Printing assembly and structural regulation of graphene towards three-dimensional flexible micro-supercapacitors

Flexible, high-performance miniature supercapacitors that offer reliable energy storage and output are desirable for use in portable and wearable electronics. Herein, we developed micro-supercapacitors with three-dimensional electrodes by printing assembly of graphene. By controlling the microstructures and macroscopic architectures of the graphene electrodes, superior electrochemical performance was achieved; especially, we demonstrated an advancement to address the limitation of areal capacitance. The unique three-dimensional graphene structure also provides this new class of micro-supercapacitors with exceptional mechanical flexibility. With these remarkable features, facile integration of the micro-supercapacitor array into flexible printed circuits was demonstrated. This printing assembly approach will pave the way to explore energy storage systems with diverse structures and extended functionalities.

[1]  Lili Liu,et al.  A Universal Strategy to Prepare Functional Porous Graphene Hybrid Architectures , 2014, Advanced materials.

[2]  Shu‐Hong Yu,et al.  Graphene-based macroscopic assemblies and architectures: an emerging material system. , 2014, Chemical Society reviews.

[3]  Klaus Müllen,et al.  Ultrathin Printable Graphene Supercapacitors with AC Line‐Filtering Performance , 2015, Advanced materials.

[4]  Sheng Yang,et al.  Ultraflexible In‐Plane Micro‐Supercapacitors by Direct Printing of Solution‐Processable Electrochemically Exfoliated Graphene , 2016, Advanced materials.

[5]  L. Qu,et al.  Solution-Processed Ultraelastic and Strong Air-Bubbled Graphene Foams. , 2016, Small.

[6]  M. El‐Kady,et al.  Scalable fabrication of high-power graphene micro-supercapacitors for flexible and on-chip energy storage , 2013, Nature Communications.

[7]  Joong Tark Han,et al.  3D Printing of Reduced Graphene Oxide Nanowires , 2015, Advanced materials.

[8]  Yi Cui,et al.  Self-assembled three-dimensional and compressible interdigitated thin-film supercapacitors and batteries , 2015, Nature Communications.

[9]  Zheye Zhang,et al.  Functionalized carbonaceous fibers for high performance flexible all-solid-state asymmetric supercapacitors , 2015 .

[10]  R. Ruoff,et al.  Graphene, related two-dimensional crystals, and hybrid systems for energy conversion and storage , 2015, Science.

[11]  Yongsung Ji,et al.  High‐Performance Pseudocapacitive Microsupercapacitors from Laser‐Induced Graphene , 2016, Advanced materials.

[12]  Liangbing Hu,et al.  Three-Dimensional Printable High-Temperature and High-Rate Heaters. , 2016, ACS nano.

[13]  J. Choi,et al.  3D macroporous graphene frameworks for supercapacitors with high energy and power densities. , 2012, ACS nano.

[14]  Y. Gogotsi,et al.  Synthesis of Two‐Dimensional Materials for Capacitive Energy Storage , 2016, Advanced materials.

[15]  Jiangtao Hu,et al.  3D‐Printed Cathodes of LiMn1−xFexPO4 Nanocrystals Achieve Both Ultrahigh Rate and High Capacity for Advanced Lithium‐Ion Battery , 2016 .

[16]  Klaus Müllen,et al.  3D Graphene Foams Cross‐linked with Pre‐encapsulated Fe3O4 Nanospheres for Enhanced Lithium Storage , 2013, Advanced materials.

[17]  Yanlin Song,et al.  Three-dimensional multi-recognition flexible wearable sensor via graphene aerogel printing. , 2016, Chemical communications.

[18]  J. A. Lewis.  Direct Ink Writing of 3D Functional Materials , 2006 .

[19]  Tian Li,et al.  Graphene Oxide‐Based Electrode Inks for 3D‐Printed Lithium‐Ion Batteries , 2016, Advanced materials.

[20]  Yunqi Liu,et al.  One-pot self-assembled three-dimensional TiO2-graphene hydrogel with improved adsorption capacities and photocatalytic and electrochemical activities. , 2013, ACS applied materials & interfaces.

[21]  M. El‐Kady,et al.  Graphene-based materials for flexible supercapacitors. , 2015, Chemical Society reviews.

[22]  Dan Li,et al.  Biomimetic superelastic graphene-based cellular monoliths , 2012, Nature Communications.

[23]  G. Shi,et al.  Graphene Hydrogels Deposited in Nickel Foams for High‐Rate Electrochemical Capacitors , 2012, Advanced materials.

