Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion

Kuksenok, Olga; Balazs, Anna C.

doi:10.1038/srep09569

Title: Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion

Abstract

Human motion is enabled by the concerted expansion and contraction of interconnected muscles that are powered by inherent biochemical reactions. One of the challenges in the field of biomimicry is eliciting this form of motion from purely synthetic materials, which typically do not generate internalized reactions to drive mechanical action. Moreover, for practical applications, this bio-inspired motion must be readily controllable. Herein, we develop a computational model to design a new class of polymer gels where structural reconfigurations and internalized reactions are intimately linked to produce autonomous motion, which can be directed with light. These gels contain both spirobenzopyran (SP) chromophores and the ruthenium catalysts that drive the oscillatory Belousov-Zhabotinsky (BZ) reaction. Importantly, both the SP moieties and the BZ reaction are photosensitive. When these dual-functionalized gels are exposed to non-uniform illumination, the localized contraction of the gel (due to the SP moieties) in the presence of traveling chemical waves (due to the BZ reaction) leads to new forms of spontaneous, self-sustained movement, which cannot be achieved by either of the mono-functionalized networks.

Authors:

Kuksenok, Olga ^[1]; Balazs, Anna C. ^[1]

Univ. of Pittsburgh, PA (United States). Chemical Engineering Dept.

Publication Date:: Thu Apr 30 00:00:00 EDT 2015

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

Sponsoring Org.:: USDOE

OSTI Identifier:: 1184794

Grant/Contract Number:: FG02-90ER45438

Resource Type:: Accepted Manuscript

Journal Name:: Scientific Reports

Additional Journal Information:: Journal Volume: 5; Journal ID: ISSN 2045-2322

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Kuksenok, Olga, and Balazs, Anna C. Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion.  United States: N. p., 2015. 
Web.  doi:10.1038/srep09569.

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                    Kuksenok, Olga, & Balazs, Anna C. Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion.  United States.  https://doi.org/10.1038/srep09569

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                    Kuksenok, Olga, and Balazs, Anna C. Thu .  
"Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion".  United States.  https://doi.org/10.1038/srep09569.  https://www.osti.gov/servlets/purl/1184794.

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@article{osti_1184794,

  title        = {Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion},

  author       = {Kuksenok, Olga and Balazs, Anna C.},

  abstractNote = {Human motion is enabled by the concerted expansion and contraction of interconnected muscles that are powered by inherent biochemical reactions. One of the challenges in the field of biomimicry is eliciting this form of motion from purely synthetic materials, which typically do not generate internalized reactions to drive mechanical action. Moreover, for practical applications, this bio-inspired motion must be readily controllable. Herein, we develop a computational model to design a new class of polymer gels where structural reconfigurations and internalized reactions are intimately linked to produce autonomous motion, which can be directed with light. These gels contain both spirobenzopyran (SP) chromophores and the ruthenium catalysts that drive the oscillatory Belousov-Zhabotinsky (BZ) reaction. Importantly, both the SP moieties and the BZ reaction are photosensitive. When these dual-functionalized gels are exposed to non-uniform illumination, the localized contraction of the gel (due to the SP moieties) in the presence of traveling chemical waves (due to the BZ reaction) leads to new forms of spontaneous, self-sustained movement, which cannot be achieved by either of the mono-functionalized networks.},

  doi          = {10.1038/srep09569},

  journal      = {Scientific Reports},

  number       = ,

  volume       = 5,

  place        = {United States},

  year         = {Thu Apr 30 00:00:00 EDT 2015},

  month        = {Thu Apr 30 00:00:00 EDT 2015}

}

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https://doi.org/10.1038/srep09569

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Synthetic homeostatic materials with chemo-mechano-chemical self-regulation
journal, July 2012

He, Ximin; Aizenberg, Michael; Kuksenok, Olga
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Isomerization of spirobenzopyrans bearing electron-donating and electron-withdrawing groups in acidic aqueous solutions
journal, January 2011

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Photophobic and phototropic movement of a self-oscillating gel
journal, January 2013

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Chemical Communications, Vol. 49, Issue 70
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Beating polymer gels coupled with a nonlinear chemical reaction
journal, June 1999

Yoshida, Ryo; Kokufuta, Etsuo; Yamaguchi, Tomohiko
Chaos: An Interdisciplinary Journal of Nonlinear Science, Vol. 9, Issue 2
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Theoretical and computational modeling of self-oscillating polymer gels
journal, March 2007

Yashin, Victor V.; Balazs, Anna C.
The Journal of Chemical Physics, Vol. 126, Issue 12
DOI: 10.1063/1.2672951

Softening of bulk modulus and negative Poisson’s ratio near the volume phase transition of polymer gels
journal, March 1991

Hirotsu, Shunsuke
The Journal of Chemical Physics, Vol. 94, Issue 5
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journal, November 2006

Yashin, V. V.; Balazs, A. C.
Science, Vol. 314, Issue 5800
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Works referencing / citing this record:

