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Journal of Applied Electrochemistry

, Volume 49, Issue 12, pp 1211–1226 | Cite as

Fishnet-like Ni–Fe–N co-modified graphene aerogel catalyst for highly efficient oxygen reduction reaction in an alkaline medium

  • Jiafeng Liang
  • Yunhan LingEmail author
  • Xiu-wen WuEmail author
  • Heloisa Andrea Acciari
  • Zhengjun Zhang
Research Article
  • 96 Downloads
Part of the following topical collections:
  1. Fuel cells

Abstract

The bimetallic nanoparticles of Ni and Fe co-modified reduced graphene oxide (rGO) aerogel were prepared by a fishnet-like one-step hydrothermal method, and the nitrogen atoms were successfully doped to the carbon layers with heat treatment of ammonia. By SEM and TEM, it could be observed that the rGO aerogel is a porous structure with particles of metal uniformly distributed on carbon sheets, and the sizes of nanoparticles were approximately 20–100 nm. The Raman results indicated that the GO was successfully reduced by ethylene glycol in the hydrothermal process. XPS results showed that nitrogen was introduced to rGO nanosheets, and Ni–Fe–NrGO possessed the higher contents of pyridinic N and graphitic N. XRD results suggested the Ni3Fe phase exists in the Ni–Fe–NrGO, which was consistent with EDX results. The electro-catalyzed oxygen reduction reaction (ORR) properties were evaluated by a rotating disk electrode (RDE). The Ni–Fe–NrGO sample showed synergistic effect with a relatively higher onset potential and diffusion-limiting current density of approximately 4.01 mA cm−2, with an electron transfer number close to 4, and exhibited an excellent ORR performance compared with the commercial Pt/C electro-catalyst.

Graphic abstract

Keywords

Graphene aerogel Nitrogen doped Synergistic effect Oxygen reduction reaction 

Notes

Acknowledgements

This work was partially supported by International cooperation on scientific and technological innovation between China and Italy governments (2016YFE0104000), the Science Challenge Project (No. tz2016004), the Fundamental Research Funds for Central Universities (No. 2652017157), the National Nature Science Foundation of China (No. 51771098), and National Energy Novel Materials Center China Academy of Engineering Physics (No. NENMCelle1703).

