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

Chen, Mao; Gu, Yuwei; Singh, Awaneesh; Zhong, Mingjiang; Jordan, Alex M.; Biswas, Santidan; Korley, LaShanda T. J.; Balazs, Anna C.; Johnson, Jeremiah A.

doi:10.1021/acscentsci.6b00335

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

Journal Article · Fri Jan 13 04:00:00 UTC 2017 · ACS Central Science

DOI: https://doi.org/10.1021/acscentsci.6b00335 · OSTI ID:1356090

Chen, Mao ^[1]; Gu, Yuwei ^[2]; Singh, Awaneesh ^[3];

^[4]; Jordan, Alex M. ^[5]; Biswas, Santidan ^[3];

^[5]; Balazs, Anna C. ^[3];

^[2]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Fudan Univ., Shanghai (China); University of Pittsburgh
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Univ. of Pittsburgh, Pittsburgh, PA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Yale Univ., New Haven, CT (United States)
Case Western Reserve Univ., Cleveland, OH (United States)

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. Furthermore, 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.

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Research Organization:: Univ. of Pittsburgh, Pittsburgh, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: FG02-90ER45438

OSTI ID:: 1356090

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Journal Issue: 2 Vol. 3; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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A Versatile 3D and 4D Printing System through Photocontrolled RAFT Polymerization Zhang, Zhiheng; Corrigan, Nathaniel; Bagheri, Ali Angewandte Chemie, Vol. 131, Issue 50 https://doi.org/10.1002/ange.201912608	journal	November 2019
Seeing the Light: Advancing Materials Chemistry through Photopolymerization Corrigan, Nathaniel; Yeow, Jonathan; Judzewitsch, Peter Angewandte Chemie International Edition, Vol. 58, Issue 16 https://doi.org/10.1002/anie.201805473	journal	April 2019
Polymer Networks: From Plastics and Gels to Porous Frameworks Gu, Yuwei; Zhao, Julia; Johnson, Jeremiah A. Angewandte Chemie International Edition, Vol. 59, Issue 13 https://doi.org/10.1002/anie.201902900	journal	March 2020
A Versatile 3D and 4D Printing System through Photocontrolled RAFT Polymerization Zhang, Zhiheng; Corrigan, Nathaniel; Bagheri, Ali Angewandte Chemie International Edition, Vol. 58, Issue 50 https://doi.org/10.1002/anie.201912608	journal	December 2019
Photocontrolled Living Polymerization Systems with Reversible Deactivations through Electron and Energy Transfer Shanmugam, Sivaprakash; Xu, Jiangtao; Boyer, Cyrille Macromolecular Rapid Communications, Vol. 38, Issue 13 https://doi.org/10.1002/marc.201700143	journal	May 2017
Photoredox-Based Actuation of an Artificial Molecular Muscle Liles, Kevin P.; Greene, Angelique F.; Danielson, Mary K. Macromolecular Rapid Communications, Vol. 39, Issue 17 https://doi.org/10.1002/marc.201700781	journal	January 2018
Non‐Tacky Fluorinated and Elastomeric STEM Networks Cuthbert, Julia; Martinez, Michael R.; Sun, Mingkang Macromolecular Rapid Communications, Vol. 40, Issue 10 https://doi.org/10.1002/marc.201800876	journal	February 2019
What happens in the dark? Assessing the temporal control of photo‐mediated controlled radical polymerizations Dolinski, Neil D.; Page, Zachariah A.; Discekici, Emre H. Journal of Polymer Science Part A: Polymer Chemistry, Vol. 57, Issue 3 https://doi.org/10.1002/pola.29247	journal	September 2018
Oxygen tolerant photopolymerization for ultralow volumes Yeow, Jonathan; Chapman, Robert; Xu, Jiangtao Polymer Chemistry, Vol. 8, Issue 34 https://doi.org/10.1039/c7py00007c	journal	January 2017
Polymer synthesis by mimicking nature's strategy: the combination of ultra-fast RAFT and the Biginelli reaction Wu, Haibo; Yang, Lei; Tao, Lei Polymer Chemistry, Vol. 8, Issue 37 https://doi.org/10.1039/c7py01313b	journal	January 2017
PET-RAFT polymerisation: towards green and precision polymer manufacturing Phommalysack-Lovan, Jamie; Chu, Yingying; Boyer, Cyrille Chemical Communications, Vol. 54, Issue 50 https://doi.org/10.1039/c8cc02783h	journal	January 2018
Externally controlled atom transfer radical polymerization Pan, Xiangcheng; Fantin, Marco; Yuan, Fang Chemical Society Reviews, Vol. 47, Issue 14 https://doi.org/10.1039/c8cs00259b	journal	January 2018
Grafting-through ROMP for gels with tailorable moduli and crosslink densities Weaver, Jessica A.; Morelly, Samantha L.; Alvarez, Nicolas J. Polymer Chemistry, Vol. 9, Issue 42 https://doi.org/10.1039/c8py01324a	journal	January 2018
Role of a polymeric component in the phase separation of ternary fluid mixtures: a dissipative particle dynamics study Singh, Amrita; Chakraborti, Anirban; Singh, Awaneesh Soft Matter, Vol. 14, Issue 21 https://doi.org/10.1039/c8sm00625c	journal	January 2018
Additive manufacturing with stimuli-responsive materials Boydston, A. J.; Cao, B.; Nelson, A. Journal of Materials Chemistry A, Vol. 6, Issue 42 https://doi.org/10.1039/c8ta07716a	journal	January 2018
Visible-light-induced metathesis reaction between diselenide and ditelluride Liu, Cheng; Xia, Jiahao; Ji, Shaobo Chemical Communications, Vol. 55, Issue 19 https://doi.org/10.1039/c9cc00252a	journal	January 2019
Visible-light-mediated, additive-free, and open-to-air controlled radical polymerization of acrylates and acrylamides Lamb, Jessica R.; Qin, K. Peter; Johnson, Jeremiah A. Polymer Chemistry, Vol. 10, Issue 13 https://doi.org/10.1039/c9py00022d	journal	January 2019
Transformation of gels via catalyst-free selective RAFT photoactivation Shanmugam, Sivaprakash; Cuthbert, Julia; Flum, Jacob Polymer Chemistry, Vol. 10, Issue 19 https://doi.org/10.1039/c9py00213h	journal	January 2019
3D printing of polymeric materials based on photo-RAFT polymerization Bagheri, Ali; Engel, Kyle Edward; Bainbridge, Chris William Anderson Polymer Chemistry, Vol. 11, Issue 3 https://doi.org/10.1039/c9py01419e	journal	January 2020
Counting loops in sidechain-crosslinked polymers from elastic solids to single-chain nanoparticles Wang, Junpeng; Wang, Rui; Gu, Yuwei Chemical Science, Vol. 10, Issue 20 https://doi.org/10.1039/c9sc01297d	journal	January 2019
Role of a polymeric component in the phase separation of ternary fluid mixtures: A dissipative particle dynamics study Singh, Amrita; Chakraborti, Anirban; Singh, Awaneesh arXiv https://doi.org/10.48550/arxiv.1804.09636	preprint	January 2018

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