Polyampholyte Hydrogels with pH Modulated Shape Memory and Spontaneous Actuation
journal, March 2018

Zhang, Yuancheng; Liao, Jiexin; Wang, Tao
Advanced Functional Materials, Vol. 28, Issue 18
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From isolated structures to continuous networks: A categorization of cytoskeleton‐based motile engineered biological microstructures
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Andorfer, Rachel; Alper, Joshua D.
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Kuksenok, Olga; Singh, Awaneesh; Balazs, Anna C.
Bioinspiration & Biomimetics, Vol. 13, Issue 3
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Title: Designing Dual-functionalized Gels for Self-reconfiguration and Autonomous Motion

Abstract

Citation Formats

Self-oscillation of polymer and photo-regulation by introducing photochromic site to induce LCST changes journal, July 2013

Rewritable Microrelief Formation on Photoresponsive Hydrogel Layers journal, May 2007

Fast-reversible light-driven hydrogels consisting of spirobenzopyran-functionalized poly(N-isopropylacrylamide) journal, January 2011

Photoresponsive polymer gel microvalves controlled by local light irradiation journal, November 2007

Photoresponsive Properties of Poly(N-isopropylacrylamide) Hydrogel Partly Modified with Spirobenzopyran journal, March 2006

Modeling the Photoinduced Reconfiguration and Directed Motion of Polymer Gels journal, July 2013

Isomerization of spirobenzopyrans bearing electron-donating and electron-withdrawing groups in acidic aqueous solutions journal, January 2011

Beating polymer gels coupled with a nonlinear chemical reaction journal, June 1999

Mechanical Oscillation Coupled with the Belousov−Zhabotinsky Reaction in Gel journal, July 2003

Oscillatory dynamics induced in a responsive gel by a non-oscillatory chemical reaction: experimental evidence journal, January 2011

Autonomous Chemomechanical Oscillations in a Hydrogel/Enzyme System Driven by Glucose journal, September 2002

Novel Hydrogels for Rhythmic Pulsatile Drug Delivery journal, August 2007

Autonomous Rhythmic Drug Delivery Systems Based on Chemical and Biochemomechanical Oscillators book, January 2009

Synthetic homeostatic materials with chemo-mechano-chemical self-regulation journal, July 2012

Chemical waves in self-oscillating gels journal, July 2000

Shape- and size-dependent patterns in self-oscillating polymer gels journal, January 2011

Using Light to Guide the Self-Sustained Motion of Active Gels journal, April 2009

Designing autonomously motile gels that follow complex paths journal, January 2010

Photophobic and phototropic movement of a self-oscillating gel journal, January 2013

Pattern Formation and Shape Changes in Self-Oscillating Polymer Gels journal, November 2006

Theoretical and computational modeling of self-oscillating polymer gels journal, March 2007

Three-dimensional model for chemoresponsive polymer gels undergoing the Belousov-Zhabotinsky reaction journal, October 2008

Self-Oscillating Gel journal, January 1996

Self-Oscillating Polymer and Gels as Novel Biomimetic Materials journal, June 2008

Photoregulated Wormlike Motion of a Gel journal, November 2008

Exploiting gradients in cross-link density to control the bending and self-propelled motion of active gels journal, January 2011

Analysis of the modified complete Oregonator accounting for oxygen sensitivity and photosensitivity of Belousov-Zhabotinskii systems journal, June 1990

Self-oscillations in chemoresponsive gels: A theoretical approach journal, June 2005

Chemo-responsive, self-oscillating gels that undergo biomimetic communication journal, January 2013

Directing the Behavior of Active, Self-Oscillating Gels with Light journal, April 2014

Softening of bulk modulus and negative Poisson’s ratio near the volume phase transition of polymer gels journal, March 1991

Theory of phase transition in polymer gels book, January 1993

Target patterns in a realistic model of the Belousov–Zhabotinskii reaction journal, September 1980

Modeling autonomously oscillating chemo-responsive gels journal, January 2010

Kinetics of solvent absorption and permeation through a highly swellable elastomeric network: Solvent Absorption and Permeation journal, December 2002

Gel systems for the Belousov-Zhabotinskii reaction journal, July 1991

Chemically-mediated communication in self-oscillating, biomimetic cilia journal, January 2012

Polymer Gels: Modeling the Photoinduced Reconfiguration and Directed Motion of Polymer Gels (Adv. Funct. Mater. 36/2013) journal, September 2013

Theory of phase transition in polymer gels book, January 1993

Modeling autonomously oscillating chemo-responsive gels journal, January 2010

Photoresponsive Properties of Poly(N-isopropylacrylamide) Hydrogel Partly Modified with Spirobenzopyran journal, March 2006

Using Light to Guide the Self-Sustained Motion of Active Gels journal, April 2009

Synthetic homeostatic materials with chemo-mechano-chemical self-regulation journal, July 2012

Isomerization of spirobenzopyrans bearing electron-donating and electron-withdrawing groups in acidic aqueous solutions journal, January 2011

