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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. Furthermore, 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 Lab. (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:
Journal Article: 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.. 2017. "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. Furthermore, 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},
url = {https://www.osti.gov/biblio/1399231}, journal = {Advanced Functional Materials},
issn = {1616-301X},
number = ,
volume = 27,
place = {United States},
year = {2017},
month = {6}
}

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Cited by: 122 works
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Works referenced in this record:

Flexible MXene/Carbon Nanotube Composite Paper with High Volumetric Capacitance
journal, November 2014


True Performance Metrics in Electrochemical Energy Storage
journal, November 2011


Carbon materials for high volumetric performance supercapacitors: design, progress, challenges and opportunities
journal, January 2016


Amine-Assisted Delamination of Nb 2 C MXene for Li-Ion Energy Storage Devices
journal, April 2015


Pseudocapacitive Electrodes Produced by Oxidant-Free Polymerization of Pyrrole between the Layers of 2D Titanium Carbide (MXene)
journal, December 2015


The advanced carbide-derived carbon based supercapacitor
journal, November 2006


Ultrahigh-power micrometre-sized supercapacitors based on onion-like carbon
journal, August 2010


Two-Dimensional Nanocrystals Produced by Exfoliation of Ti3AlC2
journal, August 2011


Synthesis and Characterization of 2D Molybdenum Carbide (MXene)
journal, February 2016


Processable aqueous dispersions of graphene nanosheets
journal, January 2008


Cation Intercalation and High Volumetric Capacitance of Two-Dimensional Titanium Carbide
journal, September 2013


Direct Chemical Synthesis of MnO 2 Nanowhiskers on Transition-Metal Carbide Surfaces for Supercapacitor Applications
journal, July 2016


Activated Graphene-Based Carbons as Supercapacitor Electrodes with Macro- and Mesopores
journal, July 2013


Photoluminescent Ti 3 C 2 MXene Quantum Dots for Multicolor Cellular Imaging
journal, February 2017


High-rate electrochemical energy storage through Li+ intercalation pseudocapacitance
journal, April 2013


Sodium-Ion Intercalation Mechanism in MXene Nanosheets
journal, February 2016


Laser Scribing of High-Performance and Flexible Graphene-Based Electrochemical Capacitors
journal, March 2012


Conductive two-dimensional titanium carbide ‘clay’ with high volumetric capacitance
journal, November 2014


Capacitance of two-dimensional titanium carbide (MXene) and MXene/carbon nanotube composites in organic electrolytes
journal, February 2016


Self-assembled Ti 3 C 2 T x MXene film with high gravimetric capacitance
journal, January 2015


2D metal carbides and nitrides (MXenes) for energy storage
journal, January 2017


Electromagnetic interference shielding with 2D transition metal carbides (MXenes)
journal, September 2016


Flexible and conductive MXene films and nanocomposites with high capacitance
journal, November 2014


Ion-Exchange and Cation Solvation Reactions in Ti 3 C 2 MXene
journal, May 2016


“Inner” and “outer” active surface of RuO2 electrodes
journal, January 1990


Synthesis of Two-Dimensional Materials for Capacitive Energy Storage
journal, June 2016


Charge- and Size-Selective Ion Sieving Through Ti 3 C 2 T x MXene Membranes
journal, September 2015


Probing the Mechanism of High Capacitance in 2D Titanium Carbide Using In Situ X-Ray Absorption Spectroscopy
journal, May 2015


Metallic 1T phase MoS2 nanosheets as supercapacitor electrode materials
journal, March 2015


High-Power and Ultralong-Life Aqueous Zinc-Ion Hybrid Capacitors Based on Pseudocapacitive Charge Storage
journal, October 2019


Works referencing / citing this record:

2D MXene Nanofilms with Tunable Gas Transport Channels
journal, June 2018


MXene‐Bonded Flexible Hard Carbon Film as Anode for Stable Na/K‐Ion Storage
journal, October 2019


Toward Superior Capacitive Energy Storage: Recent Advances in Pore Engineering for Dense Electrodes
journal, March 2018


1D Supercapacitors for Emerging Electronics: Current Status and Future Directions
journal, July 2019


MXene‐Based Composites: Synthesis and Applications in Rechargeable Batteries and Supercapacitors
journal, February 2019


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


Recent Advances in Emerging 2D Material‐Based Gas Sensors: Potential in Disease Diagnosis
journal, September 2019


Radiation‐Induced Self‐Assembly of Ti 3 C 2 T x with Improved Electrochemical Performance for Supercapacitor
journal, January 2020


Scalable Manufacturing of Large and Flexible Sheets of MXene/Graphene Heterostructures
journal, March 2019


Preparation of Ti 3 C 2 T x MXene‐Derived Quantum Dots with White/Blue‐Emitting Photoluminescence and Electrochemiluminescence
journal, October 2018


Porous g‐C 3 N 4 and MXene Dual‐Confined FeOOH Quantum Dots for Superior Energy Storage in an Ionic Liquid
journal, November 2019


The Rise of 2D Photothermal Materials beyond Graphene for Clean Water Production
journal, January 2020


MXene‐Reduced Graphene Oxide Aerogel for Aqueous Zinc‐Ion Hybrid Supercapacitor with Ultralong Cycle Life
journal, August 2019


Compressible All‐In‐One Supercapacitor with Adjustable Output Voltage Based on Polypyrrole‐Coated Melamine Foam
journal, September 2019


Antimonene Engineered Highly Deformable Freestanding Electrode with Extraordinarily Improved Energy Storage Performance
journal, October 2019


MXene Aerogel Scaffolds for High‐Rate Lithium Metal Anodes
journal, October 2018


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


MXene Aerogel Scaffolds for High-Rate Lithium Metal Anodes
journal, October 2018


2D Titanium Carbide/Reduced Graphene Oxide Heterostructures for Supercapacitor Applications
journal, April 2018


