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Title: Tailoring Fluorescence Emissions, Quantum Yields, and White Light Emitting from Nitrogen-doped Graphene and Carbon Nitride Quantum Dots

Abstract

Highly fluorescent N-doped graphene quantum dots (NGQDs) and graphitic carbon nitride quantum dots (CNQDs, g-C3N4) were synthesized using a solid-phase microwave-assisted (SPMA) technique. The SPMA method, based on the pyrolysis of citric acid and urea with different recipes, is capable of producing quantum dots with coexisting NGQDs and CNQDs at 280°C within only five minutes. The photoluminescence (PL) emissions from NGQD and CNQDs are strongly dependent on excitation wavelength and the solvent type, i.e., water, ethanol, and N-methyl pyrrolidinone. The unique design of the quantum dots possesses a multiple chromophoric band-gap structure, originated from the presence of g-C3N4, defect-related emissive traps, and grain boundaries. Thus, an appropriate excitation wavelength induces a conjugated π electron system to fulfill the most probable absorption band, resulting in wavelength-dependent emissions including ultraviolet, visible and infrared light. Here, the quantum yield of the NGQD and CNQD samples can attain as high as 68.1%. Accordingly, one light-emitting device using the combination of the NGQD and CNQD powders embedded polymeric film can emit white-like light with high power conversion efficiency.

Authors:
 [1];  [2];  [3]; ORCiD logo [4];  [5];  [6]
  1. Xiamen Univ. of Technology, Xiamen (China)
  2. Yuan Ze Univ., Taoyuan (Taiwan); Univ. of Tennessee, Knoxville, TN (United States)
  3. Univ. of Tennessee, Knoxville, TN (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Nanjing Univ. of Science and Technology, Nanjing (China)
  6. National Chiao Tung Univ., Hsinchu (Taiwan)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1558496
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 35; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Gu, Siyong, Hsieh, Chien -Te, Gandomi, Yasser Ashraf, Li, Jianlin, Yue, Xing Xing, and Chang, Jeng -Kuei. Tailoring Fluorescence Emissions, Quantum Yields, and White Light Emitting from Nitrogen-doped Graphene and Carbon Nitride Quantum Dots. United States: N. p., 2019. Web. doi:10.1039/C9NR05422G.
Gu, Siyong, Hsieh, Chien -Te, Gandomi, Yasser Ashraf, Li, Jianlin, Yue, Xing Xing, & Chang, Jeng -Kuei. Tailoring Fluorescence Emissions, Quantum Yields, and White Light Emitting from Nitrogen-doped Graphene and Carbon Nitride Quantum Dots. United States. https://doi.org/10.1039/C9NR05422G
Gu, Siyong, Hsieh, Chien -Te, Gandomi, Yasser Ashraf, Li, Jianlin, Yue, Xing Xing, and Chang, Jeng -Kuei. Fri . "Tailoring Fluorescence Emissions, Quantum Yields, and White Light Emitting from Nitrogen-doped Graphene and Carbon Nitride Quantum Dots". United States. https://doi.org/10.1039/C9NR05422G. https://www.osti.gov/servlets/purl/1558496.
@article{osti_1558496,
title = {Tailoring Fluorescence Emissions, Quantum Yields, and White Light Emitting from Nitrogen-doped Graphene and Carbon Nitride Quantum Dots},
author = {Gu, Siyong and Hsieh, Chien -Te and Gandomi, Yasser Ashraf and Li, Jianlin and Yue, Xing Xing and Chang, Jeng -Kuei},
abstractNote = {Highly fluorescent N-doped graphene quantum dots (NGQDs) and graphitic carbon nitride quantum dots (CNQDs, g-C3N4) were synthesized using a solid-phase microwave-assisted (SPMA) technique. The SPMA method, based on the pyrolysis of citric acid and urea with different recipes, is capable of producing quantum dots with coexisting NGQDs and CNQDs at 280°C within only five minutes. The photoluminescence (PL) emissions from NGQD and CNQDs are strongly dependent on excitation wavelength and the solvent type, i.e., water, ethanol, and N-methyl pyrrolidinone. The unique design of the quantum dots possesses a multiple chromophoric band-gap structure, originated from the presence of g-C3N4, defect-related emissive traps, and grain boundaries. Thus, an appropriate excitation wavelength induces a conjugated π electron system to fulfill the most probable absorption band, resulting in wavelength-dependent emissions including ultraviolet, visible and infrared light. Here, the quantum yield of the NGQD and CNQD samples can attain as high as 68.1%. Accordingly, one light-emitting device using the combination of the NGQD and CNQD powders embedded polymeric film can emit white-like light with high power conversion efficiency.},
doi = {10.1039/C9NR05422G},
journal = {Nanoscale},
number = 35,
volume = 11,
place = {United States},
year = {Fri Aug 16 00:00:00 EDT 2019},
month = {Fri Aug 16 00:00:00 EDT 2019}
}

