Electrically Controllable Actuators Based on Supramolecular Peptide Hydrogels

Hydrogel actuators that can undergo structural change upon external stimuli are highly demanded due to their potential applications in diverse fields. However, the actuators based on physically cross‐linked supramolecular hydrogels are largely unexplored. This study reports the engineering of an electrically controllable supramolecular hydrogel as an actuator from a self‐assembling short peptide, in which a catechol moiety is introduced as the stimuli‐responsive motif. This kind of electrochemically responsive hydrogel is mechanically stable and can switch its physical properties dramatically upon the applied electric field. The mechanism and reversibility of the change are studied in detail. As a proof of principle, devices are designed to perform the unidirectional expansion and rotational motion under electrical stimulations. The applications of the actuators for controllable drug release and actuation of microfluidic devices are also illustrated. It is expected that these kind of supramolecular hydrogel actuators can find broad applications as novel biosensors, artificial robots, and smart soft materials.

[1]  Bing Xu,et al.  Supramolecular hydrogels based on biofunctional nanofibers of self-assembled small molecules , 2007 .

[2]  Y. Hemar,et al.  Structure-mechanical property correlations of hydrogel forming β-sheet peptides. , 2016, Chemical Society reviews.

[3]  Yoonkey Nam,et al.  Electrochemically driven, electrode-addressable formation of functionalized polydopamine films for neural interfaces. , 2012, Angewandte Chemie.

[4]  Zhimou Yang,et al.  Glutathione-triggered formation of molecular hydrogels for 3D cell culture. , 2013, Colloids and surfaces. B, Biointerfaces.

[5]  G. Liang,et al.  In situ clicking methylglyoxal for hierarchical self-assembly of nanotubes in supramolecular hydrogel. , 2016, Nanoscale.

[6]  E. Palleau,et al.  Reversible patterning and actuation of hydrogels by electrically assisted ionoprinting , 2013, Nature Communications.

[7]  In Taek Song,et al.  Vanadyl−Catecholamine Hydrogels Inspired by Ascidians and Mussels , 2015 .

[8]  Tomoyuki Ishikawa,et al.  Rapid and reversible shape changes of molecular crystals on photoirradiation , 2007, Nature.

[9]  Lirong Kong,et al.  Carbon Nanotube and Graphene‐based Bioinspired Electrochemical Actuators , 2014, Advanced materials.

[10]  Ying Hu,et al.  Electromechanical actuation with controllable motion based on a single-walled carbon nanotube and natural biopolymer composite. , 2010, ACS nano.

[11]  Ehud Gazit,et al.  The physical properties of supramolecular peptide assemblies: from building block association to technological applications. , 2014, Chemical Society reviews.

[12]  Rein V. Ulijn,et al.  Peptide-based stimuli-responsive biomaterials. , 2006, Soft matter.

[13]  J. Aizenberg,et al.  Reversible Switching of Hydrogel-Actuated Nanostructures into Complex Micropatterns , 2007, Science.

[14]  Jinming Hu,et al.  Enzyme-responsive polymeric assemblies, nanoparticles and hydrogels. , 2012, Chemical Society reviews.

[15]  H. Koshima,et al.  Light-Driven Bending Crystals of Salicylidenephenylethylamines in Enantiomeric and Racemate Forms , 2013 .

[16]  L. Zepeda-Ruiz,et al.  Surface-chemistry-driven actuation in nanoporous gold. , 2009, Nature materials.

[17]  Jiajie Liang,et al.  The application of graphene based materials for actuators , 2012 .

[18]  Ehud Gazit,et al.  Self-assembly of short peptides to form hydrogels: design of building blocks, physical properties and technological applications. , 2014, Acta biomaterialia.

[19]  A. Piccolo,et al.  Structural characterization of isomeric dimers from the oxidative oligomerization of catechol with a biomimetic catalyst. , 2007, Biomacromolecules.

[20]  S. Fang,et al.  Electromechanical Actuators Based on Graphene and Graphene/Fe3O4 Hybrid Paper , 2011 .

[21]  S. Martin,et al.  Surface Structures of 4-Chlorocatechol Adsorbed on Titanium Dioxide , 1996 .

[22]  Yen Wei,et al.  Mouldable liquid-crystalline elastomer actuators with exchangeable covalent bonds. , 2014, Nature materials.

[23]  Choon Chiang Foo,et al.  Stretchable, Transparent, Ionic Conductors , 2013, Science.

