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Title: Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers

Abstract

Linear–bottlebrush–linear (LBBL) triblock copolymers represent an emerging system for creating multifunctional nanostructures. Their self-assembly depends on molecular architecture but remains poorly explored. We synthesize polystyrene- block-bottlebrush polydimethylsiloxane- block-polystyrene triblock copolymers with controlled molecular architecture and use them as a model system to study the self-assembly of LBBL polymers. Unlike classical stiff rod-flexible linear block copolymers that are prone to form highly ordered nanostructures such as lamellae, at small weight fractions of the linear blocks, LBBL polymers self-assemble to a disordered sphere phase, regardless of the bottlebrush stiffness. Microscopically, characteristic lengths increase with the bottlebrush stiffness by a power of 2/3, which is captured by a scaling analysis. Macroscopically, the formed nanostructures are ultrasoft, reprocessable elastomers with shear moduli of about 1 kPa, two orders of magnitude lower than that of conventional polydimethylsiloxane elastomers. Our results provide insights on exploiting the self-assembly of LBBL polymers to create soft functional nanostructures.

Authors:
 [1];  [2];  [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Virginia, Charlottesville, VA (United States)
  2. Stanford Univ., Stanford, CA (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1580235
Report Number(s):
BNL-212460-2019-JAAM
Journal ID: ISSN 2161-1653
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Macro Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 11; Journal ID: ISSN 2161-1653
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Nian, Shifeng, Lian, Huada, Gong, Zihao, Zhernenkov, Mikhail, Qin, Jian, and Cai, Li -Heng. Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers. United States: N. p., 2019. Web. doi:10.1021/acsmacrolett.9b00721.
Nian, Shifeng, Lian, Huada, Gong, Zihao, Zhernenkov, Mikhail, Qin, Jian, & Cai, Li -Heng. Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers. United States. doi:10.1021/acsmacrolett.9b00721.
Nian, Shifeng, Lian, Huada, Gong, Zihao, Zhernenkov, Mikhail, Qin, Jian, and Cai, Li -Heng. Fri . "Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers". United States. doi:10.1021/acsmacrolett.9b00721.
@article{osti_1580235,
title = {Molecular Architecture Directs Linear–Bottlebrush–Linear Triblock Copolymers to Self-Assemble to Soft Reprocessable Elastomers},
author = {Nian, Shifeng and Lian, Huada and Gong, Zihao and Zhernenkov, Mikhail and Qin, Jian and Cai, Li -Heng},
abstractNote = {Linear–bottlebrush–linear (LBBL) triblock copolymers represent an emerging system for creating multifunctional nanostructures. Their self-assembly depends on molecular architecture but remains poorly explored. We synthesize polystyrene-block-bottlebrush polydimethylsiloxane-block-polystyrene triblock copolymers with controlled molecular architecture and use them as a model system to study the self-assembly of LBBL polymers. Unlike classical stiff rod-flexible linear block copolymers that are prone to form highly ordered nanostructures such as lamellae, at small weight fractions of the linear blocks, LBBL polymers self-assemble to a disordered sphere phase, regardless of the bottlebrush stiffness. Microscopically, characteristic lengths increase with the bottlebrush stiffness by a power of 2/3, which is captured by a scaling analysis. Macroscopically, the formed nanostructures are ultrasoft, reprocessable elastomers with shear moduli of about 1 kPa, two orders of magnitude lower than that of conventional polydimethylsiloxane elastomers. Our results provide insights on exploiting the self-assembly of LBBL polymers to create soft functional nanostructures.},
doi = {10.1021/acsmacrolett.9b00721},
journal = {ACS Macro Letters},
number = 11,
volume = 8,
place = {United States},
year = {2019},
month = {11}
}

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