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Title: Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization

Abstract

Abstract Multiple‐color‐emissive carbon dots (CDots) have potential applications in various fields such as bioimaging, light‐emitting devices, and photocatalysis. The majority of the current CDots to date exhibit excitation‐wavelength‐dependent emissions with their maximum emission limited at the blue‐light region. Here, a synthesis of multiple‐color‐emission CDots by controlled graphitization and surface function is reported. The CDots are synthesized through controlled thermal pyrolysis of citric acid and urea. By regulating the thermal‐pyrolysis temperature and ratio of reactants, the maximum emission of the resulting CDots gradually shifts from blue to red light, covering the entire light spectrum. Specifically, the emission position of the CDots can be tuned from 430 to 630 nm through controlling the extent of graphitization and the amount of surface functional groups, COOH. The relative photoluminescence quantum yields of the CDots with blue, green, and red emission reach up to 52.6%, 35.1%, and 12.9%, respectively. Furthermore, it is demonstrated that the CDots can be uniformly dispersed into epoxy resins and be fabricated as transparent CDots/epoxy composites for multiple‐color‐ and white‐light‐emitting devices. This research opens a door for developing low‐cost CDots as alternative phosphors for light‐emitting devices.

Authors:
 [1];  [2];  [2];  [3];  [3];  [4]; ORCiD logo [2]
  1. Beijing Univ. of Technology (China). Beijing Key Lab. for Green Catalysis and Separation. Dept. of Chemistry and Chemical Engineering. College of Environmental and Energy Engineering; Changchun Inst. of Optics, Fine Mechanics and Physics (China). State Key Lab. of Luminescence and Applications; Univ. of Chinese Academy of Sciences, Beijing (China)
  2. Beijing Univ. of Technology (China). Beijing Key Lab. for Green Catalysis and Separation. Dept. of Chemistry and Chemical Engineering. College of Environmental and Energy Engineering
  3. Beijing Univ. of Technology (China). Beijing Key Lab. for Green Catalysis and Separation. Dept. of Chemistry and Chemical Engineering. College of Environmental and Energy Engineering; Beijing Guangqumen High School (China)
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Beijing Univ. of Technology (China); Changchun Inst. of Optics, Fine Mechanics and Physics (China); University of Chinese Academy of Sciences, Beijing (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA); National Natural Science Foundation of China (NSFC); Beijing High Talent Program (China); Beijing Natural Science Foundation (China); China Postdoctoral Science Foundation; Beijing Postdoctoral Research Foundation (China); Dongguan Program for International S&T Cooperation (China)
OSTI Identifier:
1469628
Alternate Identifier(s):
OSTI ID: 1410375
Report Number(s):
SAND-2018-9737J
Journal ID: ISSN 0935-9648; 667622
Grant/Contract Number:  
NA0003525; 21671011; KZ201710005002; 2015508102006
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 1; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; carbon dots; effective conjugation length; light-emitting devices; multiple-color emission; phosphors

Citation Formats

Miao, Xiang, Qu, Dan, Yang, Dongxue, Nie, Bing, Zhao, Yikang, Fan, Hongyou, and Sun, Zaicheng. Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization. United States: N. p., 2017. Web. doi:10.1002/adma.201704740.
Miao, Xiang, Qu, Dan, Yang, Dongxue, Nie, Bing, Zhao, Yikang, Fan, Hongyou, & Sun, Zaicheng. Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization. United States. https://doi.org/10.1002/adma.201704740
Miao, Xiang, Qu, Dan, Yang, Dongxue, Nie, Bing, Zhao, Yikang, Fan, Hongyou, and Sun, Zaicheng. Mon . "Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization". United States. https://doi.org/10.1002/adma.201704740. https://www.osti.gov/servlets/purl/1469628.
@article{osti_1469628,
title = {Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization},
author = {Miao, Xiang and Qu, Dan and Yang, Dongxue and Nie, Bing and Zhao, Yikang and Fan, Hongyou and Sun, Zaicheng},
abstractNote = {Abstract Multiple‐color‐emissive carbon dots (CDots) have potential applications in various fields such as bioimaging, light‐emitting devices, and photocatalysis. The majority of the current CDots to date exhibit excitation‐wavelength‐dependent emissions with their maximum emission limited at the blue‐light region. Here, a synthesis of multiple‐color‐emission CDots by controlled graphitization and surface function is reported. The CDots are synthesized through controlled thermal pyrolysis of citric acid and urea. By regulating the thermal‐pyrolysis temperature and ratio of reactants, the maximum emission of the resulting CDots gradually shifts from blue to red light, covering the entire light spectrum. Specifically, the emission position of the CDots can be tuned from 430 to 630 nm through controlling the extent of graphitization and the amount of surface functional groups, COOH. The relative photoluminescence quantum yields of the CDots with blue, green, and red emission reach up to 52.6%, 35.1%, and 12.9%, respectively. Furthermore, it is demonstrated that the CDots can be uniformly dispersed into epoxy resins and be fabricated as transparent CDots/epoxy composites for multiple‐color‐ and white‐light‐emitting devices. This research opens a door for developing low‐cost CDots as alternative phosphors for light‐emitting devices.},
doi = {10.1002/adma.201704740},
journal = {Advanced Materials},
number = 1,
volume = 30,
place = {United States},
year = {Mon Nov 27 00:00:00 EST 2017},
month = {Mon Nov 27 00:00:00 EST 2017}
}

