Scalable Manufactured Self-Healing Strain Sensors Based on Ion-Intercalated Graphene Nanosheets and Interfacial Coordination.

Desirable mechanical strength and self-healing performance are very important to highly sensitive and stretchable sensors to meet their practical applications. However, balancing these two key performance parameters is still a great challenge. Herein, we present a simple, large-scale, and cost-efficient route to fabricate autonomously self-healing strain sensors with satisfactory mechanical properties. Specifically, ion-intercalated mechanical milling was utilized to realize the large-scale preparation of graphene nanosheets (GNs). Then, a well-organized GN-nanostructured network was constructed in a rubber matrix based on interfacial metal-ligand coordination. The resultant nanocomposites show desirable mechanical properties (∼5 times higher than that of control sample without interfacial coordination), excellent self-healing performance (even healable in various harsh conditions, for example, underwater, at subzero temperature or exposed in acidic and alkaline conditions), and ultrahigh sensitivity (gauge factor ≈ 45 573.1). The elaborately designed strain sensors offer a feasible approach for the scalable production of self-healing strain-sensing devices, making it promising for further applications, including artificial skin, smart robotics, and other electrical devices.

[1]  Qingchuan Tao,et al.  Multiple Hydrogen Bonding Enables the Self-Healing of Sensors for Human-Machine Interactions. , 2017, Angewandte Chemie.

[2]  Jeongdai Jo,et al.  A photonic sintering derived Ag flake/nanoparticle-based highly sensitive stretchable strain sensor for human motion monitoring. , 2018, Nanoscale.

[3]  R. Sun,et al.  Recent Advancements in Flexible and Stretchable Electrodes for Electromechanical Sensors: Strategies, Materials, and Features. , 2017, ACS applied materials & interfaces.

[4]  Xinxing Zhang,et al.  A cephalopod-inspired mechanoluminescence material with skin-like self-healing and sensing properties , 2019, Materials Horizons.

[5]  Li Zhang,et al.  Highly Stretchable Room-Temperature Self-Healing Conductors Based on Wrinkled Graphene Films for Flexible Electronics. , 2019, ACS applied materials & interfaces.

[6]  Wei Huang,et al.  Stretchable Ti3C2Tx MXene/Carbon Nanotube Composite Based Strain Sensor with Ultrahigh Sensitivity and Tunable Sensing Range. , 2017, ACS nano.

[7]  Xinxing Zhang,et al.  Arbitrarily 3D Configurable Hygroscopic Robots with a Covalent–Noncovalent Interpenetrating Network and Self‐Healing Ability , 2019, Advanced materials.

[8]  Canhui Lu,et al.  In-situ reduction of graphene oxide-wrapped porous polyurethane scaffolds: Synergistic enhancement of mechanical properties and piezoresistivity , 2019, Composites Part A: Applied Science and Manufacturing.

[9]  Zhenqiang Ma,et al.  Cellulose nanofibril/reduced graphene oxide/carbon nanotube hybrid aerogels for highly flexible and all-solid-state supercapacitors. , 2015, ACS applied materials & interfaces.

[10]  Zhanhu Guo,et al.  Multistimuli-Responsive Intrinsic Self-Healing Epoxy Resin Constructed by Host–Guest Interactions , 2018, Macromolecules.

[11]  Jonathan Seppala,et al.  A healable supramolecular polymer blend based on aromatic pi-pi stacking and hydrogen-bonding interactions. , 2010, Journal of the American Chemical Society.

[12]  Lei Liu,et al.  Direct exfoliation of graphite in water with addition of ammonia solution. , 2017, Journal of colloid and interface science.

[13]  Y. Arao,et al.  Efficient solvent systems for improving production of few-layer graphene in liquid phase exfoliation , 2017 .

[14]  D. Weitz,et al.  Tough Self‐Healing Elastomers by Molecular Enforced Integration of Covalent and Reversible Networks , 2017, Advanced materials.