[24]  B. Scrosati,et al.  The role of graphene for electrochemical energy storage. , 2015, Nature materials.

[25]  Yunqi Liu,et al.  Facile Synthesis of 3D MnO2–Graphene and Carbon Nanotube–Graphene Composite Networks for High‐Performance, Flexible, All‐Solid‐State Asymmetric Supercapacitors , 2014 .

[26]  Won Suk Chang,et al.  Three-Dimensional Printing of Highly Conductive Carbon Nanotube Microarchitectures with Fluid Ink. , 2016, ACS nano.

[27]  Fei Xiao,et al.  Hierarchically structured MnO2/graphene/carbon fiber and porous graphene hydrogel wrapped copper wire for fiber-based flexible all-solid-state asymmetric supercapacitors , 2015, Journal of Materials Chemistry A.

[28]  Jiujun Zhang,et al.  A Review of Graphene‐Based Nanostructural Materials for Both Catalyst Supports and Metal‐Free Catalysts in PEM Fuel Cell Oxygen Reduction Reactions , 2014 .

[29]  M. El‐Kady,et al.  Laser Scribing of High-Performance and Flexible Graphene-Based Electrochemical Capacitors , 2012, Science.

[30]  Z. Yin,et al.  Three-dimensional graphene materials: preparation, structures and application in supercapacitors , 2014 .

[31]  Chee Kai Chua,et al.  Layer-by-layer printing of laminated graphene-based interdigitated microelectrodes for flexible planar micro-supercapacitors , 2015 .

[32]  Eduardo Saiz,et al.  Printing in Three Dimensions with Graphene , 2015, Advanced materials.

[33]  G. Shi,et al.  Base‐Induced Liquid Crystals of Graphene Oxide for Preparing Elastic Graphene Foams with Long‐Range Ordered Microstructures , 2016, Advanced materials.

[34]  Martin Pumera,et al.  3D-printing technologies for electrochemical applications. , 2016, Chemical Society reviews.

[35]  Alexandra M. Golobic,et al.  Highly compressible 3D periodic graphene aerogel microlattices , 2015, Nature Communications.

[36]  Alexandra L. Rutz,et al.  Three-dimensional printing of high-content graphene scaffolds for electronic and biomedical applications. , 2015, ACS nano.

[37]  Feng Zhang,et al.  3D Printing of Graphene Aerogels. , 2016, Small.

[38]  John A Rogers,et al.  Holographic patterning of high-performance on-chip 3D lithium-ion microbatteries , 2015, Proceedings of the National Academy of Sciences.

[39]  Yongsheng Chen,et al.  An overview of the applications of graphene-based materials in supercapacitors. , 2012, Small.

[40]  J. Coleman,et al.  2D‐Crystal‐Based Functional Inks , 2016, Advanced materials.

[41]  Zhiqiang Niu,et al.  All‐Solid‐State Flexible Ultrathin Micro‐Supercapacitors Based on Graphene , 2013, Advanced materials.

[42]  Zhiqiang Niu,et al.  Structural diversity of bulky graphene materials. , 2014, Small.

[43]  Yunqi Liu,et al.  Freestanding graphene paper supported three-dimensional porous graphene-polyaniline nanocomposite synthesized by inkjet printing and in flexible all-solid-state supercapacitor. , 2014, ACS applied materials & interfaces.

[44]  Yang Xu,et al.  Three-dimensional macro-structures of two-dimensional nanomaterials. , 2016, Chemical Society reviews.

[45]  M. Beidaghi,et al.  Micro‐Supercapacitors Based on Interdigital Electrodes of Reduced Graphene Oxide and Carbon Nanotube Composites with Ultrahigh Power Handling Performance , 2012 .

[46]  Yanlin Song,et al.  Flexible Circuits and Soft Actuators by Printing Assembly of Graphene. , 2016, ACS applied materials & interfaces.

[47]  Fang Qian,et al.  Supercapacitors Based on Three-Dimensional Hierarchical Graphene Aerogels with Periodic Macropores. , 2016, Nano letters.

[48]  J. Lewis,et al.  3D Printing of Interdigitated Li‐Ion Microbattery Architectures , 2013, Advanced materials.

[49]  Zheye Zhang,et al.  Advanced solid-state asymmetric supercapacitors based on 3D graphene/MnO2 and graphene/polypyrrole hybrid architectures , 2015 .

[50]  Klaus Müllen,et al.  Graphene-based in-plane micro-supercapacitors with high power and energy densities , 2013, Nature Communications.