Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration
Abstract
Recent experiments have shown that nitrogen doping enhances capacitance in carbon electrode supercapacitors. However, a detailed study of the effect of N-doping on capacitance is still lacking. In this paper, we study the doping concentration and the configuration effect on the electric double-layer (EDL) capacitance, quantum capacitance, and total capacitance. It is found that pyridinic and graphitic nitrogens can increase the total capacitance by increasing quantum capacitance, but pyrrolic configuration limits the total capacitance due to its much lower quantum capacitance than the other two configurations. We also find that, unlike the graphitic and pyridinic nitrogens, the pyrrolic configuration's quantum capacitance does not depend on the nitrogen concentration, which may explain why some capacitance versus voltage measurements of N-doped graphene exhibit a V-shaped curve similar to that of undoped graphene. Our investigation provides a deeper understanding of the capacitance enhancement of the N-doping effect in carbon electrodes and suggests a potentially effective way to optimize the capacitance by controlling the type of N-doping.
- Authors:
-
- Univ. of California, Riverside, CA (United States)
- Vanderbilt Univ., Nashville, TN (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:
- 1261372
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 18; Journal Issue: 6; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhan, Cheng, Cummings, Peter, and Jiang, De-en. Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration. United States: N. p., 2016.
Web. doi:10.1039/C5CP06952A.
Zhan, Cheng, Cummings, Peter, & Jiang, De-en. Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration. United States. https://doi.org/10.1039/C5CP06952A
Zhan, Cheng, Cummings, Peter, and Jiang, De-en. Fri .
"Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration". United States. https://doi.org/10.1039/C5CP06952A. https://www.osti.gov/servlets/purl/1261372.
@article{osti_1261372,
title = {Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration},
author = {Zhan, Cheng and Cummings, Peter and Jiang, De-en},
abstractNote = {Recent experiments have shown that nitrogen doping enhances capacitance in carbon electrode supercapacitors. However, a detailed study of the effect of N-doping on capacitance is still lacking. In this paper, we study the doping concentration and the configuration effect on the electric double-layer (EDL) capacitance, quantum capacitance, and total capacitance. It is found that pyridinic and graphitic nitrogens can increase the total capacitance by increasing quantum capacitance, but pyrrolic configuration limits the total capacitance due to its much lower quantum capacitance than the other two configurations. We also find that, unlike the graphitic and pyridinic nitrogens, the pyrrolic configuration's quantum capacitance does not depend on the nitrogen concentration, which may explain why some capacitance versus voltage measurements of N-doped graphene exhibit a V-shaped curve similar to that of undoped graphene. Our investigation provides a deeper understanding of the capacitance enhancement of the N-doping effect in carbon electrodes and suggests a potentially effective way to optimize the capacitance by controlling the type of N-doping.},
doi = {10.1039/C5CP06952A},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 6,
volume = 18,
place = {United States},
year = {Fri Jan 08 00:00:00 EST 2016},
month = {Fri Jan 08 00:00:00 EST 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 91 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Carbon-based materials as supercapacitor electrodes
journal, January 2009
- Zhang, Li Li; Zhao, X. S.
- Chemical Society Reviews, Vol. 38, Issue 9
Supercapacitor Devices Based on Graphene Materials
journal, July 2009
- Wang, Yan; Shi, Zhiqiang; Huang, Yi
- The Journal of Physical Chemistry C, Vol. 113, Issue 30
Anomalous Increase in Carbon Capacitance at Pore Sizes Less Than 1 Nanometer
journal, September 2006
- Chmiola, J.
- Science, Vol. 313, Issue 5794
Influence of pore structure on electric double-layer capacitance of template mesoporous carbons
journal, June 2004
- Fuertes, Antonio B.; Pico, Fernando; Rojo, Jose M.
