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

Gu, Siyong; Hsieh, Chien -Te; Gandomi, Yasser Ashraf; Li, Jianlin; Yue, Xing Xing; Chang, Jeng -Kuei

doi:10.1039/C9NR05422G

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

Journal Article · Fri Aug 16 00:00:00 EDT 2019 · Nanoscale

DOI:https://doi.org/10.1039/C9NR05422G· OSTI ID:1558496

Gu, Siyong ^[1]; Hsieh, Chien -Te ^[2]; Gandomi, Yasser Ashraf ^[3];

^[4]; Yue, Xing Xing ^[5]; Chang, Jeng -Kuei ^[6]

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)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Nanjing Univ. of Science and Technology, Nanjing (China)
National Chiao Tung Univ., Hsinchu (Taiwan)

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

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:: 1558496

Journal Information:: Nanoscale, Vol. 11, Issue 35; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 36 works

Citation information provided by
Web of Science

References (59)

Practical access to bandgap-like N-doped carbon dots with dual emission unzipped from PAN@PMMA core–shell nanoparticles Wang, Youfu; Dong, Luhua; Xiong, Rulin Journal of Materials Chemistry C, Vol. 1, Issue 46 https://doi.org/10.1039/c3tc30949e	journal	January 2013
Facile Synthetic Method for Pristine Graphene Quantum Dots and Graphene Oxide Quantum Dots: Origin of Blue and Green Luminescence Liu, Fei; Jang, Min-Ho; Ha, Hyun Dong Advanced Materials, Vol. 25, Issue 27 https://doi.org/10.1002/adma.201300233	journal	May 2013
Liquid Type Nontoxic Photoluminescent Nanomaterials for High Color Quality White-Light-Emitting Diode Lin, Chih-Hao; Pai, Yung-Min; Lee, Chun-Fu Nanoscale Research Letters, Vol. 13, Issue 1 https://doi.org/10.1186/s11671-018-2835-4	journal	December 2018
Carbon quantum dots: synthesis, properties and applications Wang, Youfu; Hu, Aiguo Journal of Materials Chemistry C, Vol. 2, Issue 34 https://doi.org/10.1039/C4TC00988F	journal	January 2014
A green heterogeneous synthesis of N-doped carbon dots and their photoluminescence applications in solid and aqueous states Xu, Minghan; He, Guili; Li, Zhaohui Nanoscale, Vol. 6, Issue 17 https://doi.org/10.1039/C4NR02792B	journal	January 2014
Enhanced photoelectrochemical performance of quantum dot-sensitized TiO ₂ nanotube arrays with Al ₂ O ₃ overcoating by atomic layer deposition Zeng, Min; Peng, Xiange; Liao, Jianjun Physical Chemistry Chemical Physics, Vol. 18, Issue 26 https://doi.org/10.1039/C6CP01299J	journal	January 2016
Controlled Formation of Sharp Zigzag and Armchair Edges in Graphitic Nanoribbons Jia, X.; Hofmann, M.; Meunier, V. Science, Vol. 323, Issue 5922 https://doi.org/10.1126/science.1166862	journal	March 2009
Blue Photoluminescence from Chemically Derived Graphene Oxide Eda, Goki; Lin, Yun-Yue; Mattevi, Cecilia Advanced Materials, Vol. 22, Issue 4, p. 505-509 https://doi.org/10.1002/adma.200901996	journal	January 2010
Formation Mechanism of Carbogenic Nanoparticles with Dual Photoluminescence Emission Krysmann, Marta J.; Kelarakis, Antonios; Dallas, Panagiotis Journal of the American Chemical Society, Vol. 134, Issue 2 https://doi.org/10.1021/ja204661r	journal	December 2011