[24]  Stephen Marshall,et al.  Biocatalytic induction of supramolecular order , 2010, Nature Chemistry.

[25]  Qiang Zhao,et al.  An instant multi-responsive porous polymer actuator driven by solvent molecule sorption , 2014, Nature Communications.

[26]  Giseop Kwak,et al.  Fluorescent Actuator Based on Microporous Conjugated Polymer with Intramolecular Stack Structure , 2012, Advanced materials.

[27]  P. Calvert,et al.  Multilayer Hydrogels as Muscle‐Like Actuators , 2000 .

[28]  Huaimin Wang,et al.  Rational design of a tetrameric protein to enhance interactions between self-assembled fibers gives molecular hydrogels. , 2012, Angewandte Chemie.

[29]  Jingfeng Jiang,et al.  pH Responsive and Oxidation Resistant Wet Adhesive based on Reversible Catechol–Boronate Complexation , 2016, Chemistry of materials : a publication of the American Chemical Society.

[30]  Moon Jeong Park,et al.  Fast low-voltage electroactive actuators using nanostructured polymer electrolytes , 2013, Nature Communications.

[31]  Giao T. M. Nguyen,et al.  Graphitic carbon nitride nanosheet electrode-based high-performance ionic actuator , 2015, Nature Communications.

[32]  Jianwu Zhang,et al.  Phenothiazine as an aromatic capping group to construct a short peptide-based 'super gelator'. , 2013, Chemical communications.

[33]  Huaimin Wang,et al.  BSA-stabilized molecular hydrogels of a hydrophobic compound. , 2012, Nanoscale.

[34]  G. Liang,et al.  Peptide-based nanostructures for cancer diagnosis and therapy. , 2014, Current medicinal chemistry.

[35]  Derek N. Woolfson,et al.  Rational design and application of responsive α-helical peptide hydrogels , 2009, Nature materials.

[36]  Leonid Ionov,et al.  Unusual and Superfast Temperature‐Triggered Actuators , 2015, Advanced materials.

[37]  T. Weil,et al.  Precise Control of Polydopamine Film Formation by Electropolymerization , 2014 .

[38]  T. Osakai,et al.  Unusually large numbers of electrons for the oxidation of polyphenolic antioxidants. , 2001, Biochimica et biophysica acta.

[39]  Bruce P. Lee,et al.  Mussel-Inspired Adhesives and Coatings. , 2011, Annual review of materials research.

[40]  Bing Xu,et al.  Giant volume change of active gels under continuous flow. , 2014, Journal of the American Chemical Society.

[41]  Bing Xu,et al.  Molecular hydrogels of therapeutic agents. , 2009, Chemical Society reviews.

[42]  Megan L. McCain,et al.  A tissue-engineered jellyfish with biomimetic propulsion , 2012, Nature Biotechnology.

[43]  Seon Jeong Kim,et al.  Torsional Carbon Nanotube Artificial Muscles , 2011, Science.

[44]  Jong-Man Kim,et al.  An Electrolyte-Free Conducting Polymer Actuator that Displays Electrothermal Bending and Flapping Wing Motions under a Magnetic Field. , 2016, ACS applied materials & interfaces.

[45]  D. Waldeck,et al.  Manipulating Mechanical Properties with Electricity: Electroplastic Elastomer Hydrogels. , 2012, ACS macro letters.

[46]  Haifeng Yu,et al.  Photocontrollable Liquid‐Crystalline Actuators , 2011, Advanced materials.

[47]  Malav S. Desai,et al.  Light-controlled graphene-elastin composite hydrogel actuators. , 2013, Nano letters.

[48]  Jun Feng,et al.  Large-area graphene realizing ultrasensitive photothermal actuator with high transparency: new prototype robotic motions under infrared-light stimuli , 2011 .

[49]  Todd A. Gisby,et al.  Multi-functional dielectric elastomer artificial muscles for soft and smart machines , 2012 .

[50]  Na Li,et al.  Electromechanical actuator with controllable motion, fast response rate, and high-frequency resonance based on graphene and polydiacetylene. , 2012, ACS nano.

[51]  M. Spiteller,et al.  Oligomerization of humic phenolic monomers by oxidative coupling under biomimetic catalysis. , 2006, Environmental science & technology.

[52]  D. Beebe,et al.  Flow control with hydrogels. , 2004, Advanced drug delivery reviews.