[15]  Xin Li,et al.  Carbon Nanocoil-Based Fast-Response and Flexible Humidity Sensor for Multifunctional Applications. , 2019, ACS applied materials & interfaces.

[16]  Wanchul Seung,et al.  Active Matrix Electronic Skin Strain Sensor Based on Piezopotential‐Powered Graphene Transistors , 2015, Advanced materials.

[17]  Lijie Li,et al.  Ultra-high sensitivity strain sensor based on piezotronic bipolar transistor , 2018, Nano Energy.

[18]  Benjamin C. K. Tee,et al.  An electrically and mechanically self-healing composite with pressure- and flexion-sensitive properties for electronic skin applications. , 2012, Nature nanotechnology.

[19]  S. Orrego,et al.  Ultrasensitive, flexible, and low-cost nanoporous piezoresistive composites for tactile pressure sensing. , 2019, Nanoscale.

[20]  Zhong Lin Wang,et al.  Large‐Area All‐Textile Pressure Sensors for Monitoring Human Motion and Physiological Signals , 2017, Advanced materials.

[21]  Chunya Wang,et al.  Carbonized Cotton Fabric for High‐Performance Wearable Strain Sensors , 2017 .

[22]  Quankang Wang,et al.  A Bioinspired Mineral Hydrogel as a Self‐Healable, Mechanically Adaptable Ionic Skin for Highly Sensitive Pressure Sensing , 2017, Advanced materials.

[23]  Xiaodong Wu,et al.  Self-healing strain sensors based on nanostructured supramolecular conductive elastomers , 2017 .

[24]  Shaohui Li,et al.  A Stretchable and Self‐Healing Energy Storage Device Based on Mechanically and Electrically Restorative Liquid‐Metal Particles and Carboxylated Polyurethane Composites , 2018, Advanced materials.

[25]  Jin-shui Yao,et al.  Molecular interactions in gelatin/chitosan composite films. , 2017, Food chemistry.

[26]  Qiang Liu,et al.  High-Performance Strain Sensors with Fish-Scale-Like Graphene-Sensing Layers for Full-Range Detection of Human Motions. , 2016, ACS nano.

[27]  Woo Jin Hyun,et al.  Highly stretchable and wearable graphene strain sensors with controllable sensitivity for human motion monitoring. , 2015, ACS applied materials & interfaces.

[28]  Babak Ziaie,et al.  Highly stretchable and sensitive unidirectional strain sensor via laser carbonization. , 2015, ACS applied materials & interfaces.

[29]  Yong Lin,et al.  Ultrasensitive Cracking-Assisted Strain Sensors Based on Silver Nanowires/Graphene Hybrid Particles. , 2016, ACS applied materials & interfaces.

[30]  D. Kaplan,et al.  Multilayered Magnetic Gelatin Membrane Scaffolds. , 2015, ACS applied materials & interfaces.

[31]  S. Zhang,et al.  An efficient multiple healing conductive composite via host-guest inclusion. , 2015, Chemical communications.

[32]  Yitai Qian,et al.  Ferric chloride-graphite intercalation compounds as anode materials for Li-ion batteries. , 2014, ChemSusChem.

[33]  Biqiong Chen,et al.  Synthesis of Multiwalled Carbon Nanotube-Reinforced Polyborosiloxane Nanocomposites with Mechanically Adaptive and Self-Healing Capabilities for Flexible Conductors. , 2016, ACS applied materials & interfaces.

[34]  Jessica J. Cash,et al.  Room-Temperature Self-Healing Polymers Based on Dynamic-Covalent Boronic Esters , 2015 .

[35]  C. Buckley,et al.  A Thermoreversible Supramolecular Polyurethane with Excellent Healing Ability at 45 °C , 2015 .

[36]  Yangyang Han,et al.  Self-Healing, Highly Sensitive Electronic Sensors Enabled by Metal-Ligand Coordination and Hierarchical Structure Design. , 2017, ACS applied materials & interfaces.

