Skip to main content
SpringerLink
Log in

Tuning the photoluminescence of graphene quantum dots by co-doping of nitrogen and sulfur

  • Research Paper
  • Published:
Journal of Nanoparticle Research Aims and scope Submit manuscript

Abstract

Nitrogen and sulfur co-doped graphene quantum dots (NS-GQDs) were successfully synthesized using a facile, inexpensive, and environmentally friendly hydrothermal reaction of aqueous ammonia, S powder, and graphene quantum dots. The NS-GQDs with oxygen-rich functional groups have a high quantum yield of 41% and a diameter of 1–5 nm. The photoluminescence (PL) properties of the nitrogen-doped graphene quantum dots (N-GQDs) and NS-GQD were investigated. The results showed that the PL emission of the NS-GQD exhibits a clear blue shift of 54 nm compared to that of the N-GQDs.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  • Chen Y, Wang J, Liu H, Banis MN, Li R, Sun X, Sham T-K, Ye S, Knights S (2011) Nitrogen doping effects on carbon nanotubes and the origin of the enhanced electrocatalytic activity of supported Pt for proton-exchange membrane fuel cells. J Phys Chem C 115:3769–3776

    Article  Google Scholar 

  • Chien CT, Li SS, Lai WJ, Yeh YC, Chen HA, Chen IS, Chen LC, Chen KH, Nemoto T, Isoda S, Chen M, Fujita T, Eda G, Yamaguchi H, Chhowalla M, Chen CW (2012) Tunable photoluminescence from graphene oxide. Angew Chem Int Ed 51:6662–6666

    Article  Google Scholar 

  • Dong Y, Pang H, Yang HB, Guo C, Shao J, Chi Y, Li CM, Yu T (2013) Carbon-based dots co-doped with nitrogen and sulfur for high quantum yield and excitation-independent emission. Angew Chem Int Ed 52:7800–7804

    Article  Google Scholar 

  • Eda G, Lin YY, Mattevi C, Yamaguchi H, Chen HA, Chen IS, Chen CW, Chhowalla M (2010) Blue photoluminescence from chemically derived graphene oxide. Adv Mater 22:505–509

    Article  Google Scholar 

  • Feng Q, Tang N, Liu F, Cao Q, Zheng W, Ren W, Wan X, Du Y (2013) Obtaining high localized spin magnetic moments by fluorination of reduced graphene oxide. ACS Nano 7:6729–6734

    Article  Google Scholar 

  • Gupta V, Chaudhary N, Srivastava R, Sharma GD, Bhardwaj R, Chand S (2011) Luminscent graphene quantum dots for organic photovoltaic devices. J Am Chem Soc 133:9960–9963

    Article  Google Scholar 

  • Hao YN, Guo HL, Tian L, Kang XF (2015) Enhanced photoluminescence of pyrrolic-nitrogen enriched graphene quantum dots. RSC Adv 5:43750–43755

    Article  Google Scholar 

  • Hu CF, Liu YL, Yang YH, Cui JH, Huang ZR, Wang YL, Yang LF, Wang HB, Xiao Y, Rong JH (2013) One-step preparation of nitrogen-doped graphene quantum dots from oxidized debris of graphene oxide. J Mater Chem B 1:39–42

    Article  Google Scholar 

  • Ji L, Yan J, Mietek J, Zhang QS (2012) Sulfur and nitrogen dual-doped mesoporous graphene electrocatalyst for oxygen reduction with synergistically enhanced performance. Angew Chem Int Ed 51:11640–11641

    Article  Google Scholar 

  • Kim S, Hwang SW, Kim MK, Dong YS, Dong HS, Chang OK, Yang SB, Park JH, Hwang E, Choi SH (2012) Anomalous behaviors of visible luminescence from graphene quantum dots: interplay between size and shape. ACS Nano 6:8203–8208

    Article  Google Scholar 

  • Li LS, Yan X (2010) Colloidal graphene quantum dots. J Phys Chem Lett 1:2572–2576

    Article  Google Scholar 

  • Li Y, Hu Y, Zhao Y, Shi GQ, Deng LE, Hou YB, Qu LT (2011) An electrochemical avenue to green-luminescent graphene quantum dots as potential electron-acceptors for photovoltaics. Adv Mater 23:776–779

    Article  Google Scholar 

  • Li Y, Zhao Y, Cheng HH, Hu Y, Shi GQ, Dai LM, Qu LT (2012) Nitrogen-doped graphene quantum dots with oxygen-rich functional groups. J Am Chem Soc 134:15–18

    Article  Google Scholar 

  • Liu RL, Wu DQ, Feng XL, Mullen K (2011) Bottom-up fabrication of photoluminescent graphene quantum dots with uniform morphology. J Am Chem Soc 133:15221–15223

    Article  Google Scholar 

  • Liu Q, Guo B, Rao Z, Zhang B, Gong JR (2013) Strong two-photon-induced fluorescence from photostable, biocompatible nitrogen-doped graphene quantum dots for cellular and deep-tissue imaging. Nano Lett 13:2436–2441

    Article  Google Scholar 

  • Mueller ML, Yan X, McGuire JA, Li LS (2010) Triplet states and electronic relaxation in photoexcited graphene quantum dots. Nano Lett 10:2679–2682

    Article  Google Scholar 

  • Neubeck S, Ponomarenko LA, Freitag F, Giesbers AJM, Zeitler U, Morozov SV, Blake P, Geim AK, Novoselov KS (2010) From one electron to one hole: quasiparticle counting in graphene quantum dots determined by electrochemical and plasma etching. Small 6:1469–1473