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Works referenced in this record:

Practical access to bandgap-like N-doped carbon dots with dual emission unzipped from PAN@PMMA core–shell nanoparticles
journal, January 2013

  • Wang, Youfu; Dong, Luhua; Xiong, Rulin
  • Journal of Materials Chemistry C, Vol. 1, Issue 46
  • DOI: 10.1039/c3tc30949e

Facile Synthetic Method for Pristine Graphene Quantum Dots and Graphene Oxide Quantum Dots: Origin of Blue and Green Luminescence
journal, May 2013


Liquid Type Nontoxic Photoluminescent Nanomaterials for High Color Quality White-Light-Emitting Diode
journal, December 2018


Carbon quantum dots: synthesis, properties and applications
journal, January 2014

  • Wang, Youfu; Hu, Aiguo
  • Journal of Materials Chemistry C, Vol. 2, Issue 34
  • DOI: 10.1039/C4TC00988F

A green heterogeneous synthesis of N-doped carbon dots and their photoluminescence applications in solid and aqueous states
journal, January 2014


Enhanced photoelectrochemical performance of quantum dot-sensitized TiO 2 nanotube arrays with Al 2 O 3 overcoating by atomic layer deposition
journal, January 2016

  • Zeng, Min; Peng, Xiange; Liao, Jianjun
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 26
  • DOI: 10.1039/C6CP01299J

Controlled Formation of Sharp Zigzag and Armchair Edges in Graphitic Nanoribbons
journal, March 2009


Blue Photoluminescence from Chemically Derived Graphene Oxide
journal, January 2010

  • Eda, Goki; Lin, Yun-Yue; Mattevi, Cecilia
  • Advanced Materials, Vol. 22, Issue 4, p. 505-509
  • DOI: 10.1002/adma.200901996

Formation Mechanism of Carbogenic Nanoparticles with Dual Photoluminescence Emission
journal, December 2011

  • Krysmann, Marta J.; Kelarakis, Antonios; Dallas, Panagiotis
  • Journal of the American Chemical Society, Vol. 134, Issue 2
  • DOI: 10.1021/ja204661r

Amino-functionalized graphene quantum dots: origin of tunable heterogeneous photoluminescence
journal, January 2014

  • Sandeep Kumar, G.; Roy, Rajarshi; Sen, Dipayan
  • Nanoscale, Vol. 6, Issue 6
  • DOI: 10.1039/c3nr05376h

Anomalous Behaviors of Visible Luminescence from Graphene Quantum Dots: Interplay between Size and Shape
journal, August 2012

  • Kim, Sung; Hwang, Sung Won; Kim, Min-Kook
  • ACS Nano, Vol. 6, Issue 9
  • DOI: 10.1021/nn302878r

Greenlighting Photoelectrochemical Oxidation of Water by Iron Oxide
journal, November 2014

  • Kim, Dong Wook; Riha, Shannon C.; DeMarco, Erica J.
  • ACS Nano, Vol. 8, Issue 12
  • DOI: 10.1021/nn503869n

Carbon Nanoparticle-based Fluorescent Bioimaging Probes
journal, March 2013

  • Bhunia, Susanta Kumar; Saha, Arindam; Maity, Amit Ranjan
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep01473

Tailoring color emissions from N-doped graphene quantum dots for bioimaging applications
journal, December 2015

  • Qu, Dan; Zheng, Min; Li, Jing
  • Light: Science & Applications, Vol. 4, Issue 12
  • DOI: 10.1038/lsa.2015.137

Highly efficient photoluminescent graphene oxide with tunable surface properties
journal, January 2010

  • Mei, Qingsong; Zhang, Kui; Guan, Guijian
  • Chemical Communications, Vol. 46, Issue 39
  • DOI: 10.1039/c0cc02374d

A low-temperature solid-phase method to synthesize highly fluorescent carbon nitride dots with tunable emission
journal, January 2013

  • Zhou, Juan; Yang, Yong; Zhang, Chun-yang
  • Chemical Communications, Vol. 49, Issue 77
  • DOI: 10.1039/c3cc42266f

Graphene quantum dots and their possible energy applications: A review
journal, September 2016


