skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots

Abstract

Adopting a solid-phase microwave-assisted technique followed by thermal pyrolysis of N-functionalized graphene quantum dots, novel nitrogen-doped graphite-like (NGL) electrode materials were synthesized in this work and served as the anode for Li-ion batteries. The NGL anode demonstrated reversible capacity of 530 mAh g-1 at 0.1C, superior rate capability at high C rate operation (420 mAh g-1 at 5C), remarkable initial coulombic efficiency (>95.7%), and excellent cyclic stability along with high efficiency (>99.1%) during entire cycling. The NGL anode nanostructure enables improved lithium ion mobility and reversible Li+ storage during cycling. The analysis of the Ragone plots revealed that the specific energy of NGL anode reaches to ca. 840 Wh kg-1 at the power density of 4200 W kg-1. The diffusion coefficient of Li ions was measured as 1.69 × 10-9 cm2 s-1 for the NGL anode material, substantially improving over commonly used graphite electrodes (15–26 times higher Li+ diffusivity). The high-rate cyclability as well as the cyclic stability of the NGL anodes were also confirmed via long-term cycling of full pouch cells assembled with ternary cathode and NGL anode. The robust design of the NGL anode materials introduced in this work, paves the way for designing next-generation lithium-ion batteries operatingmore » at ultra-high C rates.« less

Authors:
 [1];  [2]; ORCiD logo [3];  [4];  [5]; ORCiD logo [6];  [7]
  1. Xiamen Univ. of Technology (China)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Yuan Ze Univ., Taoyuan (Taiwan); Univ. of Tennessee, Knoxville, TN (United States)
  4. Yuan Ze Univ., Taoyuan (Taiwan)
  5. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  7. National Chiao Tung Univ., Hsinchu (Taiwan)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE; Taiwan Ministry of Science and Technology (MOST); Chang Gung Medical Foundation
OSTI Identifier:
1648881
Grant/Contract Number:  
AC05-00OR22725; CMRPD2E0082
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Electrochimica Acta
Additional Journal Information:
Journal Volume: 354; Journal Issue: N/A; Journal ID: ISSN 0013-4686
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Nitrogen doping; Graphite-like anodes; Lithium ion battery; Graphene quantum dots; Rate capability

Citation Formats

Gu, Siyong, Christensen, Tommiejean, Hsieh, Chien-Te, Mallick, Bikash Chandra, Gandomi, Yasser Ashraf, Li, Jianlin, and Chang, Jeng-Kuei. Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots. United States: N. p., 2020. Web. doi:10.1016/j.electacta.2020.136642.
Gu, Siyong, Christensen, Tommiejean, Hsieh, Chien-Te, Mallick, Bikash Chandra, Gandomi, Yasser Ashraf, Li, Jianlin, & Chang, Jeng-Kuei. Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots. United States. https://doi.org/10.1016/j.electacta.2020.136642
Gu, Siyong, Christensen, Tommiejean, Hsieh, Chien-Te, Mallick, Bikash Chandra, Gandomi, Yasser Ashraf, Li, Jianlin, and Chang, Jeng-Kuei. 2020. "Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots". United States. https://doi.org/10.1016/j.electacta.2020.136642. https://www.osti.gov/servlets/purl/1648881.
@article{osti_1648881,
title = {Improved lithium storage capacity and high rate capability of nitrogen-doped graphite-like electrode materials prepared from thermal pyrolysis of graphene quantum dots},
author = {Gu, Siyong and Christensen, Tommiejean and Hsieh, Chien-Te and Mallick, Bikash Chandra and Gandomi, Yasser Ashraf and Li, Jianlin and Chang, Jeng-Kuei},
abstractNote = {Adopting a solid-phase microwave-assisted technique followed by thermal pyrolysis of N-functionalized graphene quantum dots, novel nitrogen-doped graphite-like (NGL) electrode materials were synthesized in this work and served as the anode for Li-ion batteries. The NGL anode demonstrated reversible capacity of 530 mAh g-1 at 0.1C, superior rate capability at high C rate operation (420 mAh g-1 at 5C), remarkable initial coulombic efficiency (>95.7%), and excellent cyclic stability along with high efficiency (>99.1%) during entire cycling. The NGL anode nanostructure enables improved lithium ion mobility and reversible Li+ storage during cycling. The analysis of the Ragone plots revealed that the specific energy of NGL anode reaches to ca. 840 Wh kg-1 at the power density of 4200 W kg-1. The diffusion coefficient of Li ions was measured as 1.69 × 10-9 cm2 s-1 for the NGL anode material, substantially improving over commonly used graphite electrodes (15–26 times higher Li+ diffusivity). The high-rate cyclability as well as the cyclic stability of the NGL anodes were also confirmed via long-term cycling of full pouch cells assembled with ternary cathode and NGL anode. The robust design of the NGL anode materials introduced in this work, paves the way for designing next-generation lithium-ion batteries operating at ultra-high C rates.},
doi = {10.1016/j.electacta.2020.136642},
url = {https://www.osti.gov/biblio/1648881}, journal = {Electrochimica Acta},
issn = {0013-4686},
number = N/A,
volume = 354,
place = {United States},
year = {Mon Jun 22 00:00:00 EDT 2020},
month = {Mon Jun 22 00:00:00 EDT 2020}
}

Works referenced in this record:

