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Angewandte Chemie. international edition 84건

  1. [해외논문]   Photocontrol in Complex Polymeric Materials: Fact or Illusion?   SCI SCIE

    Jerca, Valentin Victor (Supramolecular Chemistry Group, Centre of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281-S4, 9000, Gent, Belgium) , Hoogenboom, Richard (Supramolecular Chemistry Group, Centre of Macromolecular Chemistry (CMaC), Department of Organic and Macromolecular Chemistry, Ghent University, Krijgslaan 281-S4, 9000, Gent, Belgium)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 7945 - 7947 , 2018 , 1433-7851 ,

    초록

    Photoswitches : Exciting recent progress realized in the field of light‐controlled polymeric materials is highlighted. It is discussed how the rational choice of azobenzene molecules and their incorporation into complex materials by making use of physical interactions can lead to genuine photocontrollable polymeric systems.

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  2. [해외논문]   The Pre‐exponential Factor in Electrochemistry   SCI SCIE

    He, Zheng‐ (Hefei National Laboratory for Physical Sciences at Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China) , Da (Hefei National Laboratory for Physical Sciences at Microscale, Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China) , Chen, Yan‐ (Institute of Theoretical Chemistry, Ulm University, Germany) , Xia (Institute of Theoretical Chemistry, Ulm University, Germany) , Santos, Elizabeth , Schmickler, Wolfgang
    Angewandte Chemie. international edition v.57 no.27 ,pp. 7948 - 7956 , 2018 , 1433-7851 ,

    초록

    Abstract Like many branches of science, not to mention culture in general, electrochemistry has a number of recurring topics: Areas of research that are popular for a certain time, then fade away as their possibilities seem to have been exhausted, only to return decades later as progress in experimental or theoretical techniques offer new possibilities for their investigation. A prime example are fuel cells, which have undergone five such cycles, but here we discuss a general concept of kinetics—the pre‐exponential factor of a rate constant—which has undergone two such cycles. The first cycle was in the 1950–1980s, when the methods of electrochemical kinetics were developed, and the interpretation was based on transition‐state theory. The second was triggered by the re‐discovery of Kramers theory for reactions in condensed phases. This Minireview will show that the time has come for a third cycle based on recent progress in electrocatalysis.

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  3. [해외논문]   Photobiocatalysis: Activating Redox Enzymes by Direct or Indirect Transfer of Photoinduced Electrons   SCI SCIE

    Lee, Sahng Ha (Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 335 Science Road, Daejeon, 305-701, Republic of Korea) , Choi, Da Som (Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 335 Science Road, Daejeon, 305-701, Republic of Korea) , Kuk, Su Keun (Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 335 Science Road, Daejeon, 305-701, Republic of Korea) , Park, Chan Beum (Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 335 Science Road, Daejeon, 305-701, Republic of Korea)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 7958 - 7985 , 2018 , 1433-7851 ,

    초록

    Abstract Biocatalytic transformation has received increasing attention in the green synthesis of chemicals because of the diversity of enzymes, their high catalytic activities and specificities, and mild reaction conditions. The idea of solar energy utilization in chemical synthesis through the combination of photocatalysis and biocatalysis provides an opportunity to make the “green” process greener. Oxidoreductases catalyze redox transformation of substrates by exchanging electrons at the enzyme′s active site, often with the aid of electron mediator(s) as a counterpart. Recent progress indicates that photoinduced electron transfer using organic (or inorganic) photosensitizers can activate a wide spectrum of redox enzymes to catalyze fuel‐forming reactions (e.g., H 2 evolution, CO 2 reduction) and synthetically useful reductions (e.g., asymmetric reduction, oxygenation, hydroxylation, epoxidation, Baeyer–Villiger oxidation). This Review provides an overview of recent advances in light‐driven activation of redox enzymes through direct or indirect transfer of photoinduced electrons.