Recent advances in graphene quantum dots for sensing
journal, November 2013


Synthesis of graphene quantum dot/metal–organic framework nanocomposites as yellow phosphors for white light-emitting diodes
journal, January 2018

  • Pan, Dengyu; Wang, Lijun; Li, Zhen
  • New Journal of Chemistry, Vol. 42, Issue 7
  • DOI: 10.1039/C7NJ04909A

Facile One-Pot Synthesis of Nanoporous Carbon Nitride Solids by Using Soft Templates
journal, April 2010


Recent Advances of Graphitic Carbon Nitride-Based Structures and Applications in Catalyst, Sensing, Imaging, and LEDs
journal, June 2017


Carbon Dots for Optical Imaging in Vivo
journal, August 2009

  • Yang, Sheng-Tao; Cao, Li; Luo, Pengju G.
  • Journal of the American Chemical Society, Vol. 131, Issue 32
  • DOI: 10.1021/ja904843x

Tailoring the bandgap of N-rich graphitic carbon nitride for enhanced photocatalytic activity
journal, June 2017


Size-Dependent Evolution of Graphene Nanopores Under Thermal Excitation
journal, August 2012


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

  • Jin, Zhong; Yao, Jun; Kittrell, Carter
  • ACS Nano, Vol. 5, Issue 5
  • DOI: 10.1021/nn200766e

Photocatalytic reduction of carbon dioxide to methanol using a ruthenium trinuclear polyazine complex immobilized on graphene oxide under visible light irradiation
journal, January 2014

  • Kumar, Pawan; Sain, Bir; Jain, Suman L.
  • Journal of Materials Chemistry A, Vol. 2, Issue 29
  • DOI: 10.1039/c4ta01494d

Layer-by-layer assembly of nitrogen-doped graphene quantum dots monolayer decorated one-dimensional semiconductor nanoarchitectures for solar-driven water splitting
journal, January 2016

  • Zeng, Zhiping; Xiao, Fang-Xing; Gui, Xuchun
  • Journal of Materials Chemistry A, Vol. 4, Issue 42
  • DOI: 10.1039/C6TA05469B

Efficiency Enhancement of Perovskite Solar Cells through Fast Electron Extraction: The Role of Graphene Quantum Dots
journal, February 2014

  • Zhu, Zonglong; Ma, Jiani; Wang, Zilong
  • Journal of the American Chemical Society, Vol. 136, Issue 10
  • DOI: 10.1021/ja4132246

Graphitic carbon nitride materials: variation of structure and morphology and their use as metal-free catalysts
journal, January 2008

  • Thomas, Arne; Fischer, Anna; Goettmann, Frederic
  • Journal of Materials Chemistry, Vol. 18, Issue 41
  • DOI: 10.1039/b800274f

Photo-Fenton Reaction of Graphene Oxide: A New Strategy to Prepare Graphene Quantum Dots for DNA Cleavage
journal, July 2012

  • Zhou, Xuejiao; Zhang, Yan; Wang, Chong
  • ACS Nano, Vol. 6, Issue 8
  • DOI: 10.1021/nn301629v

A facile microwave-assisted fabrication of fluorescent carbon nitride quantum dots and their application in the detection of mercury ions
journal, December 2015

  • Cao, Xiaotong; Ma, Jie; Lin, Yanping
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 151
  • DOI: 10.1016/j.saa.2015.07.034

Luminescent graphene quantum dots as new fluorescent materials for environmental and biological applications
journal, February 2014


Graphene quantum dots: an emerging material for energy-related applications and beyond
journal, January 2012

  • Zhang, Zhipan; Zhang, Jing; Chen, Nan
  • Energy & Environmental Science, Vol. 5, Issue 10
  • DOI: 10.1039/c2ee22982j

Elucidating Quantum Confinement in Graphene Oxide Dots Based On Excitation-Wavelength-Independent Photoluminescence
journal, May 2016

  • Yeh, Te-Fu; Huang, Wei-Lun; Chung, Chung-Jen
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 11
  • DOI: 10.1021/acs.jpclett.6b00752

Highly efficient carbon quantum dot suspensions and membranes for sensitive/selective detection and adsorption/recovery of mercury ions from aqueous solutions
journal, July 2019

  • Fu, Chun-Chieh; Hsieh, Chien-Te; Juang, Ruey-Shin
  • Journal of the Taiwan Institute of Chemical Engineers, Vol. 100
  • DOI: 10.1016/j.jtice.2019.04.012

Selective band gap manipulation of graphene oxide by its reduction with mild reagents
journal, November 2015