Materials processing for lithium-ion batteries
journal, March 2011


Issues and challenges facing rechargeable lithium batteries
journal, November 2001


Effect of High Voltage on the Structure and Electrochemistry of LiNi 0.5 Mn 0.5 O 2 :  A Joint Experimental and Theoretical Study
journal, October 2006


Electrospun SnO2 and TiO2 Composite Nanofibers for Lithium Ion Batteries
journal, January 2014


Pulse Microwave Deposition of Cobalt Oxide Nanoparticles on Graphene Nanosheets as Anode Materials for Lithium Ion Batteries
journal, July 2012


Synthesis of ZnO@Graphene composites as anode materials for lithium ion batteries
journal, November 2013


Silicon@graphene composite prepared by spray–drying method as anode for lithium ion batteries
journal, July 2019


Pitch carbon and LiF co-modified Si-based anode material for lithium ion batteries
journal, August 2017


Improved storage capacity and rate capability of Fe3O4–graphene anodes for lithium-ion batteries
journal, December 2011


Folded Structured Graphene Paper for High Performance Electrode Materials
journal, January 2012


Graphene nanosheets for enhanced lithium storage in lithium ion batteries
journal, July 2009


Electrochemical performance of graphene nanosheets as anode material for lithium-ion batteries
journal, June 2009


Electrochemical storage of energy in carbon nanotubes and nanostructured carbons
journal, August 2002


A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries
journal, September 2010


Versatile Graphene Quantum Dots with Tunable Nitrogen Doping
journal, December 2013


Large-Scale Growth and Characterizations of Nitrogen-Doped Monolayer Graphene Sheets
journal, April 2011


3D nitrogen-doped carbon supported non-precious metals electrocatalyst for oxygen reduction reaction
journal, April 2020


Pure nitrogen-doped graphene aerogel with rich micropores yields high ORR performance
journal, March 2019


Full-faradaic-active nitrogen species doping enables high-energy-density carbon-based supercapacitor
journal, September 2020


Electro-spun graphene-enriched carbon fibres with high nitrogen-contents for electrochemical water desalination
journal, February 2018


Nitrogen-doped mesoporous carbon as an anode material for high performance potassium-ion batteries
journal, April 2020


Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots
journal, January 2019


Superior Cathode Performance of Nitrogen-Doped Graphene Frameworks for Lithium Ion Batteries
journal, March 2017


Synergistic effect of S,N-co-doped mesoporous carbon materials with high performance for oxygen-reduction reaction and Li-ion batteries
journal, January 2015


Toward N-Doped Graphene via Solvothermal Synthesis
journal, March 2011


Edge-functionalized and substitutionally doped graphene nanoribbons: Electronic and spin properties
journal, April 2008


Fabrication of well-aligned carbon nanofiber array and its gaseous-phase adsorption behavior
journal, February 2004


A simple drain current model for Schottky-barrier carbon nanotube field effect transistors
journal, September 2007


Synthesis of carbon nanotubes over Ni- and Co-supported CaCO3 catalysts using catalytic chemical vapor deposition
journal, April 2009


Bottom-up synthesis of nitrogen-doped graphene sheets for ultrafast lithium storage
journal, January 2014


Improved Graphite Anode for Lithium-Ion Batteries Chemically
journal, January 1996


Nitrogen doping and chirality of carbon nanotubes
journal, December 2004


Electronic Transport and Mechanical Properties of Phosphorus- and Phosphorus−Nitrogen-Doped Carbon Nanotubes
journal, June 2009


Nitrogen-Doped Graphene: Efficient Growth, Structure, and Electronic Properties
journal, December 2011


Large reversible capacity of high quality graphene sheets as an anode material for lithium-ion batteries
journal, April 2010


Nitrogen-doped porous hard carbons derived from shaddock peel for high-capacity lithium-ion battery anodes
journal, April 2020


Sulfur and Nitrogen Dual-Doped Mesoporous Graphene Electrocatalyst for Oxygen Reduction with Synergistically Enhanced Performance
journal, October 2012


Nitrogen-doped graphene nanosheets as anode materials for lithium ion batteries: a first-principles study
journal, January 2012


High lithium anodic performance of highly nitrogen-doped porous carbon prepared from a metal-organic framework
journal, November 2014


Nitrogen-Doped Multiwall Carbon Nanotubes for Lithium Storage with Extremely High Capacity
journal, April 2012


Long-term cyclability of LiFePO4/carbon composite cathode material for lithium-ion battery applications
journal, October 2009


Effects of TiO2 coating on high-temperature cycle performance of LiFePO4-based lithium-ion batteries
journal, October 2008


Electrochemical performance of lithium iron phosphate cathodes at various temperatures
journal, January 2014


Lithium Intercalation into Mechanically Milled Natural Graphite: Electrochemical and Kinetic Characterization
journal, January 2002


Pulse Laser Deposition and Electrochemical Characterization of LiFePO 4 −C Composite Thin Films
journal, May 2008


An Electrochemical Impedance Spectroscopic Study of the Electronic and Ionic Transport Properties of Spinel LiMn 2 O 4
journal, April 2010


Intercalation Mechanism of Lithium Ions into Graphite Layers Studied by Nuclear Magnetic Resonance and Impedance Experiments
journal, January 2001


Charge/discharge cycling behavior of pitch-based carbon fiber in organic electrolyte solutions
journal, September 1993


Li diffusion through doped and defected graphene
journal, January 2013