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Citrate-Based Fluorescent Biomaterials
journal, July 2018

  • Shan, Dingying; Hsieh, Jer-Tsong; Bai, Xiaochun
  • Advanced Healthcare Materials, Vol. 7, Issue 18
  • DOI: 10.1002/adhm.201800532

Conversion of Carbon Dots from Fluorescence to Ultralong Room-Temperature Phosphorescence by Heating for Security Applications
journal, May 2018


Recent Advances in Carbon‐Based Metal‐Free Electrocatalysts
journal, December 2018


Hot‐Tailoring of Carbon Nitride Dots with Redshifted Photoluminescence for Visual Double Text Encryption and Bioimaging
journal, June 2019

  • Yang, Mengran; Mei, Hao; Shen, Yanfei
  • Chemistry – A European Journal, Vol. 25, Issue 43
  • DOI: 10.1002/chem.201901748

N‐doped C‐dot embedded fluorescent and thermo‐responsive p(NIPAAm) microgel composites
journal, February 2019

  • Demirci, Sahin; Sahiner, Nurettin
  • Polymer Composites, Vol. 40, Issue 10
  • DOI: 10.1002/pc.25249

Synthesis and Applications of Red-Emissive Carbon Dots
journal, February 2019

  • Wang, Jianying; Zhu, Yuhua; Wang, Lei
  • The Chemical Record, Vol. 19, Issue 10
  • DOI: 10.1002/tcr.201800172

The fluorescence mechanism of carbon dots, and methods for tuning their emission color: a review
journal, July 2019


Ultra-small amorphous carbon dots: preparation, photoluminescence properties, and their application as TiO2 photosensitizers
journal, December 2018


Nitrogen-doped carbon dots derived from electrospun carbon nanofibers for Cu( ii ) ion sensing
journal, January 2019

  • Li, Yang; Liu, Zhicheng; Bai, Lu
  • New Journal of Chemistry, Vol. 43, Issue 4
  • DOI: 10.1039/c8nj06069j

Carbon dot-based white and yellow electroluminescent light emitting diodes with a record-breaking brightness
journal, January 2018

  • Xu, Jiacong; Miao, Yanqin; Zheng, Jingxia
  • Nanoscale, Vol. 10, Issue 23
  • DOI: 10.1039/c8nr01834k

Formation and origin of multicenter photoluminescence in zeolite-based carbogenic nanodots
journal, January 2018


Langmuir–Blodgett self-assembly of ultrathin graphene quantum dot films with modulated optical properties
journal, January 2018

  • Wang, Jingyun; Yan, Hao; Liu, Zhongqun
  • Nanoscale, Vol. 10, Issue 41
  • DOI: 10.1039/c8nr05159c

Influence of surface chemistry on optical, chemical and electronic properties of blue luminescent carbon dots
journal, January 2019

  • Ren, Jian; Weber, Fabian; Weigert, Florian
  • Nanoscale, Vol. 11, Issue 4
  • DOI: 10.1039/c8nr08595a

Highly photoluminescent carbon dots derived from linseed and their applications in cellular imaging and sensing
journal, January 2018

  • Song, Yang; Yan, Xu; Li, Zhaohui
  • Journal of Materials Chemistry B, Vol. 6, Issue 19
  • DOI: 10.1039/c8tb00116b

A sensitive “ON–OFF” fluorescent probe based on carbon dots for Fe 2+ detection and cell imaging
journal, January 2020

  • Wei, Shanshan; Tan, Lihong; Yin, Xiangyu
  • The Analyst, Vol. 145, Issue 6
  • DOI: 10.1039/c9an02309g

Continuous synthesis of carbon dots with full spectrum fluorescence and the mechanism of their multiple color emission
journal, January 2019


Pressure-triggered aggregation-induced emission enhancement in red emissive amorphous carbon dots
journal, January 2019

  • Wang, Qi; Zhang, Shijie; Wang, Boyang
  • Nanoscale Horizons, Vol. 4, Issue 5
  • DOI: 10.1039/c9nh00287a

Synthesis of dual-emission fluorescent carbon quantum dots and their ratiometric fluorescence detection for arginine in 100% water solution
journal, January 2019

  • Wang, Yuying; Liu, Hanxiao; Song, Huanhuan
  • New Journal of Chemistry, Vol. 43, Issue 33
  • DOI: 10.1039/c9nj02806d

