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Angewandte Chemie. international edition 84건

  1. [해외논문]   Blurring the Lines between Host and Guest: A Chimeric Receptor Derived from Cucurbituril and Triptycene   SCI SCIE

    Lu, Xiaoyong (Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA) , Samanta, Soumen K. (Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA) , Zavalij, Peter Y. (Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA) , Isaacs, Lyle (Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8073 - 8078 , 2018 , 1433-7851 ,

    초록

    Abstract We report the synthesis and X‐ray crystal structure of a cucurbituril–triptycene chimeric receptor ( 1 ). Host 1 binds to guests typical of CB[6]–CB[8], but also binds to larger guests such as blue box ( 20 ) and the Fujita square ( 22 ). Intriguingly, the geometries of the 1 ⋅ 20 and 1 ⋅ 22 complexes blur the lines between host and guest in that both components fulfill both roles within each complex. The fluorescence output of 1 is fully quenched by the formation of complexes with pyridinium‐derived guests.

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  2. [해외논문]   Synthesis, Structure, Bonding, and Reactivity of Metal Complexes Comprising Diborane(4) and Diborene(2): [{Cp*Mo(CO)2}2{μ‐η2:η2‐B2H4}] and [{Cp*M(CO)2}2B2H2M(CO)4], M=Mo,W   SCI SCIE

    Mondal, Bijan (Department of Chemistry, Indian Institute of Technology Madras, Chennai, 600 036, India) , Bag, Ranjit (Department of Chemistry, Indian Institute of Technology Madras, Chennai, 600 036, India) , Ghorai, Sagar (Inorganic and Physical Chemistry Department, Indian Institute of Science, Bangalore, 560012, India) , Bakthavachalam, K. (Department of Chemistry, Indian Institute of Technology Madras, Chennai, 600 036, India) , Jemmis, Eluvathingal D. (Inorganic and Physical Chemistry Department, Indian Institute of Science, Bangalore, 560012, India) , Ghosh, Sundargopal (Department of Chemistry, Indian Institute of Technology Madras, Chennai, 600 036, India)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8079 - 8083 , 2018 , 1433-7851 ,

    초록

    Abstract The reaction of [(Cp*Mo) 2 (μ‐Cl) 2 B 2 H 6 ] ( 1 ) with CO at room temperature led to the formation of the highly fluxional species [{Cp*Mo(CO) 2 } 2 {μ‐η 2 :η 2 ‐B 2 H 4 }] ( 2 ). Compound 2, to the best of our knowledge, is the first example of a bimetallic diborane(4) conforming to a singly bridged C s structure. Theoretical studies show that 2 mimics the Cotton dimolybdenum–alkyne complex [{CpMo(CO) 2 } 2 C 2 H 2 ]. In an attempt to replace two hydrogen atoms of diborane(4) in 2 with a 2e [W(CO) 4 ] fragment, [{Cp*Mo(CO) 2 } 2 B 2 H 2 W(CO) 4 ] ( 3 ) was isolated upon treatment with [W(CO) 5 ⋅thf]. Compound 3 shows the intriguing presence of [B 2 H 2 ] with a short B−B length of 1.624(4) A. We isolated the tungsten analogues of 3 , [{Cp*W(CO) 2 } 2 B 2 H 2 W(CO) 4 ] ( 4 ) and [{Cp*W(CO) 2 } 2 B 2 H 2 Mo(CO) 4 ] ( 5 ), which provided direct proof of the existence of the tungsten analogue of 2 .

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  3. [해외논문]   Synthesis, Characterization, and Functionalization of 1‐Boraphenalenes   SCI SCIE

    Kahan, Rachel J. (School of Chemistry, University of Manchester, Manchester, M13 9PL, UK) , Crossley, Daniel L. (School of Chemistry, University of Manchester, Manchester, M13 9PL, UK) , Cid, Jessica (School of Chemistry, University of Manchester, Manchester, M13 9PL, UK) , Radcliffe, James E. (School of Chemistry, University of Manchester, Manchester, M13 9PL, UK) , Ingleson, Michael J. (School of Chemistry, University of Manchester, Manchester, M13 9PL, UK)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8084 - 8088 , 2018 , 1433-7851 ,

    초록

    Abstract 1‐Boraphenalenes have been synthesized by reaction of BBr 3 with 1‐(aryl‐ethynyl)naphthalenes, 1‐ethynylnaphthalene, and 1‐(pent‐1‐yn‐1‐yl)naphthalene and they can be selectively functionalized at boron or carbon to form bench‐stable products. All of these 1‐boraphenalenes have LUMOs localized on the planar C 12 B core that are closely comparable in character to isoelectronic phenalenyl cations. In contrast to the comparable LUMOs, the aromatic stabilization of the C 5 B ring in 1‐boraphenalenes is dramatically lower than the C 6 rings in phenalenyl cations. This is due to the occupied orbitals of π symmetry being less delocalised in the 1‐boraphenalenes.