- Journal of Power Sources, Vol. 133, Issue 2
Electrochemical energy storage in ordered porous carbon materials
journal, May 2005
- Vix-Guterl, Cathie; Frackowiak, Elzbieta; Jurewicz, Krzysztof
- Carbon, Vol. 43, Issue 6
Graphene-Based Ultracapacitors
journal, October 2008
- Stoller, Meryl D.; Park, Sungjin; Zhu, Yanwu
- Nano Letters, Vol. 8, Issue 10
Electrochemical interfacial capacitance in multilayer graphene sheets: Dependence on number of stacking layers
journal, September 2009
- Wang, Da-Wei; Li, Feng; Wu, Zhong-Shuai
- Electrochemistry Communications, Vol. 11, Issue 9
Interfacial capacitance of single layer graphene
journal, January 2011
- Stoller, Meryl D.; Magnuson, Carl W.; Zhu, Yanwu
- Energy & Environmental Science, Vol. 4, Issue 11
Tailoring the physical properties of nanocomposite films by the insertion of graphene and other nanoparticles
journal, April 2014
- Alzari, V.; Sanna, V.; Biccai, S.
- Composites Part B: Engineering, Vol. 60
Valley-degenerate two-dimensional electrons in the lowest Landau level
journal, January 2014
- Kott, Tomasz M.; Hu, Binhui; Brown, S. H.
- Physical Review B, Vol. 89, Issue 4
Quantum Capacitance of Aryldiazonium Modified Large Area Few-Layer Graphene Electrodes
journal, November 2015
- Brooksby, Paula A.; Farquhar, Anna K.; Dykstra, Haidee M.
- The Journal of Physical Chemistry C, Vol. 119, Issue 46
Mapping Local Quantum Capacitance and Charged Impurities in Graphene via Plasmonic Impedance Imaging
journal, September 2015
- Shan, Xiaonan; Chen, Shan; Wang, Hui
- Advanced Materials, Vol. 27, Issue 40
On the influence of polarization effects in predicting the interfacial structure and capacitance of graphene-like electrodes in ionic liquids
journal, January 2015
- Paek, Eunsu; Pak, Alexander J.; Hwang, Gyeong S.
- The Journal of Chemical Physics, Vol. 142, Issue 2
A Computational Study of the Interfacial Structure and Capacitance of Graphene in [BMIM][PF 6 ] Ionic Liquid
journal, November 2012
- Paek, Eunsu; Pak, Alexander J.; Hwang, Gyeong S.
- Journal of The Electrochemical Society, Vol. 160, Issue 1
Tailoring graphene-based electrodes from semiconducting to metallic to increase the energy density in supercapacitors
journal, October 2015
- Vatamanu, Jenel; Ni, Xiaojuan; Liu, Feng
- Nanotechnology, Vol. 26, Issue 46
Nitrogen doping of graphene and its effect on quantum capacitance, and a new insight on the enhanced capacitance of N-doped carbon
journal, January 2012
- Zhang, Li Li; Zhao, Xin; Ji, Hengxing
- Energy & Environmental Science, Vol. 5, Issue 11, p. 9618-9625
Synthesis of Nitrogen-Doped Graphene Using Embedded Carbon and Nitrogen Sources
journal, January 2011
- Zhang, Chaohua; Fu, Lei; Liu, Nan
- Advanced Materials, Vol. 23, Issue 8
Nitrogen-Doped Graphene for High-Performance Ultracapacitors and the Importance of Nitrogen-Doped Sites at Basal Planes
journal, June 2011
- Jeong, Hyung Mo; Lee, Jung Woo; Shin, Weon Ho
- Nano Letters, Vol. 11, Issue 6
Low-temperature preparation of nitrogen-doped graphene for supercapacitors
journal, May 2013
- Cao, Hailiang; Zhou, Xufeng; Qin, Zhihong
- Carbon, Vol. 56
Nitrogen-doped graphene for supercapacitor with long-term electrochemical stability
journal, June 2014
- Wang, Kai; Li, Liwei; Zhang, Tiezhu
- Energy, Vol. 70
Crumpled Nitrogen-Doped Graphene Nanosheets with Ultrahigh Pore Volume for High-Performance Supercapacitor
journal, August 2012
- Wen, Zhenhai; Wang, Xinchen; Mao, Shun
- Advanced Materials, Vol. 24, Issue 41
Highly concentrated, stable nitrogen-doped graphene for supercapacitors: Simultaneous doping and reduction
journal, February 2012
- Jiang, Baojiang; Tian, Chungui; Wang, Lei
- Applied Surface Science, Vol. 258, Issue 8, p. 3438-3443
Nitrogen-doped graphene with high nitrogen level via a one-step hydrothermal reaction of graphene oxide with urea for superior capacitive energy storage
journal, January 2012
- Sun, Li; Wang, Lei; Tian, Chungui
- RSC Advances, Vol. 2, Issue 10
Nitrogen-doped and crumpled graphene sheets with improved supercapacitance
journal, January 2014
- Zou, Yuqin; Kinloch, Ian A.; Dryfe, Robert A. W.