Amino-functionalized graphene quantum dots: origin of tunable heterogeneous photoluminescence Sandeep Kumar, G.; Roy, Rajarshi; Sen, Dipayan Nanoscale, Vol. 6, Issue 6 https://doi.org/10.1039/c3nr05376h	journal	January 2014
Anomalous Behaviors of Visible Luminescence from Graphene Quantum Dots: Interplay between Size and Shape Kim, Sung; Hwang, Sung Won; Kim, Min-Kook ACS Nano, Vol. 6, Issue 9 https://doi.org/10.1021/nn302878r	journal	August 2012
Greenlighting Photoelectrochemical Oxidation of Water by Iron Oxide Kim, Dong Wook; Riha, Shannon C.; DeMarco, Erica J. ACS Nano, Vol. 8, Issue 12 https://doi.org/10.1021/nn503869n	journal	November 2014
Carbon Nanoparticle-based Fluorescent Bioimaging Probes Bhunia, Susanta Kumar; Saha, Arindam; Maity, Amit Ranjan Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep01473	journal	March 2013
Tailoring color emissions from N-doped graphene quantum dots for bioimaging applications Qu, Dan; Zheng, Min; Li, Jing Light: Science & Applications, Vol. 4, Issue 12 https://doi.org/10.1038/lsa.2015.137	journal	December 2015
Highly efficient photoluminescent graphene oxide with tunable surface properties Mei, Qingsong; Zhang, Kui; Guan, Guijian Chemical Communications, Vol. 46, Issue 39 https://doi.org/10.1039/c0cc02374d	journal	January 2010
A low-temperature solid-phase method to synthesize highly fluorescent carbon nitride dots with tunable emission Zhou, Juan; Yang, Yong; Zhang, Chun-yang Chemical Communications, Vol. 49, Issue 77 https://doi.org/10.1039/c3cc42266f	journal	January 2013
Graphene quantum dots and their possible energy applications: A review Bak, Sora; Kim, Doyoung; Lee, Hyoyoung Current Applied Physics, Vol. 16, Issue 9 https://doi.org/10.1016/j.cap.2016.03.026	journal	September 2016
Recent advances in graphene quantum dots for sensing Sun, Hanjun; Wu, Li; Wei, Weili Materials Today, Vol. 16, Issue 11 https://doi.org/10.1016/j.mattod.2013.10.020	journal	November 2013
Synthesis of graphene quantum dot/metal–organic framework nanocomposites as yellow phosphors for white light-emitting diodes Pan, Dengyu; Wang, Lijun; Li, Zhen New Journal of Chemistry, Vol. 42, Issue 7 https://doi.org/10.1039/C7NJ04909A	journal	January 2018
Facile One-Pot Synthesis of Nanoporous Carbon Nitride Solids by Using Soft Templates Wang, Yong; Wang, Xinchen; Antonietti, Markus ChemSusChem, Vol. 3, Issue 4 https://doi.org/10.1002/cssc.200900284	journal	April 2010
Recent Advances of Graphitic Carbon Nitride-Based Structures and Applications in Catalyst, Sensing, Imaging, and LEDs Wang, Aiwu; Wang, Chundong; Fu, Li Nano-Micro Letters, Vol. 9, Issue 4 https://doi.org/10.1007/s40820-017-0148-2	journal	June 2017
Carbon Dots for Optical Imaging in Vivo Yang, Sheng-Tao; Cao, Li; Luo, Pengju G. Journal of the American Chemical Society, Vol. 131, Issue 32 https://doi.org/10.1021/ja904843x	journal	August 2009
Highly luminescent S, N co-doped graphene quantum dots with broad visible absorption bands for visible light photocatalysts Qu, Dan; Zheng, Min; Du, Peng Nanoscale, Vol. 5, Issue 24 https://doi.org/10.1039/c3nr04402e	journal	January 2013
Tailoring the bandgap of N-rich graphitic carbon nitride for enhanced photocatalytic activity Dillip, G. R.; Sreekanth, T. V. M.; Joo, S. W. Ceramics International, Vol. 43, Issue 8 https://doi.org/10.1016/j.ceramint.2017.02.057	journal	June 2017
