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Angewandte Chemie. international edition 84건

  1. [해외논문]   Multipronged Biomimetic Approach To Create Optically Tunable Nanoparticles   SCI SCIE

    Harmatys, Kara M. (Princess Margaret Cancer Centre, University Health Network, 101 College St., PMCRT 5-354, Toronto, ON, Canada) , Chen, Juan (Princess Margaret Cancer Centre, University Health Network, 101 College St., PMCRT 5-354, Toronto, ON, Canada) , Charron, Danielle M. (Princess Margaret Cancer Centre, University Health Network, 101 College St., PMCRT 5-354, Toronto, ON, Canada) , MacLaughlin, Christina M. (Princess Margaret Cancer Centre, University Health Network, 101 College St., PMCRT 5-354, Toronto, ON, Canada) , Zheng, Gang (Princess Margaret Cancer Centre, University Health Network, 101 College St., PMCRT 5-354, Toronto, ON, Canada)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8125 - 8129 , 2018 , 1433-7851 ,

    초록

    Abstract Current biomimetics for medical applications use a single biomimetic approach to imitate natural structures, which can be insufficient for reconstructing structurally complex natural systems. Multipronged efforts may resolve these complexities. To achieve interesting nanostructure‐driven optical properties, a dual‐biomimetic system contained within a single nanoagent was engineered to recapitulate chlorosomes, efficient light‐harvesting organelles that have unique dye assemblies and tunable photonic properties. A series of chlorin dyes was synthesized, and these hydrophobic assemblies were stabilized inside a high‐density lipoprotein, a second biomimetic that enabled in vivo utility. This system resulted in tunable tumor imaging of intact (photoacoustic) and disrupted (activatable fluorescence) nanostructures. The successful demonstration of this multipronged biomimetic approach opens the door for reconstruction of complex natural systems for biomedical applications.

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  2. [해외논문]   Real‐Time Probing of Nanowire Assembly Kinetics at the Air–Water Interface by In Situ Synchrotron X‐Ray Scattering   SCI SCIE

    He, Zhen (Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, Hefei Science Center of CAS, University of Science and Technology of China, Hefei, 230026, China) , Jiang, Hui‐ (Department of Chemical Physics & Hefei National Research Center for Physical Sciences at Microscales, iChEM, University of Science and Technology of China, Hefei, 230026, China) , Jun (School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China) , Wu, Long‐ (Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, Hefei Science Ce) , Long , Liu, Jian‐ , Wei , Wang, Geng , Wang, Xiao , Wang, Jin‐ , Long , Hou, Zhong‐ , Huai , Chen, Gang , Yu, Shu‐ , Hong
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8130 - 8134 , 2018 , 1433-7851 ,

    초록

    Abstract Although many assembly strategies have been used to successfully construct well‐aligned nanowire (NW) assemblies, the understanding of their assembly kinetics has remained elusive, which restricts the development of NW‐based device and circuit fabrication. Now a versatile strategy that combines interfacial assembly and synchrotron‐based grazing‐incidence small‐angle X‐ray scattering (GISAXS) is presented to track the assembly evolution of the NWs in real time. During the interface assembly process, the randomly dispersed NWs gradually aggregate to form small ordered NW‐blocks and finally are constructed into well‐defined NW monolayer driven by the conformation entropy. The NW assembly mechanism can be well revealed by the thermodynamic analysis and large‐scale molecular dynamics theoretical evaluation. These findings point to new opportunities for understanding NW assembly kinetics and manipulating NW assembled structures by bottom‐up strategy.

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  3. [해외논문]   Stabilized Vanadium Catalyst for Olefin Polymerization by Site Isolation in a Metal–Organic Framework   SCI SCIE

    Comito, Robert J. (Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA) , Wu, Zhenwei (Davidson School of Chemical Engineering, Purdue University, 480 Stadium Mall Dr., West Lafayette, IN, 47907, USA) , Zhang, Guanghui (Davidson School of Chemical Engineering, Purdue University, 480 Stadium Mall Dr., West Lafayette, IN, 47907, USA) , Lawrence III, John A. (Aramco Research Center—, Boston, Aramco Services Company, 400 Technology Square, Cambridge, MA, 02139, USA) , Korzyń (Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA, 02139, USA) , ski, Maciej D. (Department of Chemistry, Eugene F. Merkert Chemistry Center, Boston College, Chestnut Hill, MA, 02467, USA) , Kehl, Jeffrey A. (Davidson School of Chemical Engineering, Purdue University, 480 Stadium Mall) , Miller, Jeffrey T. , Dincă , , Mircea
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8135 - 8139 , 2018 , 1433-7851 ,

