Skip to main content

Advertisement

SpringerLink
Log in

Synthesis of 3D nitrogen-doped graphene quantum dots and reduced graphene oxide composites by a hydrothermal method for supercapacitors anodes

  • Research
  • Published:
Ionics Aims and scope Submit manuscript

Abstract

This work reports a feasible method to fabricate a simple chemical functionalization of graphene oxide (GO) electrode. The hydrothermal synthesis of nitrogen-doped graphene quantum dots modified reduced graphene oxide (NGDQs/rGO-2) using ammonium citrate and graphene oxide (GO) as raw materials. Ammonium citrate effectively acts as a nitrogen dopant cum reducing agent for graphene which remarkably enhances its electrochemical properties. Diffraction of X-rays (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscope (TEM), and X-ray photoelectron spectroscopy (XPS) were employed to characterize the structure and properties of the (NGDQs/rGO-2), and the NGDQs/rGO-2 was used as the electrode to test the electrochemical performance. According to the electrochemical test results, when the molar ratio of NGDQs to rGO is 1:2, the specific capacitance can reach 357 F/g at a current density of 1 A/g; after 1000 cycles, the capacitance retention rate is 82%. For comparison, under the same current density condition, the specific capacitance of the rGO electrode is only 74 F/g. By assembling a symmetrical supercapacitor for double electrode test, the specific capacitance can reach 237 F/g at a low current density of 0.5 A/g. As the current density increases, the capacitance decreases slightly. When the current density is 1 A/g, the specific capacitance is 113 A/g. Thus, the synthesized NGDQs/rGO-2 using this simple, cost-effective, environment friendly method could be a potential candidate for high performance energy-storage applications.

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
Fig. 6
Fig. 7
Fig. 8
Fig. 9

Similar content being viewed by others

Data availability

All data generated or analysed during this study are included in this published article [and its supplementary information files].

References

  1. Nguyen TH, Yang D, Zhu B, Lin H, Ma TY, Jia BH (2021) Doping mechanism directed graphene applications for energy conversion and storage. J Mater Chem A 9:7366–7395

    CAS  Google Scholar 

  2. Zhao SQ, Guo ZQ, Yan K, Wan SW, He FR, Sun B, Wang GX (2020) Towards high-energy-density lithium-ion batteries: strategies for developing high-capacity lithium-rich cathode materials. Energy Stor Mater 34:716–734

    Google Scholar 

  3. Wang Y, Gan SJ, Meng J, Yang JJ, Li J, Liu H, Shi L, Chen L (2021) Layered nanofiber yarn for high-performance flexible all-solid supercapacitor electrodes. J Phys Chem C 125:1190–1199

    CAS  Google Scholar 

  4. Grahame DC (1947) The electrical double layer and the theory of electrocapillarity. Chem Rev 41:441–501

    CAS  PubMed  Google Scholar 

  5. Liu YN, Li HL, Wang X, Lv T, Dong KY, Chen ZL, Yang YL, Cao SK, Chen T (2021) Flexible supercapacitors with high capacitance retention at temperatures from -20 to 100 °C based on DMSO-doped polymer hydrogel electrolytes. J Mater Chem A 9:12051–12059

    CAS  Google Scholar 

  6. González A, Goikolea E, Barrena JA, Mysyk R (2016) Review on supercapacitors: technologies and materials. Renew Sustain Energy Rev 58:1189–1206

    Google Scholar 

  7. Wang HM, Yang HR, Diao YF, Lu Y, Chrulski K, D’Acry JM (2021) Solid-state precursor impregnation for enhanced capacitance in hierarchical flexible poly (3, 4-ethylenedioxythiophene) supercapacitors. ACS Nano 15:7799–7810

    CAS  PubMed  Google Scholar 

  8. Chebrolu VT, Balakrishnan B, Cho I, Bak JS, Kim HJ (2020) A unique core–shell structured ZnO/NiO heterojunction to improve the performance of supercapacitors produced using a chemical bath deposition approach. Dalton Trans 49:14432–14444

