Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy

Garcia, Antonio; Saluga, Shannon J.; Dibble, David J.; López, Pía A.; Saito, Nozomi; Blum, Suzanne A.

doi:10.1002/anie.202010101

Title: Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy

Abstract

Abstract The chemoselectivity of molecular catalysts underpins much of modern synthetic organic chemistry. However, little is known about the selectivity of individual catalysts because this single‐catalyst‐level behavior is hidden by the bulk catalytic behavior. Here, for the first time, the selectivity of individual molecular catalysts for two different reactions is imaged in real time at the single‐catalyst level. This imaging is achieved through fluorescence microscopy paired with spectral probes that produce a snapshot of the instantaneous chemoselectivity of a single catalyst for either a single‐chain‐elongation or a single‐chain‐termination event during ruthenium‐catalyzed polymerization. Superresolution imaging of multiple selectivity events, each at a different single‐molecular ruthenium catalyst, indicates that catalyst selectivity may be unexpectedly spatially and time‐variable.

Authors:

^[1];

^[1]; Dibble, David J. ^[1];

^[1]; Saito, Nozomi ^[1];

^[1]

Univ. of California, Irvine, CA (United States)

Publication Date:: Thu Oct 08 00:00:00 EDT 2020

Research Org.:: Univ. of California, Irvine, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1836111

Alternate Identifier(s):: OSTI ID: 1786073

Grant/Contract Number:: SC0016467

Resource Type:: Accepted Manuscript

Journal Name:: Angewandte Chemie (International Edition)

Additional Journal Information:: Journal Name: Angewandte Chemie (International Edition); Journal Volume: 60; Journal Issue: 3; Journal ID: ISSN 1433-7851

Publisher:: Wiley

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; polymerization; selectivity; fluorescence microscopy; molecular catalysis; single-molecule superresolution fluorescence microscopy; polydispersity

Citation Formats


                    Garcia, Antonio, Saluga, Shannon J., Dibble, David J., López, Pía A., Saito, Nozomi, and Blum, Suzanne A. Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy.  United States: N. p., 2020. 
Web.  doi:10.1002/anie.202010101.

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                    Garcia, Antonio, Saluga, Shannon J., Dibble, David J., López, Pía A., Saito, Nozomi, & Blum, Suzanne A. Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy.  United States.  https://doi.org/10.1002/anie.202010101

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                    Garcia, Antonio, Saluga, Shannon J., Dibble, David J., López, Pía A., Saito, Nozomi, and Blum, Suzanne A. Thu .  
"Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy".  United States.  https://doi.org/10.1002/anie.202010101.  https://www.osti.gov/servlets/purl/1836111.

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@article{osti_1836111,

  title        = {Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy},

  author       = {Garcia, Antonio and Saluga, Shannon J. and Dibble, David J. and López, Pía A. and Saito, Nozomi and Blum, Suzanne A.},

  abstractNote = {Abstract The chemoselectivity of molecular catalysts underpins much of modern synthetic organic chemistry. However, little is known about the selectivity of individual catalysts because this single‐catalyst‐level behavior is hidden by the bulk catalytic behavior. Here, for the first time, the selectivity of individual molecular catalysts for two different reactions is imaged in real time at the single‐catalyst level. This imaging is achieved through fluorescence microscopy paired with spectral probes that produce a snapshot of the instantaneous chemoselectivity of a single catalyst for either a single‐chain‐elongation or a single‐chain‐termination event during ruthenium‐catalyzed polymerization. Superresolution imaging of multiple selectivity events, each at a different single‐molecular ruthenium catalyst, indicates that catalyst selectivity may be unexpectedly spatially and time‐variable.},

  doi          = {10.1002/anie.202010101},

  journal      = {Angewandte Chemie (International Edition)},

  number       = 3,

  volume       = 60,

  place        = {United States},

  year         = {Thu Oct 08 00:00:00 EDT 2020},

  month        = {Thu Oct 08 00:00:00 EDT 2020}

}

Copy to clipboard

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Title: Does Selectivity of Molecular Catalysts Change with Time? Polymerization Imaged by Single-Molecule Spectroscopy

Abstract

Citation Formats

Correlating Pyrene Excimer Formation with Polymer Chain Dynamics in Solution. Possibilities and Limitations journal, September 2007

Controlled/"living" radical polymerization. atom transfer radical polymerization in the presence of transition-metal complexes journal, May 1995

Noninvasive Nanoscopy Uncovers the Impact of the Hierarchical Porous Structure on the Catalytic Activity of Single Dealuminated Mordenite Crystals journal, August 2015

Distinguishing Alternative Reaction Pathways by Single-Molecule Fluorescence Spectroscopy journal, April 2013

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The Convergence of Synthetic Organic and Polymer Chemistries journal, August 2005

Single-molecule, single-particle fluorescence imaging of TiO2-based photocatalytic reactions journal, January 2010

Imaging Intracellular Fluorescent Proteins at Nanometer Resolution journal, September 2006

Efficient and Facile End Group Control of Living Ring-Opening Metathesis Polymers via Single Addition of Functional Cyclopropenes journal, May 2018

ROMP−ATRP Block Copolymers Prepared from Monotelechelic Poly(oxa)norbornenes Using a Difunctional Terminating Agent journal, July 2008

Olefin polymer technologies—History and recent progress at The Dow Chemical Company journal, August 2008

Single polymer growth dynamics journal, October 2017

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Propylene polymerization through supported metallocene/ MAO catalysts: Kinetic analysis and modelling journal, October 1995