Size-Dependent Evolution of Graphene Nanopores Under Thermal Excitation Xu, Tao; Yin, Kuibo; Xie, Xiao Small, Vol. 8, Issue 22 https://doi.org/10.1002/smll.201200979	journal	August 2012
Large-Scale Growth and Characterizations of Nitrogen-Doped Monolayer Graphene Sheets Jin, Zhong; Yao, Jun; Kittrell, Carter ACS Nano, Vol. 5, Issue 5 https://doi.org/10.1021/nn200766e	journal	April 2011
Photocatalytic reduction of carbon dioxide to methanol using a ruthenium trinuclear polyazine complex immobilized on graphene oxide under visible light irradiation Kumar, Pawan; Sain, Bir; Jain, Suman L. Journal of Materials Chemistry A, Vol. 2, Issue 29 https://doi.org/10.1039/c4ta01494d	journal	January 2014
Layer-by-layer assembly of nitrogen-doped graphene quantum dots monolayer decorated one-dimensional semiconductor nanoarchitectures for solar-driven water splitting Zeng, Zhiping; Xiao, Fang-Xing; Gui, Xuchun Journal of Materials Chemistry A, Vol. 4, Issue 42 https://doi.org/10.1039/C6TA05469B	journal	January 2016
Efficiency Enhancement of Perovskite Solar Cells through Fast Electron Extraction: The Role of Graphene Quantum Dots Zhu, Zonglong; Ma, Jiani; Wang, Zilong Journal of the American Chemical Society, Vol. 136, Issue 10 https://doi.org/10.1021/ja4132246	journal	February 2014
Graphitic carbon nitride materials: variation of structure and morphology and their use as metal-free catalysts Thomas, Arne; Fischer, Anna; Goettmann, Frederic Journal of Materials Chemistry, Vol. 18, Issue 41 https://doi.org/10.1039/b800274f	journal	January 2008
Photo-Fenton Reaction of Graphene Oxide: A New Strategy to Prepare Graphene Quantum Dots for DNA Cleavage Zhou, Xuejiao; Zhang, Yan; Wang, Chong ACS Nano, Vol. 6, Issue 8 https://doi.org/10.1021/nn301629v	journal	July 2012
A facile microwave-assisted fabrication of fluorescent carbon nitride quantum dots and their application in the detection of mercury ions Cao, Xiaotong; Ma, Jie; Lin, Yanping Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 151 https://doi.org/10.1016/j.saa.2015.07.034	journal	December 2015
Luminescent graphene quantum dots as new fluorescent materials for environmental and biological applications Lin, Liping; Rong, Mingcong; Luo, Feng TrAC Trends in Analytical Chemistry, Vol. 54 https://doi.org/10.1016/j.trac.2013.11.001	journal	February 2014
Graphene quantum dots: an emerging material for energy-related applications and beyond Zhang, Zhipan; Zhang, Jing; Chen, Nan Energy & Environmental Science, Vol. 5, Issue 10 https://doi.org/10.1039/c2ee22982j	journal	January 2012
Elucidating Quantum Confinement in Graphene Oxide Dots Based On Excitation-Wavelength-Independent Photoluminescence Yeh, Te-Fu; Huang, Wei-Lun; Chung, Chung-Jen The Journal of Physical Chemistry Letters, Vol. 7, Issue 11 https://doi.org/10.1021/acs.jpclett.6b00752	journal	May 2016
Highly efficient carbon quantum dot suspensions and membranes for sensitive/selective detection and adsorption/recovery of mercury ions from aqueous solutions Fu, Chun-Chieh; Hsieh, Chien-Te; Juang, Ruey-Shin Journal of the Taiwan Institute of Chemical Engineers, Vol. 100 https://doi.org/10.1016/j.jtice.2019.04.012	journal	July 2019