    CAS  PubMed  Google Scholar 

  9. Xie LJ, Su FY, Xie LF, Guo XQ, Wang ZB, Kong QQ, Sun GH, Ahmad A, Li XM, Yi ZL, Chen CM (2020) Effect of pore structure and doping species on charge storage mechanisms in porous carbon-based supercapacitors. Mater Chem Front 4:2610–2634

    CAS  Google Scholar 

  10. Peres NMR (2009) The electronic properties of graphene and its bilayer. Vacuum 83:1248–1252

    CAS  Google Scholar 

  11. Sundar JV, Subramanian V (2013) Novel chemistry for the selective oxidation of benzyl alcohol by graphene oxide and N-doped graphene. Org Lett 15:5920–5923

    Google Scholar 

  12. Zhu YW, Murali S, Cai WW, Li XS, Suk JW, Potts JR, Ruoff RS (2010) Graphene and graphene oxide: synthesis, properties, and applications. Adv Mater 22:3906–3924

    CAS  PubMed  Google Scholar 

  13. Zhou QX, Ju WW, Yong YL, Zhang Q, Liu JL (2020) Effect of the N/P/S and transition-metal co-doping on the quantum capacitance of supercapacitor electrodes based on mono-and multilayer graphene. Carbon 170:368–379

    CAS  Google Scholar 

  14. Bardi N, Giannakopoulou T, Vavouliotis A, Trapalis C (2020) Electrodeposited films of graphene, carbon nanotubes, and their mixtures for supercapacitor applications. ACS Appl Nano Mater 3:10003–10013

    CAS  Google Scholar 

  15. Zhao ZY, Liu ZH, Zhong QS, Qin YJ, Xu AZ, Li W, Shi JH (2020) In situ synthesis of trifluoroacetic acid-doped polyaniline/reduced graphene oxide composites for high-performance all-solid-state supercapacitors. ACS Appl Energy Mater 3:8774–8785

    CAS  Google Scholar 

  16. Zhao J, Zhu JY, Li YT, Wang LX, Dong Y, Jiang ZM, Fan CW, Cao YL, Sheng R, Liu AJ, Zhang S, Song HH, Jia DZ, Fan ZJ (2020) Graphene quantum dot reinforced electrospun carbon nanofiber fabrics with high surface area for ultrahigh rate supercapacitors. ACS Appl Mater Interfaces 12:11669–11678

    CAS  PubMed  Google Scholar 

  17. Huang QT, Lin XF, Tong LL, Tong QX (2020) Graphene quantum dots/multiwalled carbon nanotubes composite-based electrochemical sensor for detecting dopamine release from living cells. ACS Sustain Chem Eng 8:1644–1650

    Google Scholar 

  18. Kaur M, Ubhi MK, Grewal JK, Sharma VK (2021) Boron-and phosphorous-doped graphene nanosheets and quantum dots as sensors and catalysts in environmental applications: a review. Environ Chem Lett 19:4375–4392

    CAS  Google Scholar 

  19. Yu ZC, Ma WH, Wu T, Wen J, Zhang Y, Wang LY, He YQ, Chu HT, Hu MG (2020) Coumarin-modifed graphene quantum dots as a sensing platform for multicomponent detection and its applications in fruits and living Cells. ACS Omega 5:7369–7378

    CAS  PubMed  PubMed Central  Google Scholar 

  20. Zhang B, Xiao CH, Xiang Y, Dong BT, Ding SJ, Tang YH (2016) Nitrogen-doped graphene quantum dots anchored on thermally reduced graphene oxide as an electrocatalyst for the oxygen reduction reaction. ChemElectroChem 3:864–870

    CAS  Google Scholar 

  21. Luo Y, Li M, Sun L, Xu YJ, Hu GH, Tang T, Wen JF, Li XY (2017) Tuning the photoluminescence of graphene quantum dots by co-doping of nitrogen and sulfur. J Nanopart Res 19:363

    Google Scholar 

  22. Ma YY, Yuan WY, Bai YH, Wu H, Cheng LF (2019) The toughening design of pseudocapacitive materials via graphene quantum dots: towards enhanced cycling stability for supercapacitors. Carbon 154:292–300