- J. Mater. Chem. A, Vol. 2, Issue 45
Experimental comparison of N(1s) X-ray photoelectron spectroscopy binding energies of hard and elastic amorphous carbon nitride films with reference organic compounds
journal, January 2003
- Gammon, W. J.; Kraft, O.; Reilly, A. C.
- Carbon, Vol. 41, Issue 10
Visualizing Individual Nitrogen Dopants in Monolayer Graphene
journal, August 2011
- Zhao, L.; He, R.; Rim, K. T.
- Science, Vol. 333, Issue 6045
Joint Density-Functional Theory: Ab Initio Study of Cr 2 O 3 Surface Chemistry in Solution
journal, August 2005
- Petrosyan, S. A.; Rigos, A. A.; Arias, T. A.
- The Journal of Physical Chemistry B, Vol. 109, Issue 32
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Pseudopotentials for high-throughput DFT calculations
journal, January 2014
- Garrity, Kevin F.; Bennett, Joseph W.; Rabe, Karin M.
- Computational Materials Science, Vol. 81
The missing term in effective pair potentials
journal, November 1987
- Berendsen, H. J. C.; Grigera, J. R.; Straatsma, T. P.
- The Journal of Physical Chemistry, Vol. 91, Issue 24
Interionic potentials of mean force for SrCl2 in polarizable water
journal, November 1994
- Smith, David E.; Dang, Liem X.
- Chemical Physics Letters, Vol. 230, Issue 1-2
An ab Initio CFF93 All-Atom Force Field for Polycarbonates
journal, April 1994
- Sun, Huai; Mumby, Stephen J.; Maple, Jon R.
- Journal of the American Chemical Society, Vol. 116, Issue 7
Ab initio characterizations of molecular structures, conformation energies, and hydrogen-bonding properties for polyurethane hard segments
journal, October 1993
- Sun, H.
- Macromolecules, Vol. 26, Issue 22
GROMACS 4: Algorithms for Highly Efficient, Load-Balanced, and Scalable Molecular Simulation
journal, February 2008
- Hess, Berk; Kutzner, Carsten; van der Spoel, David
- Journal of Chemical Theory and Computation, Vol. 4, Issue 3
Ewald summation for systems with slab geometry
journal, August 1999
- Yeh, In-Chul; Berkowitz, Max L.
- The Journal of Chemical Physics, Vol. 111, Issue 7
Particle mesh Ewald: An N ⋅log( N ) method for Ewald sums in large systems
journal, June 1993
- Darden, Tom; York, Darrin; Pedersen, Lee
- The Journal of Chemical Physics, Vol. 98, Issue 12
Surface Corrugation Effects on the Water–Graphene Interfacial and Confinement Behavior
journal, October 2013
- Chialvo, Ariel A.; Vlcek, Lukas; Cummings, Peter T.
