Title: Three-Dimensional Printable, Extremely Soft, Stretchable, and Reversible Elastomers from Molecular Architecture-Directed Assembly

Abstract

3D printing elastomers enables the fabrication of many technologically important structures and devices such as tissue scaffolds, sensors, actuators, and soft robots. However, conventional 3D printable elastomers are intrinsically stiff; moreover, the process of printing often requires external mechanical support and/or post-treatment. In this work, we exploit the self-assembly of a responsive linear-bottlebrush-linear triblock copolymer to create stimuli-reversible, extremely soft, and stretchable elastomers and demonstrate their applicability as inks for in situ direct-write printing 3D structures without the aid of external mechanical support or post-treatment. By developing a procedure for controlled synthesis of such architecturally designed block copolymers, we create elastomers with extensibility up to 600% and Young’s moduli down to ~10² Pa, 10⁶ times softer than plastics and more than 102 times softer than all existing 3D printable elastomers. Moreover, the elastomers are thermostable and remain to be solid up to 180 °C, yet they are 100% solvent-reprocessable. Their extreme softness, stretchability, thermostability, and solvent-reprocessability bode well for future applications.

Authors:

Nian, Shifeng  ^[1];

• Search DOE PAGES for author "Nian, Shifeng"
• Search DOE PAGES for ORCID "0000-0002-2243-6329"

Zhu, Jinchang ^[1]; Zhang, Haozhe ^[2]; Gong, Zihao ^[1]; Freychet, Guillaume ^[3]; Zhernenkov, Mikhail  ^[3];

• Search DOE PAGES for author "Zhernenkov, Mikhail"
• Search DOE PAGES for ORCID "0000-0003-3604-0672"

Xu, Baoxing  ^[2];

• Search DOE PAGES for author "Xu, Baoxing"
• Search DOE PAGES for ORCID "0000-0002-2591-8737"

Cai, Li-Heng  ^[4]

• Search DOE PAGES for author "Cai, Li-Heng"
• Search DOE PAGES for ORCID "0000-0002-6806-0566"

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+ Show Author Affiliations

1. Univ. of Virginia, Charlottesville, VA (United States). Soft Biomatter Lab.
2. Univ. of Virginia, Charlottesville, VA (United States)
3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
4. Univ. of Virginia, Charlottesville, VA (United States). Soft Biomatter Lab.; Univ. of Virginia, Charlottesville, VA (United States)

Publication Date:

Wed Mar 31 00:00:00 EDT 2021

Research Org.:

Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1778811

Report Number(s):

BNL-221305-2021-JAAM
Journal ID: ISSN 0897-4756

Grant/Contract Number:  

SC0012704

Resource Type:

Accepted Manuscript

Journal Name:

Chemistry of Materials

Additional Journal Information:

Journal Volume: 33; Journal Issue: 7; Journal ID: ISSN 0897-4756

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; Stress; solution chemistry; elastomers; copolymers; deformation; 3D printing; chemical engineering and industrial chemistry; materials; polymers