The formation mechanism and fluorophores of carbon dots synthesized via a bottom-up route
journal, January 2020

  • Qu, Dan; Sun, Zaicheng
  • Materials Chemistry Frontiers, Vol. 4, Issue 2
  • DOI: 10.1039/c9qm00552h

Full color carbon dots through surface engineering for constructing white light-emitting diodes
journal, January 2019

  • Cai, Wei; Zhang, Ting; Xu, Meng
  • Journal of Materials Chemistry C, Vol. 7, Issue 8
  • DOI: 10.1039/c9tc00274j

Luminescence modulation of carbon dots assemblies
journal, January 2019

  • Liu, Yun; Zhang, Zhi-ying; Nie, Shi-dong
  • Journal of Materials Chemistry C, Vol. 7, Issue 21
  • DOI: 10.1039/c9tc01792e

Solvent-controlled and solvent-dependent strategies for the synthesis of multicolor carbon dots for pH sensing and cell imaging
journal, January 2019

  • Bai, Jianliang; Ma, Yusha; Yuan, Guojun
  • Journal of Materials Chemistry C, Vol. 7, Issue 31
  • DOI: 10.1039/c9tc02422k

Cobalt–carbon/silica nanocomposites prepared by pyrolysis of a cobalt 2,2′-bipyridine terephthalate complex for remediation of cationic dyes
journal, January 2020

  • Alotaibi, Nusaybah; Hammud, Hassan H.; Karnati, Ranjith Kumar
  • RSC Advances, Vol. 10, Issue 30
  • DOI: 10.1039/d0ra02752a

Small molecules derived carbon dots: synthesis and applications in sensing, catalysis, imaging, and biomedicine
journal, August 2019


Self-Protective Room-Temperature Phosphorescence of Fluorine and Nitrogen Codoped Carbon Dots
journal, July 2018

  • Long, Peng; Feng, Yiyu; Cao, Chen
  • Advanced Functional Materials, Vol. 28, Issue 37
  • DOI: 10.1002/adfm.201800791

Carbon Dots with Dual‐Emissive, Robust, and Aggregation‐Induced Room‐Temperature Phosphorescence Characteristics
journal, December 2019


Sustainable Synthesis of Bright Green Fluorescent Nitrogen‐Doped Carbon Quantum Dots from Alkali Lignin
journal, August 2019


Preparation, functionalization and characterization of engineered carbon nanodots
journal, September 2019


Nitrogen-doped carbon dots encapsulated in the mesoporous channels of SBA-15 with solid-state fluorescence and excellent stability
journal, January 2019

  • Chang, Qing; Yang, Shanshan; Xue, Chaorui
  • Nanoscale, Vol. 11, Issue 15
  • DOI: 10.1039/c9nr01224a

A postmodification strategy to modulate the photoluminescence of carbon dots from blue to green and red: synthesis and applications
journal, January 2019

  • Zheng, Min; Qiao, Lihong; Su, Ya
  • Journal of Materials Chemistry B, Vol. 7, Issue 24
  • DOI: 10.1039/c9tb00544g

Tuning Carbon Dots’ Optoelectronic Properties with Polymers
journal, November 2018


Supramolecular Chiral Nanoarchitectonics
journal, March 2020

  • Ariga, Katsuhiko; Mori, Taizo; Kitao, Takashi
  • Advanced Materials, Vol. 32, Issue 41
  • DOI: 10.1002/adma.201905657

Preparation of Multicolor Photoluminescent Carbon Dots by Tuning Surface States
journal, April 2019

  • Jiang, Kai; Feng, Xiangyu; Gao, Xiaolu
  • Nanomaterials, Vol. 9, Issue 4
  • DOI: 10.3390/nano9040529

Red Room-Temperature Phosphorescence of CDs@Zeolite Composites Triggered by Heteroatoms in Zeolite Frameworks
journal, January 2019


Hydrophobic carbon dots with blue dispersed emission and red aggregation-induced emission
journal, April 2019


Small molecules derived carbon dots: synthesis and applications in sensing, catalysis, imaging, and biomedicine
journal, August 2019


Facile Preparation of Stable Solid-State Carbon Quantum Dots with Multi-Peak Emission
journal, February 2020

  • Zheng, Yanning; Zheng, Jingxia; Wang, Junli
  • Nanomaterials, Vol. 10, Issue 2
  • DOI: 10.3390/nano10020303

Preparation of Multicolor Photoluminescent Carbon Dots by Tuning Surface States
journal, April 2019

  • Jiang, Kai; Feng, Xiangyu; Gao, Xiaolu
  • Nanomaterials, Vol. 9, Issue 4
  • DOI: 10.3390/nano9040529

Tuning Carbon Dots’ Optoelectronic Properties with Polymers
journal, November 2018