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Kinetics of polymer looping with macromolecular crowding: effects of volume fraction and crowder size journal, January 2015

Introduction to Polymers book, June 2011

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Breaking the diffraction resolution limit by stimulated emission: stimulated-emission-depletion fluorescence microscopy journal, January 1994

Equilibrium Structure and Dynamics of Self-Associating Single Polymers journal, September 2011

Single Turnover at Molecular Polymerization Catalysts Reveals Spatiotemporally Resolved Reactions journal, September 2017

Kinetics of the Same Reaction Monitored over Nine Orders of Magnitude in Concentration: When Are Unique Subensemble and Single‐Turnover Reactivity Displayed? journal, August 2018

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Nanoscale Colocalization of Fluorogenic Probes Reveals the Role of Oxygen Vacancies in the Photocatalytic Activity of Tungsten Oxide Nanowires journal, January 2020

Evidence for Dynamic Chemical Kinetics at Individual Molecular Ruthenium Catalysts journal, January 2018

Kinetics of the Same Reaction Monitored over Nine Orders of Magnitude in Concentration: When Are Unique Subensemble and Single‐Turnover Reactivity Displayed? journal, August 2018

Single Turnover at Molecular Polymerization Catalysts Reveals Spatiotemporally Resolved Reactions journal, September 2017

Optical detection and spectroscopy of single molecules in a solid journal, May 1989

Correlating Pyrene Excimer Formation with Polymer Chain Dynamics in Solution. Possibilities and Limitations
journal, September 2007

Controlled/"living" radical polymerization. atom transfer radical polymerization in the presence of transition-metal complexes
journal, May 1995

Noninvasive Nanoscopy Uncovers the Impact of the Hierarchical Porous Structure on the Catalytic Activity of Single Dealuminated Mordenite Crystals
journal, August 2015

Distinguishing Alternative Reaction Pathways by Single-Molecule Fluorescence Spectroscopy
journal, April 2013

Beyond Dispersity: Deterministic Control of Polymer Molecular Weight Distribution
journal, February 2016

The Convergence of Synthetic Organic and Polymer Chemistries
journal, August 2005

Single-molecule, single-particle fluorescence imaging of TiO2-based photocatalytic reactions
journal, January 2010

Imaging Intracellular Fluorescent Proteins at Nanometer Resolution
journal, September 2006

Efficient and Facile End Group Control of Living Ring-Opening Metathesis Polymers via Single Addition of Functional Cyclopropenes
journal, May 2018

ROMP−ATRP Block Copolymers Prepared from Monotelechelic Poly(oxa)norbornenes Using a Difunctional Terminating Agent
journal, July 2008

Olefin polymer technologies—History and recent progress at The Dow Chemical Company
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Sub-particle reaction and photocurrent mapping to optimize catalyst-modified photoanodes
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Propylene polymerization through supported metallocene/ MAO catalysts: Kinetic analysis and modelling
journal, October 1995

Organic and Organometallic Chemistry at the Single-Molecule, -Particle, and -Molecular-Catalyst-Turnover Level by Fluorescence Microscopy
journal, July 2019

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Introduction to Polymers
book, June 2011

Direkte Beobachtung alternativer Reaktionswege an einzelnen Molekülen
journal, April 2013

Breaking the diffraction resolution limit by stimulated emission: stimulated-emission-depletion fluorescence microscopy
journal, January 1994

Equilibrium Structure and Dynamics of Self-Associating Single Polymers
journal, September 2011

Single Turnover at Molecular Polymerization Catalysts Reveals Spatiotemporally Resolved Reactions
journal, September 2017

Kinetics of the Same Reaction Monitored over Nine Orders of Magnitude in Concentration: When Are Unique Subensemble and Single‐Turnover Reactivity Displayed?
journal, August 2018

Long Range Polymer Chain Dynamics Studied by Fluorescence Quenching
journal, August 2016

Proposed method for molecular optical imaging
journal, January 1995

Spatially resolved observation of crystal-face-dependent catalysis by single turnover counting
journal, February 2006

Evidence for Dynamic Chemical Kinetics at Individual Molecular Ruthenium Catalysts
journal, January 2018

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journal, March 2019

Control of the Termination Mechanism in Radical Polymerization by Viscosity: Selective Disproportionation in Viscous Media
journal, December 2016

Single-Molecule Investigation of Initiation Dynamics of an Organometallic Catalyst
journal, March 2016

Far-Field Optical Nanoscopy
journal, May 2007

Phase Separation Polymerization of Dicyclopentadiene Characterized by In Operando Fluorescence Microscopy
journal, August 2013

Fluorescence microscopy with diffraction resolution barrier broken by stimulated emission
journal, July 2000

50th Anniversary Perspective : Living Polymerization—Emphasizing the Molecule in Macromolecules
journal, September 2017

Mechanism and Activity of Ruthenium Olefin Metathesis Catalysts
journal, July 2001

Nanoscale Colocalization of Fluorogenic Probes Reveals the Role of Oxygen Vacancies in the Photocatalytic Activity of Tungsten Oxide Nanowires
journal, January 2020

Evidence for Dynamic Chemical Kinetics at Individual Molecular Ruthenium Catalysts
journal, January 2018

Kinetics of the Same Reaction Monitored over Nine Orders of Magnitude in Concentration: When Are Unique Subensemble and Single‐Turnover Reactivity Displayed?
journal, August 2018

Single Turnover at Molecular Polymerization Catalysts Reveals Spatiotemporally Resolved Reactions
journal, September 2017

Optical detection and spectroscopy of single molecules in a solid
journal, May 1989