Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots
Abstract
Tunable photoluminescent nitrogen-doped graphene and graphitic carbon nitride (g-C3N4) quantum dots are synthesized via a facile solid-phase microwave-assisted (SPMA) technique utilizing the pyrolysis of citric acid and urea precursors. The atomic ratio, surface functionalization, and atomic structure of as-prepared quantum dots strongly depend on the ratio of citric acid to urea. The quantum dots have a homogeneous particle size and tend to form a circle and/or ellipse shape to minimize the edge free energy. The atomic ratio of surface nitrogen to carbon (N/C) in the quantum dots can reach as high as 1.74, among the highest values reported in the literature. The SPMA technique is capable of producing high-quality quantum dots with photoluminescence (PL) emission at various wavelengths on a pilot scale. The atomic structures of the N-doped graphene and g-C3N4 quantum dots are investigated using molecular dynamics simulations. Increasing the urea concentration increases the tendency of in-plane N (i.e., quaternary N) substitution over that of other amino functionalizations, such as pyrrolic and pyridinic N. The PL emission can be precisely tuned via a one-step SPMA method by adjusting the precursor composition. A high quantum yield of 38.7% is achieved with N-doped graphene quantum dots, indicating the substantial influence ofmore »
- Authors:
-
[1];
[2];
[3];
[4];
[5];
[6];
[7];
[9]
- Xiamen Univ. of Technology, Xiamen (China)
- Yuan Ze Univ., Taoyuan (Taiwan); Univ. of Tennessee, Knoxville, TN (United States)
- Univ. of Tennessee, Knoxville, TN (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); National Chiao Tung Univ., Hsinchu (Taiwan)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Michigan Technological Univ., Houghton, MI (United States); California State Univ., Northridge (United States)
- California State Univ., Northridge (United States)
- Michigan Technological Univ., Houghton, MI (United States)
- 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:
- 1515647
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry C
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 18; Journal ID: ISSN 2050-7526
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Gu, Siyong, Hsieh, Chien-Te, Ashraf Gandomi, Yasser, Chang, Jeng-Kuei, Li, Ju, Li, Jianlin, Zhang, Houan, Guo, Qing, Lau, Kah Chun, and Pandey, Ravindra. Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots. United States: N. p., 2019.
Web. doi:10.1039/C9TC00233B.
Gu, Siyong, Hsieh, Chien-Te, Ashraf Gandomi, Yasser, Chang, Jeng-Kuei, Li, Ju, Li, Jianlin, Zhang, Houan, Guo, Qing, Lau, Kah Chun, & Pandey, Ravindra. Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots. United States. https://doi.org/10.1039/C9TC00233B
Gu, Siyong, Hsieh, Chien-Te, Ashraf Gandomi, Yasser, Chang, Jeng-Kuei, Li, Ju, Li, Jianlin, Zhang, Houan, Guo, Qing, Lau, Kah Chun, and Pandey, Ravindra. Tue .
"Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots". United States. https://doi.org/10.1039/C9TC00233B. https://www.osti.gov/servlets/purl/1515647.
@article{osti_1515647,
title = {Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots},
author = {Gu, Siyong and Hsieh, Chien-Te and Ashraf Gandomi, Yasser and Chang, Jeng-Kuei and Li, Ju and Li, Jianlin and Zhang, Houan and Guo, Qing and Lau, Kah Chun and Pandey, Ravindra},
abstractNote = {Tunable photoluminescent nitrogen-doped graphene and graphitic carbon nitride (g-C3N4) quantum dots are synthesized via a facile solid-phase microwave-assisted (SPMA) technique utilizing the pyrolysis of citric acid and urea precursors. The atomic ratio, surface functionalization, and atomic structure of as-prepared quantum dots strongly depend on the ratio of citric acid to urea. The quantum dots have a homogeneous particle size and tend to form a circle and/or ellipse shape to minimize the edge free energy. The atomic ratio of surface nitrogen to carbon (N/C) in the quantum dots can reach as high as 1.74, among the highest values reported in the literature. The SPMA technique is capable of producing high-quality quantum dots with photoluminescence (PL) emission at various wavelengths on a pilot scale. The atomic structures of the N-doped graphene and g-C3N4 quantum dots are investigated using molecular dynamics simulations. Increasing the urea concentration increases the tendency of in-plane N (i.e., quaternary N) substitution over that of other amino functionalizations, such as pyrrolic and pyridinic N. The PL emission can be precisely tuned via a one-step SPMA method by adjusting the precursor composition. A high quantum yield of 38.7% is achieved with N-doped graphene quantum dots, indicating the substantial influence of the N- and O-rich edge groups on the enhancement of PL efficiency. A bandgap structure is introduced to describe the interstate (π*–π) transition of quantum dots. This work presents a novel approach for engineering the chemical composition and atomic structure of graphene and g-C3N4 quantum dots, facilitating their research and applications in optical, electronic, and biomedical devices.},
doi = {10.1039/C9TC00233B},
journal = {Journal of Materials Chemistry C},
number = 18,
volume = 7,
place = {United States},
year = {Tue Jan 01 00:00:00 EST 2019},
month = {Tue Jan 01 00:00:00 EST 2019}
}
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