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Title: Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/C5CP06952A· OSTI ID:1261372
 [1];  [2];  [1]
  1. Univ. of California, Riverside, CA (United States)
  2. Vanderbilt Univ., Nashville, TN (United States)

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.

Research Organization:
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 Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1261372
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Vol. 18, Issue 6; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 91 works
Citation information provided by
Web of Science

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Computational Insights into Materials and Interfaces for Capacitive Energy Storage journal April 2017
Substrate Effects in Graphene-Based Electric Double-Layer Capacitors: The Pivotal Interplays between Ions and Solvents journal September 2017
Enhancement of quantum capacitance by chemical modification of graphene supercapacitor electrodes: a study by first principles journal September 2019
Trade-off between quantum capacitance and thermodynamic stability of defected graphene: an implication for supercapacitor electrodes journal March 2018
Nano-Architecture of nitrogen-doped graphene films synthesized from a solid CN source journal February 2018
Pyridinic-nitrogen highly doped nanotubular carbon arrays grown on a carbon cloth for high-performance and flexible supercapacitors journal January 2018
Adsorption of metal atoms on silicene: stability and quantum capacitance of silicene-based electrode materials journal January 2019
One-step synthesis of nitrogen-doped wood derived carbons as advanced electrodes for supercapacitor applications journal January 2019
Investigating the asymmetry in the EDL response of C 60 /graphene supercapacitors journal January 2019
Exploring doped or vacancy-modified graphene-based electrodes for applications in asymmetric supercapacitors journal January 2020
A nitrogen and phosphorus enriched pyridine bridged inorganic–organic hybrid material for supercapacitor application journal January 2019
Tuning the nanostructure of nitrogen-doped graphene laminates for forward osmosis desalination journal January 2019
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
A comparative study of room temperature ionic liquids and their organic solvent mixtures near charged electrodes journal September 2016
Route to achieving enhanced quantum capacitance in functionalized graphene based supercapacitor electrodes journal August 2019
One step hydrothermal synthesis of 3D CoS 2 @MoS 2 -NG for high performance supercapacitors journal May 2018
Theoretical Study on the Quantum Capacitance Origin of Graphene Cathodes in Lithium Ion Capacitors journal October 2018

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