    Article  Google Scholar 

  • Pan D, Zhang J, Li Z, Wu M (2010) Hydrothermal route for cutting graphene sheets into blue-luminescent graphene quantum dots. Adv Mater 22:734–738

    Article  Google Scholar 

  • Qu D, Zheng M, Du P, Zhou Y, Zhang LG, Li D, Tan HQ, Zhao Z, Xie ZG, Sun ZC (2013) Highly luminescent S, N co-doped graphene quantum dots with broad visible absorption bands for visible light photocatalysts. Nanoscale 5:12272–12277

    Article  Google Scholar 

  • Qu D, Zheng M, Zhang L, Zhao H, Xie Z, Jing X, Haddad RE, Fan H, Sun Z (2014) Formation mechanism and optimization of highly luminescent N-doped graphene quantum dots. Sci Rep 4:5294

    Article  Google Scholar 

  • Shen JH, Zhu YH, Chen C, Yang XL, Li CZ (2011) Facile preparation and upconversion luminescence of graphene quantum dots. Chem Commun 47:2580–2582

    Article  Google Scholar 

  • Su Y, Zhang Y, Zhuang X, Li S, Wu D, Zhang F, Feng X (2013) Low-temperature synthesis of nitrogen/sulfur co-doped three-dimensional graphene frameworks as efficient metal-free electrocatalyst for oxygen reduction reaction. Carbon 62:296–301

    Article  Google Scholar 

  • Wang Y, Zhang L, Liang RP, Bai JM, Qiu JD (2013) Using graphene quantum dots as photoluminescent probes for protein kinase sensing. Anal Chem 85:9148–9155

    Article  Google Scholar 

  • Wang L, Wang Y, Xu T, Liao H, Yao C, Liu Y, Li Z, Chen Z, Pan D, Sun L, Wu M (2014) Gram-scale synthesis of single-crystalline graphene quantum dots with superior optical properties. Nat Commun 5:5357–5357

    Article  Google Scholar 

  • Wang HX, Xiao J, Yang Z, Tang H, Zhu ZT, Zhao M, Liu Y, Zhang C, Zhang HL (2015) Rational design of nitrogen and sulfur co-doped carbon dots for efficient photoelectrical conversion applications. J Mater Chem A 3:11287–11293

    Article  Google Scholar 

  • Xue M, Zhang L, Zou M, Lan C, Zhan Z, Zhao S (2015) Nitrogen and sulfur co-doped carbon dots: a facile and green fluorescence probe for free chlorine. Sensors Actuators B Chem 219:50–56

  • Yan X, Cui X, Li B, Li LS (2010) Large, solution-processable graphene quantum dots as light absorbers for photovoltaics. Nano Lett 10:1869–1873

    Article  Google Scholar 

  • Yang Z, Yao Z, Li G, Fang G, Nie H, Liu Z, Zhou X, Chen X, Huang S (2011) Sulfur-doped graphene as an efficient metal-free cathode catalyst for oxygen reduction. ACS Nano 6:205–211

    Article  Google Scholar 

  • Yang SW, Sun J, Li XB, Zhou W, Wang ZY, He P, Ding GQ, Xie XM, Kang ZH, Jiang MH (2014) Large-scale fabrication of heavy doped carbon quantum dots with tunable-photoluminescence and sensitive fluorescence detection. J Mater Chem A 2:8660–8667

    Article  Google Scholar 

  • Zhang ZZ, Chang K (2008) Tuning of energy levels and optical properties of graphene quantum dots. Phys Rev B 77:235411

    Article  Google Scholar 

  • Zhang BX, Gao H, Li XL (2014) Synthesis and optical properties of nitrogen and sulfur co-doped graphene quantum dots. New J Chem 38:4615–4621

    Article  Google Scholar 

  • Zhu SJ, Zhang JH, Qiao CY, Tang SJ, Li YF, Yuan WJ, Li B, Tian L, Liu F, Hu R, Gao HN, Wei HT, Zhang H, Sun HC, Yang B (2011) Strongly green-photoluminescent graphene quantum dots for bioimaging applications. Chem Commun 47:6858–6860

    Article  Google Scholar 

  • Zhu S, Zhang J, Liu X, Li B, Wang X, Tang S, Meng Q, Li Y, Shi C, Hu R, Yang B (2012) Graphene quantum dots with controllable surface oxidation, tunable fluorescence and up-conversion emission. RSC Adv 2:2717–2720

    Article  Google Scholar 

Download references

Funding

This study was funded by NSFC (No. 11364010, 51662004 and 11764011) and Guangxi Natural Science Foundation (No. 2016GXNSFAA380008 and 2015GXNSFBA139002), P. R. China.

Author information

Authors and Affiliations

  1. College of Science, Guilin University of Technology, Guilin, 541004, China

    Yi Luo, Ming Li, Lang Sun, Yongjie Xu, Guanghui Hu, Tao Tang, Jianfeng Wen & Xinyu Li

Authors
  1. Yi Luo
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Ming Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Lang Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Yongjie Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Guanghui Hu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Tao Tang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Jianfeng Wen
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Xinyu Li
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Ming Li or Tao Tang.

Ethics declarations

Conflict of interests

The authors declare that they have no conflict of interests.

Electronic supplementary material

ESM 1

(DOCX 67 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Luo, Y., Li, M., Sun, L. et al. Tuning the photoluminescence of graphene quantum dots by co-doping of nitrogen and sulfur. J Nanopart Res 19, 363 (2017). https://doi.org/10.1007/s11051-017-4059-4

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s11051-017-4059-4

Keywords

Search

Navigation