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Assembly of highly stable aqueous dispersions and flexible films of nitrogen-doped graphene for high-performance stretchable supercapacitors

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Abstract

Here, we propose a route for production of highly stable nitrogen-doped graphene (NG) aqueous dispersions and flexible NG films. The NG dispersions are formed through sonication of NG hydrogels in methyl orange solution and stabilized through electrostatic repulsion without using any polymeric or surfactant stabilizer. The flexible NG films are formed by vacuum filtration of as-prepared NG dispersions and transferred onto stretchable and adhesive polyacrylate for the fabrication of stretchable supercapacitors. The supercapacitor exhibits high gravimetric specific capacitances of 315 F g−1 under no strain and 300 F g−1 under 30% applied strain at a current density of 1 A g−1. The fabrication of aqueous dispersions and stretchable NG films makes NG materials attractive for a diversity of applications in stretchable electronics.

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References

  1. Simon P, GoGotSi Y (2008) Materials for electrochemical capacitors. Nat Mater 7:845–854

    Article  Google Scholar 

  2. Winter M, Brodd RJ (2004) What are batteries, fuel cells, and supercapacitors? Chem Rev 104:4245–4270

    Article  Google Scholar 

  3. Miller JR, Simon P (2008) Electrochemical capacitors for energy management. Science 321:651–652

    Article  Google Scholar 

  4. Chen PC, Shen G, Shi Y, Chen H, Zhou C (2010) Preparation and characterization of flexible asymmetric supercapacitors based on transition-metal-oxide nanowire/single-walled carbon nanotube hybrid thin-film electrodes. ACS Nano 4:4403–4411

    Article  Google Scholar 

  5. Tarascon J-M, Armand M (2001) Issues and challenges facing rechargeable lithium batteries. Nature 414:359–367

    Article  Google Scholar 

  6. Tang Z, Tang CH, Gong H (2012) A high energy density asymmetric supercapacitor from nano-architectured Ni(OH)2/carbon nanotube electrodes. Adv Funct Mater 22:1272–1278

    Article  Google Scholar 

  7. Huang H, Lei C, Luo G, Cheng Z, Li G, Tang S, Du Y (2016) Facile synthesis of nitrogen-doped graphene on Ni foam for high-performance supercapacitors. J Mater Sci 51:6348–6356. doi:10.1007/s10853-016-9931-6

    Article  Google Scholar 

  8. Zhou Q, Zhang M, Chen J, Hong J-D, Shi G (2016) Nitrogen-doped holey graphene film-based ultrafast electrochemical capacitors. ACS Appl Mater Interfaces 8:20741–20747

    Article  Google Scholar 

  9. Chen T, Xue Y, Roy AK, Dai L (2014) Transparent and stretchable high-performance supercapacitors based on wrinkled graphene electrodes. ACS Nano 8:1039–1046

    Article  Google Scholar 

  10. Chee WK, Lim HN, Zainal Z, Huang NM, Harrison I, Andou Y (2016) Flexible graphene-based supercapacitors: a review. J Phys Chem 120:4153–4172

    Google Scholar 

  11. Li N, Lv T, Yao Y, Li H, Liu K, Chen T (2017) Compact graphene/MoS2 composite films for highly flexible and stretchable all-solid-state supercapacitors. J Mater Chem A 5:3267

    Article  Google Scholar 

  12. Ullah Z, Li Q, Wang R, Zeng Q, Li W, Liu L (2016) Graphene/Ag-NWs electrodes for highly transparent and extremely stretchable supercapacitor. IEEE trans nanotechnol. doi:10.1109/TNANO.2016.2634556

    Google Scholar 

  13. Liu YS, Li J, Li WZ, Li YM, Chen QY, Zhan FQ (2015) Nitrogen-doped graphene aerogel-supported spinel CoMn2O4 nanoparticles as an efficient catalyst for oxygen reduction reaction. J Power Sources 299:492–500

    Article  Google Scholar 

  14. Zheng FC, Yang Y, Chen QW (2014) High lithium anodic performance of highly nitrogen-doped porous carbon prepared from a metal-organic framework. Nat Commun 5:5261–5271

    Article  Google Scholar 

  15. Heydari A, Gharibi H (2016) Fabrication of electrocatalyst based on nitrogen doped graphene as highly efficient and durable support for using in polymer electrolyte fuel cell. J Power Sources 325:808–815

    Article  Google Scholar 

  16. Guo HL, Su P, Kang XF, Ning SK (2013) Synthesis and characterization of nitrogen-doped graphene hydrogels by hydrothermal route with urea as reducing-doping agents. J Mater Chem A 1:2248–2255

    Article  Google Scholar 

  17. Huang SF, Terakura K, Ozaki T, Ikeda T, Boero M, Oshima M, Ozaki J, Miyata S (2009) First-principles calculation of the electronic properties of graphene clusters doped with nitrogen and boron: analysis of catalytic activity for the oxygen reduction reaction. Phys Rev B 80:235410

    Article  Google Scholar 

  18. Wang Y, Shao YY, Matson DW, Li JH, Lin YH (2010) Nitrogen-doped graphene and its application in electrochemical biosensing. ACS Nano 4:1790–1798

    Article  Google Scholar 

  19. Wang X, Li X, Zhang L, Yoon Y, Weber PK, Wang H, Guo J, Dai H (2009) N-doping of graphene through electrothermal reactions with ammonia. Science 324:768–771

    Article  Google Scholar 

  20. Jeong HM, Lee JW, Shin WH, Choi YJ, Shin HJ, Kang JK, Choi JW (2011) Nitrogen-doped graphene for high-performance ultracapacitors and the importance of nitrogen-doped sites at basal planes. Nano Lett 11:2472–2477

