High‐Fidelity Bioelectronic Muscular Actuator Based on Graphene‐Mediated and TEMPO‐Oxidized Bacterial Cellulose

High-performance electoactive artificial muscles with biofriendly, biodegradable, and biocompatible functionalities have attracted enormous attention in the era of human friendly electronic devices such as wearable electronics, soft haptic devices, and implantable or disposal biomedical devices. Here, a high-fidelity bioelectronic soft actuator is reported based on biofriendly 2,2,6,6-tetramethylpiperidine-1-oxyl radical-oxidized bacterial cellulose (TOBC), chemically modified graphene, and ionic liquid [EMIM][BF4] as plasticizer, thereby realizing large deformable, faster, biodegradable, air working, and highly durable TOBC-IL-G muscular actuator. Especially, the TOBC-IL-G(0.10 wt%) membrane shows a dramatic increment of the ionic conductivity up to 120%, of specific capacitance up to 95%, of tensile modulus up to 63%, and of tensile strength up to 60%, for TOBC-IL, resulting in 2.3 times larger bending deformation without serious back-relaxation phenomena. The developed high-performance and durable bioelectronic muscular actuator can be a promising candidate for satisfying the tight requirements of human-related bioengineering as well as biomimetic robotics and biomedical active devices.

[1]  S. Nemat-Nasser,et al.  Comparative experimental study of ionic polymer–metal composites with different backbone ionomers and in various cation forms , 2003 .

[2]  Ying Hu,et al.  Graphene‐Stabilized Silver Nanoparticle Electrochemical Electrode for Actuator Design , 2013, Advanced materials.

[3]  Mihai Irimia-Vladu,et al.  "Green" electronics: biodegradable and biocompatible materials and devices for sustainable future. , 2014, Chemical Society reviews.

[4]  A. Isogai,et al.  Wood cellulose nanofibrils prepared by TEMPO electro-mediated oxidation , 2011 .

[5]  H. Yano,et al.  Synthesis of silver nanoparticles templated by TEMPO-mediated oxidized bacterial cellulose nanofibers. , 2009, Biomacromolecules.

[6]  Akira Isogai,et al.  TEMPO-oxidized cellulose nanofibers. , 2011, Nanoscale.

[7]  Wei Chen,et al.  Biocompatible Composite Actuator: A Supramolecular Structure Consisting of the Biopolymer Chitosan, Carbon Nanotubes, and an Ionic Liquid , 2010, Advanced materials.

[8]  Sungryul Yun,et al.  Discovery of Cellulose as a Smart Material , 2006 .

[9]  I. Oh,et al.  Bacterial cellulose actuator with electrically driven bending deformation in hydrated condition , 2010 .

[10]  I. Oh,et al.  Dry‐Type Artificial Muscles Based on Pendent Sulfonated Chitosan and Functionalized Graphene Oxide for Greatly Enhanced Ionic Interactions and Mechanical Stiffness , 2013 .

[11]  I. Oh,et al.  Electrospun fullerenol-cellulose biocompatible actuators. , 2011, Biomacromolecules.

[12]  T. Fukushima,et al.  Fully plastic actuator through layer-by-layer casting with ionic-liquid-based bucky gel. , 2005, Angewandte Chemie.

[13]  I. Oh,et al.  Fullerenol-based electroactive artificial muscles utilizing biocompatible polyetherimide. , 2011, ACS nano.

[14]  Mihai Irimia-Vladu,et al.  Green and biodegradable electronics , 2012 .

[15]  K. Yoshino,et al.  A mechanically strong, flexible and conductive film based on bacterial cellulose/graphene nanocomposite. , 2012, Carbohydrate polymers.

[16]  A. Isogai,et al.  Preparation and characterization of TEMPO-oxidized cellulose nanofibril films with free carboxyl groups , 2011 .

[17]  Akira Isogai,et al.  Cellulose nanofibers prepared by TEMPO-mediated oxidation of native cellulose. , 2007, Biomacromolecules.

[18]  Ray H. Baughman,et al.  Playing Nature's Game with Artificial Muscles , 2005, Science.

[19]  Il-Kwon Oh,et al.  Novel electroactive PVA-TOCN actuator that is extremely sensitive to low electrical inputs , 2014 .

[20]  M. Schramm,et al.  Synthesis of cellulose by Acetobacter xylinum. II. Preparation of freeze-dried cells capable of polymerizing glucose to cellulose. , 1954, The Biochemical journal.

[21]  H. Okuzaki,et al.  Electrochemical characterization of PEDOT-PSS-Sorbitol electrodes. Sorbitol changes cation to anion interchange during reactions , 2011 .

[22]  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.

[23]  B. Evans,et al.  Palladium-bacterial cellulose membranes for fuel cells. , 2003, Biosensors & bioelectronics.

[24]  Q. Hao,et al.  In situ deposition of platinum nanoparticles on bacterial cellulose membranes and evaluation of PEM fuel cell performance , 2009 .

[25]  I. Oh,et al.  Electroactive bio-composite actuators based on cellulose acetate nanofibers with specially chopped polyaniline nanoparticles through electrospinning , 2013 .

[26]  Timothy O'Connor,et al.  Plasticization of PEDOT:PSS by Common Additives for Mechanically Robust Organic Solar Cells and Wearable Sensors , 2015 .

[27]  Kinji Asaka,et al.  Recent advances in ionic polymer–metal composite actuators and their modeling and applications , 2013 .

[28]  Seung-Hyeon Moon,et al.  Preparation and characterization of acrylic acid-treated bacterial cellulose cation-exchange membrane , 2004 .

[29]  M. Berggren,et al.  Electrocardiographic Recording with Conformable Organic Electrochemical Transistor Fabricated on Resorbable Bioscaffold , 2014, Advanced materials.

[30]  Zhiqiang Fang,et al.  Novel nanostructured paper with ultrahigh transparency and ultrahigh haze for solar cells. , 2014, Nano letters.

[31]  T. Otero,et al.  Structural Electrochemistry: Conductivities and Ionic Content from Rising Reduced Polypyrrole Films , 2014 .

[32]  I. Oh,et al.  Electro-active hybrid actuators based on freeze-dried bacterial cellulose and PEDOT:PSS , 2013 .

[33]  F. Carpi,et al.  Biomedical applications of electroactive polymer actuators , 2009 .

[34]  Larry R. Dalton,et al.  Pneumatic carbon nanotube actuators , 2002 .

[35]  I. Oh,et al.  Bio‐Inspired All‐Organic Soft Actuator Based on a π–π Stacked 3D Ionic Network Membrane and Ultra‐Fast Solution Processing , 2014 .

[36]  I. Oh,et al.  A Biomimetic Actuator Based on an Ionic Networking Membrane of Poly(styrene‐alt‐maleimide)‐Incorporated Poly(vinylidene fluoride) , 2008 .