Engineering Carbon Nanostructures and Architectures for High Performance and Multifunctional Electrodes

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1 Engineering Carbon Nanostructures and Architectures for High Performance and Multifunctional Electrodes Yung Joon Jung Department of Mechanical & Industrial Engineering Northeastern University, Boston, MA 02115

2 High Performance and Multifunctional Electrodes Multifunctional Electronics Flexible and transparent smart phone, flexible computer, Flexible electronic newspaper (Wearable Electronics) Devices require mechanically flexible, functional, and high performance energy storage systems Electrode Materials 3D Nanostructures Electro-Mechanical Stability Optical Transparency etc.

SP 2 Carbon Nanostructured Materials Mechanical

bonding High elastic modulus (1 TPa) and High

Mobility Highly conductive w/wo mechanical

Optically Transparent In-plane Properties of

3 SP 2 Carbon Nanostructured Materials Mechanical Properties Strong sp2 Carbon-Carbon covalent bonding High elastic modulus (1 TPa) and High strength Electrical and Optical Properties High Mobility Highly conductive w/wo mechanical deformation High current density (10 9 A/cm 2 ) Optically Transparent In-plane Properties of Graphitic Carbon Good thermal conductivity (<3000W/mK) Good chemical stability

lower pulling resistance, electron and phonon scatterings at these unconnected junctions Transforming physical

4 Engineering SP2 Nanostructure Limitation of current CNT/graphene based networks Built on weak van der Waals interactions between CNTs, CNTs-Graphene Lower mechanical strength, electrical and thermal conductivities due to a lower pulling resistance, electron and phonon scatterings at these unconnected junctions Transforming physical Junctions into covalently bonded sp 2 Chemical Junctions Terrones, Ajayan et al., PRL, 2002 J. Tour et al., Nature Communications, 2012

Jung et al, Nature Communications, 2014 1) Initial I-V characterization is performed to

5 Engineering SP2 Nanostructure Restructuring sp 2 Lattice and Network Structure A voltage-induced electrical fusion of SWCNTs H. Jung et al, Nature Communications, ) Initial I-V characterization is performed to find the maximum current density and breakdown voltage (V b ) 2) The electrical polarity is then switched periodically in the range of V b.

6 Engineering SP2 Nanostructure Restructuring sp 2 Lattice Structure H. Jung et al, Nature Communications 2014

7 Engineering SP2 Nanostructure

8 Engineering Nanostructure and Morphology Pristine CNT fiber Thermal Conductivity 15W/mK 100μm 100nm Supported by NSF-DMREF Program (Materials Genome Initiative) Fused CNT fiber Thermal Conductivity W/mK 100µm 100 nm J. Hao et al, Unpublished

9 Engineering Nanostructure and Morphology Before Fusion After Fusion

I D /I G ratio I D /I G ratio I D /I G ratio Intensity Engineering Nanostructure and Morphology

50 60 70 2 (degree) 0.30 0.25 0.27 Original fiber 9V_2.5Hz_200s@20 C 9V_2.5Hz_400s@20 C 9V_2.

5Hz_800s@300 C 0.30 0.25 0.27 Original fiber 3V_2.5Hz_800s@20 C 6V_2.5Hz_800s@20 C 9V_2.

10 I D /I G ratio I D /I G ratio I D /I G ratio Intensity Engineering Nanostructure and Morphology Fused fiber (002) Original fiber Fused fiber Outer area Inner area (100) 10 nm 10 nm (degree) Original fiber 9V_2.5Hz_200s@20 C 9V_2.5Hz_400s@20 C 9V_2.5Hz_800s@20 C Original fiber 9V_2.5Hz_800s@20 C 9V_2.5Hz_800s@200 C 9V_2.5Hz_800s@300 C Original fiber 3V_2.5Hz_800s@20 C 6V_2.5Hz_800s@20 C 9V_2.5Hz_800s@20 C

Engineering 3D Nanoscale Architecture Carbon Nanocups Graphitic nanostructures having smaller length/diameter (L/D) aspect ratio, nanoscale cup morphology, can effectively

11 Engineering 3D Nanoscale Architecture Carbon Nanocups Graphitic nanostructures having smaller length/diameter (L/D) aspect ratio, nanoscale cup morphology, can effectively contain other nanomaterials and polymers, leading to multi-component hybrid nanostructures. Multifunctional Nanosystems Energy Storage Nanogram Quantity Container Multifunctional Sensors

12 Engineering 3D Nanoscale Architecture Fabrication Process The length of nanochannels are controlled by second anodizing time. Thermal CVD of Carbon 80 nm 50 nm H. Chun, et. al., ACS Nano (2009) H. Jung et al. Scientific Reports (2011) 50 nm 50 nm 100 nm