- The Journal of Physical Chemistry C, Vol. 117, Issue 45
Surface Strain Effects on the Water–Graphene Interfacial and Confinement Behavior
journal, August 2014
- Chialvo, Ariel A.; Vlcek, Lukas; Cummings, Peter T.
- The Journal of Physical Chemistry C, Vol. 118, Issue 34
Atomistic Insight on the Charging Energetics in Subnanometer Pore Supercapacitors
journal, September 2010
- Feng, Guang; Qiao, Rui; Huang, Jingsong
- The Journal of Physical Chemistry C, Vol. 114, Issue 41
Quantum Effects on the Capacitance of Graphene-Based Electrodes
journal, September 2015
- Zhan, Cheng; Neal, Justin; Wu, Jianzhong
- The Journal of Physical Chemistry C, Vol. 119, Issue 39
Review on Recent Progress in Nitrogen-Doped Graphene: Synthesis, Characterization, and Its Potential Applications
journal, April 2012
- Wang, Haibo; Maiyalagan, Thandavarayan; Wang, Xin
- ACS Catalysis, Vol. 2, Issue 5
Nitrogen-Doped Graphene Materials for Supercapacitor Applications
journal, February 2014
- Lu, Yanhong; Huang, Yi; Zhang, Mingjie
- Journal of Nanoscience and Nanotechnology, Vol. 14, Issue 2
Nitrogen-doped graphene: beyond single substitution and enhanced molecular sensing
journal, August 2012
- Lv, Ruitao; Li, Qing; Botello-Méndez, Andrés R.
- Scientific Reports, Vol. 2, Issue 1
Introduction of nitrogen with controllable configuration into graphene via vacancies and edges
journal, January 2013
- Wang, Bin; Tsetseris, Leonidas; Pantelides, Sokrates T.
- Journal of Materials Chemistry A, Vol. 1, Issue 47
On the Origin of the Enhanced Supercapacitor Performance of Nitrogen-Doped Graphene
journal, March 2013
- Paek, Eunsu; Pak, Alexander J.; Kweon, Kyoung E.
- The Journal of Physical Chemistry C, Vol. 117, Issue 11
On the Influence of Surface Topography on the Electric Double Layer Structure and Differential Capacitance of Graphite/Ionic Liquid Interfaces
journal, August 2011
- Vatamanu, Jenel; Cao, Liulei; Borodin, Oleg
- The Journal of Physical Chemistry Letters, Vol. 2, Issue 17
Molecular Simulations of the Electric Double Layer Structure, Differential Capacitance, and Charging Kinetics for N -Methyl- N -propylpyrrolidinium Bis(fluorosulfonyl)imide at Graphite Electrodes
journal, March 2011
- Vatamanu, Jenel; Borodin, Oleg; Smith, Grant D.
- The Journal of Physical Chemistry B, Vol. 115, Issue 12
Molecular Insights into the Potential and Temperature Dependences of the Differential Capacitance of a Room-Temperature Ionic Liquid at Graphite Electrodes
journal, October 2010
- Vatamanu, Jenel; Borodin, Oleg; Smith, Grant D.
