Single Turnover at Molecular Polymerization Catalysts Reveals Spatiotemporally Resolved Reactions

被引:37
作者
Easter, Quinn T. [1 ]
Blum, Suzanne A. [1 ]
机构
[1] Univ Calif Irvine, Dept Chem, Irvine, CA 92617 USA
关键词
fluorescence microscopy; molecular catalysts; reaction mechanisms; single molecules; HETEROGENEITIES; REACTIVITY; DYNAMICS; NANOPARTICLES; ADSORPTION; UNCOVERS; KINETICS; TIME;
D O I
10.1002/anie.201708284
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Multiple active individual molecular ruthenium catalysts have been pinpointed within growing polynorbornene, thereby revealing information on the reaction dynamics and location that is unavailable through traditional ensemble experiments. This is the first single-turnover imaging of a molecular catalyst by fluorescence microscopy and allows detection of individual monomer reactions at an industrially important molecular ruthenium ring-opening metathesis polymerization (ROMP) catalyst under synthetically relevant conditions (e.g. unmodified industrial catalyst, ambient pressure, condensed phase, ca. 0.03m monomer). These results further establish the key fundamentals of this imaging technique for characterizing the reactivity and location of active molecular catalysts even when they are the minor components.
引用
收藏
页码:13772 / 13775
页数:4
相关论文
共 53 条
[41]   Distinguishing Alternative Reaction Pathways by Single-Molecule Fluorescence Spectroscopy [J].
Rybina, Arina ;
Lang, Carolin ;
Wirtz, Marcel ;
Grussmayer, Kristin ;
Kurz, Anton ;
Maier, Frank ;
Schmitt, Alexander ;
Trapp, Oliver ;
Jung, Gregor ;
Herten, Dirk-Peter .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (24) :6322-6325
[42]   Sub-particle reaction and photocurrent mapping to optimize catalyst-modified photoanodes [J].
Sambur, Justin B. ;
Chen, Tai-Yen ;
Choudhary, Eric ;
Chen, Guanqun ;
Nissen, Erin J. ;
Thomas, Elayne M. ;
Zou, Ningmu ;
Chen, Peng .
NATURE, 2016, 530 (7588) :77-+
[43]   Nanoscopic heterogeneities in adsorption and electron transfer processes of perylene diimide dye on TiO2 nanoparticles studied by single-molecule fluorescence spectroscopy [J].
Tachikawa, Takashi ;
Cui, Shi-Cong ;
Top, Sachiko ;
Fujitsuka, Mamoru ;
Majima, Tetsuro .
CHEMICAL PHYSICS LETTERS, 2007, 443 (4-6) :313-318
[44]   Single-Molecule Fluorescence Detection of Effective Adsorption Sites at the Metal Oxide-Solution Interface [J].
Tachikawa, Takashi ;
Ohsaka, Tatsuya ;
Bian, Zhenfeng ;
Majima, Tetsuro .
JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (21) :11219-11228
[45]   Single-Molecule, Single-Particle Approaches for Exploring the Structure and Kinetics of Nanocatalysts [J].
Tachikawa, Takashi ;
Majima, Tetsuro .
LANGMUIR, 2012, 28 (24) :8933-8943
[46]   Labeling and Single-Molecule Methods To Monitor G Protein-Coupled Receptor Dynamics [J].
Tian, He ;
Furstenberg, Alexandre ;
Huber, Thomas .
CHEMICAL REVIEWS, 2017, 117 (01) :186-245
[47]   Desmethyl Macrolides: Synthesis and Evaluation of 4,8,10-Tridesmethyl Telithromycin [J].
Velvadapu, Venkata ;
Paul, Tapas ;
Wagh, Bharat ;
Klepacki, Dorota ;
Guvench, Olgun ;
MacKerell, Alexander, Jr. ;
Andrade, Rodrigo B. .
ACS MEDICINAL CHEMISTRY LETTERS, 2011, 2 (01) :68-72
[48]   Chemical Imaging of Spatial Heterogeneities in Catalytic Solids at Different Length and Time Scales [J].
Weckhuysen, Bert M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (27) :4910-4943
[49]   Fluorescence spectroscopy of single biomolecules [J].
Weiss, S .
SCIENCE, 1999, 283 (5408) :1676-1683
[50]   A two-color fluorogenic carbene complex for tagging olefins via metathesis reaction [J].
Wirtz, Marcel ;
Grueter, Andreas ;
Heib, Florian ;
Huch, Volker ;
Zapp, Josef ;
Herten, Dirk-Peter ;
Schmitt, Michael ;
Jung, Gregor .
METHODS AND APPLICATIONS IN FLUORESCENCE, 2015, 3 (04)