References

  1. 1.
    Wang Y, Yin X, Shen H, Jiang H, Yu J, Zhang Y et al (2018) Co3O4@g-C3N4 supported on N-doped graphene as effective electrocatalyst for oxygen reduction reaction. Int J Hydrogen Energy 43:20687–20695Google Scholar
  2. 2.
    Suh WK, Ganesan P, Son B, Kim H, Shanmugam S (2016) Graphene supported Pt–Ni nanoparticles for oxygen reduction reaction in acidic electrolyte. Int J Hydrogen Energy 41:12983–12994Google Scholar
  3. 3.
    Ratso S, Kruusenberg I, Vikkisk M, Joost U, Shulga E, Kink I et al (2014) Highly active nitrogen-doped few-layer graphene/carbon nanotube composite electrocatalyst for oxygen reduction reaction in alkaline media. Carbon 73:361–370Google Scholar
  4. 4.
    Kramm UI, Herranz J, Larouche N, Arruda TM, Lefèvre M, Jaouen F et al (2012) Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cells. Phys Chem Chem Phys 14:11673–11688PubMedPubMedCentralGoogle Scholar
  5. 5.
    He C, Zhang JJ, Shen PK (2014) Nitrogen-self-doped graphene-based non-precious metal catalyst with superior performance to Pt/C catalyst toward oxygen reduction reaction. J Mater Chem A 2:3231–3236Google Scholar
  6. 6.
    He D, Xiong Y, Yang J, Chen X, Deng Z, Pan M et al (2015) Nanocarbon-intercalated and Fe–N-codoped graphene as a highly active noble-metal-free bifunctional electrocatalyst for oxygen reduction and evolution. J Mater Chem A 5:1930–1934Google Scholar
  7. 7.
    Lee JY, Na YK, Dong YS, Park HY, Lee SS, Kwon SJ et al (2017) Nitrogen-doped graphene-wrapped iron nanofragments for high-performance oxygen reduction electrocatalysts. J Nanopart Res 19:98Google Scholar
  8. 8.
    Fu X, Liu Y, Cao X, Jin J, Liu Q, Zhang J (2013) FeCo–N x embedded graphene as high performance catalysts for oxygen reduction reaction. Appl Catal B 130:143–151Google Scholar
  9. 9.
    Darabdhara G, Das MR, Amin MA, Mersal GAM, Mostafa NY, El-Rehim SSA et al (2018) Au Ni alloy nanoparticles supported on reduced graphene oxide as highly efficient electrocatalysts for hydrogen evolution and oxygen reduction reactions. Int J Hydrogen Energy 43:1424–1438Google Scholar
  10. 10.
    Li J, Chen J, Wang H, Ren Y, Liu K, Tang Y et al (2017) Fe/N co-doped carbon materials with controllable structure as highly efficient electrocatalysts for oxygen reduction reaction in Al-air batteries. Energy Storage Mater 8:49–58Google Scholar
  11. 11.
    Liu Y, Wu YY, Lv GJ, Pu T, He XQ, Cui LL (2013) Iron(II) phthalocyanine covalently functionalized graphene as a highly efficient non-precious-metal catalyst for the oxygen reduction reaction in alkaline media. Electrochim Acta 112:269–278Google Scholar
  12. 12.
    Guo J, Yan X, Liu Q, Li Q, Xu X, Kang L et al (2018) The synthesis and synergistic catalysis of iron phthalocyanine and its graphene-based axial complex for enhanced oxygen reduction. Nano Energy 46:347–355Google Scholar
  13. 13.
    Merzougui B, Hachimi A, Akinpelu A, Bukola S, Shao M (2013) A Pt-free catalyst for oxygen reduction reaction based on Fe–N multiwalled carbon nanotube composites. Electrochim Acta 107:126–132Google Scholar
  14. 14.
    Qi Z, Li Y, Li Y, Huang K, Qin W, Zhang J (2017) Hierarchical hybrid of Ni3N/N-doped reduced graphene oxide nanocomposite as a noble metal free catalyst for oxygen reduction reaction. Appl Surf Sci 400:245–253Google Scholar
  15. 15.
    Yang Z-Y, Zhang Y-X, Jing L, Zhao Y-F, Yan Y-M, Sun K-N (2013) Beanpod-shaped Fe–C–N composite as promising ORR catalyst for fuel cells operated in neutral media. J Mater Chem A 2:2623–2627Google Scholar
  16. 16.
    Hu E, Yu XY, Chen F, Wu Y, Hu Y, Lou XWD (2017) Graphene layers-wrapped Fe/Fe5C2 nanoparticles supported on N-doped graphene nanosheets for highly efficient oxygen reduction. Adv Energy Mater 8(9):1702476Google Scholar
  17. 17.
    Videla AHAM, Ban S, Specchia S, Zhang L, Zhang J (2014) Non-noble Fe–Nx electrocatalysts supported on the reduced graphene oxide for oxygen reduction reaction. Carbon 76:386–400Google Scholar
