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Title: Silica–Conjugated Polymer Hybrid Fluorescent Nanoparticles: Preparation by Surface-Initiated Polymerization and Spectroscopic Studies

Abstract

Organic/inorganic hybrid nanoscale materials possess fascinating optical, electronic, magnetic, and catalytic properties that are promising for a variety of practical applications. Such properties can be dramatically affected by the hierarchical structure and molecular organization in the nanomaterials. Herein, we employed surface-initiated Kumada catalyst-transfer polymerization to prepare hybrid materials consisting of shells of conjugated polymers (CPs)—polythiophene or poly(p-phenylene)—and their block copolymers covalently attached to the surface of silica nanoparticles. Because of the controlled chain-growth mechanism of surface-initiated polymerization, we obtained structurally well-defined CP blocks in the diblock copolymer shells, which produced distinct spectroscopic properties related to the intraparticle excitation energy transfer between the nanoscale polymer shell components, as well as the formation of interfacial exciplex states. Finally, the spectroscopic phenomena were further understood via time-resolved transient absorption spectroscopy studies. Overall, the surface-initiated polymerization provided an efficient tool to prepare structurally defined and highly stable organic polymer shell–inorganic core nanoparticles with tunable spectroscopic characteristics not achievable from corresponding single-component systems.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [1];  [1];  [1]; ORCiD logo [3];  [4]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Louisiana State Univ., Baton Rouge, LA (United States). Dept. of Chemistry
  2. Georgia Inst. of Technology, Atlanta, GA (United States). School of Materials Science and Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
  4. Indiana Univ., Bloomington, IN (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1460211
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 12; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chatterjee, Sourav, Karam, Tony E., Rosu, Cornelia, Wang, Chun-Han, Youm, Sang Gil, Li, Xin, Do, Changwoo, Losovyj, Yaroslav, Russo, Paul S., Haber, Louis H., and Nesterov, Evgueni E. Silica–Conjugated Polymer Hybrid Fluorescent Nanoparticles: Preparation by Surface-Initiated Polymerization and Spectroscopic Studies. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b00313.
Chatterjee, Sourav, Karam, Tony E., Rosu, Cornelia, Wang, Chun-Han, Youm, Sang Gil, Li, Xin, Do, Changwoo, Losovyj, Yaroslav, Russo, Paul S., Haber, Louis H., & Nesterov, Evgueni E. Silica–Conjugated Polymer Hybrid Fluorescent Nanoparticles: Preparation by Surface-Initiated Polymerization and Spectroscopic Studies. United States. https://doi.org/10.1021/acs.jpcc.8b00313
Chatterjee, Sourav, Karam, Tony E., Rosu, Cornelia, Wang, Chun-Han, Youm, Sang Gil, Li, Xin, Do, Changwoo, Losovyj, Yaroslav, Russo, Paul S., Haber, Louis H., and Nesterov, Evgueni E. Thu . "Silica–Conjugated Polymer Hybrid Fluorescent Nanoparticles: Preparation by Surface-Initiated Polymerization and Spectroscopic Studies". United States. https://doi.org/10.1021/acs.jpcc.8b00313. https://www.osti.gov/servlets/purl/1460211.
@article{osti_1460211,
title = {Silica–Conjugated Polymer Hybrid Fluorescent Nanoparticles: Preparation by Surface-Initiated Polymerization and Spectroscopic Studies},
author = {Chatterjee, Sourav and Karam, Tony E. and Rosu, Cornelia and Wang, Chun-Han and Youm, Sang Gil and Li, Xin and Do, Changwoo and Losovyj, Yaroslav and Russo, Paul S. and Haber, Louis H. and Nesterov, Evgueni E.},
abstractNote = {Organic/inorganic hybrid nanoscale materials possess fascinating optical, electronic, magnetic, and catalytic properties that are promising for a variety of practical applications. Such properties can be dramatically affected by the hierarchical structure and molecular organization in the nanomaterials. Herein, we employed surface-initiated Kumada catalyst-transfer polymerization to prepare hybrid materials consisting of shells of conjugated polymers (CPs)—polythiophene or poly(p-phenylene)—and their block copolymers covalently attached to the surface of silica nanoparticles. Because of the controlled chain-growth mechanism of surface-initiated polymerization, we obtained structurally well-defined CP blocks in the diblock copolymer shells, which produced distinct spectroscopic properties related to the intraparticle excitation energy transfer between the nanoscale polymer shell components, as well as the formation of interfacial exciplex states. Finally, the spectroscopic phenomena were further understood via time-resolved transient absorption spectroscopy studies. Overall, the surface-initiated polymerization provided an efficient tool to prepare structurally defined and highly stable organic polymer shell–inorganic core nanoparticles with tunable spectroscopic characteristics not achievable from corresponding single-component systems.},
doi = {10.1021/acs.jpcc.8b00313},
journal = {Journal of Physical Chemistry. C},
number = 12,
volume = 122,
place = {United States},
year = {2018},
month = {3}
}

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Figures / Tables:

Scheme 1 Scheme 1: Preparation of Ni(II) external catalytic initiator and its use in the synthesis of regioregular poly(3-alkylthiophene)s by controlled chain-growth Kumada catalyst-transfer polymerization.

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