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Title: On-chip and freestanding elastic carbon films for micro-supercapacitors

Abstract

Integration of electrochemical capacitors with silicon-based electronics is a major challenge, limiting energy storage on a chip. We describe a wafer-scale process for manufacturing strongly adhering carbide-derived carbon films and interdigitated micro-supercapacitors with embedded titanium carbide current collectors, fully compatible with current microfabrication and silicon-based device technology. Capacitance of those films reaches 410 farads per cubic centimeter/200 millifarads per square centimeter in aqueous electrolyte and 170 farads per cubic centimeter/85 millifarads per square centimeter in organic electrolyte. We also demonstrate preparation of self-supported, mechanically stable, micrometer-thick porous carbon films with a Young’s modulus of 14.5 gigapascals, with the possibility of further transfer onto flexible substrates. Lastly, these materials are interesting for applications in structural energy storage, tribology, and gas separation.

Authors:
 [1];  [2];  [3];  [1];  [1];  [1];  [4];  [5];  [1];  [1];  [3];  [6];  [1]
  1. Univ. Paul Sabatier-Toulouse III, Toulouse (France); Reseau sur le Stockage Electrochimique de l'Energie (France)
  2. Reseau sur le Stockage Electrochimique de l'Energie (France); Univ. Lille 1 Science et Technologies, Villeneuve d'Ascq cedex (France)
  3. Univ. Paul Sabatier (IPS)-CNRS, Univ. de Toulouse, Toulouse (France)
  4. Univ. Paul Sabatier (IPS)-CNRS, Univ. de Toulouse, Toulouse (France); Univ. de Toulouse, Toulouse Cedex (France)
  5. Reseau sur le Stockage Electrochimique de l'Energie (France); Univ. de Picardie Jules Verne, Amiens (France)
  6. Drexel Univ., Philadelphia, PA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1346630
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 351; Journal Issue: 6274; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Huang, Peihua, Lethien, C., Pinaud, S., Brousse, K., Laloo, R., Turq, V., Respaud, M., Demortiere, A., Daffos, B., Taberna, Pierre -Louis, Chaudret, B., Gogotsi, Yury G., and Simon, Patrice. On-chip and freestanding elastic carbon films for micro-supercapacitors. United States: N. p., 2016. Web. doi:10.1126/science.aad3345.
Huang, Peihua, Lethien, C., Pinaud, S., Brousse, K., Laloo, R., Turq, V., Respaud, M., Demortiere, A., Daffos, B., Taberna, Pierre -Louis, Chaudret, B., Gogotsi, Yury G., & Simon, Patrice. On-chip and freestanding elastic carbon films for micro-supercapacitors. United States. https://doi.org/10.1126/science.aad3345
Huang, Peihua, Lethien, C., Pinaud, S., Brousse, K., Laloo, R., Turq, V., Respaud, M., Demortiere, A., Daffos, B., Taberna, Pierre -Louis, Chaudret, B., Gogotsi, Yury G., and Simon, Patrice. Thu . "On-chip and freestanding elastic carbon films for micro-supercapacitors". United States. https://doi.org/10.1126/science.aad3345. https://www.osti.gov/servlets/purl/1346630.
@article{osti_1346630,
title = {On-chip and freestanding elastic carbon films for micro-supercapacitors},
author = {Huang, Peihua and Lethien, C. and Pinaud, S. and Brousse, K. and Laloo, R. and Turq, V. and Respaud, M. and Demortiere, A. and Daffos, B. and Taberna, Pierre -Louis and Chaudret, B. and Gogotsi, Yury G. and Simon, Patrice},
abstractNote = {Integration of electrochemical capacitors with silicon-based electronics is a major challenge, limiting energy storage on a chip. We describe a wafer-scale process for manufacturing strongly adhering carbide-derived carbon films and interdigitated micro-supercapacitors with embedded titanium carbide current collectors, fully compatible with current microfabrication and silicon-based device technology. Capacitance of those films reaches 410 farads per cubic centimeter/200 millifarads per square centimeter in aqueous electrolyte and 170 farads per cubic centimeter/85 millifarads per square centimeter in organic electrolyte. We also demonstrate preparation of self-supported, mechanically stable, micrometer-thick porous carbon films with a Young’s modulus of 14.5 gigapascals, with the possibility of further transfer onto flexible substrates. Lastly, these materials are interesting for applications in structural energy storage, tribology, and gas separation.},
doi = {10.1126/science.aad3345},
journal = {Science},
number = 6274,
volume = 351,
place = {United States},
year = {2016},
month = {2}
}

