Advertisement

One-step ball milling-prepared nano Fe2O3 and nitrogen-doped graphene with high oxygen reduction activity and its application in microbial fuel cells

  • Xingguo Guo
  • Qiuying Wang
  • Ting Xu
  • Kajia Wei
  • Mengxi Yin
  • Peng Liang
  • Xia Huang
  • Xiaoyuan ZhangEmail author
Research Article
  • 8 Downloads

Abstract

Developing high activity, low-cost and long durability catalysts for oxygen reduction reaction is of great significance for the practical application of microbial fuel cells. The full exposure of active sites in catalysts can enhance catalytic activity dramatically. Here, novel Fe-N-doped graphene is successfully synthesized via a one-step in situ ball milling method. Pristine graphite, ball milling graphene, N-doped graphene and Fe-N-doped graphene are applied in air cathodes, and enhanced performance is observed in microbial fuel cells with graphene-based catalysts. Particularly, Fe-N-doped graphene achieves the highest oxygen reduction reaction activity, with a maximum power density of 1380±20 mW/m2 in microbial fuel cells and a current density of 23.8 A/m2 at −0.16 V in electrochemical tests, which are comparable to commercial Pt and 390% and 640% of those of pristine graphite. An investigation of the material characteristics reveals that the superior performance of Fe-N-doped graphene results from the full exposure of Fe2O3 nanoparticles, pyrrolic N, pyridinic N and excellent Fe-N-G active sites on the graphene matrix. This work not only suggests the strategy of maximally exposing active sites to optimize the potential of catalysts but also provides promising catalysts for the use of microbial fuel cells in sustainable energy generation.

Keywords

Microbial fuel cells Air cathodes Nano Fe2O3 and nitrogen-doped graphene Oxygen reduction reaction 

Notes

Acknowledgements

This research was supported by the National Natural Science Foundation of China (Grant No. 51778326) and the special fund of Tsinghua University Initiative Scientific Research Program. We thank Prof. Rufan Zhang at Tsinghua University for valuable comments and suggestions.

