images put this understanding into question...
February 17, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28212019/complete-nutrient-removal-coupled-to-nitrous-oxide-production-as-a-bioenergy-source-by-denitrifying-polyphosphate-accumulating-organisms
#16
Han Gao, Miaomiao Liu, James S Griffin, Longcheng Xu, Da Xiang, Yaniv D Scherson, Wen-Tso Liu, George F Wells
Coupled Aerobic-anoxic Nitrous Decomposition Operation (CANDO) is a promising emerging bioprocess for wastewater treatment that enables direct energy recovery from nitrogen (N) in three steps: (1) ammonium oxidation to nitrite; (2) denitrification of nitrite to nitrous oxide (N2O); and (3) N2O conversion to N2 with energy generation. However, CANDO does not currently target phosphorus (P) removal. Here, we demonstrate that denitrifying polyphosphate accumulating organism (PAO) enrichment cultures are capable of catalyzing simultaneous biological N and P removal coupled to N2O generation in a 2nd generation CANDO process, CANDO+P...
February 17, 2017: Environmental Science & Technology
https://www.readbyqxmd.com/read/28212014/metal-free-synthesis-of-c-4-substituted-pyridine-derivatives-using-pyridine-boryl-radicals-via-a-radical-addition-coupling-mechanism-a-combined-computational-and-experimental-study
#17
Guoqiang Wang, Jia Cao, Liuzhou Gao, Wenxin Chen, Wenhao Huang, Xu Cheng, Shuhua Li
Density functional theory investigations revealed that the pyridine-boryl radical generated in situ using 4-cyanopyridine and bis(pinacolato)diboron could be used as a bifunctional "reagent", which serves as not only a pyridine precursor but also a boryl radical. With the unique reactivity of such radicals, 4-substituted pyridine derivatives could be synthesized using α, β-unsaturated ketones and 4-cyanopyridine via a novel radical addition/C-C coupling mechanism. Several controlled experiments were conducted to provide supportive evidence for the proposed mechanism...
February 17, 2017: Journal of the American Chemical Society
https://www.readbyqxmd.com/read/28211966/formation-of-organometallic-intermediate-states-in-on-surface-ullmann-couplings
#18
Dennis Barton, Hong-Ying Gao, Philipp Alexander Held, Armido Studer, Harald Fuchs, Nikos L Doltsinis, Johannes Neugebauer
Possible origins of the formation of organometallic intermediates in on-surface Ullmann couplings have been investigated by surface tunneling microscopy (STM) and density functional theory (DFT) calculations. We consider the case of iodobenzenes on the coinage metals Au, Ag and Cu. We found experimental evidence for the formation of surface vacancies and the presence of metal adatoms in these coupling reactions, which are taken as a hint for the reactive extraction of surface atoms by adsorbates. In a second step, we demonstrate by ab initio molecular dynamics calculations for aryl-iodides on copper that metal atoms can be pulled out of the surface to form metalorganic species...
February 17, 2017: Chemistry: a European Journal
https://www.readbyqxmd.com/read/28211892/high-throughput-in-situ-cell-electroporation-microsystem-for-parallel-delivery-of-single-guide-rnas-into-mammalian-cells
#19
Shengtai Bian, Yicen Zhou, Yawei Hu, Jing Cheng, Xiaofang Chen, Youchun Xu, Peng Liu
Arrayed genetic screens mediated by the CRISPR/Cas9 technology with single guide RNA (sgRNA) libraries demand a high-throughput platform capable of transfecting diverse cell types at a high efficiency in a genome-wide scale for detection and analysis of sophisticated cellular phenotypes. Here we developed a high-throughput in situ cell electroporation (HiCEP) microsystem which leveraged the superhydrophobic feature of the microwell array to achieve individually controlled conditions in each microwell and coupled an interdigital electrode array chip with the microwells in a modular-based scheme for highly efficient delivery of exogenous molecules into cells...
February 13, 2017: Scientific Reports
https://www.readbyqxmd.com/read/28211844/a-tool-named-iris-for-versatile-high-throughput-phenotyping-in-microorganisms
#20
George Kritikos, Manuel Banzhaf, Lucia Herrera-Dominguez, Alexandra Koumoutsi, Morgane Wartel, Matylda Zietek, Athanasios Typas
Advances in our ability to systematically introduce and track controlled genetic variance in microorganisms have, in the past decade, fuelled high-throughput reverse genetics approaches. When coupled to quantitative readouts, such approaches are extremely powerful at elucidating gene function and providing insights into the underlying pathways and the overall cellular network organization. Yet, until now, all efforts to quantify microbial macroscopic phenotypes have been restricted to monitoring growth in a small number of model microorganisms...
February 17, 2017: Nature Microbiology
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