An Approach To Fabricate PDMS Encapsulated All-Solid-State Advanced Asymmetric Supercapacitor Device with Vertically Aligned Hierarchical Zn-Fe-Co Ternary Oxide Nanowire and Nitrogen Doped Graphene Nanosheet for High Power Device Applications.

We highlight the design and fabrication of a polydimethylsiloxane (PDMS) encapsulated advanced all-solid-state asymmetric supercapacitor (ASC) device consisting of hierarchical mesoporous zinc-iron-cobalt ternary oxide (ZICO) nanowire coated nickel (Ni) foam (ZICO@Ni foam) as a promising positive electrode and nitrogen doped graphene coated Ni foam (N-G@Ni foam) as negative electrode in the presence of PVA-KOH gel electrolyte. Owing to outstanding electrochemical behavior and ultrahigh specific capacitance of ZICO (≈ 2587.4 F/g at 1 A/g) and N-G (550 F/g at 1 A/g) along with their mutual synergistic outputs, the assembled all-solid-state ASC device exhibits an outstanding energy density of ≈40.5 Wh/kg accompanied by a remarkable long-term cycle stability with ≈95% specific capacitance retention even after 5000 charge-discharge cycles. The exclusive hierarchical ZICO nanowires were synthesized by a facile two-step process comprising of a hydrothermal protocol followed by an annealing treatment on a quartz substrate. While Zn2+ gives the stability of the oxide system, Fe and Co ions provide better electronic conductivity and capacitive response under vigorous cyclic condition. The extraordinary performance of as-fabricated ASC device resembles its suitability for the construction of advanced energy storage devices in modern electronic industries.

[1]  C. Das,et al.  α MnMoO₄/graphene hybrid composite: high energy density supercapacitor electrode material. , 2014, Dalton transactions.

[2]  Yogendra Kumar Mishra,et al.  Performance of High Energy Density Symmetric Supercapacitor Based on Sputtered MnO2 Nanorods , 2016 .

[3]  Q. Li,et al.  Hierarchical mushroom-like CoNi2S4 arrays as a novel electrode material for supercapacitors , 2014 .

[4]  S. Kim,et al.  Chemically modified graphene based supercapacitors for flexible and miniature devices , 2015, Electronic Materials Letters.

[5]  Yi Shi,et al.  Preparation and characterization of flexible asymmetric supercapacitors based on transition-metal-oxide nanowire/single-walled carbon nanotube hybrid thin-film electrodes. , 2010, ACS nano.

[6]  Sebastian Wille,et al.  Fabrication of Macroscopically Flexible and Highly Porous 3D Semiconductor Networks from Interpenetrating Nanostructures by a Simple Flame Transport Approach , 2013 .

[7]  A. Burke.  Ultracapacitors: why, how, and where is the technology , 2000 .

[8]  Lei Zhang,et al.  A review of electrode materials for electrochemical supercapacitors. , 2012, Chemical Society reviews.

[9]  H. Alshareef,et al.  Substrate dependent self-organization of mesoporous cobalt oxide nanowires with remarkable pseudocapacitance. , 2012, Nano letters.

[10]  Boyang Liu,et al.  New energy storage option: toward ZnCo2O4 nanorods/nickel foam architectures for high-performance supercapacitors. , 2013, ACS applied materials & interfaces.

[11]  Feng Li,et al.  High-energy MnO2 nanowire/graphene and graphene asymmetric electrochemical capacitors. , 2010, ACS nano.

[12]  Yongyao Xia,et al.  A new concept hybrid electrochemical surpercapacitor: Carbon/LiMn2O4 aqueous system , 2005 .

[13]  H. Martínez,et al.  High‐Performing Monometallic Cobalt Layered Double Hydroxide Supercapacitor with Defined Local Structure , 2014 .

[14]  Qiaobao Zhang,et al.  Three-dimensional hierarchical Co3O4/CuO nanowire heterostructure arrays on nickel foam for high-performance lithium ion batteries , 2014 .