Selective band gap manipulation of graphene oxide by its reduction with mild reagents Velasco-Soto, M. A.; Pérez-García, S. A.; Alvarez-Quintana, J. Carbon, Vol. 93 https://doi.org/10.1016/j.carbon.2015.06.013	journal	November 2015
Graphene Quantum Dots Coated VO ₂ Arrays for Highly Durable Electrodes for Li and Na Ion Batteries Chao, Dongliang; Zhu, Changrong; Xia, Xinhui Nano Letters, Vol. 15, Issue 1 https://doi.org/10.1021/nl504038s	journal	December 2014
Deep Ultraviolet to Near-Infrared Emission and Photoresponse in Layered N-Doped Graphene Quantum Dots Tang, Libin; Ji, Rongbin; Li, Xueming ACS Nano, Vol. 8, Issue 6 https://doi.org/10.1021/nn501796r	journal	May 2014
Nitrogen-Doped Carbon Dots: A Facile and General Preparation Method, Photoluminescence Investigation, and Imaging Applications Xu, Yang; Wu, Ming; Liu, Yang Chemistry - A European Journal, Vol. 19, Issue 7 https://doi.org/10.1002/chem.201203641	journal	January 2013
Microwave growth and tunable photoluminescence of nitrogen-doped graphene and carbon nitride quantum dots Gu, Siyong; Hsieh, Chien-Te; Ashraf Gandomi, Yasser Journal of Materials Chemistry C, Vol. 7, Issue 18 https://doi.org/10.1039/C9TC00233B	journal	January 2019
Catalyst-Free Growth of Three-Dimensional Graphene Flakes and Graphene/g-C ₃ N ₄ Composite for Hydrocarbon Oxidation Chen, Ke; Chai, Zhigang; Li, Cong ACS Nano, Vol. 10, Issue 3 https://doi.org/10.1021/acsnano.6b00113	journal	February 2016
Nitrogen-Doped ZnO Nanowire Arrays for Photoelectrochemical Water Splitting Yang, Xunyu; Wolcott, Abraham; Wang, Gongming Nano Letters, Vol. 9, Issue 6 https://doi.org/10.1021/nl900772q	journal	June 2009
Silver nanorods attached to graphene sheets as anode materials for lithium-ion batteries Hsieh, Chien-Te; Lin, Chi-Yuan; Chen, Yu-Fu Carbon, Vol. 62 https://doi.org/10.1016/j.carbon.2013.06.002	journal	October 2013
Significantly enhanced electrochemical performance of lithium titanate anode for lithium ion battery by the hybrid of nitrogen and sulfur co-doped graphene quantum dots Ruiyi, Li; Yuanyuan, Jiang; Xiaoyan, Zhou Electrochimica Acta, Vol. 178 https://doi.org/10.1016/j.electacta.2015.08.018	journal	October 2015
Synthesis and characterization of nitrogen-rich carbon nitride nanobelts by pyrolysis of melamine Yang, Jinghai; Wu, Xingtong; Li, Xuefei Applied Physics A, Vol. 105, Issue 1 https://doi.org/10.1007/s00339-011-6471-4	journal	May 2011
Facile bulk production of highly blue fluorescent graphitic carbon nitride quantum dots and their application as highly selective and sensitive sensors for the detection of mercuric and iodide ions in aqueous media Barman, Sudip; Sadhukhan, Mriganka Journal of Materials Chemistry, Vol. 22, Issue 41 https://doi.org/10.1039/c2jm35501a	journal	January 2012
Versatile Graphene Quantum Dots with Tunable Nitrogen Doping Dai, Yunqian; Long, Huan; Wang, Xiaotian Particle & Particle Systems Characterization, Vol. 31, Issue 5 https://doi.org/10.1002/ppsc.201300268	journal	December 2013
Carbon quantum dots/TiO2 composites for efficient photocatalytic hydrogen evolution Yu, Huijun; Zhao, Yufei; Zhou, Chao Journal of Materials Chemistry A, Vol. 2, Issue 10 https://doi.org/10.1039/c3ta14108j	journal	January 2014