Photophobic and phototropic movement of a self-oscillating gel journal, January 2013

Beating polymer gels coupled with a nonlinear chemical reaction journal, June 1999

Theoretical and computational modeling of self-oscillating polymer gels journal, March 2007

Softening of bulk modulus and negative Poisson’s ratio near the volume phase transition of polymer gels journal, March 1991

Pattern Formation and Shape Changes in Self-Oscillating Polymer Gels journal, November 2006

Polyampholyte Hydrogels with pH Modulated Shape Memory and Spontaneous Actuation journal, March 2018

From isolated structures to continuous networks: A categorization of cytoskeleton‐based motile engineered biological microstructures journal, February 2019

Designing polymer gels and composites that undergo bio-inspired phototactic reconfiguration and motion journal, April 2018

Self-oscillation of polymer and photo-regulation by introducing photochromic site to induce LCST changes
journal, July 2013

Rewritable Microrelief Formation on Photoresponsive Hydrogel Layers
journal, May 2007

Fast-reversible light-driven hydrogels consisting of spirobenzopyran-functionalized poly(N-isopropylacrylamide)
journal, January 2011

Photoresponsive polymer gel microvalves controlled by local light irradiation
journal, November 2007

Photoresponsive Properties of Poly(N-isopropylacrylamide) Hydrogel Partly Modified with Spirobenzopyran
journal, March 2006

Modeling the Photoinduced Reconfiguration and Directed Motion of Polymer Gels
journal, July 2013

Isomerization of spirobenzopyrans bearing electron-donating and electron-withdrawing groups in acidic aqueous solutions
journal, January 2011

Beating polymer gels coupled with a nonlinear chemical reaction
journal, June 1999

Mechanical Oscillation Coupled with the Belousov−Zhabotinsky Reaction in Gel
journal, July 2003

Oscillatory dynamics induced in a responsive gel by a non-oscillatory chemical reaction: experimental evidence
journal, January 2011

Autonomous Chemomechanical Oscillations in a Hydrogel/Enzyme System Driven by Glucose
journal, September 2002

Novel Hydrogels for Rhythmic Pulsatile Drug Delivery
journal, August 2007

Autonomous Rhythmic Drug Delivery Systems Based on Chemical and Biochemomechanical Oscillators
book, January 2009

Synthetic homeostatic materials with chemo-mechano-chemical self-regulation
journal, July 2012

Chemical waves in self-oscillating gels
journal, July 2000

Shape- and size-dependent patterns in self-oscillating polymer gels
journal, January 2011

Using Light to Guide the Self-Sustained Motion of Active Gels
journal, April 2009

Designing autonomously motile gels that follow complex paths
journal, January 2010

Photophobic and phototropic movement of a self-oscillating gel
journal, January 2013

Pattern Formation and Shape Changes in Self-Oscillating Polymer Gels
journal, November 2006

Theoretical and computational modeling of self-oscillating polymer gels
journal, March 2007

Three-dimensional model for chemoresponsive polymer gels undergoing the Belousov-Zhabotinsky reaction
journal, October 2008

Self-Oscillating Gel
journal, January 1996

Self-Oscillating Polymer and Gels as Novel Biomimetic Materials
journal, June 2008

Photoregulated Wormlike Motion of a Gel
journal, November 2008

Exploiting gradients in cross-link density to control the bending and self-propelled motion of active gels
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Directing the Behavior of Active, Self-Oscillating Gels with Light
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Softening of bulk modulus and negative Poisson’s ratio near the volume phase transition of polymer gels
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Theory of phase transition in polymer gels
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Target patterns in a realistic model of the Belousov–Zhabotinskii reaction
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Modeling autonomously oscillating chemo-responsive gels
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Kinetics of solvent absorption and permeation through a highly swellable elastomeric network: Solvent Absorption and Permeation
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Gel systems for the Belousov-Zhabotinskii reaction
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Theory of phase transition in polymer gels
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Modeling autonomously oscillating chemo-responsive gels
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Photoresponsive Properties of Poly(N-isopropylacrylamide) Hydrogel Partly Modified with Spirobenzopyran
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Using Light to Guide the Self-Sustained Motion of Active Gels
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Synthetic homeostatic materials with chemo-mechano-chemical self-regulation
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Isomerization of spirobenzopyrans bearing electron-donating and electron-withdrawing groups in acidic aqueous solutions
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Photophobic and phototropic movement of a self-oscillating gel
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Beating polymer gels coupled with a nonlinear chemical reaction
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Theoretical and computational modeling of self-oscillating polymer gels
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Softening of bulk modulus and negative Poisson’s ratio near the volume phase transition of polymer gels
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Pattern Formation and Shape Changes in Self-Oscillating Polymer Gels
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Polyampholyte Hydrogels with pH Modulated Shape Memory and Spontaneous Actuation
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From isolated structures to continuous networks: A categorization of cytoskeleton‐based motile engineered biological microstructures
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