[15]  François Béguin,et al.  A High‐Performance Carbon for Supercapacitors Obtained by Carbonization of a Seaweed Biopolymer , 2006 .

[16]  Sandip Maiti,et al.  An Approach to Design Highly Durable Piezoelectric Nanogenerator Based on Self‐Poled PVDF/AlO‐rGO Flexible Nanocomposite with High Power Density and Energy Conversion Efficiency , 2016 .

[17]  Q. Li,et al.  Facile synthesis of ZnCo2O4 nanowire cluster arrays on Ni foam for high-performance asymmetric supercapacitors , 2014 .

[18]  Yunlong Zhao,et al.  Hierarchical MnMoO(4)/CoMoO(4) heterostructured nanowires with enhanced supercapacitor performance. , 2011, Nature communications.

[19]  C. F. Ng,et al.  Synthesis of free-standing metal sulfide nanoarrays via anion exchange reaction and their electrochemical energy storage application. , 2014, Small.

[20]  Qiang Zhang,et al.  Advanced Asymmetric Supercapacitors Based on Ni(OH)2/Graphene and Porous Graphene Electrodes with High Energy Density , 2012 .

[21]  F. Wei,et al.  Asymmetric Supercapacitors Based on Graphene/MnO2 and Activated Carbon Nanofiber Electrodes with High Power and Energy Density , 2011 .

[22]  Wei-bin Zhang,et al.  Nickel vanadate and nickel oxide nanohybrid on nickel foam as pseudocapacitive electrodes for electrochemical capacitors , 2014 .

[23]  L. Ricardez‐Sandoval,et al.  Pyrrolic-structure enriched nitrogen doped graphene for highly efficient next generation supercapacitors , 2013 .

[24]  Hongcai Gao,et al.  High-performance asymmetric supercapacitor based on graphene hydrogel and nanostructured MnO2. , 2012, ACS applied materials & interfaces.

[25]  Jong-Huy Kim,et al.  Polypyrrole/carbon composite electrode for high-power electrochemical capacitors , 2006 .

[26]  H. Alshareef,et al.  One-step electrodeposited nickel cobalt sulfide nanosheet arrays for high-performance asymmetric supercapacitors. , 2014, ACS nano.

[27]  Jiaoyang Li,et al.  Ultrathin Mesoporous NiCo2O4 Nanosheets Supported on Ni Foam as Advanced Electrodes for Supercapacitors , 2012 .

[28]  R. Chandra,et al.  Silicon Carbide Nanocauliflowers for Symmetric Supercapacitor Devices , 2016 .

[29]  S. Xie,et al.  Asymmetric Supercapacitors Based on Graphene/MnO2 Nanospheres and Graphene/MoO3 Nanosheets with High Energy Density , 2013 .

[30]  Joonwon Lim,et al.  Nitrogen-doped carbon nanotubes and graphene composite structures for energy and catalytic applications. , 2014, Chemical communications.

[31]  Meenakshi Sharma,et al.  Heavily nitrogen doped, graphene supercapacitor from silk cocoon , 2015 .

[32]  Y. Sung,et al.  Controlled growth of high-quality TiO2 nanowires on sapphire and silica , 2006 .

[33]  C. Das,et al.  Solid State Flexible Asymmetric Supercapacitor Based on Carbon Fiber Supported Hierarchical Co(OH)xCO3 and Ni(OH)2. , 2015, Langmuir : the ACS journal of surfaces and colloids.

[34]  H.Q. Li,et al.  Ordered Whiskerlike Polyaniline Grown on the Surface of Mesoporous Carbon and Its Electrochemical Capacitance Performance , 2006 .

[35]  François Béguin,et al.  Optimisation of an asymmetric manganese oxide/activated carbon capacitor working at 2 V in aqueous medium , 2006 .

[36]  Jia-Yaw Chang,et al.  Comparative Study of Individual and Mixed Aqueous Electrolytes with ZnFe2O4 Nano–flakes Thin Film as an Electrode for Supercapacitor Application , 2016 .

[37]  Yuping Wu,et al.  Polypyrrole-coated α-MoO3 nanobelts with good electrochemical performance as anode materials for aqueous supercapacitors , 2013 .