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  4. [해외논문]   Two Amphoteric Silver Carbene Clusters   SCI SCIE

    Tskhovrebov, Alexander G. (Max-Planck-Institut für Kohlenforschung, 45470, Mülheim/Ruhr, Germany) , Goddard, Richard (Max-Planck-Institut für Kohlenforschung, 45470, Mülheim/Ruhr, Germany) , Fü (Max-Planck-Institut für Kohlenforschung, 45470, Mülheim/Ruhr, Germany) , rstner, Alois
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8089 - 8094 , 2018 , 1433-7851 ,

    초록

    Abstract Two highly labile silver carbene cluster complexes are described, which are unique in that they mark the transition point at which the carbene center transmutes from a fairly common NHC‐like nucleophilic behavior to an electrophilic character befitting reactive silver carbene intermediates of relevance in various catalytic transformations. This amphoteric character is the distinguishing attribute of a μ‐bridged donor/donor carbene entity that connects two silver atoms of triangular or tetrahedral metallic core units.

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  5. [해외논문]   Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process   SCI SCIE

    Chowdhury, Abhishek Dutta (Inorganic Chemistry and Catalysis Group, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands) , Paioni, Alessandra Lucini (NMR Spectroscopy group, Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH, Utrecht, The Netherlands) , Houben, Klaartje (NMR Spectroscopy group, Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH, Utrecht, The Netherlands) , Whiting, Gareth T. (Inorganic Chemistry and Catalysis Group, Debye Institute for Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584, CG, Utrecht, The Netherlands) , Baldus, Marc (NMR Spectroscopy group, Bijvoet Center for Biomolecular Research, Utrecht University, Padualaan 8, 3584 CH, Utrecht, The Netherlands) , Weckhuysen, Bert M. (Inorganic Chemistry and Catalysis Group, Debye Institute for Nanomaterials Scienc)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8095 - 8099 , 2018 , 1433-7851 ,

    초록

    Abstract After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the “direct mechanism”‐derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H‐SAPO‐34 catalyst, using a combination of advanced solid‐state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on‐line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C−C bond‐containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon‐based co‐catalytic organic reaction centers.

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  6. [해외논문]   Identification of an Asexual Reproduction Inducer of Phytopathogenic and Toxigenic Fusarium   SCI SCIE

    Qi, Jianhua (College of Pharmaceutical Sciences, Zhejiang University, Yu Hang Tang Road 866, Hangzhou, 310058, P. R. China) , Cheng, Lihong (College of Pharmaceutical Sciences, Zhejiang University, Yu Hang Tang Road 866, Hangzhou, 310058, P. R. China) , Sun, Yujuan (College of Pharmaceutical Sciences, Zhejiang University, Yu Hang Tang Road 866, Hangzhou, 310058, P. R. China) , Hirata, Yushi (Graduate School of Bioagricultural Sciences, Nagoya University, Chikusa-ku, Nagoya, 464-8601, Japan) , Ushida, Naoki (Graduate School of Bioagricultural Sciences, Nagoya University, Chikusa-ku, Nagoya, 464-8601, Japan) , Ma, Zhonghua (Institute of Biotechnology, Zhejiang University, Yu Hang Tang Road 866, Hangzhou, 310058, P. R. China) , Osada, Hiroyuki (Chemical Biology Research Group, RIKEN Center for Sustainable Resource Science, Wako-shi, Saitama, 351-0198, Japan) , Nishikawa, Toshio , Xiang, Lan
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8100 - 8104 , 2018 , 1433-7851 ,

    초록

    Abstract Asexual and sexual reproduction are the most important biological events in the life cycle of phytopathogenic and toxigenic Fusarium and are responsible for disease epidemics. However, the signaling molecules which induce the asexual reproduction of Fusarium are unknown. Herein we describe the structure elucidation, including the absolute configuration, of Fusarium asexual reproduction inducer (FARI), a new sesquiterpene derivative, by spectroscopic analysis, total synthesis, and conidium‐inducing assays of synthetic isomers. We have also uncovered the universality of FARI among Fusarium species. Moreover, a mechanism‐of‐action study suggested that the Gpmk1 and LaeA signaling pathways are required for conidium formation induced by FARI; conversely, the Mgv1 of mitogen‐activated protein kinase is not involved in conidium formation. FARI exhibited conidium‐inducing activity at an extremely low dose and high stereoselectivity, which may suggest the presence of a stereospecific target.

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  7. [해외논문]   Light‐Induced Reversible Reconfiguration of DNA‐Based Constitutional Dynamic Networks: Application to Switchable Catalysis   SCI SCIE

    Wang, Shan (Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem, 91904, Israel) , Yue, Liang (Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew University of Jerusalem, Jerusalem, 91904, Israel) , Li, Zi‐ (Key Laboratory for Advanced Materials, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China) , Yuan (Key Laboratory for Advanced Materials, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China) , Zhang, Junji (Key Laboratory for Advanced Materials, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China) , Tian, He (Institute of Chemistry, The Center for Nanoscience and Nanotechnology, The Hebrew U) , Willner, Itamar
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8105 - 8109 , 2018 , 1433-7851 ,

    초록

    Abstract The light‐induced reversible and cyclic reconfiguration of constitutional dynamic networks, consisting of supramolecular nucleic acid structures as constituents and a photoisomerizable trans / cis ‐azobenzene‐functionalized nucleic acid as the trigger is demonstrated. In addition, the cyclic photochemical reconfiguration of the constitutional dynamic networks guides the switchable on/off operation of an emerging hemin/G‐quadruplex DNAzyme.