Engineering 3D Nanoscale Architecture TOP view BOTTOM view 400 nm 100 nm 400 nm 100 nm 3D Carbon

S/m High surface area and highly disordered graphitic layers provides the effective permeation of

Unique nanoscale cup feature enables the easy access and faster transport of ions at the

High current carrying capability, substantial mechanical strength, and small effective electrode

13 Engineering 3D Nanoscale Architecture TOP view BOTTOM view 400 nm 100 nm 400 nm 100 nm 3D Carbon Nanostructured Film for Supercapacitor Electrodes Electrically Conductive: Surface Conductivity: 117 S/m High surface area and highly disordered graphitic layers provides the effective permeation of the polymer electrolyte and their conformal packaging with electrodes. Unique nanoscale cup feature enables the easy access and faster transport of ions at the electrode/electrolyte interface resulting in higher power capability. High current carrying capability, substantial mechanical strength, and small effective electrode thickness (5-10 nm: 80-85% Transmittance at 550nm wavelength) allow us to build optically transparent and mechanically flexible reliable thin-film (solid state) energy storage devices.

Scientific Reports 2012) CNC films: Outer graphene layers are acting as current

14 Flexible and Transparent Supercapacitors (a) concave and (b, c) convex and (d-f) branched nanocup films (H. Jung et al. Scientific Reports 2012) CNC films: Outer graphene layers are acting as current collectors and the Innermost layer exposed electrolyte is acting an electrode. Polymer electrolyte (PVA-H 3 PO 4 ) is acting as both electrolyte and separator.

15 Flexible and Transparent Supercapacitors (a) Cyclic voltammetry (CV) measured with mvs -1 scan rates. (b) Galvanostatic charge/discharge (CD) results measured at a constant current density of 5 µacm -2. The capacitances by the geometrical area calculated from CD curves are 409 µf cm -2. (c) The capacitance change as a function of temperature

16 Flexible and Transparent Supercapacitors Normalized capacitance as a function of cycle-number (10,000) and w/wo the mechanical deformation (45 bending). (SG: single layer graphene, RMGO: reduced multilayer graphene oxide, HGO: hydrated graphitic oxide, LSG-EC: laser-scribed graphene electrochemical capacitor) Jung, Ajayan et al. Scientific Reports 2012

Acknowledgement NSF-Designing Materials to

1434824-Materials Genome Initiative) NSF ECCS-1202376

Army under grant W911NF-10-2-0098, subaward

17 Acknowledgement NSF-Designing Materials to Revolutionize and Engineer our Future (DMREF Materials Genome Initiative) NSF ECCS NSF CHN-Center for Highrate Nanomanufacturing, NEU US Army under grant W911NF , subaward Ministry of Energy, Industry, and Trade (MOEIT) Republic of Korea

Acknowledgement Contributions from Our Group Members Prof. Hyunyoung Jung (KNUST, Korea) Prof. MyungGwan Hahm (Inha University, Korea) Dr. Younglae Kim (Intel, Portland) Prof. Bo Li (Villanova Univ.

18 Acknowledgement Contributions from Our Group Members Prof. Hyunyoung Jung (KNUST, Korea) Prof. MyungGwan Hahm (Inha University, Korea) Dr. Younglae Kim (Intel, Portland) Prof. Bo Li (Villanova Univ. PA.) Prof. Rodrigo Lavall (Federal Univ. of Minas Gerais, Brazil) Sanghyun Hong (PhD), Ji Hao (PhD), Heyhee Kim (PhD), Sen Gao (PhD), Jeonghoon Nam (PhD) Zane Gavin (UG), Alexander Keklak (UG) Collaborators Prof. S. Kar (NEU), Prof. P. Ajayan (Rice Univ.), Prof. A. Busnaina (NEU), Prof. Y. Homma (Tokyo Univ. Science) Dr. C. Ahn (KAIST-NanoFab), Dr. Ann Chiramonti (NIST), Prof. G.H. Gilmer (CSM) Prof. Dongsik Kim (POSTECH), Prof. M. Upmanyu (NEU), Prof. C. Livermore (NEU) Prof. Jonghwan Suhr (SKKU), Dr. Sung Lee (KRICT), Prof. Y. Kwon (KyungHee Univ.), Dr. Jeremy Robinson (Naval Research Lab.) Prof. David Luzzi (NEU)

R ecently there has been significant interest in using carbon based nanomaterials as supercapacitor electrodes

R ecently there has been significant interest in using carbon based nanomaterials as supercapacitor electrodes SUBJECT AREAS: MATERIALS SCIENCE PHYSICS APPLIED PHYSICS ELECTROCHEMISTRY Transparent, flexible supercapacitors from nano-engineered carbon films Hyun Young Jung 1, Majid B. Karimi 1, Myung Gwan Hahm 2,3,