  18. 18.
    Chen C, Liu M, Rao H, Liu Y, Lin S, Sun J-K et al (2019) Doped porous carbon nanostructures with N-Co-O catalytic active sites for efficient electrocatalytic oxygen reduction reaction. Appl Surf Sci 463:386–394Google Scholar
  19. 19.
    Wang DC, Huang NB, Sun Y, Zhan S, Zhang JJ (2017) GO clad Co3O4(Co3O4@GO) as ORR catalyst of anion exchange membrane fuel cell. Int J Hydrogen Energy 42:20216–20223Google Scholar
  20. 20.
    Wang J, Wang G, Miao S, Li J, Bao X (2015) Graphene-supported iron-based nanoparticles encapsulated in nitrogen-doped carbon as a synergistic catalyst for hydrogen evolution and oxygen reduction reactions. Faraday Discuss 176:135–151Google Scholar
  21. 21.
    Novoselov KS, Geim AK, Morozov SV, Jiang D, Zhang Y, Dubonos SV et al (2004) Electric field effect in atomically thin carbon films. Science 306:666–669PubMedGoogle Scholar
  22. 22.
    Geim AK, Novoselov KS (2007) The rise of graphene. Nat Mater 6:183–191PubMedGoogle Scholar
  23. 23.
    Hummers SW Jr, Offeman RE (1958) Preparation of graphitic oxide. J Am Chem Soc 80:1339Google Scholar
  24. 24.
    Dreyer DR, Park S, Bielawski CW, Ruoff RS (2009) The chemistry of graphene oxide. Chem Soc Rev 39:228–240PubMedGoogle Scholar
  25. 25.
    Liu X, Yu Y, Niu Y, Bao S, Hu W (2017) Cobalt nanoparticle decorated graphene aerogel for efficient oxygen reduction reaction electrocatalysis. Int J Hydrogen Energy 42:5930–5937Google Scholar
  26. 26.
    Sirirak R, Jarulertwathana B, Laokawee V, Susingrat W, Sarakonsri T (2016) FeNi alloy supported on nitrogen-doped graphene catalysts by polyol process for oxygen reduction reaction (ORR) in proton exchange membrane fuel cell (PEMFC) cathode. Res Chem Intermed 43:2905–2919Google Scholar
  27. 27.
    Cui X, Yang S, Yan X, Leng J, Shuang S, Ajayan PM et al (2016) Pyridinic-nitrogen-dominated graphene aerogels with Fe–N–C coordination for highly efficient oxygen reduction reaction. Adv Func Mater 26:5708–5717Google Scholar
  28. 28.
    Hossen MM, Artyushkova K, Atanassov P, Serov A (2018) Synthesis and characterization of high performing Fe–N–C catalyst for oxygen reduction reaction (ORR) in alkaline exchange membrane fuel cells. J Power Sources 375:214–221Google Scholar
  29. 29.
    Yu D, He X (2016) 3D cobalt-embedded nitrogen-doped graphene xerogel as an efficient electrocatalyst for oxygen reduction reaction in an alkaline medium. J Appl Electrochem 47(1):1–11Google Scholar
  30. 30.
    Wu Y, Shi Q, Li Y, Lai Z, Yu H, Wang H et al (2014) Nitrogen-doped graphene-supported cobalt carbonitride@oxide core-shell nanoparticles as a non-noble metal electrocatalyst for oxygen reduction reaction. J Mater Chem A 3:1142–1151Google Scholar
  31. 31.
    Min WC, Chang HC (2017) Carbon nanofibers as parent materials for a graphene-based Fe–N–C catalyst for the oxygen reduction reaction. Catal Today 295:125–131Google Scholar
  32. 32.
    Liang J, Wu XW, Ling Y, Yu S, Zhang Z (2018) Trilaminar structure hydrophobic graphene oxide decorated organosilane composite coatings for corrosion protection. Surf Coat Technol 339:65–77Google Scholar
  33. 33.
    Chen C, Zhang X, Zhou Z-Y, Yang X-D, Zhang X-S, Sun S-G (2016) Highly active Fe, N co-doped graphene nanoribbon/carbon nanotube composite catalyst for oxygen reduction reaction. Electrochim Acta 222:1922–1930Google Scholar
  34. 34.
    Pan F, Zhao Q, Wang J, Zhang J (2016) High-performance Fe-N-doped graphene electrocatalysts with pH-dependent active sites for oxygen reduction reaction. ChemElectroChem 2:2032–2040Google Scholar
  35. 35.
    Li T, Peng Y, Li K, Zhang R, Zheng L, Xia D et al (2015) Enhanced activity and stability of binuclear iron (III) phthalocyanine on graphene nanosheets for electrocatalytic oxygen reduction in acid. J Power Sources 293:511–518Google Scholar
  36. 36.