- Journal of the American Chemical Society, Vol. 132, Issue 42
Stability and Core-Level Signature of Nitrogen Dopants in Carbonaceous Materials
journal, August 2015
- Tian, Ziqi; Dai, Sheng; Jiang, De-en
- Chemistry of Materials, Vol. 27, Issue 16
Works referencing / citing this record:
Computational Insights into Materials and Interfaces for Capacitive Energy Storage
journal, April 2017
- Zhan, Cheng; Lian, Cheng; Zhang, Yu
- Advanced Science, Vol. 4, Issue 7
Substrate Effects in Graphene-Based Electric Double-Layer Capacitors: The Pivotal Interplays between Ions and Solvents
journal, September 2017
- Yang, Huachao; Bo, Zheng; Yang, Jinyuan
- ChemElectroChem, Vol. 4, Issue 11
Enhancement of quantum capacitance by chemical modification of graphene supercapacitor electrodes: a study by first principles
journal, September 2019
- Sruthi, T.; Tarafder, Kartick
- Bulletin of Materials Science, Vol. 42, Issue 6
Trade-off between quantum capacitance and thermodynamic stability of defected graphene: an implication for supercapacitor electrodes
journal, March 2018
- Srivastava, Anurag; SanthiBhushan, Boddepalli
- Applied Nanoscience, Vol. 8, Issue 4
Nano-Architecture of nitrogen-doped graphene films synthesized from a solid CN source
journal, February 2018
- Maddi, Chiranjeevi; Bourquard, Florent; Barnier, Vincent
- Scientific Reports, Vol. 8, Issue 1
Pyridinic-nitrogen highly doped nanotubular carbon arrays grown on a carbon cloth for high-performance and flexible supercapacitors
journal, January 2018
- Li, Rui; Li, Xiaodong; Chen, Jin
- Nanoscale, Vol. 10, Issue 8
Adsorption of metal atoms on silicene: stability and quantum capacitance of silicene-based electrode materials
journal, January 2019
- Xu, Q.; Yang, G. M.; Fan, Xiaofeng
- Physical Chemistry Chemical Physics, Vol. 21, Issue 8
One-step synthesis of nitrogen-doped wood derived carbons as advanced electrodes for supercapacitor applications
journal, January 2019
- Meng, Qi; Ge, Huilin; Yao, Weitang
- New Journal of Chemistry, Vol. 43, Issue 9
Investigating the asymmetry in the EDL response of C 60 /graphene supercapacitors
journal, January 2019
- Fileti, Eudes Eterno; Colherinhas, Guilherme
- Physical Chemistry Chemical Physics, Vol. 21, Issue 28
Exploring doped or vacancy-modified graphene-based electrodes for applications in asymmetric supercapacitors
journal, January 2020
- da Silva, Débora A. C.; Paulista Neto, Antenor J.; Pascon, Aline M.
- Physical Chemistry Chemical Physics, Vol. 22, Issue 7
A nitrogen and phosphorus enriched pyridine bridged inorganic–organic hybrid material for supercapacitor application
journal, January 2019
- Dhiman, Nisha; Mohanty, Paritosh
- New Journal of Chemistry, Vol. 43, Issue 42
Tuning the nanostructure of nitrogen-doped graphene laminates for forward osmosis desalination
journal, January 2019
- Song, Jun-ho; Shon, Ho Kyong; Wang, Peng
- Nanoscale, Vol. 11, Issue 45
An ecofriendly route to synthesize C-Mo 2 C and C/N-Mo 2 C utilizing waste polyethene for efficient hydrogen evolution reaction (HER) activity and high performance capacitors
journal, January 2020
- Mir, Rameez Ahmad; Pandey, O. P.
- Sustainable Energy & Fuels, Vol. 4, Issue 2
A comparative study of room temperature ionic liquids and their organic solvent mixtures near charged electrodes
journal, September 2016
- Vatamanu, Jenel; Vatamanu, Mihaela; Borodin, Oleg
- Journal of Physics: Condensed Matter, Vol. 28, Issue 46
Route to achieving enhanced quantum capacitance in functionalized graphene based supercapacitor electrodes
journal, August 2019
- Sruthi, T.; Kartick, Tarafder
- Journal of Physics: Condensed Matter, Vol. 31, Issue 47
One step hydrothermal synthesis of 3D CoS 2 @MoS 2 -NG for high performance supercapacitors
journal, May 2018
- Meng, Qi; Chen, Yizhi; Zhu, Wenkun
- Nanotechnology, Vol. 29, Issue 29
Theoretical Study on the Quantum Capacitance Origin of Graphene Cathodes in Lithium Ion Capacitors
journal, October 2018
- Su, Fangyuan; Huo, Li; Kong, Qingqiang
- Catalysts, Vol. 8, Issue 10