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Title: Flexible MXene/Graphene Films for Ultrafast Supercapacitors with Outstanding Volumetric Capacitance

Abstract

A strategy to prepare flexible and conductive MXene/graphene (reduced graphene oxide, rGO) supercapacitor electrodes by using electrostatic self‐assembly between positively charged rGO modified with poly(diallyldimethylammonium chloride) and negatively charged titanium carbide MXene nanosheets is presented. After electrostatic assembly, rGO nanosheets are inserted in‐between MXene layers. As a result, the self‐restacking of MXene nanosheets is effectively prevented, leading to a considerably increased interlayer spacing. Accelerated diffusion of electrolyte ions enables more electroactive sites to become accessible. The freestanding MXene/rGO‐5 wt% electrode displays a volumetric capacitance of 1040 F cm −3 at a scan rate of 2 mV s −1 , an impressive rate capability with 61% capacitance retention at 1 V s −1 and long cycle life. Moreover, the fabricated binder‐free symmetric supercapacitor shows an ultrahigh volumetric energy density of 32.6 Wh L −1 , which is among the highest values reported for carbon and MXene based materials in aqueous electrolytes. This work provides fundamental insight into the effect of interlayer spacing on the electrochemical performance of 2D hybrid materials and sheds light on the design of next‐generation flexible, portable and highly integrated supercapacitors with high volumetric and rate performances.

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2];  [2];  [2]; ORCiD logo [2]
  1. Drexel Univ., Philadelphia, PA (United States); Harbin Engineering Univ., Harbin (China)
  2. Drexel Univ., Philadelphia, PA (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1399231
Alternate Identifier(s):
OSTI ID: 1401090
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 27; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; energy density; graphene; MXene; supercapacitors; volumetric performance

Citation Formats

Yan, Jun, Ren, Chang E., Maleski, Kathleen, Hatter, Christine B., Anasori, Babak, Urbankowski, Patrick, Sarycheva, Asya, and Gogotsi, Yury G. Flexible MXene/Graphene Films for Ultrafast Supercapacitors with Outstanding Volumetric Capacitance. United States: N. p., 2017. Web. doi:10.1002/adfm.201701264.
Yan, Jun, Ren, Chang E., Maleski, Kathleen, Hatter, Christine B., Anasori, Babak, Urbankowski, Patrick, Sarycheva, Asya, & Gogotsi, Yury G. Flexible MXene/Graphene Films for Ultrafast Supercapacitors with Outstanding Volumetric Capacitance. United States. https://doi.org/10.1002/adfm.201701264
Yan, Jun, Ren, Chang E., Maleski, Kathleen, Hatter, Christine B., Anasori, Babak, Urbankowski, Patrick, Sarycheva, Asya, and Gogotsi, Yury G. Fri . "Flexible MXene/Graphene Films for Ultrafast Supercapacitors with Outstanding Volumetric Capacitance". United States. https://doi.org/10.1002/adfm.201701264. https://www.osti.gov/servlets/purl/1399231.
@article{osti_1399231,
title = {Flexible MXene/Graphene Films for Ultrafast Supercapacitors with Outstanding Volumetric Capacitance},
author = {Yan, Jun and Ren, Chang E. and Maleski, Kathleen and Hatter, Christine B. and Anasori, Babak and Urbankowski, Patrick and Sarycheva, Asya and Gogotsi, Yury G.},
abstractNote = {A strategy to prepare flexible and conductive MXene/graphene (reduced graphene oxide, rGO) supercapacitor electrodes by using electrostatic self‐assembly between positively charged rGO modified with poly(diallyldimethylammonium chloride) and negatively charged titanium carbide MXene nanosheets is presented. After electrostatic assembly, rGO nanosheets are inserted in‐between MXene layers. As a result, the self‐restacking of MXene nanosheets is effectively prevented, leading to a considerably increased interlayer spacing. Accelerated diffusion of electrolyte ions enables more electroactive sites to become accessible. The freestanding MXene/rGO‐5 wt% electrode displays a volumetric capacitance of 1040 F cm −3 at a scan rate of 2 mV s −1 , an impressive rate capability with 61% capacitance retention at 1 V s −1 and long cycle life. Moreover, the fabricated binder‐free symmetric supercapacitor shows an ultrahigh volumetric energy density of 32.6 Wh L −1 , which is among the highest values reported for carbon and MXene based materials in aqueous electrolytes. This work provides fundamental insight into the effect of interlayer spacing on the electrochemical performance of 2D hybrid materials and sheds light on the design of next‐generation flexible, portable and highly integrated supercapacitors with high volumetric and rate performances.},
doi = {10.1002/adfm.201701264},
journal = {Advanced Functional Materials},
number = ,
volume = 27,
place = {United States},
year = {Fri Jun 30 00:00:00 EDT 2017},
month = {Fri Jun 30 00:00:00 EDT 2017}
}