Surface Chemistry Routes to Modulate the Photoluminescence of Graphene Quantum Dots: From Fluorescence Mechanism to Up-Conversion Bioimaging Applications Zhu, Shoujun; Zhang, Junhu; Tang, Shijia Advanced Functional Materials, Vol. 22, Issue 22 https://doi.org/10.1002/adfm.201201499	journal	July 2012
Graphene quantum dots: emergent nanolights for bioimaging, sensors, catalysis and photovoltaic devices Shen, Jianhua; Zhu, Yihua; Yang, Xiaoling Chemical Communications, Vol. 48, Issue 31 https://doi.org/10.1039/c2cc00110a	journal	January 2012
Yellow fluorescent graphene quantum dots as a phosphor for white tunable light-emitting diodes Yin, Luqiao; Zhou, Jipeng; Li, Weitao RSC Advances, Vol. 9, Issue 16 https://doi.org/10.1039/C8RA10353D	journal	January 2019
Optical fiber sensor for Hg(II) based on carbon dots Gonçalves, Helena M. R.; Duarte, Abel J.; Esteves da Silva, Joaquim C. G. Biosensors and Bioelectronics, Vol. 26, Issue 4 https://doi.org/10.1016/j.bios.2010.07.018	journal	December 2010
Graphene Quantum Dots Derived from Carbon Fibers Peng, Juan; Gao, Wei; Gupta, Bipin Kumar Nano Letters, Vol. 12, Issue 2 https://doi.org/10.1021/nl2038979	journal	January 2012
Electrophoretic fabrication of highly robust, efficient, and benign heterojunction photoelectrocatalysts based on graphene-quantum-dot sensitized TiO2 nanotube arrays Pan, Dengyu; Xi, Chen; Li, Zhen Journal of Materials Chemistry A, Vol. 1, Issue 11 https://doi.org/10.1039/c3ta00059a	journal	January 2013
Tailoring the Electronic Properties of Graphene Quantum Dots by P Doping and Their Enhanced Performance in Metal-Free Composite Photocatalyst Qian, Jiajia; Shen, Chao; Yan, Jing The Journal of Physical Chemistry C, Vol. 122, Issue 1 https://doi.org/10.1021/acs.jpcc.7b08702	journal	December 2017
Focusing on luminescent graphene quantum dots: current status and future perspectives Li, Lingling; Wu, Gehui; Yang, Guohai Nanoscale, Vol. 5, Issue 10 https://doi.org/10.1039/c3nr33849e	journal	January 2013
Principles of fluorescence spectroscopy Ricchelli, Fernanda Journal of Photochemistry and Photobiology B: Biology, Vol. 3, Issue 2 https://doi.org/10.1016/1011-1344(89)80070-3	journal	April 1989
Blue photoluminescence from chemically derived graphene oxide Eda, Goki; Lin, Yun-Yue; Mattevi, Cecilia arXiv https://doi.org/10.48550/arxiv.0909.2456	preprint	January 2009

Similar Records

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 · OSTI ID:1558496

Gu, Siyong; Hsieh, Chien-Te; Ashraf Gandomi, Yasser; +7 more

Luminescent carbon quantum dots with high quantum yield as a single white converter for white light emitting diodes

Journal Article · Mon Nov 23 00:00:00 EST 2015 · Applied Physics Letters · OSTI ID:1558496

Feng, X. T.; Zhang, Y.; Zhang, F.; +1 more

Monolithic phosphor-free InGaN/GaN quantum dot wavelength converter white light emitting diodes

Journal Article · Mon Sep 15 00:00:00 EDT 2014 · Applied Physics Letters · OSTI ID:1558496

Jahangir, Shafat; Bhattacharya, Pallab; Pietzonka, Ines; +1 more

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY

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

Citation Formats

References (59)

Similar Records

Related Subjects