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The Road Towards Planar Microbatteries and Micro‐Supercapacitors: From 2D to 3D Device Geometries
journal, June 2019


Asymmetric Flexible MXene-Reduced Graphene Oxide Micro-Supercapacitor
journal, November 2017

  • Couly, Cedric; Alhabeb, Mohamed; Van Aken, Katherine L.
  • Advanced Electronic Materials, Vol. 4, Issue 1
  • DOI: 10.1002/aelm.201700339

Hollow TiN nanotrees derived from a surface-induced Kirkendall effect and their application in high-power supercapacitors
journal, January 2019

  • Wen, Wei; Yao, Jincheng; Tan, Hua
  • Journal of Materials Chemistry A, Vol. 7, Issue 37
  • DOI: 10.1039/c9ta07642e

Scalable Production of Graphene Inks via Wet‐Jet Milling Exfoliation for Screen‐Printed Micro‐Supercapacitors
journal, February 2019

  • Bellani, Sebastiano; Petroni, Elisa; Del Rio Castillo, Antonio Esau
  • Advanced Functional Materials, Vol. 29, Issue 14
  • DOI: 10.1002/adfm.201807659

Recent Progress in Micro‐Supercapacitor Design, Integration, and Functionalization
journal, December 2018


High Power In-Plane Micro-Supercapacitors Based on Mesoporous Polyaniline Patterned Graphene
journal, February 2017


Graphene-Based Planar Microsupercapacitors: Recent Advances and Future Challenges
journal, October 2018

  • Liang, Jiaxing; Mondal, Anjon Kumar; Wang, Da-Wei
  • Advanced Materials Technologies, Vol. 4, Issue 1
  • DOI: 10.1002/admt.201800200

NiMn 2 O 4 Nanosheet-Decorated Hierarchically Porous Polyaromatic Carbon Spheres for High-Performance Supercapacitors
journal, March 2017


Unconventional supercapacitors from nanocarbon-based electrode materials to device configurations
journal, January 2016

  • Liu, Lili; Niu, Zhiqiang; Chen, Jun
  • Chemical Society Reviews, Vol. 45, Issue 15
  • DOI: 10.1039/c6cs00041j

Ionogel-based sodium ion micro-batteries with a 3D Na-ion diffusion mechanism enable ultrahigh rate capability
journal, January 2020

  • Zheng, Shuanghao; Huang, Huijuan; Dong, Yanfeng
  • Energy & Environmental Science, Vol. 13, Issue 3
  • DOI: 10.1039/c9ee03219c

A true cable assembly with a carbon nanotube sheath and nickel wire core: a fully flexible electrode integrating energy storage and electrical conduction
journal, January 2018

  • Ye, Huating; Wang, Kai; Zhou, Juntao
  • Journal of Materials Chemistry A, Vol. 6, Issue 3
  • DOI: 10.1039/c7ta08758f

Conductive Metal–Organic Frameworks Selectively Grown on Laser‐Scribed Graphene for Electrochemical Microsupercapacitors
journal, April 2019

  • Wu, Hao; Zhang, Wenli; Kandambeth, Sharath
  • Advanced Energy Materials, Vol. 9, Issue 21
  • DOI: 10.1002/aenm.201900482

Nitrogen-rich hierarchical porous carbon materials with interconnected channels for high stability supercapacitors
journal, January 2019

  • Sun, Zhenjie; Wang, Wenjie; Zhang, Jiamin
  • New Journal of Chemistry, Vol. 43, Issue 4
  • DOI: 10.1039/c8nj05552a

Stimulus-Responsive Micro-Supercapacitors with Ultrahigh Energy Density and Reversible Electrochromic Window
journal, December 2016


Boosting the Energy Density of Carbon-Based Aqueous Supercapacitors by Optimizing the Surface Charge
journal, March 2017

  • Yu, Minghao; Lin, Dun; Feng, Haobin
  • Angewandte Chemie International Edition, Vol. 56, Issue 20
  • DOI: 10.1002/anie.201701737

Designed formation of hollow particle-based nitrogen-doped carbon nanofibers for high-performance supercapacitors
journal, January 2017

  • Chen, Li-Feng; Lu, Yan; Yu, Le
  • Energy & Environmental Science, Vol. 10, Issue 8
  • DOI: 10.1039/c7ee00488e

3D-Printed, Superelastic Polypyrrole-Graphene Electrodes with Ultrahigh Areal Capacitance for Electrochemical Energy Storage
journal, June 2018