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journal, February 2019

  • Wang, Yuanming; Wang, Xue; Li, Xiaolong
  • Advanced Functional Materials, Vol. 29, Issue 14
  • DOI: 10.1002/adfm.201900326

3D Macroscopic Architectures from Self‐Assembled MXene Hydrogels
journal, June 2019

  • Shang, Tongxin; Lin, Zifeng; Qi, Changsheng
  • Advanced Functional Materials, Vol. 29, Issue 33
  • DOI: 10.1002/adfm.201903960

Pristine Titanium Carbide MXene Films with Environmentally Stable Conductivity and Superior Mechanical Strength
journal, November 2019

  • Chen, Hongwu; Wen, Yeye; Qi, Yingyi
  • Advanced Functional Materials, Vol. 30, Issue 5
  • DOI: 10.1002/adfm.201906996

3D Printing of Freestanding MXene Architectures for Current‐Collector‐Free Supercapacitors
journal, July 2019


Ultrastrong and Highly Conductive MXene‐Based Films for High‐Performance Electromagnetic Interference Shielding
journal, November 2019

  • Liu, Ji; Liu, Zhangshuo; Zhang, Hao‐Bin
  • Advanced Electronic Materials, Vol. 6, Issue 1
  • DOI: 10.1002/aelm.201901094

Scalable Water-Based Production of Highly Conductive 2D Nanosheets with Ultrahigh Volumetric Capacitance and Rate Capability
journal, March 2018

  • Jeon, Hyeonyeol; Jeong, Jae-Min; Kang, Heon Gyu
  • Advanced Energy Materials, Vol. 8, Issue 18
  • DOI: 10.1002/aenm.201800227

Flexible Nitrogen-Doped 2D Titanium Carbides (MXene) Films Constructed by an Ex Situ Solvothermal Method with Extraordinary Volumetric Capacitance
journal, September 2018

  • Yang, Chenhui; Tang, Yi; Tian, Yapeng
  • Advanced Energy Materials, Vol. 8, Issue 31
  • DOI: 10.1002/aenm.201802087

Ultrahigh-Capacity and Fire-Resistant LiFePO 4 -Based Composite Cathodes for Advanced Lithium-Ion Batteries
journal, January 2019


High‐Performance Electrocatalytic Conversion of N 2 to NH 3 Using Oxygen‐Vacancy‐Rich TiO 2 In Situ Grown on Ti 3 C 2 T x MXene
journal, February 2019

  • Fang, Yanfeng; Liu, Zaichun; Han, Jingrui
  • Advanced Energy Materials, Vol. 9, Issue 16
  • DOI: 10.1002/aenm.201803406

Regulating Fast Anionic Redox for High-Voltage Aqueous Hydrogen-Ion-based Energy Storage
journal, December 2018

  • Wang, Shengping; Zhao, Xiaoli; Yan, Xiaojun
  • Angewandte Chemie, Vol. 131, Issue 1
  • DOI: 10.1002/ange.201811220

Recent Progress of MXene-Based Nanomaterials in Flexible Energy Storage and Electronic Devices
journal, December 2018

  • Yang, Qi; Wang, Yukun; Li, Xinliang
  • Energy & Environmental Materials, Vol. 1, Issue 4
  • DOI: 10.1002/eem2.12023

Freestanding Lamellar Porous Carbon Stacks for Low‐Temperature‐Foldable Supercapacitors
journal, July 2019


Construction of cobaltous oxide/nickel–iron oxide electrodes with great cycle stability and high energy density for advanced asymmetry supercapacitor
journal, November 2019

  • Zhao, Yan; Chen, Yuan; Liu, Qingqing
  • Journal of Materials Science: Materials in Electronics, Vol. 30, Issue 24
  • DOI: 10.1007/s10854-019-02495-3

Electromagnetic simulation of MXene-based plasmonic metamaterials with enhanced optical absorption
journal, January 2020

  • Jakšić, Zoran; Obradov, Marko; Tanasković, Dragan
  • Optical and Quantum Electronics, Vol. 52, Issue 2
  • DOI: 10.1007/s11082-020-2227-8

Polyoxometalate-coupled MXene nanohybrid via poly(ionic liquid) linkers and its electrode for enhanced supercapacitive performance
journal, January 2018

