Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots

Gu, Siyong; Hsieh, Chien-Te; Ashraf Gandomi, Yasser; Chang, Jeng-Kuei; Li, Ju; Li, Jianlin; Zhang, Houan; Guo, Qing; Lau, Kah Chun; Pandey, Ravindra

doi:10.1039/C9TC00233B

Title: Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots

Journal Article · Tue Jan 01 00:00:00 EST 2019 · Journal of Materials Chemistry C

DOI:https://doi.org/10.1039/C9TC00233B· OSTI ID:1515647

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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)

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.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1515647

Journal Information:: Journal of Materials Chemistry C, Vol. 7, Issue 18; ISSN 2050-7526

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 53 works

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