    Article  Google Scholar 

  21. Li XF, Geng DS, Zhang Y, Meng XB, Li RY, Sun XL (2011) Superior cycle stability of nitrogen-doped graphene nanosheets as anodes for lithium ion batteries. Electrochem Commun 13:822–825

    Article  Google Scholar 

  22. Wang K, Li L, Zhang T, Liu Z (2014) Nitrogen-doped graphene for supercapacitor with long-term electrochemical stability. Energy 70:612–617

    Article  Google Scholar 

  23. Sun L, Wang L, Tian CG, Tan TX, Xie Y, Shi KY, Li MT, Fu HG (2012) Nitrogen-doped graphene with high nitrogen level via a one-step hydrothermal reaction of graphene oxide with urea for superior capacitive energy storage. RSC Adv 2:4498–4506

    Article  Google Scholar 

  24. Zhao Y, Hu CG, Hu Y, Cheng HH, Shi GQ, Qu LT (2012) A versatile ultralight, nitrogen-doped graphene framework. Angew Chem 51:11371–11375

    Article  Google Scholar 

  25. Lin ZY, Waller GH, Liu Y, Liu ML, Wong C (2013) 3D Nitrogen-doped graphene prepared by pyrolysis of graphene oxide with polypyrrole for electrocatalysis of oxygen reduction reaction. Nano Energy 2:241–248

    Article  Google Scholar 

  26. Long DH, Li W, Ling LC, Miyawaki J, Mochida I, Yoon SH (2010) Preparation of nitrogen-doped graphene sheets by a combined chemical and hydrothermal reduction of graphene oxide. Langmuir 26:16096–16102

    Article  Google Scholar 

  27. Lu YH, Zhang F, Zhang TF, Leng K, Zhang L, Yang X, Ma YF, Huang Y, Zhang MJ, Chen YS (2013) Synthesis and supercapacitor performance studies of N-doped graphene materials using o-phenylenediamine as the double-N precursor. Carbon 63:508–516

    Article  Google Scholar 

  28. Chen P, Yang JJ, Li SS, Wang Z, Xiao TY, Qian YH, Yu SH (2013) Hydrothermal synthesis of macroscopic nitrogen-doped graphene hydrogels for ultrafast supercapacitor. Nano Energy 2:249–256

    Article  Google Scholar 

  29. Li D, Müller MB, Gilje S, Kaner RB, Wallace GD (2008) Processable aqueous dispersions of graphene nanosheets. Nat Nanotechnol 3:101–105

    Article  Google Scholar 

  30. Hunter RJ (2001) Electrokinetics and the zetapotential. Foundations of colloid science. Oxford University Press Inc., New York

    Google Scholar 

  31. Liu SW, Liu C, Wang WG, Cheng B, Yu JG (2012) Unique photocatalytic oxidation reactivity and selectivity of TiO2–graphene nanocomposites. Nanoscale 4:3193–3200

    Article  Google Scholar 

  32. Deng DH, Pan XL, Yu L, Cui Y, Jiang YP, Qi J, Li WX, Fu Q, Ma XC, Xue QK, Sun GQ, Bao XH (2011) Toward N-doped graphene via solvothermal synthesis. Chem Mater 23:1188–1193

    Article  Google Scholar 

  33. Kudin KN, Ozbas B, Schniepp HC, Prud’homme RK, Aksay IA, Car R (2008) Raman spectra of graphite oxide and functionalized graphene sheets. Nano Lett 8:36–41

    Article  Google Scholar 

  34. Wen ZH, Wang XC, Mao S, Bo Z, Kim H, Cui SM, Lu GH, Feng XL, Chen JH (2012) Crumpled nitrogen-doped graphene nanosheets with ultrahigh pore volume for high-performance supercapacitor. Adv Mater 24:5610–5616

    Article  Google Scholar 

  35. Xu YX, Lin ZY, Huang XQ, Liu Y, Huang Y, Duan XF (2013) Flexible solid-state supercapacitors based on three-dimensional graphene hydrogel films. ACS Nano 7:4042–4049

    Article  Google Scholar 

Download references

Acknowledgements

The authors acknowledge financial support by the National Natural Science Foundation of China (Grant Nos. 11474310, 61605237), the Projects of Jiangsu province and Suzhou city (Grant Nos. BE2014061, BE2016006-3, BK20150366, BK20150367, ZXG201410, SYG201629, and SYG201623), and CAS-TWAS President’s Fellowship for Z. Ullah (Student ID: 2013A8017808100). The authors are also grateful for the technical support of Nano-X, the Platforms of Characterization & Test, and Nanofabrication Facility from Suzhou Institute of Nano-Tech and Nano-Bionics, and the Suzhou Industrial Park Initiative Platform Development for Suzhou Municipal Key Lab for New Energy Technology.

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Author notes

  1. Qi Zeng, Zaka Ullah and Mingliang Chen contributed equally to this work.

Authors and Affiliations

  1. College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, 215123, Jiangsu, China

    Qi Zeng & Guanhong Tao

  2. Key Laboratory of Nanodevices and Applications-CAS and Collaborative Innovation Center of Suzhou Nano Science and Technology, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, 215123, Jiangsu, China

    Qi Zeng, Zaka Ullah, Mingliang Chen, Huitao Zhang, Rubing Wang, Lina Gao, Liwei Liu & Qi Li

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  1. Qi Zeng
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  2. Zaka Ullah
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Correspondence to Guanhong Tao or Qi Li.

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Zeng, Q., Ullah, Z., Chen, M. et al. Assembly of highly stable aqueous dispersions and flexible films of nitrogen-doped graphene for high-performance stretchable supercapacitors. J Mater Sci 52, 12751–12760 (2017). https://doi.org/10.1007/s10853-017-1336-7

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