[38]  Rujia Zou,et al.  Electrochemical Energy Storage Application and Degradation Analysis of Carbon-Coated Hierarchical NiCo2S4 Core-Shell Nanowire Arrays Grown Directly on Graphene/Nickel Foam , 2016, Scientific Reports.

[39]  Lili Zhang,et al.  Carbon-based materials as supercapacitor electrodes. , 2009, Chemical Society reviews.

[40]  Mathieu Toupin,et al.  Charge Storage Mechanism of MnO2 Electrode Used in Aqueous Electrochemical Capacitor , 2004 .

[41]  J. Tu,et al.  Spinel manganese-nickel-cobalt ternary oxide nanowire array for high-performance electrochemical capacitor applications. , 2014, ACS applied materials & interfaces.

[42]  Deyang Qu,et al.  Studies of the activated carbons used in double-layer supercapacitors , 2002 .

[43]  Joonwon Lim,et al.  Dopant-specific unzipping of carbon nanotubes for intact crystalline graphene nanostructures , 2016, Nature Communications.

[44]  Srinivasan Sampath,et al.  Hydrogel-polymer electrolytes for electrochemical capacitors: an overview , 2009 .

[45]  Meilin Liu,et al.  Nickel-cobalt hydroxide nanosheets coated on NiCo2O4 nanowires grown on carbon fiber paper for high-performance pseudocapacitors. , 2013, Nano letters.

[46]  T. Maiyalagan,et al.  Review on Recent Progress in Nitrogen-Doped Graphene: Synthesis, Characterization, and Its Potential Applications , 2012 .

[47]  Yongchang Liu,et al.  Facile synthesis of hierarchical porous ZnCo2O4 microspheres for high-performance supercapacitors , 2015 .

[48]  Qiaobao Zhang,et al.  Hierarchical Mesoporous Zinc-Nickel-Cobalt Ternary Oxide Nanowire Arrays on Nickel Foam as High-Performance Electrodes for Supercapacitors. , 2015, ACS applied materials & interfaces.

[49]  John R. Miller,et al.  Electrochemical Capacitors for Energy Management , 2008, Science.

[50]  Tiezhu Zhang,et al.  Nitrogen-doped graphene for supercapacitor with long-term electrochemical stability , 2014 .

[51]  J. Xu,et al.  Flexible asymmetric supercapacitors based upon Co9S8 nanorod//Co3O4@RuO2 nanosheet arrays on carbon cloth. , 2013, ACS nano.

[52]  Y. Tong,et al.  Co3O4/Ni(OH)2 composite mesoporous nanosheet networks as a promising electrode for supercapacitor applications , 2012 .

[53]  C. Das,et al.  Reduced Graphene Oxide/Manganese Carbonate Hybrid Composite: High Performance Supercapacitor Electrode Material , 2014 .

[54]  Joonwon Lim,et al.  High Energy Density All Solid State Asymmetric Pseudocapacitors Based on Free Standing Reduced Graphene Oxide-Co3O4 Composite Aerogel Electrodes. , 2016, ACS applied materials & interfaces.

[55]  B. Chowdari,et al.  Nanophase ZnCo2O4 as a High Performance Anode Material for Li‐Ion Batteries , 2007 .

[56]  Bo‐wei Ju,et al.  Supercapacitive behaviors of activated mesocarbon microbeads coated with polyaniline , 2012 .

[57]  Chongwu Zhou,et al.  Hierarchical three-dimensional ZnCo₂O₄ nanowire arrays/carbon cloth anodes for a novel class of high-performance flexible lithium-ion batteries. , 2012, Nano letters.

[58]  M. Dargusch,et al.  Green Synthesis of Porous Three-Dimensional Nitrogen-Doped Graphene Foam for Electrochemical Applications. , 2016, ACS applied materials & interfaces.

[59]  Huanlei Wang,et al.  Asymmetric capacitor based on superior porous Ni–Zn–Co oxide/hydroxide and carbon electrodes , 2010 .