Supplementary material

11783_2019_1209_MOESM1_ESM.pdf (404 kb)
Supporting Information

References

  1. Jain A, He Z (2018). “NEW” resource recovery from wastewater using bioelectrochemical systems: Moving forward with functions. Frontiers of Environmental Science & Engineering, 12(4): 3–15CrossRefGoogle Scholar
  2. Bashyam R, Zelenay P (2006). A class of non-precious metal composite catalysts for fuel cells. Nature, 443(7107): 63–66CrossRefGoogle Scholar
  3. Cao C, Wei L, Wang G, Shen J (2017a). Superiority of boron, nitrogen and iron ternary doped carbonized graphene oxide-based catalysts for oxygen reduction in microbial fuel cells. Nanoscale, 9(10): 3537–3546CrossRefGoogle Scholar
  4. Cao C, Wei L, Zhai Q, Ci J, Li W, Wang G, Shen J (2017b). Gas-flow tailoring fabrication of graphene-like Co-Nx-C nanosheet supported sub-10 nm PtCo nanoalloys as synergistic catalyst for air-cathode microbial fuel cells. ACS Applied Materials & Interfaces, 9(27): 22465–22475CrossRefGoogle Scholar
  5. Chen X, Li F, Zhang N, An L, Xia D (2013). Mechanism of oxygen reduction reaction catalyzed by Fe(Co)-Nx/C. Physical chemistry chemical physics, 15(44): 19330–19336CrossRefGoogle Scholar
  6. Chen Z, Higgins D, Yu A, Zhang L, Zhang J (2011). A review on non-precious metal electrocatalysts for PEM fuel cells. Energy & Environmental Science, 4(9): 3167–3192CrossRefGoogle Scholar
  7. Chen Z Y, Li Y N, Lei L L, Bao S J, Wang M Q, Liu H, Zhao Z L, Xu M (2017). Investigation of Fe2N@Carbon encapsulated in N-doped graphene-like carbon as a catalyst in sustainable zinc-air batteries. Catalysis Science & Technology, 7(23): 5670–5676CrossRefGoogle Scholar
  8. Choi C H, Choi W S, Kasian O, Mechler A K, Sougrati M T, Brüller S, Strickland K, Jia Q, Mukerjee S, Mayrhofer K J J, Jaouen F (2017). Unraveling the nature of sites active toward hydrogen peroxide reduction in Fe-N-C catalysts. Angewandte Chemie International Edition, 56(30): 8809–8812CrossRefGoogle Scholar
  9. Chuong N D, Thanh T D, Kim N H, Lee J H (2018). Hierarchical heterostructures of ultrasmall Fe2O3-encapsulated MoS2/N-graphene as an effective catalyst for oxygen reduction reaction. ACS Applied Materials & Interfaces, 10(29): 24523–24532CrossRefGoogle Scholar
  10. Durán F G, Barbero B P, Cadús L E, Rojas C, Centeno M A, Odriozola J A (2009). Manganese and iron oxides as combustion catalysts of volatile organic compounds. Applied Catalysis B: Environmental, 92(1–2): 194–201CrossRefGoogle Scholar
  11. Ferrari A C, Meyer J C, Scardaci V, Casiraghi C, Lazzeri M, Mauri F, Piscanec S, Jiang D, Novoselov K S, Roth S, Geim A K (2006). Raman spectrum of graphene and graphene layers. Physical Review Letters, 97(18): 187401(1)–187401(4)CrossRefGoogle Scholar
  12. Guo D, Shibuya R, Akiba C, Saji S, Kondo T, Nakamura J (2016). Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts. Science, 351(6271): 361–365CrossRefGoogle Scholar
  13. Guo X, Jia J, Dong H, Wang Q, Xu T, Fu B, Ran R, Liang P, Huang X, Zhang X (2019a). Hydrothermal synthesis of Fe-Mn bimetallic nanocatalysts as high-efficiency cathode catalysts for microbial fuel cells. Journal of Power Sources, 414: 444–452CrossRefGoogle Scholar
  14. He D, Xiong Y, Yang J, Chen X, Deng Z, Pan M, Li Y, Mu S (2017). Nanocarbon-intercalated and Fe-N-codoped graphene as a highly active noble-metal-free bifunctional electrocatalyst for oxygen reduction and evolution. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 5(5): 1930–1934CrossRefGoogle Scholar
  15. Hossen M M, 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. Journal of Power Sources, 375: 214–221CrossRefGoogle Scholar
  16. Huang K, Zhang L, Xu T, Wei H, Zhang R, Zhang X, Ge B, Lei M, Ma J-Y, Liu L-M, Wu H (2019). 60 °C solution synthesis of atomically dispersed cobalt electrocatalyst with superior performance. Nature Communications, 10(1): 606(601–610)CrossRefGoogle Scholar
  17. Jiang C, Liu L, Crittenden J C. (2016). An electrochemical process that uses an Fe0/TiO2 cathode to degrade typical dyes and antibiotics and a bio-anode that produces electricity. Frontiers of Environmental Science & Engineering, 10(4): 25–32CrossRefGoogle Scholar
  18. Jiang Z J, Jiang Z, Chen W (2014). The role of holes in improving the performance of nitrogen-doped holey graphene as an active electrode material for supercapacitor and oxygen reduction reaction. Journal of Power Sources, 251: 55–65CrossRefGoogle Scholar
  19. Lai L, Potts J R, Zhan D, Wang L, Poh C K, Tang C, Gong H, Shen Z, Lin J, Ruoff R S (2012). Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction. Energy & Environmental Science, 5(7): 7936–7942CrossRefGoogle Scholar