  • Chen, Shu; Xiang, Yuanfang; Banks, M. Katherine
  • Nanoscale, Vol. 10, Issue 42
  • DOI: 10.1039/c8nr05760e

Electrolyte-assisted hydrothermal synthesis of holey graphene films for all-solid-state supercapacitors
journal, January 2018

  • Liu, Daoqing; Li, Qianwei; Zhao, Huazhang
  • Journal of Materials Chemistry A, Vol. 6, Issue 24
  • DOI: 10.1039/c8ta02580k

Surface modification of biomass-derived hard carbon by grafting porous carbon nanosheets for high-performance supercapacitors
journal, January 2018

  • Dong, Shian; He, Xiaojun; Zhang, Hanfang
  • Journal of Materials Chemistry A, Vol. 6, Issue 33
  • DOI: 10.1039/c8ta04080j

Silicon quantum dot-assisted synthesis of MoS 2 /rGO sandwich structures with excellent supercapacitive performance
journal, January 2019

  • Wu, Jinzhu; Li, Beibei; Feng, Yaxiu
  • New Journal of Chemistry, Vol. 43, Issue 22
  • DOI: 10.1039/c9nj01232j

A fully inkjet-printed transparent humidity sensor based on a Ti 3 C 2 /Ag hybrid for touchless sensing of finger motion
journal, January 2019


Macroporous three-dimensional MXene architectures for highly efficient solar steam generation
journal, January 2019

  • Zhao, Xing; Zha, Xiang-Jun; Pu, Jun-Hong
  • Journal of Materials Chemistry A, Vol. 7, Issue 17
  • DOI: 10.1039/c9ta00176j

Designing chemical bonds between active materials and current collectors for packaging a high-performance supercapacitor
journal, December 2019


Effects of biaxial strain and functional groups on SiC/ti 3 C 2 heterostructure: a first principle calculation
journal, November 2019


Interfacial and electronic properties of heterostructures of MXene and graphene
journal, February 2019


2D/2D SnS 2 /MoS 2 layered heterojunction for enhanced supercapacitor performance
journal, September 2019

  • Wang, Bo; Hu, Rong; Zhang, Jun
  • Journal of the American Ceramic Society, Vol. 103, Issue 2
  • DOI: 10.1111/jace.16778

Advances in Two-Dimensional MXenes for Nitrogen Electrocatalytic Reduction to Ammonia
journal, February 2020

  • Yu, Lan-lan; Qin, Jiang-zhou; Zhao, Wen-jun
  • International Journal of Photoenergy, Vol. 2020
  • DOI: 10.1155/2020/5251431

Strategies to Enhance the Performance of Electrochemical Capacitors Based on Carbon Materials
journal, May 2019

  • Salinas-Torres, David; Ruiz-Rosas, Ramiro; Morallón, Emilia
  • Frontiers in Materials, Vol. 6
  • DOI: 10.3389/fmats.2019.00115

Hollow MXene Sphere/Reduced Graphene Aerogel Composites for Piezoresistive Sensor with Ultra‐High Sensitivity
journal, December 2019

  • Zhu, Meng; Yue, Yang; Cheng, Yongfa
  • Advanced Electronic Materials, Vol. 6, Issue 2
  • DOI: 10.1002/aelm.201901064

Two‐Dimensional Transition Metal Carbides and Nitrides (MXenes): Synthesis, Properties, and Electrochemical Energy Storage Applications
journal, March 2020

  • Zhang, Chuanfang (John); Ma, Yonglu; Zhang, Xuetao
  • ENERGY & ENVIRONMENTAL MATERIALS, Vol. 3, Issue 1
  • DOI: 10.1002/eem2.12058

Highly Conductive Ti 3 C 2 T x MXene Hybrid Fibers for Flexible and Elastic Fiber-Shaped Supercapacitors
journal, January 2019


A nanoporous MXene film enables flexible supercapacitors with high energy storage
journal, January 2018

  • Fan, Zhimin; Wang, Youshan; Xie, Zhimin
  • Nanoscale, Vol. 10, Issue 20
  • DOI: 10.1039/c8nr01550c

Ti 2 C 3 T x nanosheets as photothermal agents for near-infrared responsive hydrogels
journal, January 2018

  • Yang, Changyu; Xu, Danyun; Peng, WenChao
  • Nanoscale, Vol. 10, Issue 32
  • DOI: 10.1039/c8nr05301d

Mixed transition metal oxide nanowire arrays enabling hybrid capacitor performance enhancement
journal, January 2019