Ultra-Stable Asymmetric Supercapacitors Constructed by In-Situ Electro-Oxidation Activated Ni@CNTs Composites
journal, August 2018


Thermally Reduced Graphene/MXene Film for Enhanced Li‐ion Storage
journal, June 2018


Electrochemical Behavior of Ti 3 C 2 T x MXene in Environmentally Friendly Methanesulfonic Acid Electrolyte
journal, August 2019


Free‐standing Reduced Graphene Oxide/MoO 3‐ x Composite Film with High Performance for Flexible Supercapacitors
journal, August 2019


Recent Advances in Layered Ti 3 C 2 T x MXene for Electrochemical Energy Storage
journal, February 2018


High-Performance Biscrolled MXene/Carbon Nanotube Yarn Supercapacitors
journal, August 2018


A MXene‐Based Wearable Biosensor System for High‐Performance In Vitro Perspiration Analysis
journal, April 2019


Delaminating Vanadium Carbides for Zinc‐Ion Storage: Hydrate Precipitation and H + /Zn 2+ Co‐Action Mechanism
journal, August 2019


Layered BiOBr/Ti3C2 MXene composite with improved visible-light photocatalytic activity
journal, October 2018


Monolithic carbon nanosheets with rich pores for high-capacitance supercapacitor
journal, November 2019


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


Plate-to-Layer Bi2MoO6/MXene-Heterostructured Anode for Lithium-Ion Batteries
journal, September 2019


Intercalated metal–organic frameworks with high electronic conductivity as negative electrode materials for hybrid capacitors
journal, October 2018


Highly packed graphene–CNT films as electrodes for aqueous supercapacitors with high volumetric performance
journal, January 2018


High-capacitance Ti 3 C 2 T x MXene obtained by etching submicron Ti 3 AlC 2 grains grown in molten salt
journal, January 2018


Seawater electrolyte-mediated high volumetric MXene-based electrochemical symmetric supercapacitors
journal, January 2018


Flexible Ti 3 C 2 T x /PEDOT:PSS films with outstanding volumetric capacitance for asymmetric supercapacitors
journal, January 2019


3D Ti 3 C 2 T x aerogels with enhanced surface area for high performance supercapacitors
journal, January 2018


Hybrid carbon nanostructured fibers: stepping stone for intelligent textile-based electronics
journal, January 2019


Concisely modularized assembling of graphene-based thin films with promising electrode performance
journal, January 2019


Polypyrrole–MXene coated textile-based flexible energy storage device
journal, January 2018


A flexible VOCs sensor based on a 3D Mxene framework with a high sensing performance
journal, January 2018


Exploring the synergy of 2D MXene-supported black phosphorus quantum dots in hydrogen and oxygen evolution reactions
journal, January 2018


Carbon-intercalated Ti 3 C 2 T x MXene for high-performance electrochemical energy storage
journal, January 2018


Ti 3 C 2 T x (T = F, OH) MXene nanosheets: conductive 2D catalysts for ambient electrohydrogenation of N 2 to NH 3
journal, January 2018


MXene-derived TiO 2 /reduced graphene oxide composite with an enhanced capacitive capacity for Li-ion and K-ion batteries
journal, January 2019


A recyclable route to produce biochar with a tailored structure and surface chemistry for enhanced charge storage
journal, January 2019


MXene and MXene-based composites: synthesis, properties and environment-related applications
journal, January 2020


Highly fluorescent Ti 3 C 2 MXene quantum dots for macrophage labeling and Cu 2+ ion sensing
journal, January 2019


Exploring the microscopic mechanism of pseudocapacitance with electronic structures in monolayer 1T-MoS 2 electrodes for supercapacitors
journal, January 2019


Nitrogen-doped carbon sheets coated on CoNiO 2 @textile carbon as bifunctional electrodes for asymmetric supercapacitors
journal, January 2019


Surface nitrogen-modified 2D titanium carbide (MXene) with high energy density for aqueous supercapacitor applications
journal, January 2019


Ionic liquid pre-intercalated MXene films for ionogel-based flexible micro-supercapacitors with high volumetric energy density
journal, January 2019


Pursuit of a high-capacity and long-life Mg-storage cathode by tailoring sandwich-structured MXene@carbon nanosphere composites
journal, January 2019


Multivalent metal ion hybrid capacitors: a review with a focus on zinc-ion hybrid capacitors
journal, January 2019


Excellent air and water stability of two-dimensional black phosphorene/MXene heterostructure
journal, March 2019


NiFe 2 O 4 nanoparticles on reduced graphene oxide for supercapacitor electrodes with improved capacitance
journal, September 2019


Two-Dimensional Titanium Carbides (Ti3C2Tx) Functionalized by Poly(m-phenylenediamine) for Efficient Adsorption and Reduction of Hexavalent Chromium
journal, December 2019


Hydrothermal Synthesis of Co-Doped NiSe2 Nanowire for High-Performance Asymmetric Supercapacitors
journal, August 2018


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


Stamping of Flexible, Coplanar Micro-Supercapacitors Using MXene Inks
journal, January 2018


Engineering 3D Ion Transport Channels for Flexible MXene Films with Superior Capacitive Performance
journal, February 2019


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


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


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


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


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


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


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


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


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


Knittable energy storing fiber with high volumetric performance made from predominantly MXene nanosheets
journal, January 2017


The mechanism of ultrafast supercapacitors
journal, January 2018


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


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


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


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


An MnO 2 –Ti 3 C 2 T x MXene nanohybrid: an efficient and durable electrocatalyst toward artificial N 2 fixation to NH 3 under ambient conditions
journal, January 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


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


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


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


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


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


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


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


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


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


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