  • Qi, Zhen; Ye, Jianchao; Chen, Wen
  • Advanced Materials Technologies, Vol. 3, Issue 7
  • DOI: 10.1002/admt.201800053

Flexible Fiber and Fabric Batteries
journal, February 2018

  • Zhang, Chenjun; Zhu, Jixin; Lin, Huijuan
  • Advanced Materials Technologies, Vol. 3, Issue 10
  • DOI: 10.1002/admt.201700302

Oxygen-Deficient Bismuth Oxide/Graphene of Ultrahigh Capacitance as Advanced Flexible Anode for Asymmetric Supercapacitors
journal, May 2017

  • Liu, Rong; Ma, Lina; Niu, Gudan
  • Advanced Functional Materials, Vol. 27, Issue 29
  • DOI: 10.1002/adfm.201701635

Microsupercapacitors as miniaturized energy-storage components for on-chip electronics
journal, November 2016

  • Kyeremateng, Nana Amponsah; Brousse, Thierry; Pech, David
  • Nature Nanotechnology, Vol. 12, Issue 1
  • DOI: 10.1038/nnano.2016.196

On‐Chip MXene Microsupercapacitors for AC‐Line Filtering Applications
journal, May 2019


3D printed graphene/nickel electrodes for high areal capacitance electrochemical storage
journal, January 2019

  • Li, Guijun; Mo, Xiaoyong; Law, Wing-Cheung
  • Journal of Materials Chemistry A, Vol. 7, Issue 8
  • DOI: 10.1039/c8ta11121a

Multidimensional materials and device architectures for future hybrid energy storage
journal, September 2016

  • Lukatskaya, Maria R.; Dunn, Bruce; Gogotsi, Yury
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12647

Dual-phase nanostructuring of layered metal oxides for high-performance aqueous rechargeable potassium ion microbatteries
journal, September 2019


Layered coating of ultraflexible graphene-based electrodes for high-performance in-plane quasi-solid-state micro-supercapacitors
journal, January 2019

  • Du, Jingwei; Mu, Xuemei; Zhao, Yirong
  • Nanoscale, Vol. 11, Issue 30
  • DOI: 10.1039/c9nr03917a

Energy storage on demand: ultra-high-rate and high-energy-density inkjet-printed NiO micro-supercapacitors
journal, January 2019

  • Giannakou, Pavlos; Masteghin, Mateus G.; Slade, Robert C. T.
  • Journal of Materials Chemistry A, Vol. 7, Issue 37
  • DOI: 10.1039/c9ta07878a

Direct Laser Etching Free‐Standing MXene‐MoS 2 Film for Highly Flexible Micro‐Supercapacitor
journal, September 2019

  • Chen, Xing; Wang, Siliang; Shi, Junjie
  • Advanced Materials Interfaces, Vol. 6, Issue 22
  • DOI: 10.1002/admi.201901160

Electropolymerization and energy storage of poly[Ni(salphen)]/MWCNT composite materials for supercapacitors
journal, October 2016

  • Chen, Cheng; Zhu, Zhixun; Li, Xinping
  • Journal of Applied Polymer Science, Vol. 134, Issue 7
  • DOI: 10.1002/app.44464

2D Ultrathin MXene-Based Drug-Delivery Nanoplatform for Synergistic Photothermal Ablation and Chemotherapy of Cancer
journal, February 2018

  • Han, Xiaoxia; Huang, Ju; Lin, Han
  • Advanced Healthcare Materials, Vol. 7, Issue 9
  • DOI: 10.1002/adhm.201701394

Challenges and opportunities for supercapacitors
journal, October 2019

  • Huang, Shifei; Zhu, Xianglin; Sarkar, Samrat
  • APL Materials, Vol. 7, Issue 10
  • DOI: 10.1063/1.5116146

Charge storage mechanisms of electrospun Mn 3 O 4 nanofibres for high-performance supercapacitors
journal, January 2017

  • Suktha, Phansiri; Phattharasupakun, Nutthaphon; Dittanet, Peerapan
  • RSC Advances, Vol. 7, Issue 16
  • DOI: 10.1039/c6ra28499j

Multifunctional Energy Storage and Conversion Devices
journal, July 2016


Planar integration of flexible micro-supercapacitors with ultrafast charge and discharge based on interdigital nanoporous gold electrodes on a chip
journal, January 2016

  • Zhang, Chao; Xiao, Jian; Qian, Lihua
  • Journal of Materials Chemistry A, Vol. 4, Issue 24
  • DOI: 10.1039/c6ta02219g