  • Zhao, Depeng; Dai, Meizhen; Tong, Yongli
  • CrystEngComm, Vol. 21, Issue 38
  • DOI: 10.1039/c9ce01169b

The solvent-free mechanochemical synthesis of mildly oxidized graphene oxide and its application as a novel conductive surfactant
journal, January 2019

  • Chen, Jianhui; Chen, Wufeng; Song, Dongcheng
  • New Journal of Chemistry, Vol. 43, Issue 18
  • DOI: 10.1039/c9nj00529c

Few-layered Ti 3 C 2 T x MXenes coupled with Fe 2 O 3 nanorod arrays grown on carbon cloth as anodes for flexible asymmetric supercapacitors
journal, January 2019

  • Li, Fei; Liu, Yi-Lin; Wang, Gui-Gen
  • Journal of Materials Chemistry A, Vol. 7, Issue 39
  • DOI: 10.1039/c9ta08144e

Printable Nanomaterials for the Fabrication of High-Performance Supercapacitors
journal, July 2018


Modified MXene/Holey Graphene Films for Advanced Supercapacitor Electrodes with Superior Energy Storage
journal, August 2018


Ultrathin Titanate Nanosheets/Graphene Films Derived from Confined Transformation for Excellent Na/K Ion Storage
journal, June 2018


Regulating Fast Anionic Redox for High-Voltage Aqueous Hydrogen-Ion-based Energy Storage
journal, December 2018

  • Wang, Shengping; Zhao, Xiaoli; Yan, Xiaojun
  • Angewandte Chemie International Edition, Vol. 58, Issue 1
  • DOI: 10.1002/anie.201811220

An MXene/CNTs@P nanohybrid with stable Ti–O–P bonds for enhanced lithium ion storage
journal, January 2019

  • Zhang, Shixue; Liu, Huan; Cao, Bin
  • Journal of Materials Chemistry A, Vol. 7, Issue 38
  • DOI: 10.1039/c9ta07357d

Assembling 2D MXenes into Highly Stable Pseudocapacitive Electrodes with High Power and Energy Densities
journal, December 2018

  • VahidMohammadi, Armin; Mojtabavi, Mehrnaz; Caffrey, Nuala Mai
  • Advanced Materials, Vol. 31, Issue 8
  • DOI: 10.1002/adma.201806931

2D Stacks of MXene Ti 3 C 2 and 1T‐Phase WS 2 with Enhanced Capacitive Behavior
journal, May 2019

  • Vyskočil, Jan; Mayorga‐Martinez, Carmen C.; Szőkölová, Kateřina
  • ChemElectroChem, Vol. 6, Issue 15
  • DOI: 10.1002/celc.201900643

Carbon nanotubes enhance flexible MXene films for high-rate supercapacitors
journal, September 2019


All-Solid-State Supercapacitors Based on Flexible Co3O4 Nanoflowers/rGO Nanocomposites
journal, July 2018


Electrostatic Self-assembly of 0D–2D SnO2 Quantum Dots/Ti3C2Tx MXene Hybrids as Anode for Lithium-Ion Batteries
journal, August 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

A general way to fabricate transition metal dichalcogenide/oxide-sandwiched MXene nanosheets as flexible film anodes for high-performance lithium storage
journal, January 2019

  • Wang, Chuang; Zhu, Xiao-Dong; Wang, Ke-Xin
  • Sustainable Energy & Fuels, Vol. 3, Issue 10
  • DOI: 10.1039/c9se00635d

Beyond Graphene Anode Materials for Emerging Metal Ion Batteries and Supercapacitors
journal, October 2018


Electromagnetic Shielding by MXene-Graphene-PVDF Composite with Hydrophobic, Lightweight and Flexible Graphene Coated Fabric
journal, September 2018

  • Raagulan, Kanthasamy; Braveenth, Ramanaskanda; Jang, Hee
  • Materials, Vol. 11, Issue 10
  • DOI: 10.3390/ma11101803

Nitrogen Doped Intercalation TiO2/TiN/Ti3C2Tx Nanocomposite Electrodes with Enhanced Pseudocapacitance
journal, February 2020


Printable Nanomaterials for the Fabrication of High-Performance Supercapacitors
journal, July 2018


Fabrication of Flexible, Lightweight, Magnetic Mushroom Gills and Coral-Like MXene–Carbon Nanotube Nanocomposites for EMI Shielding Application
journal, April 2019

  • Raagulan, Kanthasamy; Braveenth, Ramanaskanda; Ro Lee, Lee
  • Nanomaterials, Vol. 9, Issue 4
  • DOI: 10.3390/nano9040519