[53]  D. Waldeck,et al.  Chemical and Electrochemical Manipulation of Mechanical Properties in Stimuli-Responsive Copper-Cross-Linked Hydrogels. , 2013, ACS macro letters.

[54]  Y. Li,et al.  An enzyme-assisted nanoparticle crosslinking approach to enhance the mechanical strength of peptide-based supramolecular hydrogels. , 2013, Chemical communications.

[55]  Bing Xu,et al.  A redox responsive, fluorescent supramolecular metallohydrogel consists of nanofibers with single-molecule width. , 2013, Journal of the American Chemical Society.

[56]  M. Madou,et al.  Genetically engineered protein in hydrogels tailors stimuli-responsive characteristics , 2005, Nature Materials.

[57]  Sung Min Kang,et al.  One-step modification of superhydrophobic surfaces by a mussel-inspired polymer coating. , 2010, Angewandte Chemie.

[58]  Wouter Olthuis,et al.  Stimulus-sensitive hydrogels and their applications in chemical (micro)analysis. , 2003, The Analyst.

[59]  C. Spillmann,et al.  Liquid‐Crystalline Nano‐optomechanical Actuator , 2013 .

[60]  Sergiy Minko,et al.  Stimuli‐Responsive Porous Hydrogels at Interfaces for Molecular Filtration, Separation, Controlled Release, and Gating in Capsules and Membranes , 2010, Advanced materials.

[61]  Yi Cao,et al.  Designing the mechanical properties of peptide-based supramolecular hydrogels for biomedical applications , 2014 .

[62]  Akira Harada,et al.  Redox-generated mechanical motion of a supramolecular polymeric actuator based on host-guest interactions. , 2013, Angewandte Chemie.

[63]  Hidenori Okuzaki,et al.  Humidity‐Sensitive Polypyrrole Films for Electro‐Active Polymer Actuators , 2013 .

[64]  Patrick Onck,et al.  Metallic muscles at work: high rate actuation in nanoporous gold/polyaniline composites. , 2013, ACS nano.

[65]  Bruce P. Lee,et al.  Novel Hydrogel Actuator Inspired by Reversible Mussel Adhesive Protein Chemistry , 2014, Advanced materials.

[66]  Vesselin Shanov,et al.  A multi-wall carbon nanotube tower electrochemical actuator. , 2006, Nano letters.

[67]  Liang Dong,et al.  Autonomous microfluidics with stimuli-responsive hydrogels. , 2007, Soft matter.

[68]  P. Janmey,et al.  Nonlinear elasticity in biological gels , 2004, Nature.

[69]  Ben Fabry,et al.  Stress controls the mechanics of collagen networks , 2015, Proceedings of the National Academy of Sciences.

[70]  Bong Hoon Kim,et al.  Electric Actuation of Nanostructured Thermoplastic Elastomer Gels with Ultralarge Electrostriction Coefficients , 2011 .

[71]  Bing Xu,et al.  Supramolecular hydrogel of a D-amino acid dipeptide for controlled drug release in vivo. , 2009, Langmuir : the ACS journal of surfaces and colloids.

[72]  Vahid Mottaghitalab,et al.  Carbon‐Nanotube‐Reinforced Polyaniline Fibers for High‐Strength Artificial Muscles , 2006 .

[73]  Il-Kwon Oh,et al.  Durable and water-floatable ionic polymer actuator with hydrophobic and asymmetrically laser-scribed reduced graphene oxide paper electrodes. , 2014, ACS nano.

[74]  Hongbo Zeng,et al.  Novel Mussel‐Inspired Injectable Self‐Healing Hydrogel with Anti‐Biofouling Property , 2015, Advanced materials.

[75]  Eduardo Mendes,et al.  Responsive biomimetic networks from polyisocyanopeptide hydrogels , 2013, Nature.

[76]  Wendelin Jan Stark,et al.  Crosslinking metal nanoparticles into the polymer backbone of hydrogels enables preparation of soft, magnetic field-driven actuators with muscle-like flexibility. , 2009, Small.

[77]  Daniela Kalafatovic,et al.  Exploring the sequence space for (tri-)peptide self-assembly to design and discover new hydrogels. , 2015, Nature chemistry.

[78]  Bo Zheng,et al.  Stimuli-responsive supramolecular polymeric materials. , 2012, Chemical Society reviews.