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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. https://doi.org/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 = {2019},
month = {8}
}

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