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  8. [해외논문]   Chemical/Light‐Powered Hybrid Micromotors with “On‐the‐Fly” Optical Brakes   SCI SCIE

    Chen, Chuanrui (Department of Nanoengineering, University of California, San Diego, La Jolla, CA, 92093, USA) , Tang, Songsong (Department of Nanoengineering, University of California, San Diego, La Jolla, CA, 92093, USA) , Teymourian, Hazhir (Department of Nanoengineering, University of California, San Diego, La Jolla, CA, 92093, USA) , Karshalev, Emil (Department of Nanoengineering, University of California, San Diego, La Jolla, CA, 92093, USA) , Zhang, Fangyu (Department of Nanoengineering, University of California, San Diego, La Jolla, CA, 92093, USA) , Li, Jinxing (Department of Nanoengineering, University of California, San Diego, La Jolla, CA, 92093, USA) , Mou, Fangzhi (State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, P. R. China) , Liang, Yuyan (Department of) , Guan, Jianguo , Wang, Joseph
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8110 - 8114 , 2018 , 1433-7851 ,

    초록

    Abstract Hybrid micromotors capable of both chemically powered propulsion and fuel‐free light‐driven actuation and offering built‐in optical brakes for chemical propulsion are described. The new hybrid micromotors are designed by combining photocatalytic TiO 2 and catalytic Pt surfaces into a Janus microparticle. The chemical reactions on the different surfaces of the Janus particle hybrid micromotor can be tailored by using chemical or light stimuli that generate counteracting propulsion forces on the catalytic Pt and photocatalytic TiO 2 sides. Such modulation of the surface chemistry on a single micromotor leads to switchable propulsion modes and reversal of the direction of motion that reflect the tuning of the local ion concentration and hence the dominant propulsion force. An intermediate Au layer (under the Pt surface) plays an important role in determining the propulsion mechanism and operation of the hybrid motor. The built‐in optical braking system allows “on‐the‐fly” control of the chemical propulsion through a photocatalytic reaction on the TiO 2 side to counterbalance the chemical propulsion force generated on the Pt side. The adaptive dual operation of these chemical/light hybrid micromotors, associated with such control of the surface chemistry, holds considerable promise for designing smart nanomachines that autonomously reconfigure their propulsion mode for various on‐demand operations.

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  9. [해외논문]   Electro‐Oxidative S−H/S−H Cross‐Coupling with Hydrogen Evolution: Facile Access to Unsymmetrical Disulfides   SCI SCIE

    Huang, Pengfei (Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China) , Wang, Pan (Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China) , Tang, Shan (Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China) , Fu, Zhuangjiong (Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China) , Lei, Aiwen (Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan, 430072, Hubei, P. R. China)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8115 - 8119 , 2018 , 1433-7851 ,

    초록

    Abstract Sulfur is an essential element because it exists widely in proteins. The disulfide bond is an important moiety in many different types of significant organic molecules. A new approach for oxidant‐ and catalyst‐free S−H/S−H cross‐coupling, with hydrogen evolution, to construct unsymmetrical disulfides was developed. Under the conditions of an undivided cell at room temperature, a series of unsymmetrical disulfides were prepared with up to 87 % yield from the direct coupling of an aryl mercaptan and alkyl mercaptan. Gram‐scale synthesis also highlights the synthetic utility of this electrochemical strategy.

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  10. [해외논문]   Self‐Reporting Inhibitors: A Single Crystallization Process To Obtain Two Optically Pure Enantiomers   SCI SCIE

    Ye, Xichong (Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China) , Cui, Jiaxi (INM—, Leibniz Institute for New Materials, Campus D22, 66123, Saarbrucken, Germany) , Li, Bowen (Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China) , Li, Na (Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China) , Zhang, Jie (Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry and Physics of) , Wan, Xinhua
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8120 - 8124 , 2018 , 1433-7851 ,

    초록

    Abstract Collection of two optically pure enantiomers in a single crystallization process can significantly increase the chiral separation efficiency but this is difficult to realize. Now a self‐reporting strategy is presented for visualizing the crystallization process by a dyed self‐assembled inhibitor made from the copolymers with tri(ethylene glycol)‐grafting polymethylsiloxane as the main chain and poly(N 6 ‐methacryloyl‐ l ‐lysine) as side chains. When applied with seeds together for the fractional crystallization of conglomerates, the inhibitors can label the formation of the secondary crystals and guide the complete separation process of two enantiomers with colorless crystals as the first product and red crystals as the second. This method leads to high optical purity of d / l ‐Asn⋅H 2 O (99.9 % ee for d ‐crystals and 99.5 % for l ‐crystals) in a single crystallization process. It requires a small amount of additives and shows excellent recyclability.

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