  20. Li Q, Chen W, Xiao H, Gong Y, Li Z, Zheng L, Zheng X, Yan W, Cheong W C, Shen R, Fu N, Gu L, Zhuang Z, Chen C, Wang D, Peng Q, Li J, Li Y (2018). Fe isolated single atoms on S, N codoped carbon by copolymer pyrolysis strategy for highly efficient oxygen reduction reaction. Advanced materials, 30(25): 1800588CrossRefGoogle Scholar
  21. Liang W, Chen J, Liu Y, Chen S (2014). Density-functional-theory calculation analysis of active sites for four-electron reduction of O2 on Fe/N-doped graphene. ACS Catalysis, 4(11): 4170–4177CrossRefGoogle Scholar
  22. Lin T, Tang Y, Wang Y, Bi H, Liu Z, Huang F, Xie X, Jiang M (2013). Scotch-tape-like exfoliation of graphite assisted with elemental sulfur and graphene-sulfur composites for high-performance lithium-sulfur batteries. Energy & Environmental Science, 6(4): 1283–1290CrossRefGoogle Scholar
  23. Liu Q, Zhou Y, Chen S, Wang Z, Hou H, Zhao F (2015). Cellulose-derived nitrogen and phosphorus dual-doped carbon as high performance oxygen reduction catalyst in microbial fuel cell. Journal of Power Sources, 273: 1189–1193CrossRefGoogle Scholar
  24. Liu X, Dai L (2016). Carbon-based metal-free catalysts. Nature Reviews Materials, 1(11): 16064(1–12)CrossRefGoogle Scholar
  25. Liu Y, Liu H, Wang C, Hou S X, Yang N (2013). Sustainable energy recovery in wastewater treatment by microbial fuel cells: Stable power generation with nitrogen-doped graphene cathode. Environmental Science & Technology, 47(23): 13889–13895CrossRefGoogle Scholar
  26. Liu Y, Zhao Y, Li K, Wang Z, Tian P, Liu D, Yang T, Wang J (2018). Activated carbon derived from chitosan as air cathode catalyst for high performance in microbial fuel cells. Journal of Power Sources, 378: 1–9CrossRefGoogle Scholar
  27. Lu X, Zeng Y, Yu M, Zhai T, Liang C, Xie S, Balogun M S, Tong Y (2014). Oxygen-deficient hematite nanorods as high-performance and novel negative electrodes for flexible asymmetric supercapacitors. Advanced materials, 26(19): 3148–3155CrossRefGoogle Scholar
  28. Malard L M, Pimenta M A, Dresselhaus G, Dresselhaus M S (2009). Raman spectroscopy in graphene. Physics Reports, 473(5–6): 51–87CrossRefGoogle Scholar
  29. Nadeem M, Yasin G, Bhatti M H, Mehmood M, Arif M, Dai L (2018). Pt-M bimetallic nanoparticles (M = Ni, Cu, Er) supported on metal organic framework-derived N-doped nanostructured carbon for hydrogen evolution and oxygen evolution reaction. Journal of Power Sources, 402: 34–42CrossRefGoogle Scholar
  30. Niu Y, Huang X, Hu W (2016). Fe3C nanoparticle decorated Fe/N doped graphene for efficient oxygen reduction reaction electrocatalysis. Journal of Power Sources, 332: 305–311CrossRefGoogle Scholar
  31. Oh W D, Lisak G, Webster R D, Liang Y N, Veksha A, Giannis A, Moo G S, Lim J W, Lim T T (2018). Insights into the thermolytic transformation of lignocellulosic biomass waste to redox-active carbocatalyst: Durability of surface active sites. Applied Catalysis B: Environmental, 233: 120–129CrossRefGoogle Scholar
  32. Qu L, Liu Y, Baek J B, Dai L (2010). Nitrogen-doped graphene as efficient metal-free electrocatalyst for oxygen reduction in fuel cells. ACS Nano, 4(3): 1321–1326CrossRefGoogle Scholar
  33. Ren G, Li Y, Guo Z, Xiao G, Zhu Y, Dai L, Jiang L (2015). A bio-inspired Co3O4-polypyrrole-graphene complex as an efficient oxygen reduction catalyst in one-step ball milling. Nano Research, 8(11): 3461–3471CrossRefGoogle Scholar
  34. Santoro C, Arbizzani C, Erable B, Ieropoulos I (2017). Microbial fuel cells: From fundamentals to applications: A review. Journal of Power Sources, 356: 225–244CrossRefGoogle Scholar
  35. Solomon E I, Stahl S S (2018). Introduction: Oxygen reduction and activation in catalysis. Chemical Reviews, 118(5): 2299–2301CrossRefGoogle Scholar
  36. Stacy J, Regmi Y N, Leonard B, Fan M (2017). The recent progress and future of oxygen reduction reaction catalysis: A review. Renewable & Sustainable Energy Reviews, 69: 401–414CrossRefGoogle Scholar
  37. Sun M, Zhai L F, Li W W, Yu H Q (2016). Harvest and utilization of chemical energy in wastes by microbial fuel cells. Chemical Society Reviews, 45(10): 2847–2870CrossRefGoogle Scholar
  38. Tang H, Cai S, Xie S, Wang Z, Tong Y, Pan M, Lu X (2016). Metal-organic-framework-derived dual metal- and nitrogen-doped carbon as efficient and robust oxygen reduction reaction catalysts for microbial fuel cells. Advanced science, 3(2): 1500265CrossRefGoogle Scholar
  39. Tian G, Zhang Q, Zhang B, Jin Y, Huang J, Su D S, Wei F (2014). Toward full exposure of “active sites”: Nanocarbon electrocatalyst with surface enriched nitrogen for superior oxygen reduction and evolution reactivity. Advanced Functional Materials, 24(38): 5956–5961CrossRefGoogle Scholar
