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Title: Living additive manufacturing: Transformation of parent gels into diversely functionalized daughter gels made possible by visible light photoredox catalysis

Abstract

Light-initiated additive manufacturing techniques typically rely on layer-by-layer addition or continuous extraction of polymers formed via nonliving, free radical polymerization methods that render the final materials “dead” toward further monomer insertion; the polymer chains within the materials cannot be reactivated to induce chain extension. An alternative “living additive manufacturing” strategy would involve the use of photocontrolled living radical polymerization to spatiotemporally insert monomers into dormant “parent” materials to generate more complex and diversely functionalized “daughter” materials. Here, we demonstrate a proof-of-concept study of living additive manufacturing using end-linked polymer gels embedded with trithiocarbonate iniferters that can be activated by photoinduced single-electron transfer from an organic photoredox catalyst in solution. This system enables the synthesis of a wide range of chemically and mechanically differentiated daughter gels from a single type of parent gel via light-controlled modification of the parent’s average composition, strand length, and/or cross-linking density. Daughter gels that are softer than their parent, stiffer than their parent, larger but with the same modulus as their parent, thermally responsive, polarity responsive, healable, and weldable are all realized.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [5];  [3]; ORCiD logo [5];  [3]; ORCiD logo [2]
+ Show Author Affiliations
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Fudan Univ., Shanghai (China)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Univ. of Pittsburgh, Pittsburgh, PA (United States)
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Yale Univ., New Haven, CT (United States)
  5. Case Western Reserve Univ., Cleveland, OH (United States)
Publication Date:
Research Org.:
Univ. of Pittsburgh, PA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1356090
Alternate Identifier(s):
OSTI ID: 1358429
Grant/Contract Number:  
FG02-90ER45438
Resource Type:
Accepted Manuscript
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 3; Journal Issue: 2; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; transfer radical polymerization; cross-linked polymers; cationic-polymerization; model networks; hydrogels; trithiocarbonate; transition; driven; growth; elasticity; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Chen, Mao, Gu, Yuwei, Singh, Awaneesh, Zhong, Mingjiang, Jordan, Alex M., Biswas, Santidan, Korley, LaShanda T. J., Balazs, Anna C., and Johnson, Jeremiah A. Living additive manufacturing: Transformation of parent gels into diversely functionalized daughter gels made possible by visible light photoredox catalysis. United States: N. p., 2017. Web. doi:10.1021/acscentsci.6b00335.
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Chen, Mao, Gu, Yuwei, Singh, Awaneesh, Zhong, Mingjiang, Jordan, Alex M., Biswas, Santidan, Korley, LaShanda T. J., Balazs, Anna C., & Johnson, Jeremiah A. Living additive manufacturing: Transformation of parent gels into diversely functionalized daughter gels made possible by visible light photoredox catalysis. United States. https://doi.org/10.1021/acscentsci.6b00335
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Chen, Mao, Gu, Yuwei, Singh, Awaneesh, Zhong, Mingjiang, Jordan, Alex M., Biswas, Santidan, Korley, LaShanda T. J., Balazs, Anna C., and Johnson, Jeremiah A. Fri . "Living additive manufacturing: Transformation of parent gels into diversely functionalized daughter gels made possible by visible light photoredox catalysis". United States. https://doi.org/10.1021/acscentsci.6b00335. https://www.osti.gov/servlets/purl/1356090.
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@article{osti_1356090,
title = {Living additive manufacturing: Transformation of parent gels into diversely functionalized daughter gels made possible by visible light photoredox catalysis},
author = {Chen, Mao and Gu, Yuwei and Singh, Awaneesh and Zhong, Mingjiang and Jordan, Alex M. and Biswas, Santidan and Korley, LaShanda T. J. and Balazs, Anna C. and Johnson, Jeremiah A.},
abstractNote = {Light-initiated additive manufacturing techniques typically rely on layer-by-layer addition or continuous extraction of polymers formed via nonliving, free radical polymerization methods that render the final materials “dead” toward further monomer insertion; the polymer chains within the materials cannot be reactivated to induce chain extension. An alternative “living additive manufacturing” strategy would involve the use of photocontrolled living radical polymerization to spatiotemporally insert monomers into dormant “parent” materials to generate more complex and diversely functionalized “daughter” materials. Here, we demonstrate a proof-of-concept study of living additive manufacturing using end-linked polymer gels embedded with trithiocarbonate iniferters that can be activated by photoinduced single-electron transfer from an organic photoredox catalyst in solution. This system enables the synthesis of a wide range of chemically and mechanically differentiated daughter gels from a single type of parent gel via light-controlled modification of the parent’s average composition, strand length, and/or cross-linking density. Daughter gels that are softer than their parent, stiffer than their parent, larger but with the same modulus as their parent, thermally responsive, polarity responsive, healable, and weldable are all realized.},
doi = {10.1021/acscentsci.6b00335},
journal = {ACS Central Science},
number = 2,
volume = 3,
place = {United States},
year = {Fri Jan 13 00:00:00 EST 2017},
month = {Fri Jan 13 00:00:00 EST 2017}
}
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Covalent Adaptable Networks (CANs): A Unique Paradigm in Cross-Linked Polymers
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Changes in Network Structure of Chemical Gels Controlled by Solvent Quality through Photoinduced Radical Reshuffling Reactions of Trithiocarbonate Units
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journal, July 2013

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Erratum: Photogated humidity-driven motility
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Copper-free click chemistry for the in situ crosslinking of photodegradable star polymers
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Cu-free click cycloaddition reactions in chemical biology
journal, January 2010

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Mesh-size control and functionalization of reorganizable chemical gels by monomer insertion into their cross-linking points
journal, January 2011

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