    초록

    Abstract Vanadium catalysts offer unique selectivity in olefin polymerization, yet are underutilized industrially owing to their poor stability and productivity. Reported here is the immobilization of vanadium by cation exchange in MFU‐4 l , thus providing a metal–organic framework (MOF) with vanadium in a molecule‐like coordination environment. This material forms a single‐site heterogeneous catalyst with methylaluminoxane and provides polyethylene with low polydispersity (PDI≈3) and the highest activity (up to 148 000 h −1 ) reported for a MOF‐based polymerization catalyst. Furthermore, polyethylene is obtained as a free‐flowing powder as desired industrially. Finally, the catalyst shows good structural integrity and retains polymerization activity for over 24 hours, both promising attributes for the commercialization of vanadium‐based polyolefins.

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  4. [해외논문]   Alloying n‐Butylamine into CsPbBr3 To Give a Two‐Dimensional Bilayered Perovskite Ferroelectric Material   SCI SCIE

    Wu, Zhenyue (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China) , Ji, Chengmin (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China) , Li, Lina (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China) , Kong, Jintao (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China) , Sun, Zhihua (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China) , Zhao, Sangen , Wang, Sasa , Hong, Maochun , Luo, Junhua
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8140 - 8143 , 2018 , 1433-7851 ,

    초록

    Abstract Cesium‐lead halide perovskites (e.g. CsPbBr 3 ) have gained attention because of their rich physical properties, but their bulk ferroelectricity remains unexplored. Herein, by alloying flexible organic cations into the cubic CsPbBr 3 , we design the first cesium‐based two‐dimensional (2D) perovskite ferroelectric material with both inorganic alkali metal and organic cations, (C 4 H 9 NH 3 ) 2 CsPb 2 Br 7 ( 1 ). Strikingly, 1 shows a high Curie temperature ( T c = 412 K) above that of BaTiO 3 (ca. 393 K) and notable spontaneous polarization (ca. 4.2 μC cm −2 ), triggered by not only the ordering of organic cations but also atomic displacement of inorganic Cs + ions. To our knowledge, such a 2D bilayered Cs + ‐based metal–halide perovskite ferroelectric material with inorganic and organic cations is unprecedented. 1 also shows photoelectric semiconducting behavior with large “on/off” ratios of photoconductivity (>10 3 ).

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  5. [해외논문]   Structure and Magnetization Dynamics of Dy−Fe and Dy−Ru Bonded Complexes   SCI SCIE

    Burns, Corey P. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Yang, Xin (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Wofford, Joshua D. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Bhuvanesh, Nattamai S. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Hall, Michael B. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Nippe, Michael (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8144 - 8148 , 2018 , 1433-7851 ,

    초록

    Abstract We present an investigation of isostructural complexes that feature unsupported direct bonds between a formally trivalent lanthanide ion (Dy 3+ ) and either a first‐row (Fe) or a second‐row (Ru) transition metal (TM) ion. The sterically rigid, yet not too bulky ligand PyCp 2 2− (PyCp 2 2− =[2,6 [2,6‐(CH 2 C 5 H 3 ) 2 C 5 H 3 N] 2− ) facilitates the isolation and characterization of PyCp 2 Dy−FeCp(CO) 2 ( 1 ; d (Dy–Fe)=2.884(2) A) and PyCp 2 Dy−RuCp(CO) 2 ( 2 ; d (Dy–Ru)=2.9508(5) A). Computational and spectroscopic studies suggest strong TM→Dy bonding interactions. Both complexes exhibit field‐induced slow magnetic relaxation with effectively identical energy barriers to magnetization reversal. However, in going from Dy−Fe to Dy−Ru bonding, we observed faster magnetic relaxation at a given temperature and larger direct and Raman coefficients, which could be due to differences in the bonding and/or spin–phonon coupling contributions to magnetic relaxation.