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  4. [해외논문]   Oxidative Coupling of Anionic Abnormal N‐Heterocyclic Carbenes: Efficient Access to Janus‐Type 4,4′‐Bis(2H‐imidazol‐2‐ylidene)s   SCI SCIE

    Grineva, Alina A. (LCC-CNRS, Université) , Valyaev, Dmitry A. (de Toulouse, CNRS, France) , Cé (LCC-CNRS, Université) , sar, Vincent (de Toulouse, CNRS, France) , Filippov, Oleg A. (LCC-CNRS, Université) , Khrustalev, Victor N. (de Toulouse, CNRS, France) , Nefedov, Sergei E. (A. N. Nesmeyanov Institute of Organoelement Compounds (INEOS), Russian Academy of Sciences, 28 Vavilov str., GSP-1, B-334, Moscow, 119991, Russia) , Lugan, Noë (Peoples Friendship University of Russia (RUDN University), 6 Miklukho Maklaya str., Moscow, 117198, Russia) , l (Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Sciences, 31 Leninsky Pr., Moscow, 119991, Russia)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 7986 - 7991 , 2018 , 1433-7851 ,

    초록

    Abstract The oxidative coupling of anionic imidazol‐4‐ylidenes protected at the C2 position with [MnCp(CO) 2 ] or BH 3 led to the corresponding 4,4′‐bis(2 H ‐imidazol‐2‐ylidene) complexes or adducts, in which the two carbene moieties are connected through a single C−C bond. Subsequent acidic treatment of the later species led to the corresponding 4,4′‐bis(imidazolium) salts in good yields. The overall procedure offers practical access to a novel class of Janus‐type bis(NHC)s. Strikingly, the coplanarity of the two NHC rings within the mesityl derivative 4,4′‐bis(IMes), favored by steric hindrance along with stabilizing intramolecular C−H⋅⋅⋅π aryl interactions, allows the alignment of the π‐systems and, as a direct consequence, significant electron communication through the bis(carbene) scaffold.

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  5. [해외논문]   Conductive Microporous Covalent Triazine‐Based Framework for High‐Performance Electrochemical Capacitive Energy Storage   SCI SCIE

    Li, Yajuan (State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, P. R. China) , Zheng, Shuanghao (Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, P. R. China) , Liu, Xue (State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, P. R. China) , Li, Pan (State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China) , Sun, Lei (State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, P. R. China) , Yang, Ruixia (State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, P. R. China) , Wang, Sen , Wu, Zhong‐ , Shuai , Bao, Xinhe , Deng, Wei‐ , Qiao
    Angewandte Chemie. international edition v.57 no.27 ,pp. 7992 - 7996 , 2018 , 1433-7851 ,

    초록

    Abstract Nitrogen‐enriched porous nanocarbon, graphene, and conductive polymers attract increasing attention for application in supercapacitors. However, electrode materials with a large specific surface area (SSA) and a high nitrogen doping concentration, which is needed for excellent supercapacitors, has not been achieved thus far. Herein, we developed a class of tetracyanoquinodimethane‐derived conductive microporous covalent triazine‐based frameworks (TCNQ‐CTFs) with both high nitrogen content (>8 %) and large SSA (>3600 m 2 g −1 ). These CTFs exhibited excellent specific capacitances with the highest value exceeding 380 F g −1 , considerable energy density of 42.8 Wh kg −1 , and remarkable cycling stability without any capacitance degradation after 10 000 cycles. This class of CTFs should hold a great potential as high‐performance electrode material for electrochemical energy‐storage systems.

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  6. [해외논문]   Designing Efficient and Ultralong Pure Organic Room‐Temperature Phosphorescent Materials by Structural Isomerism   SCI SCIE

    Xiong, Yu (HKUST Shenzhen Research Institute, No. 9 Yuexing 1st RD, South Area, Hi-tech Park Nanshan, Shenzhen, 518057, China) , Zhao, Zheng (HKUST Shenzhen Research Institute, No. 9 Yuexing 1st RD, South Area, Hi-tech Park Nanshan, Shenzhen, 518057, China) , Zhao, Weijun (HKUST Shenzhen Research Institute, No. 9 Yuexing 1st RD, South Area, Hi-tech Park Nanshan, Shenzhen, 518057, China) , Ma, Huili (Key Laboratory of Organic Solids, Beijing National Laboratory for Molecular Science, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China) , Peng, Qian (Key Laboratory of Organic Solids, Beijing National Laboratory for Molecular Science, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China) , He, Zikai (School of Science, Harbin Institute of Technology Shenzhen, HIT Campus of University Town of Shenzhen, Shenzhen, 518055, China<countr) , Zhang, Xuepeng , Chen, Yuncong , He, Xuewen , Lam, Jacky W. Y. , Tang, Ben Zhong
    Angewandte Chemie. international edition v.57 no.27 ,pp. 7997 - 8001 , 2018 , 1433-7851 ,