    CAS  Google Scholar 

  23. Kapoor S, Jha A, Ahmad H, Islam SS (2020) Avenue to large-scale production of graphene quantum dots from high-purity graphene sheets using laboratory-grade graphite electrodes. ACS Omega 5:18831–18841

    CAS  PubMed  PubMed Central  Google Scholar 

  24. Yuan WJ, Zhou Y, Li YR, Li C, Peng HL, Zhang J, Liu ZF, Dai LM, Shi GQ (2013) The edge-and basal-plane-specific electrochemistry of a single-layer graphene sheet. Sci Rep 3:1–7

    Google Scholar 

  25. Ebrahimi M, Kermanpur A, Atapour M, Adhami S, Heidari RH, Khorshidi E, Irannejad N, Rezaie B (2020) Performance enhancement of mesoscopic perovskite solar cells with GQDs-doped TiO2 electron transport layer. Sol Energy Mater Sol Cells 208:110407

    CAS  Google Scholar 

  26. Wu H, Guo ZS, Li M, Hu GH, Tang T, Wen JF, Li XY, Huang HF (2021) Enhanced pseudocapacitive performance of MoS2 by introduction of both N-GQDs and HCNT for flexible supercapacitors. Electrochim Acta 370:137758

    CAS  Google Scholar 

  27. Li Z, Bu F, Wei JJ, Yao WW, Wang L, Chen ZW, Pan DY, Wu MH (2018) Boosting the energy storage densities of supercapacitors by incorporating N-doped graphene quantum dots into cubic porous carbon. Nanoscale 10:22871–22883

    CAS  PubMed  Google Scholar 

  28. Ganganboina AB, Doong RA (2020) Nitrogen doped graphene quantum dot-decorated earth-abundant nanotubes for enhanced capacitive deionization. Environ Sci Nano 7:228–237

    CAS  Google Scholar 

  29. Chen F, Liu LL, Zhang YJ, Wu JH, Huang GX, Yang Q, Chen JJ, Yu HQ (2020) Enhanced full solar spectrum photocatalysis by nitrogen-doped graphene quantum dots decorated BiO2-x nanosheets: ultrafast charge transfer and molecular oxygen activation. Appl Catal B-Environ 277:119218

    CAS  Google Scholar 

  30. Nascimento JRD, D'Oliveira MR, Veiga AG, Chagas CA, Schmal M (2020) Synthesis of reduced graphene oxide as a support for nano copper and palladium/copper catalysts for selective NO reduction by CO. ACS Omega 5:25568–25581

    PubMed  PubMed Central  Google Scholar 

  31. Turkaslan BE, Aydin MF (2020) Optimizing parameters of graphene derivatives synthesis by modified improved Hummers. Math Methods Appl Sci 8:1–8

    Google Scholar 

  32. Aragaw BA (2020) Reduced graphene oxide-intercalated graphene oxide nano-hybrid for enhanced photoelectrochemical water reduction. J Nanostructure Chem 10:9–18

    CAS  Google Scholar 

  33. Gong XB, Wang Y, Yao K, Yang JJ, Li YN, Ge X, Xie HJ, Pan GF, Xing RG (2023) Supercapacitors based on Resveratrol/reduced graphene oxide composites. ACS Appl Nano Mater 6:4162–4169

    CAS  Google Scholar 

  34. Yap PL, Kabiri S, Auyoong YL, Tran DNH, Losic D (2019) Tuning the multifunctional surface chemistry of reduced graphene oxide via combined elemental doping and chemical modifications. ACS omega 4:19787–19798

    CAS  PubMed  PubMed Central  Google Scholar 

  35. Tarcan R, Handrea-Dragan M, Todor-Boer O, Petrovai I, Farcau C, Rusu M, Vulpoi A, Todea M, Astilean S, Botiz I (2020) A new, fast and facile synthesis method for reduced graphene oxide in N. N-dimethylformamide Synth Met 269:116576