  40. Wang Q, Lei Y, Chen Z, Wu N, Wang Y, Wang B, Wang Y (2018). Fe/Fe3C@C nanoparticles encapsulated in N-doped graphene-CNTs framework as an efficient bifunctional oxygen electrocatalyst for robust rechargeable Zn-air batteries. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 6(2): 516–526CrossRefGoogle Scholar
  41. Wang Q, Zhang X, Lv R, Chen X, Xue B, Liang P, Huang X (2016). Binder-free nitrogen-doped graphene catalyst air-cathodes for microbial fuel cells. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 4(32): 12387–12391CrossRefGoogle Scholar
  42. Xia X, Zhang F, Zhang X, Liang P, Huang X, Logan B E (2013). Use of pyrolyzed iron ethylenediaminetetraacetic acid modified activated carbon as air-cathode catalyst in microbial fuel cells. ACS Applied Materials & Interfaces, 5(16): 7862–7866CrossRefGoogle Scholar
  43. Xiao M, Zhu J, Ma L, Jin Z, Ge J, Deng X, Hou Y, He Q, Li J, Jia Q, Mukerjee S, Yang R, Jiang Z, Su D, Liu C, Xing W (2018). Microporous framework induced synthesis of single-atom dispersed Fe-N-C acidic ORR catalyst and its in situ reduced Fe-N4 active site identification revealed by X-ray absorption Spectroscopy. ACS Catalysis, 8(4): 2824–2832CrossRefGoogle Scholar
  44. Yang W, Li J, Ye D, Zhu X, Liao Q (2017). Bamboo charcoal as a cost-effective catalyst for an air-cathode of microbial fuel cells. Electrochimica Acta, 224: 585–592CrossRefGoogle Scholar
  45. Yin H, Zhang C, Liu F, Hou Y (2014). Doped graphene: Hybrid of iron nitride and nitrogen-doped graphene aerogel as synergistic catalyst for oxygen reduction reaction. Advanced Functional Materials, 24(20): 2930–2937CrossRefGoogle Scholar
  46. Yuan H, Hou Y, Aub-Reesh I M A, Chen J, He Z (2016). Oxygen reduction reaction catalysts used in microbial fuel cells for energy-efficient wastewater treatment: A review. Materials Horizons, 3(5): 382–401CrossRefGoogle Scholar
  47. Zhang B, Wen Z, Ci S, Mao S, Chen J, He Z (2014a). Synthesizing nitrogen-doped activated carbon and probing its active sites for oxygen reduction reaction in microbial fuel cells. ACS Applied Materials & Interfaces, 6(10): 7464–7470CrossRefGoogle Scholar
  48. Zhang L, Ni Y, Wang X, Zhao G (2010). Direct electrocatalytic oxidation of nitric oxide and reduction of hydrogen peroxide based on-Fe2O3 nanoparticles-chitosan composite. Talanta, 82(1): 196–201CrossRefGoogle Scholar
  49. Zhang X, Pant D, Zhang F, Liu J, He W, Logan B E (2014b). Long-term performance of chemically and physically modified activated carbons in air cathodes of microbial fuel cells. ChemElectroChem, 1(11): 1859–1866CrossRefGoogle Scholar
  50. Zhang X, Xia X, Ivanov I, Huang X, Logan B E (2014c). Enhanced activated carbon cathode performance for microbial fuel cell by blending carbon black. Environmental Science & Technology, 48(3): 2075–2081CrossRefGoogle Scholar
  51. Zhao Q, Yu H, Zhang W, Kabutey F T, Jiang J, Zhang Y, Wang K, Ding J (2017). Microbial fuel cell with high content solid wastes as substrates: A review. Frontiers of Environmental Science & Engineering, 11(2): 25–41CrossRefGoogle Scholar
  52. Wu Z Y, Xu X X, Hu B C, Liang H W, Lin Y, Chen L F, Yu S H (2015). Iron carbide nanoparticles encapsulated in mesoporous Fe-N-doped carbon nanofibers for efficient electrocatalysis. Angewandte Chemie (International ed. in English), 54(28): 8179–8183CrossRefGoogle Scholar
  53. Zhuang S, Lee E S, Lei L, Nunna B B, Kuang L, Zhang W (2016). Synthesis of nitrogen-doped graphene catalyst by high-energy wet ball milling for electrochemical systems. International Journal of Energy Research, 40(15): 2136–2149CrossRefGoogle Scholar
  54. Zhuang S, Nunna B B, Lee E S (2018). Metal organic framework-modified nitrogen-doped graphene oxygen reduction reaction catalyst synthesized by nanoscale high-energy wet ball-milling structural and electrochemical characterization. MRS Communications, 8(01): 40–48CrossRefGoogle Scholar
  55. Zitolo A, Goellner V, Armel V, Sougrati M T, Mineva T, Stievano L, Fonda E, Jaouen F (2015). Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials. Nature Materials, 14(9): 937–942CrossRefGoogle Scholar

Copyright information

© Higher Education Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020

Authors and Affiliations

  • Xingguo Guo
    • 1
  • Qiuying Wang
    • 1
  • Ting Xu
    • 1
  • Kajia Wei
    • 1
  • Mengxi Yin
    • 1
  • Peng Liang
    • 1
  • Xia Huang
    • 1
  • Xiaoyuan Zhang
    • 1
    Email author
  1. 1.State Key Joint Laboratory of Environment Simulation and Pollution Control, School of EnvironmentTsinghua UniversityBeijingChina

Personalised recommendations