Ultrafast All-Solid-State Coaxial Asymmetric Fiber Supercapacitors with a High Volumetric Energy Density
journal, January 2018

  • Pan, Zhenghui; Zhong, Jun; Zhang, Qichong
  • Advanced Energy Materials, Vol. 8, Issue 14
  • DOI: 10.1002/aenm.201702946

Copper Hydroxide Porous Nanotube Arrays Grown on Copper Foils as High-Performance Integrated Electrodes for Supercapacitors
journal, October 2017


A Nonaqueous Na‐Ion Hybrid Micro‐Supercapacitor with Wide Potential Window and Ultrahigh Areal Energy Density
journal, August 2019

  • Zhang, Panpan; Wang, Lanlan; Wang, Faxing
  • Batteries & Supercaps, Vol. 2, Issue 11
  • DOI: 10.1002/batt.201900079

MXene-on-Paper Coplanar Microsupercapacitors
journal, September 2016

  • Kurra, Narendra; Ahmed, Bilal; Gogotsi, Yury
  • Advanced Energy Materials, Vol. 6, Issue 24
  • DOI: 10.1002/aenm.201601372

Unique MOF-derived hierarchical MnO 2 nanotubes@NiCo-LDH/CoS 2 nanocage materials as high performance supercapacitors
journal, January 2019

  • Wang, Xiuhua; Huang, Feifei; Rong, Fang
  • Journal of Materials Chemistry A, Vol. 7, Issue 19
  • DOI: 10.1039/c9ta01951k

Challenges and prospects of 3D micro-supercapacitors for powering the internet of things
journal, January 2019

  • Lethien, Christophe; Le Bideau, Jean; Brousse, Thierry
  • Energy & Environmental Science, Vol. 12, Issue 1
  • DOI: 10.1039/c8ee02029a

Graphene-Based Planar On-Chip Micro-Supercapacitors with Whole Series/Parallel Configuration for Integration
journal, June 2019


Hybrid Microsupercapacitors with Vertically Scaled 3D Current Collectors Fabricated using a Simple Cut-and-Transfer Strategy
journal, September 2016

  • Jiang, Qiu; Kurra, Narendra; Xia, Chuan
  • Advanced Energy Materials, Vol. 7, Issue 1
  • DOI: 10.1002/aenm.201601257

NiO/Ni x Co 3−x O 4 porous ultrathin nanosheet/nanowire composite structures as high-performance supercapacitor electrodes
journal, January 2018

  • Jiang, Dongkai; Zheng, Maojun; You, Yuxiu
  • RSC Advances, Vol. 8, Issue 56
  • DOI: 10.1039/c8ra04827d

Flexible quasi-solid-state planar micro-supercapacitor based on cellular graphene films
journal, January 2017

  • Shao, Yuanlong; Li, Jianmin; Li, Yaogang
  • Mater. Horiz., Vol. 4, Issue 6
  • DOI: 10.1039/c7mh00441a

Scalable 2D Hierarchical Porous Carbon Nanosheets for Flexible Supercapacitors with Ultrahigh Energy Density
journal, January 2018


Metal–organic framework derived hollow materials for electrochemical energy storage
journal, January 2018

  • Xie, Xing-Chen; Huang, Ke-Jing; Wu, Xu
  • Journal of Materials Chemistry A, Vol. 6, Issue 16
  • DOI: 10.1039/c8ta00612a

All‐Solid‐State Planar Sodium‐Ion Microcapacitors with Multidirectional Fast Ion Diffusion Pathways
journal, September 2019


Sticky-note supercapacitors
journal, January 2018

  • Cao, Jingyu; Zhao, Yang; Xu, Yifan
  • Journal of Materials Chemistry A, Vol. 6, Issue 8
  • DOI: 10.1039/c7ta10756k

Rich-Mixed-Valence Ni x Co 3−x P y Porous Nanowires Interwelded Junction-Free 3D Network Architectures for Ultrahigh Areal Energy Density Supercapacitors
journal, September 2018

  • Song, Weijie; Wu, Juan; Wang, Gengjie
  • Advanced Functional Materials, Vol. 28, Issue 46
  • DOI: 10.1002/adfm.201804620

Coordination Polymer Framework Based On-Chip Micro-Supercapacitors with AC Line-Filtering Performance
journal, March 2017

  • Yang, Chongqing; Schellhammer, Karl Sebastian; Ortmann, Frank
  • Angewandte Chemie International Edition, Vol. 56, Issue 14
  • DOI: 10.1002/anie.201700679