    초록

    Abstract Pure organic materials with ultralong room‐temperature phosphorescence (RTP) are attractive alternatives to inorganic phosphors. However, they generally show inefficient intersystem crossing (ISC) owing to weak spin–orbit coupling (SOC). A design principle based on the realization of small energy gap between the lowest singlet and triplet states (ΔE ST ) and pure ππ* configuration of the lowest triplet state (T 1 ) via structural isomerism was used to obtain efficient and ultralong RTP materials. The meta isomer of carbazole‐substituted methyl benzoate exhibits an ultralong lifetime of 795.0 ms with a quantum yield of 2.1 %. Study of the structure–property relationship shows that the varied steric and conjugation effects imposed by ester substituent at different positions are responsible for the small ΔE ST and pure ππ* configuration of T 1 .

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  7. [해외논문]   Structural Basis of Outstanding Multivalent Effects in Jack Bean α‐Mannosidase Inhibition   SCI SCIE

    Howard, Eduardo (Department of Integrative Biology, Institut de Génétique et de Biologie Moléculaire et Cellulaire, CNRS, INSERM, UdS, 1 rue Laurent Fries, 67404, Illkirch CEDEX, France) , Cousido‐ (Department of Integrative Biology, Institut de Génétique et de Biologie Moléculaire et Cellulaire, CNRS, INSERM, UdS, 1 rue Laurent Fries, 67404, Illkirch CEDEX, France) , Siah, Alexandra (Laboratoire d'Innovation Moléculaire et Applications, Université) , Lepage, Mathieu L. (de Strasbourg|, Université) , Schneider, Jé (de Haute-Alsace|, CNRS|, LIMA (UMR 7042), Equipe de Synthèse Organique et Molécules Bioactives (SYBIO), ECPM, 25 rue Becquerel, 67000, Strasbourg, France) , ré (Laboratoire d'Innovation Moléculaire et Applications, Université) , my P. (de Strasbourg|, Université) , Bodlenner, Anne (de Haute-Alsace|, CNRS|, LIMA (UMR 7042), Equipe de Synthèse Organique et Molécules Bioactiv) , Mitschler, André , , Meli, Alessandra , Izzo, Irene , Alvarez, H. Ariel , Podjarny, Alberto , Compain, Philippe
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8002 - 8006 , 2018 , 1433-7851 ,

    초록

    Abstract Multivalent design of glycosidase inhibitors is a promising strategy for the treatment of diseases involving enzymatic hydrolysis of glycosidic bonds in carbohydrates. An essential prerequisite for successful applications is the atomic‐level understanding of how outstanding binding enhancement occurs with multivalent inhibitors. Herein we report the first high‐resolution crystal structures of the Jack bean α‐mannosidase (JBα‐man) in apo and inhibited states. The three‐dimensional structure of JBα‐man in complex with the multimeric cyclopeptoid‐based inhibitor displaying the largest binding enhancements reported so far provides decisive insight into the molecular mechanisms underlying multivalent effects in glycosidase inhibition.

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  8. [해외논문]   Toward Two‐Dimensional π‐Conjugated Covalent Organic Radical Frameworks   SCI SCIE

    Wu, Shaofei (Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore) , Li, Minchan (Department of Materials Science and Engineering, Southern University of Science and Technology, 518055, Shenzhen, China) , Phan, Hoa (Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore) , Wang, Dingguan (Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore) , Herng, Tun Seng (Department of Materials Science and Engineering, National University of Singapore, 119260, Singapore, Singapore) , Ding, Jun (Department of Materials Science and Engineering, National University of Singapore, 119260, Singapore, Singapore) , Lu, Zhouguang (Department of Materials Science and Engineering, Southern University of Science and Technology,) , Wu, Jishan
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8007 - 8011 , 2018 , 1433-7851 ,