[37]  H. Nasir,et al.  A flexible, ultra-sensitive strain sensor based on carbon nanocoil network fabricated by an electrophoretic method. , 2017, Nanoscale.

[38]  A. Bourlinos,et al.  Liquid-phase exfoliation of graphite towards solubilized graphenes. , 2009, Small.

[39]  Ping Zhang,et al.  A Sunlight-Degradable Autonomous Self-Healing Supramolecular Elastomer for Flexible Electronic Devices , 2018 .

[40]  Canhui Lu,et al.  Exfoliation/dispersion of low-temperature expandable graphite in nanocellulose matrix by wet co-milling. , 2017, Carbohydrate polymers.

[41]  Canhui Lu,et al.  A well-organized graphene nanostructure for versatile strain-sensing application constructed by a covalently bonded graphene/rubber interface , 2018 .

[42]  Xingrong Zeng,et al.  Thiolated Graphene@Polyester Fabric-Based Multilayer Piezoresistive Pressure Sensors for Detecting Human Motion. , 2018, ACS applied materials & interfaces.

[43]  Changlin Zhou,et al.  Hierarchically Structured Self‐Healing Sensors with Tunable Positive/Negative Piezoresistivity , 2018 .

[44]  D. Wei,et al.  Fe3+-induced oxidation and coordination cross-linking in catechol–chitosan hydrogels under acidic pH conditions , 2015 .

[45]  Jiajun Fu,et al.  Autonomous self-healing supramolecular elastomer reinforced and toughened by graphitic carbon nitride nanosheets tailored for smart anticorrosion coating applications , 2018 .

[46]  Xinxing Zhang,et al.  Templated synthesis of a 1D Ag nanohybrid in the solid state and its organized network for strain-sensing applications , 2018 .

[47]  Mehmet Turan,et al.  Parallel Microcracks-based Ultrasensitive and Highly Stretchable Strain Sensors. , 2016, ACS applied materials & interfaces.

[48]  Chengguo Hu,et al.  Tuning electrochemical behaviors of N-methyl-2-pyrrolidone liquid exfoliated graphene nanosheets by centrifugal speed-based grading , 2018 .

[49]  R. Sun,et al.  Biomimetic, recyclable, highly stretchable and self-healing conductors enabled by dual reversible bonds , 2019, Chemical Engineering Journal.

[50]  Xinxing Zhang,et al.  A naturally-derived supramolecular elastomer containing green-synthesized silver nanofibers for self-repairing E-skin sensor , 2019, Journal of Materials Chemistry C.

[51]  U. Schubert,et al.  Conditional repair by locally switching the thermal healing capability of dynamic covalent polymers with light , 2016, Nature Communications.

[52]  Run-Wei Li,et al.  Mechano-regulated metal–organic framework nanofilm for ultrasensitive and anti-jamming strain sensing , 2018, Nature Communications.

[53]  T. Trung,et al.  Flexible and Stretchable Physical Sensor Integrated Platforms for Wearable Human‐Activity Monitoringand Personal Healthcare , 2016, Advanced materials.

[54]  Olivia R. Cromwell,et al.  Self-healing multiphase polymers via dynamic metal-ligand interactions. , 2014, Journal of the American Chemical Society.

[55]  R. Sun,et al.  Highly Stretchable and Sensitive Strain Sensor Based on Facilely Prepared Three-Dimensional Graphene Foam Composite. , 2016, ACS applied materials & interfaces.

[56]  Hyung Jin Sung,et al.  Highly Stretchable, Hysteresis-Free Ionic Liquid-Based Strain Sensor for Precise Human Motion Monitoring. , 2017, ACS applied materials & interfaces.

[57]  W. Lu,et al.  Improved synthesis of graphene oxide. , 2010, ACS nano.

[58]  Yanbo Yao,et al.  A Route toward Ultrasensitive Layered Carbon Based Piezoresistive Sensors through Hierarchical Contact Design. , 2017, ACS applied materials & interfaces.