Flexible Ti 3 C 2 T x @Al electrodes with Ultrahigh Areal Capacitance: In Situ Regulation of Interlayer Conductivity and Spacing
journal, July 2018

  • Guo, Miao; Liu, Chengbin; Zhang, Zezhong
  • Advanced Functional Materials, Vol. 28, Issue 37
  • DOI: 10.1002/adfm.201803196

Microfluidic‐Architected Nanoarrays/Porous Core–Shell Fibers toward Robust Micro‐Energy‐Storage
journal, November 2019


Nanoelectrode design from microminiaturized honeycomb monolith with ultrathin and stiff nanoscaffold for high-energy micro-supercapacitors
journal, January 2020


3D porous binary-heteroatom doped carbon nanosheet/electrochemically exfoliated graphene hybrids for high performance flexible solid-state supercapacitors
journal, January 2018

  • Liu, Yuxi; Qiu, Xiaoming; Liu, Xiaobin
  • Journal of Materials Chemistry A, Vol. 6, Issue 18
  • DOI: 10.1039/c8ta01148f

Gated ion transport through layered graphene oxide membranes
journal, January 2019

  • Yang, Jinlei; Zhu, Weiwei; Zhang, Xiaopeng
  • New Journal of Chemistry, Vol. 43, Issue 19
  • DOI: 10.1039/c9nj00460b

High performance microsupercapacitors based on a nano-micro hierarchical carbon electrode by direct laser writing
journal, December 2018

  • Kwon, Soongeun; Kim, Geehong; Lim, Hyungjun
  • Applied Physics Letters, Vol. 113, Issue 24
  • DOI: 10.1063/1.5066017

A High-Performance Sodium-Ion Hybrid Capacitor Constructed by Metal-Organic Framework-Derived Anode and Cathode Materials
journal, May 2018

  • Li, Hongxia; Lang, Junwei; Lei, Shulai
  • Advanced Functional Materials, Vol. 28, Issue 30
  • DOI: 10.1002/adfm.201800757

A Flexible Quasi‐Solid‐State Bifunctional Device with Zinc‐Ion Microbattery and Photodetector
journal, May 2019


Two-dimensional materials for miniaturized energy storage devices: from individual devices to smart integrated systems
journal, January 2018

  • Zhang, Panpan; Wang, Faxing; Yu, Minghao
  • Chemical Society Reviews, Vol. 47, Issue 19
  • DOI: 10.1039/c8cs00561c

Fully inkjet printed ultrathin microsupercapacitors based on graphene electrodes and a nano-graphene oxide electrolyte
journal, January 2019

  • Sollami Delekta, Szymon; Adolfsson, Karin H.; Benyahia Erdal, Nejla
  • Nanoscale, Vol. 11, Issue 21
  • DOI: 10.1039/c9nr01427f

Energy storage: The future enabled by nanomaterials
journal, November 2019

  • Pomerantseva, Ekaterina; Bonaccorso, Francesco; Feng, Xinliang
  • Science, Vol. 366, Issue 6468
  • DOI: 10.1126/science.aan8285

All‐Solid‐State On‐Chip Supercapacitors Based on Free‐Standing 4 H ‐SiC Nanowire Arrays
journal, March 2019


Coordination Polymer Framework Based On-Chip Micro-Supercapacitors with AC Line-Filtering Performance
journal, March 2017

  • Yang, Chongqing; Schellhammer, Karl Sebastian; Ortmann, Frank
  • Angewandte Chemie, Vol. 129, Issue 14
  • DOI: 10.1002/ange.201700679

Micro-supercapacitors based on oriented coordination polymer thin films for AC line-filtering
journal, January 2018

  • Hua, Weiwei; Xiu, Jingwei; Xiu, Fei
  • RSC Advances, Vol. 8, Issue 53
  • DOI: 10.1039/c8ra06474a

3D printing-based cellular microelectrodes for high-performance asymmetric quasi-solid-state micro-pseudocapacitors
journal, January 2020

  • Wang, Teng; Tian, Xiaocong; Li, Liang
  • Journal of Materials Chemistry A, Vol. 8, Issue 4
  • DOI: 10.1039/c9ta11386j

Study of fractal electrode designs for buckypaper-based micro-supercapacitors
journal, January 2019

  • Huang, Kuan-Hua; Lin, Cheng-Te; Chen, Yun-Ting
  • Journal of Applied Physics, Vol. 125, Issue 1
  • DOI: 10.1063/1.5051702