    초록

    Abstract Reported is the synthesis, characterization, and material properties of the first π‐conjugated two‐dimensional covalent organic radical framework (CORF), PTM‐CORF , based on the stable polychlorotriphenylmethyl (PTM) radical. The covalent organic framework (COF) precursor ( PTM‐H‐COF ) was first synthesized by liquid/liquid interfacial acetylenic homocoupling of a triethynylpolychlorotriphenylmethane monomer, and showed crystalline features with a hexagonal diffraction pattern matching that of A‐B‐C stacking. Subsequent deprotonation and oxidation of the PTM units in PTM‐H‐COF gave PTM‐CORF . Magnetic measurements revealed that the neighboring PTM radicals in the PTM‐CORF are anti‐ferromagnetically coupled each other, with a moderate exchange interaction ( J = −375 cm −1 ). The PTM‐CORF has a small energy gap (ca. 0.88 eV) and a low‐lying LUMO energy level (−4.72 eV), and exhibits high electrocatalytic activity and durability toward the oxygen reduction reaction.

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  9. [해외논문]   Metal‐Catalyzed Remote Functionalization of ω‐Ene Unsaturated Ethers: Towards Functionalized Vinyl Species   SCI SCIE

    Ho, Guo‐ (Schulich Faculty of Chemistry, Technion—, Israel Institute of Technology, Haifa, 32000, Israel) , Ming (Schulich Faculty of Chemistry, Technion—, Israel Institute of Technology, Haifa, 32000, Israel) , Judkele, Lina (Schulich Faculty of Chemistry, Technion—, Israel Institute of Technology, Haifa, 32000, Israel) , Bruffaerts, Jeffrey (Schulich Faculty of Chemistry, Technion—, Israel Institute of Technology, Haifa, 32000, Israel) , Marek, Ilan
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8012 - 8016 , 2018 , 1433-7851 ,

    초록

    Abstract The combined ruthenium‐catalyzed chain walking with the nickel‐catalyzed cross‐coupling reaction of ω‐alkenyl ethers provide a unique entry to functionalized vinyl species. This transformation illustrates the power and flexibility of remote functionalization by demonstrating the compatibility of two independent reactions involving unrelated sites.

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  10. [해외논문]   Residue‐Specific Dynamics and Local Environmental Changes in Aβ40 Oligomer and Fibril Formation   SCI SCIE

    Liu, Haiyang (Department of Chemistry and Biochemistry, Florida Atlantic University, 777 Glades Road, Boca Raton, FL, 33431, USA) , Morris, Clifford (Department of Chemistry and Biochemistry, Florida Atlantic University, 777 Glades Road, Boca Raton, FL, 33431, USA) , Lantz, Richard (Department of Chemistry and Biochemistry, Florida Atlantic University, 777 Glades Road, Boca Raton, FL, 33431, USA) , Kent, Thomas W. (Department of Chemistry and Biochemistry, Florida Atlantic University, 777 Glades Road, Boca Raton, FL, 33431, USA) , Elbassal, Esmail A. (Department of Chemistry and Biochemistry, Florida Atlantic University, 777 Glades Road, Boca Raton, FL, 33431, USA) , Wojcikiewicz, Ewa P. (Department of Biomedical Science, Florida Atlantic University, 777 Glades Road, Boca Raton, FL, 33431, USA) , Du, Deguo (Department of Chemistry and Biochemistry, Florida Atlantic University, 7)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8017 - 8021 , 2018 , 1433-7851 ,

    초록

    Abstract Elucidating local dynamics of protein aggregation is crucial for understanding the mechanistic details of protein amyloidogenesis. Herein, we studied the residue‐specific dynamics and local environmental changes of Aβ40 along the course of aggregation by using para ‐cyanophenylalanine (Phe CN ) as a fluorescent and vibrational probe. Our results show that the Phe CN residues introduced at various positions all exhibited an immediate decay of fluorescence intensity, indicating a relatively synergistic process in early oligomer formation. The fast decreases in the fluorescence intensities of residues 19 and 20 in the central hydrophobic core region and residue 10 in the N‐terminal region suggest that they play crucial roles in the formation of the oligomeric core. The Phe CN 4 residue exhibits a remarkably slower decrease in fluorescence intensity, implicating its dynamic conformational characteristics in oligomer and fibril formation. Our results also suggest that the N‐terminal residues in fibrils are surrounded by a relatively hydrophobic local environment, as opposed to being solvated.

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