    Niu Y, Huang X, Hu W (2016) Fe 3 C nanoparticle decorated Fe/N doped graphene for efficient oxygen reduction reaction electrocatalysis. J Power Sources 332:305–311Google Scholar
  37. 37.
    Wang J, Zhang H, Wang C, Zhang Y, Wang J, Zhao H et al (2018) Co-synthesis of atomic Fe and few-layer graphene towards superior ORR electrocatalyst. Energy Storage Mater 12:1–7Google Scholar
  38. 38.
    Lin L, Li M, Jiang L, Li Y, Liu D, He X et al (2014) A novel iron (II) polyphthalocyanine catalyst assembled on graphene with significantly enhanced performance for oxygen reduction reaction in alkaline medium. J Power Sources 268:269–278Google Scholar
  39. 39.
    Qian L, Gu L, Yang L et al (2013) Direct growth of NiCo2O4 nanostructures on conductive substrates with enhanced electrocatalytic activity and stability for methanol oxidation. Nanoscale 5(16):7388–7396PubMedGoogle Scholar
  40. 40.
    Wu LK, Xia J, Cao HZ et al (2017) Highly active and durable cauliflower-like NiCo2O4, film for oxygen evolution with electrodeposited SiO2 as template. Int J Hydrogen Energy 42(16):10813–10825Google Scholar
  41. 41.
    Wei C, Huang Y, Chen M et al (2017) Fabrication of porous nanosheets assembled from NiCo2O4/NiO electrode for electrochemical energy storage application. J Colloid Interface Sci 504:1–11PubMedGoogle Scholar
  42. 42.
    Liangti Q, Yong L, Jong-Beom B, Liming D (2010) Nitrogen-doped graphene as efficient metal-free electrocatalyst for oxygen reduction in fuel cells. ACS Nano 4:1321–1326Google Scholar
  43. 43.
    Rethinasabapathy M, Kang S-M, Haldorai Y, Jankiraman M, Jonna N, Choe SR et al (2017) Ternary PtRuFe nanoparticles supported N-doped graphene as an efficient bifunctional catalyst for methanol oxidation and oxygen reduction reactions. Int J Hydrogen Energy 42:30738–30749Google Scholar
  44. 44.
    Zhuang W, Li M, Fan L, Han J, Xiong Y (2017) Fe/Ni–N–CNFs electrochemical catalyst for oxygen reduction reaction/oxygen evolution reaction in alkaline media. Appl Surf Sci 401:89–99Google Scholar
  45. 45.
    Faraji M, Derakhshi P, Tahvildari K, Yousefian Z (2018) High performance Fe and N-codoped graphene quantum dot supported Pd3Co catalyst with synergistically improved oxygen reduction activity and great methanol tolerance. Solid State Sci 83:152–160Google Scholar
  46. 46.
    Yan P, Liu J, Yuan S, Liu Y, Cen W, Chen Y (2018) The promotion effects of graphitic and pyridinic N combinational doping on graphene for ORR. Appl Surf Sci 445:398–403Google Scholar
  47. 47.
    Monteverde Videla AHA, Zhang L, Kim J et al (2013) Mesoporous carbons supported non-noble metal Fe–Nx electrocatalysts for PEM fuel cell oxygen reduction reaction. J Appl Electrochem 43(2):159–169Google Scholar
  48. 48.
    Kazuhide K, Kazuhito H, Shuji N (2012) Instantaneous one-pot synthesis of Fe–N-modified graphene as an efficient electrocatalyst for the oxygen reduction reaction in acidic solutions. Chem Commun 48:10213–10215Google Scholar
  49. 49.
    Palaniselvam T, Kashyap V, Bhange SN, Baek JB, Kurungot S (2016) Nanoporous graphene enriched with Fe/Co–N active sites as a promising oxygen reduction electrocatalyst for anion exchange membrane fuel cells. Adv Func Mater 26:2150–2162Google Scholar
  50. 50.
    Fu G, Cui Z, Chen Y, Li Y, Tang Y, Goodenough JB (2017) Ni3Fe–N doped carbon sheets as a bifunctional electrocatalyst for air cathodes. Adv Energy Mater 7(1):1601172Google Scholar

Copyright information

© Springer Nature B.V. 2019

Authors and Affiliations

  1. 1.The Key Laboratory of Advanced Materials, School of Materials Sciences and Engineering, Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijingPeople’s Republic of China
  2. 2.Beijing Institute of Aeronautical MaterialsBeijingPeople’s Republic of China
  3. 3.Beijing Institute of Graphene TechnologyBeijingPeople’s Republic of China
  4. 4.School of ScienceChina University of GeosciencesBeijingPeople’s Republic of China

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