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  6. [해외논문]   Cofactor Biogenesis in Cysteamine Dioxygenase: C−F Bond Cleavage with Genetically Incorporated Unnatural Tyrosine   SCI SCIE

    Wang, Yifan (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA) , Griffith, Wendell P. (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA) , Li, Jiasong (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA) , Koto, Teruaki (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA) , Wherritt, Daniel J. (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA) , Fritz, Elizabeth (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA) , Liu, Aimin (Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX, USA)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8149 - 8153 , 2018 , 1433-7851 ,

    초록

    Abstract Cysteamine dioxygenase (ADO) is a thiol dioxygenase whose study has been stagnated by the ambiguity as to whether or not it possesses an anticipated protein‐derived cofactor. Reported herein is the discovery and elucidation of a Cys‐Tyr cofactor in human ADO, crosslinked between Cys220 and Tyr222 through a thioether (C−S) bond. By genetically incorporating an unnatural amino acid, 3,5‐difluoro‐tyrosine (F 2 ‐Tyr), specifically into Tyr222 of human ADO, an autocatalytic oxidative carbon–fluorine bond activation and fluoride release were identified by mass spectrometry and 19 F NMR spectroscopy. These results suggest that the cofactor biogenesis is executed by a powerful oxidant during an autocatalytic process. Unlike that of cysteine dioxygenase, the crosslinking results in a minimal structural change of the protein and it is not detectable by routine low‐resolution techniques. Finally, a new sequence motif, C‐X‐Y‐Y(F), is proposed for identifying the Cys‐Tyr crosslink.

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  7. [해외논문]   Undoped Layered Perovskite Oxynitride Li2LaTa2O6N for Photocatalytic CO2 Reduction with Visible Light   SCI SCIE

    Oshima, Takayoshi (Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo, 152-8550, Japan) , Ichibha, Tom (School of Information Science, JAIST, Asahidai 1-1, Nomi, Ishikawa, 923-1292, Japan) , Qin, Ken Sinkou (School of Information Science, JAIST, Asahidai 1-1, Nomi, Ishikawa, 923-1292, Japan) , Muraoka, Kanemichi (Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo, 152-8550, Japan) , Vequizo, Junie Jhon M. (Graduate School of Engineering, Toyota Technological Institute, 2-12-1 Hisakata, Tempaku, Nagoya, 468-8511, Japan) , Hibino, Keisuke (Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-2 Ookayama, Meguro-ku, Tokyo, 152-8550, Japan) , Kuriki, Ryo (Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1-NE-) , Yamashita, Shunsuke , Hongo, Kenta , Uchiyama, Tomoki , Fujii, Kotaro , Lu, Daling , Maezono, Ryo , Yamakata, Akira , Kato, Hideki , Kimoto, Koji , Yashima, Masatomo , Uchimoto, Yoshiharu , Kakihana, Masato , Ishitani, Osamu , Kageyama, Hiroshi , Maeda, Kazuhiko
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8154 - 8158 , 2018 , 1433-7851 ,

    초록

    Abstract Oxynitrides are promising visible‐light‐responsive photocatalysts, but their structures are almost confined with three‐dimensional (3D) structures such as perovskites. A phase‐pure Li 2 LaTa 2 O 6 N with a layered perovskite structure was successfully prepared by thermal ammonolysis of a lithium‐rich oxide precursor. Li 2 LaTa 2 O 6 N exhibited high crystallinity and visible‐light absorption up to 500 nm. As opposed to well‐known 3D oxynitride perovskites, Li 2 LaTa 2 O 6 N supported by a binuclear Ru II complex was capable of stably and selectively converting CO 2 into formate under visible light ( λ >400 nm). Transient absorption spectroscopy indicated that, as compared to 3D oxynitrides, Li 2 LaTa 2 O 6 N possesses a lower density of mid‐gap states that work as recombination centers of photogenerated electron/hole pairs, but a higher density of reactive electrons, which is responsible for the higher photocatalytic performance of this layered oxynitride.

