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Title: Mesoporous Polymer Frameworks from End-Reactive Bottlebrush Copolymers

Reticulated nanoporous materials generated by versatile molecular framework approaches are limited to pore dimensions on the scale of the utilized rigid molecular building blocks (<5 nm). The inherent flexibility of linear polymers precludes their utilization as long framework connectors for the extension of this strategy to larger length scales. We report a method for the fabrication of mesoporous frameworks by using bottlebrush copolymers with reactive end blocks serving as rigid macromolecular interconnectors with directional reactivity. End-reactive bottlebrush copolymers with pendant alkene functionalities were synthesized by a combination of controlled radical polymerization and polymer modification protocols. Ru-catalyzed cross-metathesis cross-linking of bottlebrush copolymers with two reactive end blocks resulted in the formation of polymer frameworks where isolated cross-linked domains were interconnected with bottlebrush copolymer bridges. The resulting materials were characterized by a continuous network pore structure with average pore sizes of 9–50 nm, conveniently tunable by the length of the utilized bottlebrush copolymer building blocks. As a result, the materials fabrication strategy described in this work expands the length scale of molecular framework materials and provides access to mesoporous polymers with a molecularly tunable reticulated pore structure without the need for templating, sacrificial component etching, or supercritical fluid drying.
Authors:
 [1] ;  [2] ; ORCiD logo [1]
  1. Univ. at Buffalo, The State Univ. of New York, Buffalo, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-114443-2017-JA
Journal ID: ISSN 1936-0851
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 8; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; nanoporous materials; organic frameworks; bottlebrush copolymers; polymer networks; Center for Functional Nanomaterials; cross-linking
OSTI Identifier:
1405935

Altay, Esra, Nykypanchuk, Dmytro, and Rzayev, Javid. Mesoporous Polymer Frameworks from End-Reactive Bottlebrush Copolymers. United States: N. p., Web. doi:10.1021/acsnano.7b03214.
Altay, Esra, Nykypanchuk, Dmytro, & Rzayev, Javid. Mesoporous Polymer Frameworks from End-Reactive Bottlebrush Copolymers. United States. doi:10.1021/acsnano.7b03214.
Altay, Esra, Nykypanchuk, Dmytro, and Rzayev, Javid. 2017. "Mesoporous Polymer Frameworks from End-Reactive Bottlebrush Copolymers". United States. doi:10.1021/acsnano.7b03214. https://www.osti.gov/servlets/purl/1405935.
@article{osti_1405935,
title = {Mesoporous Polymer Frameworks from End-Reactive Bottlebrush Copolymers},
author = {Altay, Esra and Nykypanchuk, Dmytro and Rzayev, Javid},
abstractNote = {Reticulated nanoporous materials generated by versatile molecular framework approaches are limited to pore dimensions on the scale of the utilized rigid molecular building blocks (<5 nm). The inherent flexibility of linear polymers precludes their utilization as long framework connectors for the extension of this strategy to larger length scales. We report a method for the fabrication of mesoporous frameworks by using bottlebrush copolymers with reactive end blocks serving as rigid macromolecular interconnectors with directional reactivity. End-reactive bottlebrush copolymers with pendant alkene functionalities were synthesized by a combination of controlled radical polymerization and polymer modification protocols. Ru-catalyzed cross-metathesis cross-linking of bottlebrush copolymers with two reactive end blocks resulted in the formation of polymer frameworks where isolated cross-linked domains were interconnected with bottlebrush copolymer bridges. The resulting materials were characterized by a continuous network pore structure with average pore sizes of 9–50 nm, conveniently tunable by the length of the utilized bottlebrush copolymer building blocks. As a result, the materials fabrication strategy described in this work expands the length scale of molecular framework materials and provides access to mesoporous polymers with a molecularly tunable reticulated pore structure without the need for templating, sacrificial component etching, or supercritical fluid drying.},
doi = {10.1021/acsnano.7b03214},
journal = {ACS Nano},
number = 8,
volume = 11,
place = {United States},
year = {2017},
month = {8}
}