Graphene Quantum Dots Coated VO 2 Arrays for Highly Durable Electrodes for Li and Na Ion Batteries
journal, December 2014

  • Chao, Dongliang; Zhu, Changrong; Xia, Xinhui
  • Nano Letters, Vol. 15, Issue 1
  • DOI: 10.1021/nl504038s

Deep Ultraviolet to Near-Infrared Emission and Photoresponse in Layered N-Doped Graphene Quantum Dots
journal, May 2014

  • Tang, Libin; Ji, Rongbin; Li, Xueming
  • ACS Nano, Vol. 8, Issue 6
  • DOI: 10.1021/nn501796r

Nitrogen-Doped Carbon Dots: A Facile and General Preparation Method, Photoluminescence Investigation, and Imaging Applications
journal, January 2013


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

  • Gu, Siyong; Hsieh, Chien-Te; Ashraf Gandomi, Yasser
  • Journal of Materials Chemistry C, Vol. 7, Issue 18
  • DOI: 10.1039/C9TC00233B

Catalyst-Free Growth of Three-Dimensional Graphene Flakes and Graphene/g-C 3 N 4 Composite for Hydrocarbon Oxidation
journal, February 2016


Nitrogen-Doped ZnO Nanowire Arrays for Photoelectrochemical Water Splitting
journal, June 2009

  • Yang, Xunyu; Wolcott, Abraham; Wang, Gongming
  • Nano Letters, Vol. 9, Issue 6
  • DOI: 10.1021/nl900772q

Silver nanorods attached to graphene sheets as anode materials for lithium-ion batteries
journal, October 2013


Synthesis and characterization of nitrogen-rich carbon nitride nanobelts by pyrolysis of melamine
journal, May 2011


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

  • Dai, Yunqian; Long, Huan; Wang, Xiaotian
  • Particle & Particle Systems Characterization, Vol. 31, Issue 5
  • DOI: 10.1002/ppsc.201300268

Carbon quantum dots/TiO2 composites for efficient photocatalytic hydrogen evolution
journal, January 2014

  • Yu, Huijun; Zhao, Yufei; Zhou, Chao
  • Journal of Materials Chemistry A, Vol. 2, Issue 10
  • DOI: 10.1039/c3ta14108j

Surface Chemistry Routes to Modulate the Photoluminescence of Graphene Quantum Dots: From Fluorescence Mechanism to Up-Conversion Bioimaging Applications
journal, July 2012

  • Zhu, Shoujun; Zhang, Junhu; Tang, Shijia
  • Advanced Functional Materials, Vol. 22, Issue 22
  • DOI: 10.1002/adfm.201201499

Graphene quantum dots: emergent nanolights for bioimaging, sensors, catalysis and photovoltaic devices
journal, January 2012

  • Shen, Jianhua; Zhu, Yihua; Yang, Xiaoling
  • Chemical Communications, Vol. 48, Issue 31
  • DOI: 10.1039/c2cc00110a

Yellow fluorescent graphene quantum dots as a phosphor for white tunable light-emitting diodes
journal, January 2019

  • Yin, Luqiao; Zhou, Jipeng; Li, Weitao
  • RSC Advances, Vol. 9, Issue 16
  • DOI: 10.1039/C8RA10353D

Optical fiber sensor for Hg(II) based on carbon dots
journal, December 2010

  • Gonçalves, Helena M. R.; Duarte, Abel J.; Esteves da Silva, Joaquim C. G.
  • Biosensors and Bioelectronics, Vol. 26, Issue 4
  • DOI: 10.1016/j.bios.2010.07.018

Graphene Quantum Dots Derived from Carbon Fibers
journal, January 2012

  • Peng, Juan; Gao, Wei; Gupta, Bipin Kumar
  • Nano Letters, Vol. 12, Issue 2
  • DOI: 10.1021/nl2038979

Tailoring the Electronic Properties of Graphene Quantum Dots by P Doping and Their Enhanced Performance in Metal-Free Composite Photocatalyst
journal, December 2017

  • Qian, Jiajia; Shen, Chao; Yan, Jing
  • The Journal of Physical Chemistry C, Vol. 122, Issue 1
  • DOI: 10.1021/acs.jpcc.7b08702

Focusing on luminescent graphene quantum dots: current status and future perspectives
journal, January 2013

  • Li, Lingling; Wu, Gehui; Yang, Guohai
  • Nanoscale, Vol. 5, Issue 10
  • DOI: 10.1039/c3nr33849e

Principles of fluorescence spectroscopy
journal, April 1989


Blue photoluminescence from chemically derived graphene oxide
preprint, January 2009