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  8. [해외논문]   Highly Selective Directed Iridium‐Catalyzed Hydrogen Isotope Exchange Reactions of Aliphatic Amides   SCI SCIE

    Valero, Mé (Sanofi-Aventis (Deutschland) GmbH, R&D, Integrated Drug Discovery, Industriepark Höchst, 65926, Frankfurt am Main, Germany) , gane (Sanofi-Aventis (Deutschland) GmbH, R&D, Integrated Drug Discovery, Industriepark Höchst, 65926, Frankfurt am Main, Germany) , Weck, Remo (Sanofi-Aventis (Deutschland) GmbH, R&D, Integrated Drug Discovery, Industriepark Höchst, 65926, Frankfurt am Main, Germany) , Gü (Sanofi-Aventis (Deutschland) GmbH, R&D, Integrated Drug Discovery, Industriepark Höchst, 65926, Frankfurt am Main, Germany) , ssregen, Stefan (Sanofi-Aventis (Deutschland) GmbH, R&D, Integrated Drug Discovery, Industriepark Höchst, 65926, Frankfurt am Main, Germany) , Atzrodt, Jens , Derdau, Volker
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8159 - 8163 , 2018 , 1433-7851 ,

    초록

    Abstract For the first time, we describe highly selective homogeneous iridium‐catalyzed hydrogen isotope exchange (HIE) of unactivated C(sp 3 ) centers in aliphatic amides. When using the commercially available Kerr catalyst, the HIE with a series of common antibody–drug conjugate (ADC) linker side chains proceeds with high yields, high regioselectivity, and with deuterium incorporation up to 99 %. The method is fully translatable to the specific requirements of tritium chemistry and its effectiveness was demonstrated by direct tritium labelling of a maytansinoid. The scope of the method can be extended to simple amino acids, with high HIE activity observed for glycine and alanine. In di‐ and tripeptides, a very interesting protecting‐group‐dependent tunable selectivity was observed. DFT calculations gave insight into the energies of the transition states, thereby explaining the observed selectivity and the influence of the amino acid protecting groups.

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  9. [해외논문]   Magnetic Properties of a Terbium–[1]Ferrocenophane Complex: Analogies between Lanthanide–Ferrocenophane and Lanthanide–Bis‐phthalocyanine Complexes   SCI SCIE

    Latendresse, Trevor P. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Vieru, Veacheslav (Theory of Nanomaterials Group, Katholieke Universiteit Leuven, Celestijnenlaan 200F, 3001, Leuven, Belgium) , Wilkins, Branford O. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Bhuvanesh, Nattamai S. (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA) , Chibotaru, Liviu F. (Theory of Nanomaterials Group, Katholieke Universiteit Leuven, Celestijnenlaan 200F, 3001, Leuven, Belgium) , Nippe, Michael (Department of Chemistry, Texas A&M University, 3255 TAMU, College Station, TX, 77843, USA)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8164 - 8169 , 2018 , 1433-7851 ,

    초록

    Abstract A rare example of an organometallic terbium single‐ion magnet is reported. A Tb 3+ –[1]ferrocenophane complex displays a larger barrier to magnetization reversal than its isostructural Dy 3+ analogue, which is reminiscent of trends observed for lanthanide–bis‐phthalocyanine complexes. Detailed ab initio calculations support the experimental observations and suggest a significantly larger ground‐state stabilization for the non‐Kramers ion Tb 3+ in the Tb complex than for the Kramers‐ion Dy 3+ in the Dy complex.

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  10. [해외논문]   Colossal Negative Thermal Expansion in Electron‐Doped PbVO3 Perovskites   SCI SCIE

    Yamamoto, Hajime (Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan) , Imai, Takashi (Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan) , Sakai, Yuki (Kanagawa Institute of Industrial Science and Technology, 705-1 Shimoimaizumi, Ebina, 243-0435, Japan) , Azuma, Masaki (Laboratory for Materials and Structures, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, 226-8503, Japan)
    Angewandte Chemie. international edition v.57 no.27 ,pp. 8170 - 8173 , 2018 , 1433-7851 ,

    초록

    Abstract Colossal negative thermal expansion (NTE) with a volume contraction of about 8 %, the largest value reported so far for NTE materials, was observed in an electron‐doped giant tetragonal perovskite compound Pb 1− x Bi x VO 3 ( x = 0.2 and 0.3). A polar tetragonal ( P 4 mm ) to non‐polar cubic structural transition took place upon heating. The coefficient of thermal expansion (CTE) and the working temperature could be tuned by changing the Bi content, and La substitution decreased the transition temperature to room temperature. Pb 0.76 La 0.04 Bi 0.20 VO 3 exhibited a unit cell volume contraction of 6.7 % from 200 K to 420 K. Interestingly, further gigantic NTE of about 8.5 % was observed in a dilametric measurement of a Pb 0.76 La 0.04 Bi 0.20 VO 3 polycrystalline sample. The pronounced NTE in the sintered body should be attributed to an anisotropic lattice parameter change.

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