    CAS  Google Scholar 

  36. Karaman C, Bayram E, Karaman O, Akta Z (2020) Preparation of high surface area nitrogen doped graphene for the assessment of morphologic properties and nitrogen content impacts on supercapacitors. J Electroanal Chem 868:114197

    CAS  Google Scholar 

  37. Qing Y, Jiang YT, Lin H, Wang LX, Liu AJ, Cao YL, Sheng R, Guo Y, Fan CW, Zhang S, Jia DZ, Fan ZJ (2019) Boosting the supercapacitor performance of activated carbon by constructing overall conductive networks using graphene quantum dots. J Mater Chem A 7:6021–6027

    CAS  Google Scholar 

  38. Kakaei K, Hamidi M, Husseindoost S (2016) Chlorine-doped reduced graphene oxide nanosheets as an efficient and stable electrode for supercapacitor in acidic medium. J Colloid Interface Sci 479:121–126

    CAS  PubMed  Google Scholar 

  39. Zheng F, Xi CP, Xu JH, Yu Y, Yang WG, Hu PF, Li Y, Zhen Q, Bashir S, Jingbo JL (2019) Facile preparation of WO3 nano-fibers with super large aspect ratio for high performance supercapacitor. J Alloys Compd 772:933–942

    CAS  Google Scholar 

  40. Chen J, Chang B, Liu FR, Wei HM, Wei W, Liu HL, Han S (2019) Modification of porous carbon with nitrogen elements to enhance the capacitance of supercapacitors. J Mater Sci 54:11959–11971

    CAS  Google Scholar 

  41. Zhang R, Shen WZ, Zhong M, Zhang JL, Guo SW (2020) Carbon nanofibers cross-linked and decorated with graphene quantum dots as binder-free electrodes for flexible supercapacitors. J Phys Chem C 125:143–151

    Google Scholar 

  42. Xing RG, Gong XB, Zhuang XX, Li YA, Bulin CK, Ge X, Zhang BW (2022) Synthesis and improved electrochemical properties of nitrogen-doped graphene quantum dot–modifed polyaniline. J Nanopart Res 24:32

    CAS  Google Scholar 

Download references

Funding

This work was financially supported by the Natural Science Foundations of Inner Mongolia Autonomous Region (No. 2018LH05020, 2018LH02003); the Inner Mongolia Science and Technology Innovation Oriented Project (No. KCBJ2018032) and Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region (NJYT23004).

Author information

Authors and Affiliations

  1. School of Materials and Metallurgy, Inner Mongolia University of Science and Technology, Baotou, 014010, China

    Xiaobin Gong, Jingjing Yang, Kai Yao, Yanan Li, Gaofei Pan, Xin Ge, Zhe Gao & Ruiguang Xing

Authors
  1. Xiaobin Gong
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Jingjing Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Kai Yao
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Yanan Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Gaofei Pan
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Xin Ge
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Zhe Gao
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Ruiguang Xing
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

XB: Conceptualization, Methodology, Experiment, Software, Investigation, Formal Analysis, Writing—Original Draft; , JJ: Data Curation, Writing—Original Draft; K: Visualization, Investigation; YN: Resources, Supervision, Writing—Review and Editing; GF: Software, Validation; X: Visualization, Writing—Review and Editing; Z: Additional experiments Writing; RG: Conceptualization, Funding Acquisition, Resources, Supervision, Writing—Review and Editing.

Corresponding authors

Correspondence to Yanan Li or Ruiguang Xing.

Ethics declarations

Ethics approval

Written informed consent for publication of this paper was obtained from the Inner Mongolia University of Science and Technology and all authors

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

ESM 1

(DOCX 253 kb)

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Gong, X., Yang, J., Yao, K. et al. Synthesis of 3D nitrogen-doped graphene quantum dots and reduced graphene oxide composites by a hydrothermal method for supercapacitors anodes. Ionics 29, 3273–3285 (2023). https://doi.org/10.1007/s11581-023-05057-0

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11581-023-05057-0

Keywords

Search

Navigation